Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high...Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high bond energy C-H bond(4.57 eV)makes it difficult to realize methane conversion and activation under mild conditions.The photothermal synergetic strategy by combining photon energy and thermo energy provides an advanced philosophy to achieve efficient methane conversion.In this review,we overview the current pioneering studies of photothermal methane indirect conversion and present the methane direct conversion by the way of photocatalysis and thermocatalysis to provide a fundamental understanding of methane activation.Finally,we end this review with a discussion on the remaining challenges and perspectives of methane direct conversion over single-atom catalysts via photothermal synergetic strategy.展开更多
The utilization of fossil fuels has brought unprecedented prosperity and development to human society,but also caused environmental pollution and global warming triggered by excess greenhouse gases emission.For one th...The utilization of fossil fuels has brought unprecedented prosperity and development to human society,but also caused environmental pollution and global warming triggered by excess greenhouse gases emission.For one thing,the excess emission of carbon dioxide(CO_(2)),which has a negative impact on global temperature and ocean acidity,needs to be controlled.For another,the depletion of fossil fuels will eventually force people to seek alternative carbon sources to maintain a sustainable economy.Thus,using renewable energy to convert CO_(2) and biomass into value-added chemicals and fuels is a promising method to overcome urgent problems.The hy-drogenation of CO_(2) is very important to mitigate the greenhouse effect caused by CO_(2),while biomass conversion can produce alternative renewable biofuels and green chemicals.As a kind of promising catalyst,heterogeneous single-atom catalyst(SAC)has received extensive attention in the past decades.SACs combine the advantages of homogeneous catalysts with uniform active sites and heterogeneous catalysts that are easily separable.In this review,we will give a comprehensive overview of the latest progress in CO_(2) selective hydrogenation and biomass conversion via SACs.展开更多
Developing efficient and long wavelength sensitive unimolecular photoinitiators(PIs)is still facing a great challenge.In this work,a series of thioxanthone-based N-hydroxyphthalimide esters(TX-NHPIEs)were synthesized ...Developing efficient and long wavelength sensitive unimolecular photoinitiators(PIs)is still facing a great challenge.In this work,a series of thioxanthone-based N-hydroxyphthalimide esters(TX-NHPIEs)were synthesized by installing NHPIEs along the TX backbone and characterized.The investigated TX-NHPIEs have a 60 nm redshift and demonstrate sterling initiating efficiency for free radical photopolymerization(FRP)under LED@450 nm light irradiation compared with the commercialized isopropylthioxanthone(ITX).Real-time1Hnuclear magnetic resonance(1H NMR),electron spin resonance(ESR),decarboxylation and gas chromatograph-mass spectrometer(GC–MS)experiments and density functional theory(DFT)reveal that TX-NHPIEs can generate one alkyl radical and one N-centered iminyl radical,which can initiate FRP directly and indirectly,respectively.In other words,TX-NHPIEs absorb one photon and can generate two active radicals,which break through the limitations of common PIs.TX-NHPIE-Cpe demonstrates the highest initiating efficiency,and its application in coatings and 3D printing was also studied,indicating TX-NHPIEs have broad potential applications in photopolymerization processes.展开更多
Carbon dots(CDs)with superior fluorescence properties have attracted a growing number of research interests in anti-counterfeiting.However,the preparation of CDs with thermally turn-on fluorescence and full-color-emit...Carbon dots(CDs)with superior fluorescence properties have attracted a growing number of research interests in anti-counterfeiting.However,the preparation of CDs with thermally turn-on fluorescence and full-color-emitting in visible spectrum is still a big challenge due to the complicated reaction mechanism in the formation of CDs.Here,a simple precursor-oriented strategy for the preparation of multicolor CDs with heat-stimuli turn-on fluorescence is reported.Comprehensive experimental characterizations and theoretical calculations revealed that the emission wavelength of CDs can be readily tuned from 460 nm to 654 nm with selected precursors,which was ascribed to the extent of conjugated sp2-domains(core states)and the amount of oxygen-and nitrogen-containing groups bound to sp2-domains(surface states).After simply mixing two or three kinds of CDs,a full-color range of fluorescence emission was realized,and the CDs-based fluorescence inks were successfully fabricated.Particularly,all the printed patterns from the inkjet exhibited a thermal-induced enhancement in fluorescence.On this basis,combining CDs with heating-induced“turn-off”fluorescence materials can lead to multidimensional and multistage encryption.These results demonstrate that the thermochromic and photochromic CDs with much more enhanced security exhibit promising application in data storage and encryption.展开更多
Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing het...Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.展开更多
