Chuangxinmycin is an antibiotic isolated from Actinoplanes tsinanensis CPCC 200056 in the1970 s with a novel indole-dihydrothiopyran heterocyclic skeleton. Chuangxinmycin showed in vitro antibacterial activity and in ...Chuangxinmycin is an antibiotic isolated from Actinoplanes tsinanensis CPCC 200056 in the1970 s with a novel indole-dihydrothiopyran heterocyclic skeleton. Chuangxinmycin showed in vitro antibacterial activity and in vivo efficacy in mouse infection models as well as preliminary clinical trials.But the biosynthetic pathway of chuangxinmycin has been obscure since its discovery. Herein, we report the identification of a stretch of DNA from the genome of A. tsinanensis CPCC 200056 that encodes genes for biosynthesis of chuangxinmycin by bioinformatics analysis. The designated cxn cluster was then confirmed to be responsible for chuangxinmycin biosynthesis by direct cloning and heterologous expressing in Streptomyces coelicolor M1146. The cytochrome P450 CxnD was verified to be involved in the dihydrothiopyran ring closure reaction by the identification of seco-chuangxinmycin in S. coelicolor M1146 harboring the cxn gene cluster with an inactivated cxn D. Based on these results, a plausible biosynthetic pathway for chuangxinmycin biosynthesis was proposed, by hijacking the primary sulfur transfer system for sulfur incorporation. The identification of the biosynthetic gene cluster of chuangxinmycin paves the way for elucidating the detail biochemical machinery for chuangxinmycin biosynthesis, and provides the basis for the generation of novel chuangxinmycin derivatives by means of combinatorial biosynthesis and synthetic biology.展开更多
An iodine‐catalyzed sulfenylation of pyrazoles at room temperature is described,in which a variety of pyrazoles were well tolerated and the desired products were obtained in good to excellent yields.
Density effects on the growth and self-thinning of Eucalyptus urophylla stands were examined for 7 years.The reciprocal equation of the competition-density(C–D)effect was used to describe the C–D effect in even-aged...Density effects on the growth and self-thinning of Eucalyptus urophylla stands were examined for 7 years.The reciprocal equation of the competition-density(C–D)effect was used to describe the C–D effect in even-aged pure stands of E. urophylla during course of self-thinning and showed a good fit to the data. The time trajectories of mean stem volume-density nearly paralleled the y-axis during early growth stages of stands, and then began to curve left. Finally, the mean stem volume-density trajectories of the low-, middle-and high-density stands tended to follow the self-thinning lines with slopes of-2.01,-1.90 and-1.99, respectively. With increasing physical time t, the biological time s increased rapidly during early growth stages and became slow gradually during later growth stages. Realized density-initial density curves tended to become more or less flat with increasing initial density, indicating the existence of an asymptotic value for density at a given time. The coefficient e, the reciprocal of which represents the asymptotic density at a given time,increased with increasing biological time s, indicating that the asymptotic density decreased with increasing stand age.Final yield Y(t) increased gradually with increasing stand age.展开更多
In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flour...In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flourishing area, Chinese chemists have devoted great efforts to different aspects of synthetic chemistry. This review will summarize their representative work according to the following categories: C–H functionalization, synthesis of aromatic aza-heterocycles, asymmetric organic photochemical synthesis, transformations of small molecules and biomolecule-compatible reactions.展开更多
Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneo...Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous catalysis.This prediction was first experimentally demonstrated in 2016.In this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H bonds.All of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous catalysts.These pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis.展开更多
