Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing...Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou,China in 2022.Generally,the particle counts of OOM particles and the mass concentration of secondary organic carbon(SOC)exhibited similar temporal trends throughout the entire year.The OOM particles were consistently enriched in secondary ions,including ^(16)O^(−),^(26)CN^(−),^(46)NO_(2)^(−),^(62)NO_(3)^(−),and ^(97)HSO_(4)^(−).In contrast,the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October;however,the SOC ratios in fine particulate matter were quite different,suggesting that there were different mixing states of single-particle oxygenated organics.In addition,further classification results indicated that the OOM particles were more aged in October than August,even though the SOC ratios were higher in August.Furthermore,the distribution of hydrocarbon fragments exhibited a notable decrease from January to October,emphasizing the more aged state of the organics in October.In addition,the sharp increase in elemental carbon(EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics.Overall,in contrast to the bulk analysis of SOC mass concentration,the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.展开更多
A new andrographolide metabolite 1 was isolated from human urine samples after oral administration. The structure was determined to be 3-carbonylandrographolide-19-O-β-D-glu- curonide on the basis of chemical evidenc...A new andrographolide metabolite 1 was isolated from human urine samples after oral administration. The structure was determined to be 3-carbonylandrographolide-19-O-β-D-glu- curonide on the basis of chemical evidences and spectral analysis, especially by 2D-NMR techni- ques.展开更多
Oxygenated volatile organic compounds（OVOCs） emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs（TOVOCs...Oxygenated volatile organic compounds（OVOCs） emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs（TOVOCs） from orange wastes reached 1714 mg/dry kg（330 mg/wet kg）. Ethanol, methanol, ethyl acetate, methyl acetate, 2-butanone and acetaldehyde were the most abundant OVOC species with shares of 26.9%, 24.8%, 20.3%, 13.9%, 2.8%and 2.5%, respectively, in the TOVOCs released. The emission fluxes of the above top five OVOCs were quite trivial in the beginning but increased sharply to form one ＂peak emission window＂ with maximums at days 1-8 until leveling off after 10 days. This type of ＂peak emission window＂ was synchronized with the CO2 fluxes and incubation temperature of the orange wastes, indicating that released OVOCs were mainly derived from secondary metabolites of orange substrates through biotic processes rather than abiotic processes or primary volatilization of the inherent pool in oranges. Acetaldehyde instead had emission fluxes decreasing sharply from its initial maximum to nearly zero in about four days,suggesting that it was inherent rather than secondarily formed. For TOVOCs or all OVOC species except 2-butanone and acetone, over 80% of their emissions occurred during the first week, implying that organic wastes might give off a considerable amount of OVOCs during the early disposal period under aerobic conditions.展开更多
Aerosol-bound organic radicals,including environmentally persistent free radicals(EPFRs),are key components that affect climate,air quality,and human health.While putative structures have been proposed,the molecular c...Aerosol-bound organic radicals,including environmentally persistent free radicals(EPFRs),are key components that affect climate,air quality,and human health.While putative structures have been proposed,the molecular characteristics of EPFRs remain unknown.Here,we report a surrogate method to characterize EPFRs in real ambient samples using mass spectrometry.The method identifies chemically relevant oxygenated polycyclic aromatic hydrocarbons(OxPAH)that interconvert with oxygen-centered EPFR(OC-EPFR).We found OxPAH compounds most relevant to OC-EPFRs are structurally rich and diverse quinones,whose diversity is strongly associated with OC-EPFR levels.Both atmospheric oxidation and combustion contributed to OC-EPFR formation.Redundancy analysis and photochemical aging model show pyrolytic sources generated more oxidized OC-EPFRs than photolytic sources.Our study reveals the detailed molecular characteristics of OC-EPFRs and shows that oxidation states can be used to identify the origins of OC-EPFRs,offering a way to track the development and evolution of aerosol particles in the environment.展开更多
For a climate-neutral future mobility,the socalled e-fuels can play an essential part.Especially,oxygenated e-fuels containing oxygen in their chemical formula have the additional potential to burn with significantly ...For a climate-neutral future mobility,the socalled e-fuels can play an essential part.Especially,oxygenated e-fuels containing oxygen in their chemical formula have the additional potential to burn with significantly lower soot levels.In particular,polyoxymethylene dimethyl ethers or oxymethylene ethers(PODEs or OMEs)do not contain carbon-carbon bonds,prohibiting the production of soot precursors like acetylene(C2H2).These properties make OMEs a highly interesting candidate for future climate-neutral compression-ignition engines.However,to fully leverage their potential,the auto-ignition process,flame propagation,and mixing regimes of the combustion need to be understood.To achieve this,efficient oxidation mechanisms suitable for computational fluid dynamics(CFD)calculations must be developed and validated.The present work aims to highlight the improvements made by developing an adapted oxidation mechanism for OME1-6 and introducing it into a validated spray combustion CFD model for OMEs.The simulations were conducted for single-and multi-injection patterns,changing ambient temperatures,and oxygen contents.The results were validated against high-pressure and high-temperature constantpressure chamber experiments.OH*-chemiluminescence measurements accomplished the characterization of the auto-ignition process.Both experiments and simulations were conducted for two different injectors.Significant improvements concerning the prediction of the ignition delay time were accomplished while also retaining an excellent agreement for the flame lift-off length.The spatial zones of high-temperature reaction activity were also affected by the adaption of the reaction kinetics.They showed a greater tendency to form OH*radicals within the center of the spray in accordance with the experiments.展开更多
