甘草与附子配伍有减毒增效的作用。该研究从中药汤剂甘草和附子混煎过程中蛋白质自组装的现象入手,以甘草蛋白和附子主要毒性物质——乌头碱为研究对象,探析甘草附子配伍减毒机制。研究发现经分离纯化后的甘草蛋白在p H 5时可通过自组...甘草与附子配伍有减毒增效的作用。该研究从中药汤剂甘草和附子混煎过程中蛋白质自组装的现象入手,以甘草蛋白和附子主要毒性物质——乌头碱为研究对象,探析甘草附子配伍减毒机制。研究发现经分离纯化后的甘草蛋白在p H 5时可通过自组装形成粒径为(206.2±2.02)nm的稳定颗粒,且可与乌头碱形成平均粒径为(238.20±1.23)nm的甘草蛋白-乌头碱稳定颗粒。通过小鼠急性毒性实验发现注射乌头碱单体的小鼠全部死亡,而注射相同乌头碱含量的甘草蛋白-乌头碱颗粒的小鼠全部存活。对甘草蛋白-乌头碱胶体颗粒的稳定性的调查显示,该胶体颗粒在室温下较稳定,具有成为候选药物载体的可能性。综上所述,甘草蛋白可通过与乌头碱自组装而达到减毒效果。展开更多
The solar-driven catalytic conversion of CO2 to useful chemical fuels is regarded as an environmentally friendly approach to reduce the consumption of fossil fuels and mitigate the greenhouse effect.However,it is high...The solar-driven catalytic conversion of CO2 to useful chemical fuels is regarded as an environmentally friendly approach to reduce the consumption of fossil fuels and mitigate the greenhouse effect.However,it is highly intriguing and challenging to promote the selectivity and efficiency of visible-light-responsive photocatalysts that favor the adsorption of CO2 in photoreduction processes.In this work,three-dimensional hierarchical Cd0.8Zn0.2S flowers(C8Z2S-F)with ultrathin petals were successfully synthesized through an in-situ self-assembly growth process using sodium citrate as a morphology director.The flower-like Cd0.8Zn0.2S solid solution exhibited remarkable photocatalytic performance in the reduction of CO2,generating CO up to 41.4μmol g^−1 under visible-light illumination for 3 h;this was nearly three times greater than that of Cd0.8Zn0.2S nanoparticles(C8Z2S-NP)(14.7μmol g^−1).Particularly,a comparably high selectivity of 89.9%for the conversion of CO2 to CO,with a turnover number of 39.6,was obtained from the solar-driven C8Z2S-F system in the absence of any co-catalyst or sacrificial agent.Terahertz time-domain spectroscopy indicated that the introduction of flower structures enhanced the light-harvesting capacity of C8Z2S-F.The in situ diffuse reflectance infrared Fourier transform spectroscopy unveiled the existence of surface-adsorbed species and the conversion of photoreduction intermediates during the photocatalytic process.Empirical characterizations and predictions of the photocatalytic mechanism demonstrated that the flower-like Cd0.8Zn0.2S solid solution possessed desirable CO2 adsorption properties and an enhanced charge-transfer capability,thus providing a highly effective photocatalytic reduction of CO2.展开更多
MXene, a new type of two-dimensional layered transition metal carbide material differing from graphene, demonstrates intriguing chemical/physical properties and wide applications in recent years. Here, the preparation...MXene, a new type of two-dimensional layered transition metal carbide material differing from graphene, demonstrates intriguing chemical/physical properties and wide applications in recent years. Here, the preparation of the self-assembled MXene-gold nanoparticles （MXene@AuNPs） nanocomposites with tunable sizes is reported. The nano- composites are obtained via the self-reduction reactions of MXene material in a HAuCI4 solution at room temperature. The sizes of the Au particles can be well-controlled by reg- ulating the self-reduction reaction time. They can greatly in- fluence the catalytic behaviors of the MXene@AuNPs composites. MXene@AuNPs composites with optimized re- duction time show high catalytic performances and good cycle stability for model catalytic reactions of nRro-compounds, such as 2-nitrophenol and 4-nitrophenol. This work demon- strates a new approach for the preparation of tunable MXene- based self-assembled composites.展开更多
To efficiently recycle valuable metals such as chromium and nickel in stainless steel dust, self-reduction ex- periments were carried out to study the reduction mechanism of metal oxides in coal composite stainless st...To efficiently recycle valuable metals such as chromium and nickel in stainless steel dust, self-reduction ex- periments were carried out to study the reduction mechanism of metal oxides in coal composite stainless steel dust hot briquette, which is defined as a CCSB here. Self-reduction of CCSB is proceeded by volatile matter and fixed carbon contained within CCSB. Experiments were performed to study the effects of temperature and carbon to oxygen （C/OCoal） ratio on self reduction of CCSB. At 1400 and 