An efficient photo-Fenton catalyst(Fe S_(2)@HTCN)was designed by maximizing the synergistic effect of Fe S_(2)nanoparticles and hollow tubular g-C_(3)N_(4)(HTCN).Molecule self-assembly and molten salts-assisted calcin...An efficient photo-Fenton catalyst(Fe S_(2)@HTCN)was designed by maximizing the synergistic effect of Fe S_(2)nanoparticles and hollow tubular g-C_(3)N_(4)(HTCN).Molecule self-assembly and molten salts-assisted calcination were used to engineering the hollow structured g-C_(3)N_(4)before anchoring Fe S_(2)nanoparticles on the walls of HTCN via reflux method.Compared to bulk g-C_(3)N_(4),the unique structure of HTCN and heterojunction in the composite endowed FeS_(2)@HTCN with more active sites and abundant channels for electron transfer and charge separation.The enriched electrons can improve the Fe^(3+) recycling and boost Fe^(2+) catalyzed ^(·)OH production via H_(2)O_(2).As-prepared photo-Fenton catalyst was successfully applied to the treatment of industrial paint wastewater.The paint wastewater with its COD as high as 8200 mg/L can be effectively degraded with 0.2 mol/L H_(2)O_(2)in 90 min under visible light irradiation.The photoFenton system was further evaluated according to the process stability and economic benefit,proving that the strategy presented in this work would be applicable to the treatment of real wastewater.展开更多
Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multi...Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multicarbon products is still challenging.Here,we demonstrate that the high‐index crystalline surface of copper could be designed and obtained through a simple square‐wave potential treatment on copper nanowires,which is beneficial to improve the selectivity of multi‐carbon products,especially the reaction route towards ethylene.The Faradaic efficiency of C_(2+)products can reach nearly 60%,and hydrogen can be suppressed to below 20%.Density functional theory(DFT)calculations reveal that(311)high‐index facet can activate CO_(2) effectively and promote adsorption of the*COCOH intermediate on copper for ethylene formation,therefore improves the selectivity of ethylene and inhibits the competing hydrogen evolution reaction.This method can be extended to the design of other catalytic systems and has inspirations for other electrochemical catalytic reactions.展开更多
Microenvironments of the catalytic center,which play a vital role in adjusting electrocatalytic CO_(2) reduction reaction(ECO_(2) RR)activity,have received increasing attention during the past few years.However,contro...Microenvironments of the catalytic center,which play a vital role in adjusting electrocatalytic CO_(2) reduction reaction(ECO_(2) RR)activity,have received increasing attention during the past few years.However,controllable microenvironment construction and the effects of multi-microenvironment variations for improving ECO_(2) RR performance remain unclear.Herein,we summarize the representative strategies for tuning the catalyst and local microenvironments to enhance ECO_(2) RR selectivity and activity.The multifactor synergetic effects of microen-vironment regulation for enhancing CO_(2) accessibility,stabilizing key intermediates,and improving the performance of ECO_(2) RR catalysts are discussed in detail,as well as perspectives on the challenges when investigating ECO_(2) RR microenvironments.We anticipate that the discussions in this review will inspire further research in microenvironment engineering to accelerate the development of the ECO 2 RR for practical application.展开更多
The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable ...The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable low-cost electrocatalysts with high activity,high selectivity,and long-term stability by a facile and simple method.Herein,we construct this scalable Cu-based nanoarray with muti-oxidation states grown directly on nickel foam(NF)substrate(Cu_(2+1)O@Cu/NF)using a facile molten salt method combined in-situ electrochemical reduction.The as-prepared Cu_(2+1)O@Cu/NF nanoarrays reveal a high NH_(3) yield of 20.14 mg h^(−1) cm^(−2) at−0.95 V vs.a reversible hydrogen electrode(vs.RHE),Faradaic efficiency of 99.38%at−0.55 V vs.RHE in the neutral potassium phosphate(PBS)buffer solution with 50 mM NaNO_(3),which is ascribed to its electron redistribution with abundant oxygen vacancies and favorable charge/mass transfer.展开更多
Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto t...Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto the edges of two-dimensional(2D)1Tphase MoS_(2)(Pt1/1T-MOS_(2)SAC)as a proof-of-concept catalyst can efficiently convert biomass-derived MAH to SA with 100%conversion and 100%selectivity under mild conditions.The kinetic data and characterization results suggest that the catalytic performance of the edge-anchored Pt1/1T-MoS_(2)SAC originates from the facile H_(2)dissociation induced by the electron-deficient Pt1atoms and the pocket-like configuration of Pt1active site confines the adsorption configuration of MAH by the steric effect.The strategy of fabricating edge-confined catalysts offers a new direction to design novel SACs for biomass-derived transformations.展开更多