Numerous studies have focused on the reduction thermodynamics of ordinary iron ore;by contrast, the literature contains few thermodynamic studies on the gas-based reduction of vanadium titano-magnetite (VTM) in mixed ...Numerous studies have focused on the reduction thermodynamics of ordinary iron ore;by contrast, the literature contains few thermodynamic studies on the gas-based reduction of vanadium titano-magnetite (VTM) in mixed atmospheres of H2, CO, H2O, CO2, and N2. In this paper, thermodynamic studies on the reduction of oxidized VTM pellets were systematically conducted in an atmosphere of a C–H–O system as a reducing agent. The results indicate that VTM of an equivalent valence state is more difficult to reduce than ordinary iron ore. A reduction equilibrium diagram using the C–H–O system as a reducing agent was obtained;it clearly describes the reduction process. Experiments were performed to investigate the effects of the reduction temperature, the gas composition, and two types of iron ores on the reduction of oxidized VTM pellets. The results show that the final reduction degree increases with increasing reduction temperature, increasing molar ratio of H2/(H2 + CO), and decreasing H2O, CO2, and N2 contents. In addition, the reduction processes under various conditions are discussed. All of the results of the reduction experiments are consistent with those of theoretical thermodynamic analysis. This study is expected to provide valuable thermodynamic theory on the industrial applications of VTM.展开更多
We demonstrate the synthesis of C-Cl-codoped titania/attapulgite（TiO2/ATT） composites containing a mixture of TiO2 phases by a facile sol-gel method at 70 ℃ using titanium tetraisopropoxide as the TiO2 precursor an...We demonstrate the synthesis of C-Cl-codoped titania/attapulgite（TiO2/ATT） composites containing a mixture of TiO2 phases by a facile sol-gel method at 70 ℃ using titanium tetraisopropoxide as the TiO2 precursor and ATT as a support for the TiO2 nanoparticles.The photocatalytic activity of the C-Cl-codoped TiO2/ATT composites with mixed anatase/brookite/rutile phases obtained at pH= 3.0 was much higher than that of commercially available Degussa P25 for the photocatalytic degradation of acid red G under visible-light irradiation.The excellent photocatalytic activity of the developed composite originates from the nonmetal codoping,which extends the absorption edge of TiO2 into visible region,and the presence of multiple phases,which slow the recombination of photoexcited electron/hole pairs.The formation of hydroxyl radicals during the photocatalytic degradation process was detected by photoluminescence probing using terephthalic acid.A mechanism for photocatalysis over the C-Cl-codoped TiO2/ATT composites was proposed.展开更多
It remains challenging to achieve the selective cleavage of C–C bonds in lignin or lignin model compounds to produce aromatic products in high yield and selectivity.We have developed a redox-neutral photocatalytic st...It remains challenging to achieve the selective cleavage of C–C bonds in lignin or lignin model compounds to produce aromatic products in high yield and selectivity.We have developed a redox-neutral photocatalytic strategy to accomplish this goal in both b-O-4 and b-1 lignin models at room temperature(RT)via proton-coupled electron transfer(PCET)process without any pretreatments of substrate,by adjusting the alkalinity of base to obtain a lignin models/base PCET pair with a bond dissociation free energy close to 102 kcal/mol.Without breaking down C_b–Ccbond and any C–O bonds,this PCET method is 100%atom economy and produces exclusive Ca–C_bbond cleavage products,such as benzaldehydes(up to 97%)and phenyl ethers(up to 96%),in high to excellent yields and selectivities.Preliminary studies indicated that the PCET strategy is also effective for the depolymerization of native lignin at RT,thus providing significantly important foundation to the depolymerization of lignin.展开更多
In radiation measurement and digital nuclear spectrum systems,traditional nuclear signal processing circuits in nuclear electronics have been gradually replaced by digital algorithm modules with the application of hig...In radiation measurement and digital nuclear spectrum systems,traditional nuclear signal processing circuits in nuclear electronics have been gradually replaced by digital algorithm modules with the application of highperformance programmable hardware logic devices(such as FPGA or DSP).Referring to the digital realization method of inverse RC integral circuit systems,the function of the pole-zero cancellation(PZC)circuit was analyzed,a new modified cascade equivalent model of PZC was established,and the time-domain digital PZC(DPZC)recursive algorithm was derived in detail in this study.Two parameters kIand k_(D)are included in the new algorithm,where kIshould match the exponential decay time constant of the input signal to realize the pole-zero compensation,while the decay time constant of the output signal can be changed with the adjustable parameter k_(D)(which is larger than the decay time constant of the input signal).Based on the new DPZC algorithm module,two trapezoidal(triangular)shaping filters were designed and implemented.The amplitude–frequency characteristics of the output signal of the proposed trapezoidal shaping algorithm and the convolution trapezoidal shaping algorithm were compared,with fixed peaking time.The results show that the trapezoidal shaping algorithm based on DPZC can better suppress high-frequency noise.Finally,based on the Na I(Tl)scintillator(u75 mm×75 mm)detector and^(137)Cs source,the effect of the k_(D)value on the energy resolution of the DPZC trapezoidal(triangular)shaping algorithm was studied.The experimental results show that,with an increase in k_(D),the energy resolution of the system improved and reached the maximum when k_(D)was greater than 10,and the optimal energy resolution of the system was 7.72%.展开更多