1450℃, volatile matter in coal used for experiment could take the place of about 40℃ of fixed carbon in coal. Under the present experimental conditions, reduction product of chromium appears as FeCr2O2, Cr2O3, Cr7C3 , and [Cr] in turn during reduction. To evaluate the formation of met al nuggets in self reduction process of CCSB, metal nuggets containing chromium and nickel were observed in outside of reduction products under various conditions, and thermodynamic equilibrium calculation was carried out for possi hie products and formation of molten metal by fixed carbon. SEM and EDS analyses were made for metal nugget and slag in reduced product. The results reveal that it is reasonable to achieve the metal nuggets at 1450℃, 0.8 of C/OCoal ratio and 20 min of reduction time. The nugget formation can indicate one innovative process for comprehensive utilization of stainless steel dust.展开更多
The oxygen reduction reaction(ORR)activity of carbonized ZIF-8(CZ)and its Fe-doped derivatives,CZ-A(doped with ammonium iron(II)sulphate)and CZ-B(doped with iron(II)acetate),were examined in both acidic(0.5 M H_(2)SO_...The oxygen reduction reaction(ORR)activity of carbonized ZIF-8(CZ)and its Fe-doped derivatives,CZ-A(doped with ammonium iron(II)sulphate)and CZ-B(doped with iron(II)acetate),were examined in both acidic(0.5 M H_(2)SO_(4))and basic(0.1 M KOH)electrolytes using a rotating disk electrode setup.These data show that the ORR activity of the Fe-doped catalysts is higher than that of pure CZ,with a higher activity in basic than acidic electrolyte.Extensive materials characterization highlights important differences in the sample crystallinity,morphology,porosity,and chemical composition as a function of the deployed precursor.The performance of the prepared catalysts is also impacted by the Fe precursor selection,highlighting the importance of such synthetic parameters in controlling the density and identify of Fe-Nx active sites.These results demonstrate the potential application of Fe-doped carbonized ZIF-8 catalysts for the ORR in basic electrolyte and offer important knowledge for the future design of non-precious metal fuel cell electrocatalysts.展开更多
Nitrogen-doped anatase TiO 2 microsheets with 65%（001） and 35%（101） exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by ...Nitrogen-doped anatase TiO 2 microsheets with 65%（001） and 35%（101） exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by scanning electron microscopy,X-ray diffraction,N2 adsorption,X-ray photoelectron spectroscopy,UV-visible spectroscopy,and electrochemical impedance spectroscopy. Their photocatalytic activity was evaluated using the photocatalytic reduction of CO2. The N-doped TiO 2 sample exhibited a much higher visible light photocatalytic activity for CO2 reduction than its precursor TiN and commercial TiO 2（P25）. This was due to the synergistic effect of the formation of surface heterojunctions on the TiO 2 microsheet surface,enhanced visible light absorption by nitrogen-doping,and surface fluorination.展开更多
Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their m...Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.展开更多
With the strict control of sulfur content in fuels,oxidative desulfurization(ODS),a promising desulphurization technology,needs to be continuously developed.In this study,we integrated multiple approaches(fabricating ...With the strict control of sulfur content in fuels,oxidative desulfurization(ODS),a promising desulphurization technology,needs to be continuously developed.In this study,we integrated multiple approaches(fabricating a porous structure,increasing phosphomolybdic acid(PMo)loading,improving amphiphilicity,and enhancing the intrinsic activity of PMo using a reductive framework)into PAF-54 carriers to improve ODS catalytic ability.The catalytic performance suggested that PAF-54 was not simply used as a carrier for PMo by physical integration.During the binding process,electron transfer between PAF-54 and PMo formed Mo^(5+)with superior catalytic activity.Owing to the presence of PAF-54,the catalytic activity of PMo as the active component qualitatively improved to achieve rapid and efficient desulfurization.More importantly,we found that other nitrogen-rich porous organic polymers can also reduce some of Mo^(6+)in PMo during loading,and its formation mechanism was investigated.This work provides a feasible strategy for designing highly efficient DOS catalysts.展开更多
Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative stru...Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.展开更多
Bimetalic platinum-copper(Pt-Cu)alloy nanowires have emerged as a novel class of fuel cell electrocatalysts for oxygen reduction reaction(ORR)due to their intrinsic high catalytic activity and durability,but preparing...Bimetalic platinum-copper(Pt-Cu)alloy nanowires have emerged as a novel class of fuel cell electrocatalysts for oxygen reduction reaction(ORR)due to their intrinsic high catalytic activity and durability,but preparing such electrocatalysts with clean surface via facile method is still a challenge.Herein,PtCu alloy with nanowire networks(NWNs)structure is obtained by a simple modified polyol method accompanied with a salt-mediated self-assembly process in a water/ethylene glycol(EG)mixing media.The formation mechanism of PtCu NWNs including the morphological evolution and the relevant experimental parameters has been investigated systematically.We propose that a micro-interface in H2O-EG media formed with the assistance of disodium dihydrogen pyrophosphate(Na2H2P2O7)and its unique nature of coordinating with Pt^2+ or Cu^2+ play critical roles in the formation of NWNs.When tested as ORR catalyst,the PtCuNWNs/C exhibits much higher activity and durability than that of PtNWNs/C and commercial PtC,even exceeding the target of DOE in 2020.The excellent performance of PtCuNWNs/C could be attributed to the unique structure of NWNs with 2.4 nm ultrathin wavy nanowires and plentiful surface defects and the modified electronic effect caused by alloying with Cu atoms.展开更多
Incorporating metal nanodots(NDs)into heterostructures for high charge separation and transfer capacities is one of the most effective strategies for improving their photocatalytic activities.However,controlling the s...Incorporating metal nanodots(NDs)into heterostructures for high charge separation and transfer capacities is one of the most effective strategies for improving their photocatalytic activities.However,controlling the space distribution of metal NDs for optimizing charge transport pathways remains a significant challenge,particularly in two-dimensional(2D)face-to-face heterostructures.Herein,we develop a simple targeted self-reduction strategy for selectively loading Ru NDs onto the Ti_(3−x)C_(2)T_(y)(TC)surface of 2D TC/g-C_(3)N_(4)(CN)heterojunction based on the reductive Ti vacancy defects creatively increased during the preparation of TC/CN by reducing calcination.Notably,the optimized Ru/TC/CN photocatalyst exhibits an outstanding H_(2)evolution rate of 3.21 mmol·g^(−1)·h^(−1)and a high apparent quantum efficiency of 30.9%at 380 nm,which is contributed by the unidirectional transfer of the photogenerated electrons from CN to Ru active sites(CN→TC→Ru)and the suppressed backflow of electrons from Ru sites to CN,as revealed by comprehensive characterizations and density functional theory(DFT)calculations.This work provides a novel strategy for synthesizing the highly efficient photocatalysts with a controllable charge transfer paths,which will boost the development of photocatalysis.展开更多
Large high clearance self-propelled sprayers were widely used in field plant protection due to their high-efficiency operation capabilities.Influenced by the characteristics of field operations such as high power,heav...Large high clearance self-propelled sprayers were widely used in field plant protection due to their high-efficiency operation capabilities.Influenced by the characteristics of field operations such as high power,heavy weight,high ground clearance,and fast operation speed,the comprehensive requirements for the ride comfort,handling stability and road friendliness of the sprayer were increasingly strong.At the present stage,the chassis structure of the high clearance selfpropelled sprayer that attaches great importance to the improvement of comprehensive performance still has the problems of severe bumps,weak handling performance and serious road damage in complex field environments.Therefore,this paper proposes an optimization design method for hydro-pneumatic suspension system of a high clearance self-propelled