The widespread uptake of different machine perfusion(MP)strategies for liver transplant has been driven by an effort to minimize graft injury.Damage to the cholangiocytes during the liver donation,preservation,or earl...The widespread uptake of different machine perfusion(MP)strategies for liver transplant has been driven by an effort to minimize graft injury.Damage to the cholangiocytes during the liver donation,preservation,or early posttransplant period may result in stricturing of the biliary tree and inadequate biliary drainage.This problem continues to trouble clinicians,and may have catastrophic consequences for the graft and patient.Ischemic injury,as a result of compromised hepatic artery flow,is a well-known cause of biliary strictures,sepsis,and graft failure.However,very similar lesions can appear with a patent hepatic artery and these are known as ischemic type biliary lesions(ITBL)that are attributed to microcirculatory dysfunction rather than main hepatic arterial compromise.Both the warm and cold ischemic period duration appear to influence the onset of ITBL.All of the commonly used MP techniques deliver oxygen to the graft cells,and therefore may minimize the cholangiocyte injury and subsequently reduce the incidence of ITBL.As clinical experience and published evidence grows for these modalities,the impact they have on ITBL rates is important to consider.In this review,the evidence for the three commonly used MP strategies(abdominal normothermic regional perfusion[A-NRP],hypothermic oxygenated perfusion[HOPE],and normothermic machine perfusion[NMP])for ITBL prevention has been critically reviewed.Inconsistencies with ITBL definitions used in trials,coupled with variations in techniques of MP,make interpretation challenging.Overall,the evidence suggests that both HOPE and A-NRP prevent ITBL in donated after circulatory death grafts compared to cold storage.The evidence for ITBL prevention in donor after brain death grafts with any MP technique is weak.展开更多
The last decade has been notable for increasing high-quality research and dramatic improvement in outcomes with dynamic liver preservation.Robust evidence from numerous randomized controlled trials has been pooled by ...The last decade has been notable for increasing high-quality research and dramatic improvement in outcomes with dynamic liver preservation.Robust evidence from numerous randomized controlled trials has been pooled by meta-analyses,providing the highest available evidence on the protective effect of machine perfusion(MP)over static cold storage in liver transplantation(LT).Based on a protective effect with less complications and improved graft survival,the field has seen a paradigm shift in organ preservation.This editorial focuses on the role of MP in LT and how it could become the new“gold standard”.Strong collaborative efforts are needed to explore its effects on long-term outcomes.展开更多
The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hy...The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hydrogenation deoxygenation,solvent extraction,and extraction distillation,adsorption deoxygenation technology has the advantages of low cost,mild operating conditions,easy removal and recovery,and mini-mal impact on oil quality.Therefore,adsorption deoxygenation technology has devel-oped rapidly in various removal processes and has become a research hotspot in the cur-rent Fischer Tropsch oil deoxygenation.Adsorbents are the core of adsorption deoxygen-ation technology.Therefore,this article briefly introduces the adsorption mechanism and summarizes the research progress of adsorbents widely used in recent years,such as silica gel,alumina,molecular sieves,and metal organic frameworks,in adsorbing oxygen-containing compounds in Fischer Tropsch synthetic oils.And provide reference sugges-tions for further adsorption and deoxygenation directions in the future.展开更多
Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of ac...Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of acrolein,as the main by-product of this epoxidation process,is very important to achieve the high yield of PO.In this study,we perform the spin-polarized density functional theory(DFT)calculations to investigate the reaction pathway from propylene to acrolein over two representative Au surfaces,that is,Au(111)and Au(100),which incorporates propylene adsorption,methyl hydrogen activation and acrolein formation.The results show that the oxygenated species(mainly O^(*),OH^(*)and OOH^(*))are able to stabilize the adsorption of propylene to decrease the energy barrier for its activation.It is demonstrated that the OOH^(*)on Au(111)surface emerges as the most easily formed oxygenated species via the H-assisted O_(2) dissociation,which is also the most active for the cleavage of methyl CAH bond in propylene.Furthermore,three pathways of acrolein formation activated by O^(*)/OH^(*)/OOH^(*)are analyzed,in which O^(*)is found as the key species to form acrolein.Finally,Bader charge analysis was conducted to explore the reasons behind the promotion effect of the oxygenated species.The insights reported here could be valuable in the design and optimization of gold catalysts for the direct epoxidation of propylene.展开更多
Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and u...Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.展开更多
Liver transplantation(LT),an ultimate and vital method for treating end-stage liver disease,is often accompanied by ischemiareperfusion injury(IRI)resulting from warm or cold ischemia of the donor liver.Organ protecti...Liver transplantation(LT),an ultimate and vital method for treating end-stage liver disease,is often accompanied by ischemiareperfusion injury(IRI)resulting from warm or cold ischemia of the donor liver.Organ protection techniques are used to improve the quality of liver grafts(from retrieval to implantation).Reactive oxygen species(ROS)cause oxidative stress,which is considered a crucial factor in IRI after LT.Nano antioxidants capable of scavenging ROS alleviate IRI in multiple types of organs and tissues.In this study,we synthesized ceria nanoparticles(NPs)with antioxidant properties using a pyrolysis method and covered them with phospholipid-polyethylene glycol to improve their biocompatibility in vivo.We investigated the potential organprotective effect of ceria NPs and the underlying mechanisms.Ceria NPs promoted liver function recovery after LT by attenuating IRI in liver grafts in vivo.The protective effect of ceria NPs on liver grafts was investigated by applying hypothermic oxygenated machine perfusion ex vivo.Ceria NPs attenuated hypoxia reoxygenation-or H_(2)O_(2)-induced hepatocyte injury by enhancing mitochondrial activity and ROS scavenging in vitro.These effects may be associated with the activation of the nuclear factor erythroid-derived 2-related factor 2(Nrf2)/Kelch-like ECH-associated protein 1(Keap1)/heme oxygenase 1(HO-1)signaling pathway.In conclusion,ceria NPs may serve as a promising antioxidant agent for the treatment of hepatic IRI after LT.展开更多
Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozz...Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.展开更多
There is a theory that the unavoidable graft damage caused by ischemia-reperfusion injury(IRI)during liver transplantation(LT)can lead to severe IRI-related inflammation and trigger an early activation of the innate i...There is a theory that the unavoidable graft damage caused by ischemia-reperfusion injury(IRI)during liver transplantation(LT)can lead to severe IRI-related inflammation and trigger an early activation of the innate immune response mediated by T-cells,which potentially worsening the acute cellular rejection(ACR)cascade.As a result,machine perfusion(MP)has been placed great expectations for the potential to diminish post-LT ACR and other related immune responses by alleviating IRI through removing harmful substances and restoring cellular metabolism homeostasis(1,2).However,there has been much debate about MP’s benefits on ACR as relative data is limited.展开更多
The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) durin...The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) during germination by giving pre-sowing soaking treatment for 6 hours using petriplate method. Both the treatments enhanced the germination process. GA treatment was useful to increase shoot length, mobilization efficiency, emergence index, speed of germination and co-efficient of germination while oxygenated peptone showed an upper hand in root length, shoot/root ratio, biomass and vigour index. GA led to comparatively more synthesis of nucleic acids while oxygenated peptone showed more increase in total carbohydrates and soluble protein content. However, the activity of enzymes like amylase, catalase and protease showed upper hand with oxygenated peptone as compared to GA. In fact GA is costlier and can not be used in organic farming as it enters metabolic pathways of plant and alters them. Hence the use of oxygenated peptone is recommended being less expensive and usable under organic farming condition as it does not enter the plant metabolic pathways and yet brings about significant positive effect.展开更多
Biogenic volatile organic compounds(BVOCs)are widely involved in a variety of atmospheric chemical processes due to their high reactivity and species diversity.To date,however,research on BVOCs in agroecosystems,parti...Biogenic volatile organic compounds(BVOCs)are widely involved in a variety of atmospheric chemical processes due to their high reactivity and species diversity.To date,however,research on BVOCs in agroecosystems,particularly fruit trees,remains scarce despite their large cultivation area and economic interest.BVOC emissions from different organs(leaf or fruit)of apple and peach trees were investigated throughout the stages of fruit development(FS,fruit swelling;FC,fruit coloration;FM,fruit maturity;and FP,fruit postharvest)using a proton-transfer-reaction mass spectrometer.Results indicated that methanol was the most abundant compound emitted by the leaf(apple tree leaf 492.5±47.9 ng/(g·hr),peach tree leaf 938.8±154.5 ng/(g·hr)),followed by acetic acid and green leaf volatiles.Beside the above three compounds,acetaldehyde had an important contribution to the emissions from the fruit.Overall,the total BVOCs(sum of eight compounds studied in this paper)emitted by both leaf and fruit gradually decreased along the fruit development,although the effect was significant only for the leaf.The leaf(2020.8±258.8 ng/(g·hr))was a stronger BVOC emitter than the fruit(146.0±45.7 ng/(g·hr))(P=0.006),and there were no significant differences in total BVOC emission rates between apple and peach trees.These findings contribute to our understanding on BVOC emissions from different plant organs and provide important insights into the variation of BVOC emissions across different fruit developmental stages.展开更多
Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,ca...Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,carbon neutral,greenhouse gases reduction,waste utilization,energy and economic security,and fuel pluralism.Based on the understanding of molecular structure effects of biofuels on soot formation and particles morphology,the effects of alcohols,ethers,esters and biodiesel on spray and combustion process in constant volume bomb in recent years are retrospectively analyzed in this paper.For the mixture,macromolecular ester fuels and polyoxymethylene dimethyl ether(PODE)are conducive to the improvement of liquid spray,while biodiesel,small molecules,dimethyl ether(DME)and alcohols are reversed.Alcohols are advantageous to the extension of mixing time and the increasing of vapor-phase mixture.Through the influence integrated assessment,alcohols show the best performance on the spray,atomization and combustion,while biodiesels show the worst.But in terms of combustion,PODE is the best choice without considering spray and atomization.For binary alternative-diesel fuel blends,methanol or butanol is the best additive based on synthetically considerations on spray,atomization and combustion.To meet the requirements of the fuel application of diesel engine,ternary fuel or even quaternary fuel have been proposed and explored.This review can help to form a systematic understanding on fuel recombining and obtain the guide of clean and efficient fuel formulation for diesel engine.展开更多
The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered ...The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered by the lack of efficient low-cost electrocatalysts. In the current study,oxygenated boron-doped carbon(O-BC) materials were realized via a green synthetic strategy involving polymer dehalogenation and employed as electrode materials for the electrochemical synthesis of H_(2)O_(2)via a 2 e-oxygen reduction.The catalytic activity of the O-BC materials was optimized through systematic variation of the boron source(H_(2)BO_(2))dosage and annealing temperature. Electrochemical measurements revealed that the optimal sample(O-BC-2-650)exhibited a selectivity of 98% for the 2 e-oxygen reduction to H2 O_(2)and an average H_(2)O_(2)production rate of412.8 mmol g_(cat)^(-1) h^(-1)in an H-type alkaline electrolyzer. Density functional theory simulations indicated that the functionalization of active B sites with one oxygen atom provides the lowest Gibbs free energy change(ΔG) of 0.03 e V for the hydrogenation of*O_(2), while functionalization with zero or two O atoms results in much larger ΔG values(0.08 and 0.10 e V,respectively). Thus, this work details a new type of green, lowcost, and metal-free electrocatalyst for H_(2)O_(2)production.展开更多
In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for ...In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.展开更多
<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were...<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were: pure gasoline (type A), common gasoline (type C), gasoline type A + 15% (v/v) oxygenated additives (ethanol, ethyl octanoate, ethyl oleate). The experiments were performed using engine Branco 4-stroke and 2-cylinder, electric dynamometer, exhaust system, control unit composed of Multi-K unit, variable selector and load cell, stroboscope tachometer, fuel supply system and stopwatch. The rotation was conserved at 4400 rpm and wheel power varied from 3 kW to 12 kW, with intervals of 3 kW to obtain hourly consumption curves and brake specific fuel consumption. Even esters and ethanol having lower heat of combustion, hourly consumption was similar to pure gasoline (type A). In relation to the brake specific fuel consumption, increasing the wheel power had a better conversion of the mass of fuel burned into energy. Thus, this study showed that the mixture of gasoline and esters (ethyl octanoate and ethyl oleate) presented good efficiency in terms of consumption. This research contributes to the needs and to the current studi</span><span style="font-family:Verdana;">es in which industries started to add renewable products to petroleum-</span><span style="font-family:Verdana;">derived fuels;in order to obtain more sustainable fuels at lower costs.</span>展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.41827804 and 41805093)the Natural Science Foundation of Guangdong Province(China)(No.2021A1515011206)+1 种基金the State Key Laboratory of Marine Resource Utilization in the South China Sea,Hainan University(China)(No.MRUKF2023009)the State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,CAS(No.SKLLQG2218).
文摘Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou,China in 2022.Generally,the particle counts of OOM particles and the mass concentration of secondary organic carbon(SOC)exhibited similar temporal trends throughout the entire year.The OOM particles were consistently enriched in secondary ions,including ^(16)O^(−),^(26)CN^(−),^(46)NO_(2)^(−),^(62)NO_(3)^(−),and ^(97)HSO_(4)^(−).In contrast,the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October;however,the SOC ratios in fine particulate matter were quite different,suggesting that there were different mixing states of single-particle oxygenated organics.In addition,further classification results indicated that the OOM particles were more aged in October than August,even though the SOC ratios were higher in August.Furthermore,the distribution of hydrocarbon fragments exhibited a notable decrease from January to October,emphasizing the more aged state of the organics in October.In addition,the sharp increase in elemental carbon(EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics.Overall,in contrast to the bulk analysis of SOC mass concentration,the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.