Cu-based catalysts are the most promising candidates for electrochemical CO_(2)reduction(CO_(2)RR)to multi-carbon(C_(2))products.Optimizing the C-C coupling process,the rate-determining step for C_(2)product generatio...Cu-based catalysts are the most promising candidates for electrochemical CO_(2)reduction(CO_(2)RR)to multi-carbon(C_(2))products.Optimizing the C-C coupling process,the rate-determining step for C_(2)product generation,is an important strategy to improve the production and selectivity of the C_(2)products.In this study,we determined that the local electric field can promote the C-C coupling reaction and enhance CO_(2)electroreduction to C_(2)products.First,finite-element simulations indicated that the high curvature of the Cu nanoneedles results in a large local electric field on their tips.Density functional theory(DFT)calculations proved that a large electric field can promote C-C coupling.Motivated by this prediction,we prepared a series of Cu catalysts with different curvatures.The Cu nanoneedles(NNs)exhibited the largest number of curvatures,followed by the Cu nanorods(NRs),and Cu nanoparticles(NPs).The Cu NNs contained the highest concentration of adsorbed K+,which resulted in the highest local electric field on the needles.CO adsorption sensor tests indicated that the Cu NNs exhibited the strongest CO adsorption ability,and in-situ Fourier-transform infrared spectroscopy(FTIR)showed the strongest*COCO and*CO signals for the Cu NNs.These experimental results demonstrate that high-curvature nanoneedles can induce a large local electric field,thus promoting C-C coupling.As a result,the Cu NNs show a maximum FEC_(2)of 44%for CO_(2)RR at a low potential(-0.6 V vs.RHE),which is approximately 2.2 times that of the Cu NPs.This work provides an effective strategy for enhancing the production of multi-carbon products during CO_(2)RR.展开更多
Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the ...Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the conversion of corn-stalk cellulose to produce a relatively high concentration of bio-ethanol(6.1 wt%)without humin formation.A high yield of cellulose(ca.50 wt%)is extracted from corn stalk using a green solvent(80 wt%1,4-butanediol)without destroying the structure of the lignin.The first hydrothermal hydrogenolysis step uses a Ni–WO_(x)/SiO_(2)catalyst to convert the high cumulative concentration of cellulose(30 wt%)into a polyol mixture with a 56.5 C%yield of ethylene glycol(EG).The original polyol mixture is then subjected to subsequent selective aqueous-phase hydrogenolysis of the C–O bond to produce bioethanol(75%conversion,84 C%selectivity)over the modified hydrothermally stable Cu catalysts.The added Ni component favors the good dispersion of Cu nanoparticles,and the incorporated Au3+helps to stabilize the active Cu^(0)-Cu^(+)species.This multi-functional catalytic process provides an economically competitive route for the production of cellulosic ethanol from raw lignocellulose.展开更多
C/C–SiC–HfC composites were fabricated via precursor infiltration and pyrolysis using a mixture solution of organic hafnium-containing polymer and polycarbosilane as precursor. The microstructures and the phases of ...C/C–SiC–HfC composites were fabricated via precursor infiltration and pyrolysis using a mixture solution of organic hafnium-containing polymer and polycarbosilane as precursor. The microstructures and the phases of the composites were analyzed by scanning electron microscopy and X-ray diffraction. The ablation resistance of the composites was evaluated under 3,000 °C oxyacetylene torch. After ablation for 120 s, the composites exhibit good ablation properties with the linear and mass ablation rates of 9.1 9 10-4mm/s and 1.30 9 10-3g/s, which are far lower than those of the C/C–SiC composites. The excellent ablative property of the C/C–SiC–HfC composites is resulted from the formation of HfO2 molten layer on the surface of the composites, which could play a positive role in reducing heat transfer and preventing oxygen transport to the underlying carbon substrate.展开更多