sprayer based on the improved MOPSO(Multi-Objective Particle Swarm Optimization)algorithm,covering the entire process of configuration design,parameter intelligent optimization,and system verification of the high clearance self-propelled sprayer chassis.Specifically,chassis structure of the hydro-pneumatic suspension suitable for the high clearance self-propelled sprayer was designed,and a design method combining the improved MOPSO algorithm based on time-varying fusion strategy and adaptive update with the parameter optimization of hydro-pneumatic suspension based on this algorithm was proposed,and finally the software simulation and bench performance verification were carried out.The results show that the optimized hydropneumatic suspension has excellent vibration reduction effect,and the body acceleration,suspension dynamic deflection and tire deflection were increased by 16.5%,9.9%and 0.9%respectively,compared with those before optimization.The comprehensive performance of the hydro-pneumatic suspension designed in this study is better than that of the traditional suspension.展开更多
Dimensionality reduction and data visualization are useful and important processes in pattern recognition. Many techniques have been developed in the recent years. The self-organizing map （SOM） can be an efficient m...Dimensionality reduction and data visualization are useful and important processes in pattern recognition. Many techniques have been developed in the recent years. The self-organizing map （SOM） can be an efficient method for this purpose. This paper reviews recent advances in this area and related approaches such as multidimensional scaling （MDS）, nonlinear PC A, principal manifolds, as well as the connections of the SOM and its recent variant, the visualization induced SOM （ViSOM）, with these approaches. The SOM is shown to produce a quantized, qualitative scaling and while the ViSOM a quantitative or metric scaling and approximates principal curve/surface. The SOM can also be regarded as a generalized MDS to relate two metric spaces by forming a topological mapping between them. The relationships among various recently proposed techniques such as ViSOM, Isomap, LLE, and eigenmap are discussed and compared.展开更多
文摘甘草与附子配伍有减毒增效的作用。该研究从中药汤剂甘草和附子混煎过程中蛋白质自组装的现象入手,以甘草蛋白和附子主要毒性物质——乌头碱为研究对象,探析甘草附子配伍减毒机制。研究发现经分离纯化后的甘草蛋白在p H 5时可通过自组装形成粒径为(206.2±2.02)nm的稳定颗粒,且可与乌头碱形成平均粒径为(238.20±1.23)nm的甘草蛋白-乌头碱稳定颗粒。通过小鼠急性毒性实验发现注射乌头碱单体的小鼠全部死亡,而注射相同乌头碱含量的甘草蛋白-乌头碱颗粒的小鼠全部存活。对甘草蛋白-乌头碱胶体颗粒的稳定性的调查显示,该胶体颗粒在室温下较稳定,具有成为候选药物载体的可能性。综上所述,甘草蛋白可通过与乌头碱自组装而达到减毒效果。
文摘The solar-driven catalytic conversion of CO2 to useful chemical fuels is regarded as an environmentally friendly approach to reduce the consumption of fossil fuels and mitigate the greenhouse effect.However,it is highly intriguing and challenging to promote the selectivity and efficiency of visible-light-responsive photocatalysts that favor the adsorption of CO2 in photoreduction processes.In this work,three-dimensional hierarchical Cd0.8Zn0.2S flowers(C8Z2S-F)with ultrathin petals were successfully synthesized through an in-situ self-assembly growth process using sodium citrate as a morphology director.The flower-like Cd0.8Zn0.2S solid solution exhibited remarkable photocatalytic performance in the reduction of CO2,generating CO up to 41.4μmol g^−1 under visible-light illumination for 3 h;this was nearly three times greater than that of Cd0.8Zn0.2S nanoparticles(C8Z2S-NP)(14.7μmol g^−1).Particularly,a comparably high selectivity of 89.9%for the conversion of CO2 to CO,with a turnover number of 39.6,was obtained from the solar-driven C8Z2S-F system in the absence of any co-catalyst or sacrificial agent.Terahertz time-domain spectroscopy indicated that the introduction of flower structures enhanced the light-harvesting capacity of C8Z2S-F.The in situ diffuse reflectance infrared Fourier transform spectroscopy unveiled the existence of surface-adsorbed species and the conversion of photoreduction intermediates during the photocatalytic process.Empirical characterizations and predictions of the photocatalytic mechanism demonstrated that the flower-like Cd0.8Zn0.2S solid solution possessed desirable CO2 adsorption properties and an enhanced charge-transfer capability,thus providing a highly effective photocatalytic reduction of CO2.