文摘A new andrographolide metabolite 1 was isolated from human urine samples after oral administration. The structure was determined to be 3-carbonylandrographolide-19-O-β-D-glu- curonide on the basis of chemical evidences and spectral analysis, especially by 2D-NMR techni- ques.
基金supported by the Ministry of Science and Technology of China (No. 2012IM030700)the National Natural Science Foundation of China (Nos. 41025012, U0833003, 41273095 and 41103067)
文摘Oxygenated volatile organic compounds（OVOCs） emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs（TOVOCs） from orange wastes reached 1714 mg/dry kg（330 mg/wet kg）. Ethanol, methanol, ethyl acetate, methyl acetate, 2-butanone and acetaldehyde were the most abundant OVOC species with shares of 26.9%, 24.8%, 20.3%, 13.9%, 2.8%and 2.5%, respectively, in the TOVOCs released. The emission fluxes of the above top five OVOCs were quite trivial in the beginning but increased sharply to form one ＂peak emission window＂ with maximums at days 1-8 until leveling off after 10 days. This type of ＂peak emission window＂ was synchronized with the CO2 fluxes and incubation temperature of the orange wastes, indicating that released OVOCs were mainly derived from secondary metabolites of orange substrates through biotic processes rather than abiotic processes or primary volatilization of the inherent pool in oranges. Acetaldehyde instead had emission fluxes decreasing sharply from its initial maximum to nearly zero in about four days,suggesting that it was inherent rather than secondarily formed. For TOVOCs or all OVOC species except 2-butanone and acetone, over 80% of their emissions occurred during the first week, implying that organic wastes might give off a considerable amount of OVOCs during the early disposal period under aerobic conditions.
基金supported by the National Natural Science Foundation of China(92143301 and 91843301)the National Key Research and Development Program of China(2020YFF01014504)the Chinese Academy Sciences Youth Innovation Promotion Association projects。
文摘Aerosol-bound organic radicals,including environmentally persistent free radicals(EPFRs),are key components that affect climate,air quality,and human health.While putative structures have been proposed,the molecular characteristics of EPFRs remain unknown.Here,we report a surrogate method to characterize EPFRs in real ambient samples using mass spectrometry.The method identifies chemically relevant oxygenated polycyclic aromatic hydrocarbons(OxPAH)that interconvert with oxygen-centered EPFR(OC-EPFR).We found OxPAH compounds most relevant to OC-EPFRs are structurally rich and diverse quinones,whose diversity is strongly associated with OC-EPFR levels.Both atmospheric oxidation and combustion contributed to OC-EPFR formation.Redundancy analysis and photochemical aging model show pyrolytic sources generated more oxidized OC-EPFRs than photolytic sources.Our study reveals the detailed molecular characteristics of OC-EPFRs and shows that oxidation states can be used to identify the origins of OC-EPFRs,offering a way to track the development and evolution of aerosol particles in the environment.
文摘For a climate-neutral future mobility,the socalled e-fuels can play an essential part.Especially,oxygenated e-fuels containing oxygen in their chemical formula have the additional potential to burn with significantly lower soot levels.In particular,polyoxymethylene dimethyl ethers or oxymethylene ethers(PODEs or OMEs)do not contain carbon-carbon bonds,prohibiting the production of soot precursors like acetylene(C2H2).These properties make OMEs a highly interesting candidate for future climate-neutral compression-ignition engines.However,to fully leverage their potential,the auto-ignition process,flame propagation,and mixing regimes of the combustion need to be understood.To achieve this,efficient oxidation mechanisms suitable for computational fluid dynamics(CFD)calculations must be developed and validated.The present work aims to highlight the improvements made by developing an adapted oxidation mechanism for OME1-6 and introducing it into a validated spray combustion CFD model for OMEs.The simulations were conducted for single-and multi-injection patterns,changing ambient temperatures,and oxygen contents.The results were validated against high-pressure and high-temperature constantpressure chamber experiments.OH*-chemiluminescence measurements accomplished the characterization of the auto-ignition process.Both experiments and simulations were conducted for two different injectors.Significant improvements concerning the prediction of the ignition delay time were accomplished while also retaining an excellent agreement for the flame lift-off length.The spatial zones of high-temperature reaction activity were also affected by the adaption of the reaction kinetics.They showed a greater tendency to form OH*radicals within the center of the spray in accordance with the experiments.