基金supported by the National Natural Science Foundation of China (81621064, 81603006, 81402836 and 31170042)the National Mega-Project for Innovative Drugs (2015ZX09102007016 and 2017ZX09101003-006-011)the CAMS Initiative for Innovative Medicine (2016-I2M-3–012)
文摘Chuangxinmycin is an antibiotic isolated from Actinoplanes tsinanensis CPCC 200056 in the1970 s with a novel indole-dihydrothiopyran heterocyclic skeleton. Chuangxinmycin showed in vitro antibacterial activity and in vivo efficacy in mouse infection models as well as preliminary clinical trials.But the biosynthetic pathway of chuangxinmycin has been obscure since its discovery. Herein, we report the identification of a stretch of DNA from the genome of A. tsinanensis CPCC 200056 that encodes genes for biosynthesis of chuangxinmycin by bioinformatics analysis. The designated cxn cluster was then confirmed to be responsible for chuangxinmycin biosynthesis by direct cloning and heterologous expressing in Streptomyces coelicolor M1146. The cytochrome P450 CxnD was verified to be involved in the dihydrothiopyran ring closure reaction by the identification of seco-chuangxinmycin in S. coelicolor M1146 harboring the cxn gene cluster with an inactivated cxn D. Based on these results, a plausible biosynthetic pathway for chuangxinmycin biosynthesis was proposed, by hijacking the primary sulfur transfer system for sulfur incorporation. The identification of the biosynthetic gene cluster of chuangxinmycin paves the way for elucidating the detail biochemical machinery for chuangxinmycin biosynthesis, and provides the basis for the generation of novel chuangxinmycin derivatives by means of combinatorial biosynthesis and synthetic biology.
基金supported by the National Natural Science Foundation of China(21402103,21772107,31471808)the China Postdoctoral Science Foundation(150030)the Research Fund of Qingdao Agricultural University's Highlevel Person(631303)~~
文摘An iodine‐catalyzed sulfenylation of pyrazoles at room temperature is described,in which a variety of pyrazoles were well tolerated and the desired products were obtained in good to excellent yields.
基金partially supported by the Forestry Technology Popularization Demonstration Project of the Central Government of China(No.[2015]GDTK-07)
文摘Density effects on the growth and self-thinning of Eucalyptus urophylla stands were examined for 7 years.The reciprocal equation of the competition-density(C–D)effect was used to describe the C–D effect in even-aged pure stands of E. urophylla during course of self-thinning and showed a good fit to the data. The time trajectories of mean stem volume-density nearly paralleled the y-axis during early growth stages of stands, and then began to curve left. Finally, the mean stem volume-density trajectories of the low-, middle-and high-density stands tended to follow the self-thinning lines with slopes of-2.01,-1.90 and-1.99, respectively. With increasing physical time t, the biological time s increased rapidly during early growth stages and became slow gradually during later growth stages. Realized density-initial density curves tended to become more or less flat with increasing initial density, indicating the existence of an asymptotic value for density at a given time. The coefficient e, the reciprocal of which represents the asymptotic density at a given time,increased with increasing biological time s, indicating that the asymptotic density decreased with increasing stand age.Final yield Y(t) increased gradually with increasing stand age.
基金supported by the National Natural Science Foundation of China(21772052,21772053,21772129,21801176,21672099,21732003)Chinese Academy of Sciences(XDB20020200)
文摘In recent years, visible light-driven organic photochemical synthesis has attracted wide research interest from academic and industrial communities due to its features of green and sustainable chemistry. In this flourishing area, Chinese chemists have devoted great efforts to different aspects of synthetic chemistry. This review will summarize their representative work according to the following categories: C–H functionalization, synthesis of aromatic aza-heterocycles, asymmetric organic photochemical synthesis, transformations of small molecules and biomolecule-compatible reactions.
基金supported by National Natural Science Foundation of China(21606222,21776270)Postdoctoral Science Foundation(2017M621170,2016M601350)~~
文摘Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous catalysis.This prediction was first experimentally demonstrated in 2016.In this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H bonds.All of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous catalysts.These pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis.