基金supported by the National Natural Science Foundation of China (21473153 and 51771162)Support Program for the Top Young Talents of Hebei Province, China Postdoctoral Science Foundation (2015M580214)the Scientific and Technological Research and Development Program of Qinhuangdao City (201701B004)
文摘MXene, a new type of two-dimensional layered transition metal carbide material differing from graphene, demonstrates intriguing chemical/physical properties and wide applications in recent years. Here, the preparation of the self-assembled MXene-gold nanoparticles （MXene@AuNPs） nanocomposites with tunable sizes is reported. The nano- composites are obtained via the self-reduction reactions of MXene material in a HAuCI4 solution at room temperature. The sizes of the Au particles can be well-controlled by reg- ulating the self-reduction reaction time. They can greatly in- fluence the catalytic behaviors of the MXene@AuNPs composites. MXene@AuNPs composites with optimized re- duction time show high catalytic performances and good cycle stability for model catalytic reactions of nRro-compounds, such as 2-nitrophenol and 4-nitrophenol. This work demon- strates a new approach for the preparation of tunable MXene- based self-assembled composites.
基金Item Sponsored by Fundamental Research Funds for the Central Universities of China(N110202001)
文摘To efficiently recycle valuable metals such as chromium and nickel in stainless steel dust, self-reduction ex- periments were carried out to study the reduction mechanism of metal oxides in coal composite stainless steel dust hot briquette, which is defined as a CCSB here. Self-reduction of CCSB is proceeded by volatile matter and fixed carbon contained within CCSB. Experiments were performed to study the effects of temperature and carbon to oxygen （C/OCoal） ratio on self reduction of CCSB. At 1400 and 1450℃, volatile matter in coal used for experiment could take the place of about 40℃ of fixed carbon in coal. Under the present experimental conditions, reduction product of chromium appears as FeCr2O2, Cr2O3, Cr7C3 , and [Cr] in turn during reduction. To evaluate the formation of met al nuggets in self reduction process of CCSB, metal nuggets containing chromium and nickel were observed in outside of reduction products under various conditions, and thermodynamic equilibrium calculation was carried out for possi hie products and formation of molten metal by fixed carbon. SEM and EDS analyses were made for metal nugget and slag in reduced product. The results reveal that it is reasonable to achieve the metal nuggets at 1450℃, 0.8 of C/OCoal ratio and 20 min of reduction time. The nugget formation can indicate one innovative process for comprehensive utilization of stainless steel dust.
文摘The oxygen reduction reaction(ORR)activity of carbonized ZIF-8(CZ)and its Fe-doped derivatives,CZ-A(doped with ammonium iron(II)sulphate)and CZ-B(doped with iron(II)acetate),were examined in both acidic(0.5 M H_(2)SO_(4))and basic(0.1 M KOH)electrolytes using a rotating disk electrode setup.These data show that the ORR activity of the Fe-doped catalysts is higher than that of pure CZ,with a higher activity in basic than acidic electrolyte.Extensive materials characterization highlights important differences in the sample crystallinity,morphology,porosity,and chemical composition as a function of the deployed precursor.The performance of the prepared catalysts is also impacted by the Fe precursor selection,highlighting the importance of such synthetic parameters in controlling the density and identify of Fe-Nx active sites.These results demonstrate the potential application of Fe-doped carbonized ZIF-8 catalysts for the ORR in basic electrolyte and offer important knowledge for the future design of non-precious metal fuel cell electrocatalysts.