基金funding received in the form of the Catherine Marie Enright research scholarship from the Royal Australasian College of Surgeons to support his program of research
文摘The widespread uptake of different machine perfusion(MP)strategies for liver transplant has been driven by an effort to minimize graft injury.Damage to the cholangiocytes during the liver donation,preservation,or early posttransplant period may result in stricturing of the biliary tree and inadequate biliary drainage.This problem continues to trouble clinicians,and may have catastrophic consequences for the graft and patient.Ischemic injury,as a result of compromised hepatic artery flow,is a well-known cause of biliary strictures,sepsis,and graft failure.However,very similar lesions can appear with a patent hepatic artery and these are known as ischemic type biliary lesions(ITBL)that are attributed to microcirculatory dysfunction rather than main hepatic arterial compromise.Both the warm and cold ischemic period duration appear to influence the onset of ITBL.All of the commonly used MP techniques deliver oxygen to the graft cells,and therefore may minimize the cholangiocyte injury and subsequently reduce the incidence of ITBL.As clinical experience and published evidence grows for these modalities,the impact they have on ITBL rates is important to consider.In this review,the evidence for the three commonly used MP strategies(abdominal normothermic regional perfusion[A-NRP],hypothermic oxygenated perfusion[HOPE],and normothermic machine perfusion[NMP])for ITBL prevention has been critically reviewed.Inconsistencies with ITBL definitions used in trials,coupled with variations in techniques of MP,make interpretation challenging.Overall,the evidence suggests that both HOPE and A-NRP prevent ITBL in donated after circulatory death grafts compared to cold storage.The evidence for ITBL prevention in donor after brain death grafts with any MP technique is weak.
文摘The last decade has been notable for increasing high-quality research and dramatic improvement in outcomes with dynamic liver preservation.Robust evidence from numerous randomized controlled trials has been pooled by meta-analyses,providing the highest available evidence on the protective effect of machine perfusion(MP)over static cold storage in liver transplantation(LT).Based on a protective effect with less complications and improved graft survival,the field has seen a paradigm shift in organ preservation.This editorial focuses on the role of MP in LT and how it could become the new“gold standard”.Strong collaborative efforts are needed to explore its effects on long-term outcomes.
文摘The oxygen-containing compounds in Fischer Tropsch synthetic oil greatly affect the downstream deep processing of hydrocarbons,and effective removal is required.Com-pared to traditional removal technologies such as hydrogenation deoxygenation,solvent extraction,and extraction distillation,adsorption deoxygenation technology has the advantages of low cost,mild operating conditions,easy removal and recovery,and mini-mal impact on oil quality.Therefore,adsorption deoxygenation technology has devel-oped rapidly in various removal processes and has become a research hotspot in the cur-rent Fischer Tropsch oil deoxygenation.Adsorbents are the core of adsorption deoxygen-ation technology.Therefore,this article briefly introduces the adsorption mechanism and summarizes the research progress of adsorbents widely used in recent years,such as silica gel,alumina,molecular sieves,and metal organic frameworks,in adsorbing oxygen-containing compounds in Fischer Tropsch synthetic oils.And provide reference sugges-tions for further adsorption and deoxygenation directions in the future.
基金financially supported by the Research Fund for National Key Research and Development Program of China (2021YFA1501403)the National Natural Science Foundation of China (22208094,22038003,21922803,22178100)+1 种基金the Innovation Program of Shanghai Municipal Education Commission,the Program of Shanghai Academic/Technology Research Leader (21XD1421000)the Shanghai Science and Technology Innovation Action Plan (22JC1403800)。
文摘Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial interests.Fundamentally understanding the formation mechanism of acrolein,as the main by-product of this epoxidation process,is very important to achieve the high yield of PO.In this study,we perform the spin-polarized density functional theory(DFT)calculations to investigate the reaction pathway from propylene to acrolein over two representative Au surfaces,that is,Au(111)and Au(100),which incorporates propylene adsorption,methyl hydrogen activation and acrolein formation.The results show that the oxygenated species(mainly O^(*),OH^(*)and OOH^(*))are able to stabilize the adsorption of propylene to decrease the energy barrier for its activation.It is demonstrated that the OOH^(*)on Au(111)surface emerges as the most easily formed oxygenated species via the H-assisted O_(2) dissociation,which is also the most active for the cleavage of methyl CAH bond in propylene.Furthermore,three pathways of acrolein formation activated by O^(*)/OH^(*)/OOH^(*)are analyzed,in which O^(*)is found as the key species to form acrolein.Finally,Bader charge analysis was conducted to explore the reasons behind the promotion effect of the oxygenated species.The insights reported here could be valuable in the design and optimization of gold catalysts for the direct epoxidation of propylene.