基金financially supported by the Ministry of Land and Resources Public Welfare Industry Research Project, China (No. 201511062-02)
文摘Numerous studies have focused on the reduction thermodynamics of ordinary iron ore;by contrast, the literature contains few thermodynamic studies on the gas-based reduction of vanadium titano-magnetite (VTM) in mixed atmospheres of H2, CO, H2O, CO2, and N2. In this paper, thermodynamic studies on the reduction of oxidized VTM pellets were systematically conducted in an atmosphere of a C–H–O system as a reducing agent. The results indicate that VTM of an equivalent valence state is more difficult to reduce than ordinary iron ore. A reduction equilibrium diagram using the C–H–O system as a reducing agent was obtained;it clearly describes the reduction process. Experiments were performed to investigate the effects of the reduction temperature, the gas composition, and two types of iron ores on the reduction of oxidized VTM pellets. The results show that the final reduction degree increases with increasing reduction temperature, increasing molar ratio of H2/(H2 + CO), and decreasing H2O, CO2, and N2 contents. In addition, the reduction processes under various conditions are discussed. All of the results of the reduction experiments are consistent with those of theoretical thermodynamic analysis. This study is expected to provide valuable thermodynamic theory on the industrial applications of VTM.
基金supported by the National Basic Research Program of China (973 Program, 2007CB613302)the Natural Science Foundation of Hubei Province (2016CFA078)~~
文摘We demonstrate the synthesis of C-Cl-codoped titania/attapulgite（TiO2/ATT） composites containing a mixture of TiO2 phases by a facile sol-gel method at 70 ℃ using titanium tetraisopropoxide as the TiO2 precursor and ATT as a support for the TiO2 nanoparticles.The photocatalytic activity of the C-Cl-codoped TiO2/ATT composites with mixed anatase/brookite/rutile phases obtained at pH= 3.0 was much higher than that of commercially available Degussa P25 for the photocatalytic degradation of acid red G under visible-light irradiation.The excellent photocatalytic activity of the developed composite originates from the nonmetal codoping,which extends the absorption edge of TiO2 into visible region,and the presence of multiple phases,which slow the recombination of photoexcited electron/hole pairs.The formation of hydroxyl radicals during the photocatalytic degradation process was detected by photoluminescence probing using terephthalic acid.A mechanism for photocatalysis over the C-Cl-codoped TiO2/ATT composites was proposed.
基金supported by the National Natural Science Foundation of China (21975102, 21871107, 21774042, and 21422401)
文摘It remains challenging to achieve the selective cleavage of C–C bonds in lignin or lignin model compounds to produce aromatic products in high yield and selectivity.We have developed a redox-neutral photocatalytic strategy to accomplish this goal in both b-O-4 and b-1 lignin models at room temperature(RT)via proton-coupled electron transfer(PCET)process without any pretreatments of substrate,by adjusting the alkalinity of base to obtain a lignin models/base PCET pair with a bond dissociation free energy close to 102 kcal/mol.Without breaking down C_b–Ccbond and any C–O bonds,this PCET method is 100%atom economy and produces exclusive Ca–C_bbond cleavage products,such as benzaldehydes(up to 97%)and phenyl ethers(up to 96%),in high to excellent yields and selectivities.Preliminary studies indicated that the PCET strategy is also effective for the depolymerization of native lignin at RT,thus providing significantly important foundation to the depolymerization of lignin.
基金supported by the National Natural Science Foundation of China(Nos.11975060,12005026,and 12075038)the Fund of Robot Technology Used for Special Environment Key Laboratory of Sichuan Province(No.19kftk02)。
文摘In radiation measurement and digital nuclear spectrum systems,traditional nuclear signal processing circuits in nuclear electronics have been gradually replaced by digital algorithm modules with the application of highperformance programmable hardware logic devices(such as FPGA or DSP).Referring to the digital realization method of inverse RC integral circuit systems,the function of the pole-zero cancellation(PZC)circuit was analyzed,a new modified cascade equivalent model of PZC was established,and the time-domain digital PZC(DPZC)recursive algorithm was derived in detail in this study.Two parameters kIand k_(D)are included in the new algorithm,where kIshould match the exponential decay time constant of the input signal to realize the pole-zero compensation,while the decay time constant of the output signal can be changed with the adjustable parameter k_(D)(which is larger than the decay time constant of the input signal).Based on the new DPZC algorithm module,two trapezoidal(triangular)shaping filters were designed and implemented.The amplitude–frequency characteristics of the output signal of the proposed trapezoidal shaping algorithm and the convolution trapezoidal shaping algorithm were compared,with fixed peaking time.The results show that the trapezoidal shaping algorithm based on DPZC can better suppress high-frequency noise.Finally,based on the Na I(Tl)scintillator(u75 mm×75 mm)detector and^(137)Cs source,the effect of the k_(D)value on the energy resolution of the DPZC trapezoidal(triangular)shaping algorithm was studied.The experimental results show that,with an increase in k_(D),the energy resolution of the system improved and reached the maximum when k_(D)was greater than 10,and the optimal energy resolution of the system was 7.72%.