基金supported by the National Basic Research Program of China(973 Program2013CB632402)+7 种基金the National Natural Science Foundation of China(513201050015137219051402025and 21433007)the Natural Science Foundation of Hubei Province(2015CFA001)the Fundamental Research Funds for the Central Universities(WUT:2014-VII-010)the Self-Determined and Innovative Research Funds of State Key Laboratory of Advanced Technology for Material Synthesis and ProcessingWuhan University of Technology(2013-ZD-1)~~
文摘Nitrogen-doped anatase TiO 2 microsheets with 65%（001） and 35%（101） exposed faces were fabricated by the hydrothermal method using TiN as precursor in the presence of HF and HCl. The samples were characterized by scanning electron microscopy,X-ray diffraction,N2 adsorption,X-ray photoelectron spectroscopy,UV-visible spectroscopy,and electrochemical impedance spectroscopy. Their photocatalytic activity was evaluated using the photocatalytic reduction of CO2. The N-doped TiO 2 sample exhibited a much higher visible light photocatalytic activity for CO2 reduction than its precursor TiN and commercial TiO 2（P25）. This was due to the synergistic effect of the formation of surface heterojunctions on the TiO 2 microsheet surface,enhanced visible light absorption by nitrogen-doping,and surface fluorination.
文摘Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.
基金supported by Hainan Provincial Natural Science Foundation of China(220MS005)the National Key R&D Program of China(2022YFB3805902)+3 种基金the National Natural Science Foundation of China(22361017 and 22075040)the Innovation Platform for Academicians of Hainan Provincethe Specific Research Fund of the Innovation Platform for Academicians of Hainan Province(YSPTZX202321)the International Science&Technology Cooperation Program of Hainan Province(GHYF2022006)。
文摘With the strict control of sulfur content in fuels,oxidative desulfurization(ODS),a promising desulphurization technology,needs to be continuously developed.In this study,we integrated multiple approaches(fabricating a porous structure,increasing phosphomolybdic acid(PMo)loading,improving amphiphilicity,and enhancing the intrinsic activity of PMo using a reductive framework)into PAF-54 carriers to improve ODS catalytic ability.The catalytic performance suggested that PAF-54 was not simply used as a carrier for PMo by physical integration.During the binding process,electron transfer between PAF-54 and PMo formed Mo^(5+)with superior catalytic activity.Owing to the presence of PAF-54,the catalytic activity of PMo as the active component qualitatively improved to achieve rapid and efficient desulfurization.More importantly,we found that other nitrogen-rich porous organic polymers can also reduce some of Mo^(6+)in PMo during loading,and its formation mechanism was investigated.This work provides a feasible strategy for designing highly efficient DOS catalysts.
基金funded by the National Natural Science Foundation of China(No.51873004).
文摘Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.
基金the National Major Research Project(No.2018YFB0105601)the National Natural Science Foundation of China(No.21576257)+1 种基金the Natural Science Foundation-Liaoning United Fund(No.U 1508202)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB06050303).
文摘Bimetalic platinum-copper(Pt-Cu)alloy nanowires have emerged as a novel class of fuel cell electrocatalysts for oxygen reduction reaction(ORR)due to their intrinsic high catalytic activity and durability,but preparing such electrocatalysts with clean surface via facile method is still a challenge.Herein,PtCu alloy with nanowire networks(NWNs)structure is obtained by a simple modified polyol method accompanied with a salt-mediated self-assembly process in a water/ethylene glycol(EG)mixing media.The formation mechanism of PtCu NWNs including the morphological evolution and the relevant experimental parameters has been investigated systematically.We propose that a micro-interface in H2O-EG media formed with the assistance of disodium dihydrogen pyrophosphate(Na2H2P2O7)and its unique nature of coordinating with Pt^2+ or Cu^2+ play critical roles in the formation of NWNs.When tested as ORR catalyst,the PtCuNWNs/C exhibits much higher activity and durability than that of PtNWNs/C and commercial PtC,even exceeding the target of DOE in 2020.The excellent performance of PtCuNWNs/C could be attributed to the unique structure of NWNs with 2.4 nm ultrathin wavy nanowires and plentiful surface defects and the modified electronic effect caused by alloying with Cu atoms.