基金supported by the National Natural Science Foundation of China(No.52171022,No.22105214)Zhejiang Provincial Natural Science Foundation of China(Grant No.LXR22B030001)+3 种基金Fujian Institute of Innovation and Chinese Academy of Sciences.K.C.Wong Education Foundation(GJTD-2019-13)the National Key Research and Development Program of China(2019YFB2203400)Ningbo Yongjiang Talent Introduction Programme(2021A-036-B)NingBo S&T Innovation 2025 Major Special Programme(No:2020z059)and the“111 Project”(B20030).
文摘Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.
基金supported by Public Projects of Zhejiang Province(No.LGF21H030006)Major Science and Technology Projects of Hainan Province(No.ZDKJ2019009)+2 种基金the Zhejiang Provincial Natural Science Foundation of China(No.LZ21H180001)a Research Project of Jinan Microecological Biomedicine Shandong Laboratory(Nos.JNL-2022002A,JNL-2022007B,and JNL-2022023C)the National Natural Science Foundation of China(No.82000618).
文摘Liver transplantation(LT),an ultimate and vital method for treating end-stage liver disease,is often accompanied by ischemiareperfusion injury(IRI)resulting from warm or cold ischemia of the donor liver.Organ protection techniques are used to improve the quality of liver grafts(from retrieval to implantation).Reactive oxygen species(ROS)cause oxidative stress,which is considered a crucial factor in IRI after LT.Nano antioxidants capable of scavenging ROS alleviate IRI in multiple types of organs and tissues.In this study,we synthesized ceria nanoparticles(NPs)with antioxidant properties using a pyrolysis method and covered them with phospholipid-polyethylene glycol to improve their biocompatibility in vivo.We investigated the potential organprotective effect of ceria NPs and the underlying mechanisms.Ceria NPs promoted liver function recovery after LT by attenuating IRI in liver grafts in vivo.The protective effect of ceria NPs on liver grafts was investigated by applying hypothermic oxygenated machine perfusion ex vivo.Ceria NPs attenuated hypoxia reoxygenation-or H_(2)O_(2)-induced hepatocyte injury by enhancing mitochondrial activity and ROS scavenging in vitro.These effects may be associated with the activation of the nuclear factor erythroid-derived 2-related factor 2(Nrf2)/Kelch-like ECH-associated protein 1(Keap1)/heme oxygenase 1(HO-1)signaling pathway.In conclusion,ceria NPs may serve as a promising antioxidant agent for the treatment of hepatic IRI after LT.
基金financial funding from the Egyptian governmentthe financial funding from the NSERC Discovery grant。
文摘Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.
文摘There is a theory that the unavoidable graft damage caused by ischemia-reperfusion injury(IRI)during liver transplantation(LT)can lead to severe IRI-related inflammation and trigger an early activation of the innate immune response mediated by T-cells,which potentially worsening the acute cellular rejection(ACR)cascade.As a result,machine perfusion(MP)has been placed great expectations for the potential to diminish post-LT ACR and other related immune responses by alleviating IRI through removing harmful substances and restoring cellular metabolism homeostasis(1,2).However,there has been much debate about MP’s benefits on ACR as relative data is limited.
文摘The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) during germination by giving pre-sowing soaking treatment for 6 hours using petriplate method. Both the treatments enhanced the germination process. GA treatment was useful to increase shoot length, mobilization efficiency, emergence index, speed of germination and co-efficient of germination while oxygenated peptone showed an upper hand in root length, shoot/root ratio, biomass and vigour index. GA led to comparatively more synthesis of nucleic acids while oxygenated peptone showed more increase in total carbohydrates and soluble protein content. However, the activity of enzymes like amylase, catalase and protease showed upper hand with oxygenated peptone as compared to GA. In fact GA is costlier and can not be used in organic farming as it enters metabolic pathways of plant and alters them. Hence the use of oxygenated peptone is recommended being less expensive and usable under organic farming condition as it does not enter the plant metabolic pathways and yet brings about significant positive effect.
基金supported by the Open Fund by Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control(No.KHK1801)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)+1 种基金CAS President’s International Fellowship Initiative(No.PIFI-2016VBA057)the National Natural Science Foundation of China(No.41907383)。
文摘Biogenic volatile organic compounds(BVOCs)are widely involved in a variety of atmospheric chemical processes due to their high reactivity and species diversity.To date,however,research on BVOCs in agroecosystems,particularly fruit trees,remains scarce despite their large cultivation area and economic interest.BVOC emissions from different organs(leaf or fruit)of apple and peach trees were investigated throughout the stages of fruit development(FS,fruit swelling;FC,fruit coloration;FM,fruit maturity;and FP,fruit postharvest)using a proton-transfer-reaction mass spectrometer.Results indicated that methanol was the most abundant compound emitted by the leaf(apple tree leaf 492.5±47.9 ng/(g·hr),peach tree leaf 938.8±154.5 ng/(g·hr)),followed by acetic acid and green leaf volatiles.Beside the above three compounds,acetaldehyde had an important contribution to the emissions from the fruit.Overall,the total BVOCs(sum of eight compounds studied in this paper)emitted by both leaf and fruit gradually decreased along the fruit development,although the effect was significant only for the leaf.The leaf(2020.8±258.8 ng/(g·hr))was a stronger BVOC emitter than the fruit(146.0±45.7 ng/(g·hr))(P=0.006),and there were no significant differences in total BVOC emission rates between apple and peach trees.These findings contribute to our understanding on BVOC emissions from different plant organs and provide important insights into the variation of BVOC emissions across different fruit developmental stages.