文摘Cu-based catalysts are the most promising candidates for electrochemical CO_(2)reduction(CO_(2)RR)to multi-carbon(C_(2))products.Optimizing the C-C coupling process,the rate-determining step for C_(2)product generation,is an important strategy to improve the production and selectivity of the C_(2)products.In this study,we determined that the local electric field can promote the C-C coupling reaction and enhance CO_(2)electroreduction to C_(2)products.First,finite-element simulations indicated that the high curvature of the Cu nanoneedles results in a large local electric field on their tips.Density functional theory(DFT)calculations proved that a large electric field can promote C-C coupling.Motivated by this prediction,we prepared a series of Cu catalysts with different curvatures.The Cu nanoneedles(NNs)exhibited the largest number of curvatures,followed by the Cu nanorods(NRs),and Cu nanoparticles(NPs).The Cu NNs contained the highest concentration of adsorbed K+,which resulted in the highest local electric field on the needles.CO adsorption sensor tests indicated that the Cu NNs exhibited the strongest CO adsorption ability,and in-situ Fourier-transform infrared spectroscopy(FTIR)showed the strongest*COCO and*CO signals for the Cu NNs.These experimental results demonstrate that high-curvature nanoneedles can induce a large local electric field,thus promoting C-C coupling.As a result,the Cu NNs show a maximum FEC_(2)of 44%for CO_(2)RR at a low potential(-0.6 V vs.RHE),which is approximately 2.2 times that of the Cu NPs.This work provides an effective strategy for enhancing the production of multi-carbon products during CO_(2)RR.
文摘Current bio-ethanol production entails the enzymatic depolymerization of cellulose,but this process shows low efficiency and poor economy.In this work,we developed a consecutive aqueous hydrogenolysis process for the conversion of corn-stalk cellulose to produce a relatively high concentration of bio-ethanol(6.1 wt%)without humin formation.A high yield of cellulose(ca.50 wt%)is extracted from corn stalk using a green solvent(80 wt%1,4-butanediol)without destroying the structure of the lignin.The first hydrothermal hydrogenolysis step uses a Ni–WO_(x)/SiO_(2)catalyst to convert the high cumulative concentration of cellulose(30 wt%)into a polyol mixture with a 56.5 C%yield of ethylene glycol(EG).The original polyol mixture is then subjected to subsequent selective aqueous-phase hydrogenolysis of the C–O bond to produce bioethanol(75%conversion,84 C%selectivity)over the modified hydrothermally stable Cu catalysts.The added Ni component favors the good dispersion of Cu nanoparticles,and the incorporated Au3+helps to stabilize the active Cu^(0)-Cu^(+)species.This multi-functional catalytic process provides an economically competitive route for the production of cellulosic ethanol from raw lignocellulose.
基金financially supported by the National Natural Science Foundation of China(Nos.51221001 and 51272213)the Author of National Excellent Doctoral Dissertation of China(No.201036),the ‘‘111’’ project of China (No.B08040)National Basic Research program of China (No.2011CB605806)
文摘C/C–SiC–HfC composites were fabricated via precursor infiltration and pyrolysis using a mixture solution of organic hafnium-containing polymer and polycarbosilane as precursor. The microstructures and the phases of the composites were analyzed by scanning electron microscopy and X-ray diffraction. The ablation resistance of the composites was evaluated under 3,000 °C oxyacetylene torch. After ablation for 120 s, the composites exhibit good ablation properties with the linear and mass ablation rates of 9.1 9 10-4mm/s and 1.30 9 10-3g/s, which are far lower than those of the C/C–SiC composites. The excellent ablative property of the C/C–SiC–HfC composites is resulted from the formation of HfO2 molten layer on the surface of the composites, which could play a positive role in reducing heat transfer and preventing oxygen transport to the underlying carbon substrate.