基金the National Natural Science Foundation of China(No.22002142)China Postdoctoral Science Foundation(No.2020T130605)+2 种基金Natural Science Foundation of Henan Province(No.202300410436)Support Plan for College Science and Technology Innovation Team of Henan Province(No.16IRTSTHN001)the Science&Technology Innovation Talent Plan of Henan Province(No.174200510018).
文摘Incorporating metal nanodots(NDs)into heterostructures for high charge separation and transfer capacities is one of the most effective strategies for improving their photocatalytic activities.However,controlling the space distribution of metal NDs for optimizing charge transport pathways remains a significant challenge,particularly in two-dimensional(2D)face-to-face heterostructures.Herein,we develop a simple targeted self-reduction strategy for selectively loading Ru NDs onto the Ti_(3−x)C_(2)T_(y)(TC)surface of 2D TC/g-C_(3)N_(4)(CN)heterojunction based on the reductive Ti vacancy defects creatively increased during the preparation of TC/CN by reducing calcination.Notably,the optimized Ru/TC/CN photocatalyst exhibits an outstanding H_(2)evolution rate of 3.21 mmol·g^(−1)·h^(−1)and a high apparent quantum efficiency of 30.9%at 380 nm,which is contributed by the unidirectional transfer of the photogenerated electrons from CN to Ru active sites(CN→TC→Ru)and the suppressed backflow of electrons from Ru sites to CN,as revealed by comprehensive characterizations and density functional theory(DFT)calculations.This work provides a novel strategy for synthesizing the highly efficient photocatalysts with a controllable charge transfer paths,which will boost the development of photocatalysis.
基金financially supported by Major scientific and Technological Innovation Projects of Shan Dong Province(Grant No.2019JZZY010728-01)supported by Bintuan Science and Technology Program(Grant No.2022DB001)Innovative Platform of Intelligent Agricultural Equipment Design and Manufacturing(Grant No.2021XDRHXMPT29).
文摘Large high clearance self-propelled sprayers were widely used in field plant protection due to their high-efficiency operation capabilities.Influenced by the characteristics of field operations such as high power,heavy weight,high ground clearance,and fast operation speed,the comprehensive requirements for the ride comfort,handling stability and road friendliness of the sprayer were increasingly strong.At the present stage,the chassis structure of the high clearance selfpropelled sprayer that attaches great importance to the improvement of comprehensive performance still has the problems of severe bumps,weak handling performance and serious road damage in complex field environments.Therefore,this paper proposes an optimization design method for hydro-pneumatic suspension system of a high clearance self-propelled sprayer based on the improved MOPSO(Multi-Objective Particle Swarm Optimization)algorithm,covering the entire process of configuration design,parameter intelligent optimization,and system verification of the high clearance self-propelled sprayer chassis.Specifically,chassis structure of the hydro-pneumatic suspension suitable for the high clearance self-propelled sprayer was designed,and a design method combining the improved MOPSO algorithm based on time-varying fusion strategy and adaptive update with the parameter optimization of hydro-pneumatic suspension based on this algorithm was proposed,and finally the software simulation and bench performance verification were carried out.The results show that the optimized hydropneumatic suspension has excellent vibration reduction effect,and the body acceleration,suspension dynamic deflection and tire deflection were increased by 16.5%,9.9%and 0.9%respectively,compared with those before optimization.The comprehensive performance of the hydro-pneumatic suspension designed in this study is better than that of the traditional suspension.
文摘Dimensionality reduction and data visualization are useful and important processes in pattern recognition. Many techniques have been developed in the recent years. The self-organizing map （SOM） can be an efficient method for this purpose. This paper reviews recent advances in this area and related approaches such as multidimensional scaling （MDS）, nonlinear PC A, principal manifolds, as well as the connections of the SOM and its recent variant, the visualization induced SOM （ViSOM）, with these approaches. The SOM is shown to produce a quantized, qualitative scaling and while the ViSOM a quantitative or metric scaling and approximates principal curve/surface. The SOM can also be regarded as a generalized MDS to relate two metric spaces by forming a topological mapping between them. The relationships among various recently proposed techniques such as ViSOM, Isomap, LLE, and eigenmap are discussed and compared.