基金supported by the Key Research and Development Program of Shaanxi Province(2019ZDLGY15-07)the National Natural Science Foundation of China(51806020)+1 种基金the Youth Innovation Team of Shaanxi Universities(Energy Saving and New Energy Vehicles)the Special Fund for Basic Scientific Research of Central Colleges,Chang’an University(300102229104)。
文摘Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,carbon neutral,greenhouse gases reduction,waste utilization,energy and economic security,and fuel pluralism.Based on the understanding of molecular structure effects of biofuels on soot formation and particles morphology,the effects of alcohols,ethers,esters and biodiesel on spray and combustion process in constant volume bomb in recent years are retrospectively analyzed in this paper.For the mixture,macromolecular ester fuels and polyoxymethylene dimethyl ether(PODE)are conducive to the improvement of liquid spray,while biodiesel,small molecules,dimethyl ether(DME)and alcohols are reversed.Alcohols are advantageous to the extension of mixing time and the increasing of vapor-phase mixture.Through the influence integrated assessment,alcohols show the best performance on the spray,atomization and combustion,while biodiesels show the worst.But in terms of combustion,PODE is the best choice without considering spray and atomization.For binary alternative-diesel fuel blends,methanol or butanol is the best additive based on synthetically considerations on spray,atomization and combustion.To meet the requirements of the fuel application of diesel engine,ternary fuel or even quaternary fuel have been proposed and explored.This review can help to form a systematic understanding on fuel recombining and obtain the guide of clean and efficient fuel formulation for diesel engine.
基金financially supported by the National Natural Science Foundation of China (22071137)the Program for Tsingtao Al-ion Power and Energy-storage Battery Research Team in the University (17-2-1-1-zhc)。
文摘The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered by the lack of efficient low-cost electrocatalysts. In the current study,oxygenated boron-doped carbon(O-BC) materials were realized via a green synthetic strategy involving polymer dehalogenation and employed as electrode materials for the electrochemical synthesis of H_(2)O_(2)via a 2 e-oxygen reduction.The catalytic activity of the O-BC materials was optimized through systematic variation of the boron source(H_(2)BO_(2))dosage and annealing temperature. Electrochemical measurements revealed that the optimal sample(O-BC-2-650)exhibited a selectivity of 98% for the 2 e-oxygen reduction to H2 O_(2)and an average H_(2)O_(2)production rate of412.8 mmol g_(cat)^(-1) h^(-1)in an H-type alkaline electrolyzer. Density functional theory simulations indicated that the functionalization of active B sites with one oxygen atom provides the lowest Gibbs free energy change(ΔG) of 0.03 e V for the hydrogenation of*O_(2), while functionalization with zero or two O atoms results in much larger ΔG values(0.08 and 0.10 e V,respectively). Thus, this work details a new type of green, lowcost, and metal-free electrocatalyst for H_(2)O_(2)production.
基金the National Natural Science Foundation of China(No.21978183)。
文摘In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.
文摘<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were: pure gasoline (type A), common gasoline (type C), gasoline type A + 15% (v/v) oxygenated additives (ethanol, ethyl octanoate, ethyl oleate). The experiments were performed using engine Branco 4-stroke and 2-cylinder, electric dynamometer, exhaust system, control unit composed of Multi-K unit, variable selector and load cell, stroboscope tachometer, fuel supply system and stopwatch. The rotation was conserved at 4400 rpm and wheel power varied from 3 kW to 12 kW, with intervals of 3 kW to obtain hourly consumption curves and brake specific fuel consumption. Even esters and ethanol having lower heat of combustion, hourly consumption was similar to pure gasoline (type A). In relation to the brake specific fuel consumption, increasing the wheel power had a better conversion of the mass of fuel burned into energy. Thus, this study showed that the mixture of gasoline and esters (ethyl octanoate and ethyl oleate) presented good efficiency in terms of consumption. This research contributes to the needs and to the current studi</span><span style="font-family:Verdana;">es in which industries started to add renewable products to petroleum-</span><span style="font-family:Verdana;">derived fuels;in order to obtain more sustainable fuels at lower costs.</span>