Fishy odor has been a major limiting factor for the production and commercialization of loach.Herein,this study aims to develop an efficient deodorization process using single-factor experiments and Design-Expert resp...Fishy odor has been a major limiting factor for the production and commercialization of loach.Herein,this study aims to develop an efficient deodorization process using single-factor experiments and Design-Expert response surface methodology.The deodorization capability is evaluated using gas chromatography-ion mobility spec-troscopy(GS-IMS).As a result,the trehalose-sweet wine koji method was selected and the final optimal deodorization conditions were shown as follows:the compound ratio of trehalose to sweet wine koji was 51:1,the content of sweet wine koji was 0.10%,and the deodorization time was 33 min at 17℃.Under the conditions,the final trimethylamine content of loach was reduced by 89%.A total of 29 volatile compounds in loach samples before and after deodorization were identified by GC-IMS,including 11 aldehydes,8 alcohol,7 ketones,1 ester,and 2 olefins.Volatile compounds responsible for fish-like odor,such as hexanal,pentanal,heptanal,benzal-dehyde,octanal,nonanal,n-butanol,pentanol,and acetone,were decreased in intensity.Principal component and fingerprint analysis confirmed the deodorization effect of this process on loach was significant(p<0.05).Collectively,the study developed an efficient loach deodorization method,which will improve the quality of loach production.展开更多
基金This project was supported financially by the National Natural Science Foundation of China(21908079,21902009,21707052)Natural Science Foundation of Jiangsu Province(BK20201345)+3 种基金the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF2005)Startup Funding at Jiangnan University(1045210322190170,1045281602190010,1042050205204100)Jiangsu Agriculture Science and Technology Innovation Fund(CX(20)3108)Fundamental Research Funds for the Central Universities(JUSRP11905,JUSRP52004B).
文摘Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high bond energy C-H bond(4.57 eV)makes it difficult to realize methane conversion and activation under mild conditions.The photothermal synergetic strategy by combining photon energy and thermo energy provides an advanced philosophy to achieve efficient methane conversion.In this review,we overview the current pioneering studies of photothermal methane indirect conversion and present the methane direct conversion by the way of photocatalysis and thermocatalysis to provide a fundamental understanding of methane activation.Finally,we end this review with a discussion on the remaining challenges and perspectives of methane direct conversion over single-atom catalysts via photothermal synergetic strategy.
基金supported financially by the National Key R&D Program of China(2021YFB3501900)National Natural Sci-ence Foundation of China(21908079,U21A20326,22202105,22072118,22121001)+3 种基金Jiangsu Specially-Appointed Professor(1046010241211400)Natural Science Foundation of Jiangsu Province(BK20211239,BK20210608)National High-Level Young Talents Program,the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF2005)Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(BK20220023).
文摘The utilization of fossil fuels has brought unprecedented prosperity and development to human society,but also caused environmental pollution and global warming triggered by excess greenhouse gases emission.For one thing,the excess emission of carbon dioxide(CO_(2)),which has a negative impact on global temperature and ocean acidity,needs to be controlled.For another,the depletion of fossil fuels will eventually force people to seek alternative carbon sources to maintain a sustainable economy.Thus,using renewable energy to convert CO_(2) and biomass into value-added chemicals and fuels is a promising method to overcome urgent problems.The hy-drogenation of CO_(2) is very important to mitigate the greenhouse effect caused by CO_(2),while biomass conversion can produce alternative renewable biofuels and green chemicals.As a kind of promising catalyst,heterogeneous single-atom catalyst(SAC)has received extensive attention in the past decades.SACs combine the advantages of homogeneous catalysts with uniform active sites and heterogeneous catalysts that are easily separable.In this review,we will give a comprehensive overview of the latest progress in CO_(2) selective hydrogenation and biomass conversion via SACs.
基金the financial support by the National Natural Science Foundation of China(Nos.22301107,52373057)the Nature Science Foundation of Jiangsu Province(No.BK20200610)+1 种基金the Fundamental Research Funds for the Central Universities(No.JUSRP122021)Jiangsu Province"Innovation and Entrepreneurship Doctor"Talent Plan(No.JSSCBS20221053)also provided support。
文摘Developing efficient and long wavelength sensitive unimolecular photoinitiators(PIs)is still facing a great challenge.In this work,a series of thioxanthone-based N-hydroxyphthalimide esters(TX-NHPIEs)were synthesized by installing NHPIEs along the TX backbone and characterized.The investigated TX-NHPIEs have a 60 nm redshift and demonstrate sterling initiating efficiency for free radical photopolymerization(FRP)under LED@450 nm light irradiation compared with the commercialized isopropylthioxanthone(ITX).Real-time1Hnuclear magnetic resonance(1H NMR),electron spin resonance(ESR),decarboxylation and gas chromatograph-mass spectrometer(GC–MS)experiments and density functional theory(DFT)reveal that TX-NHPIEs can generate one alkyl radical and one N-centered iminyl radical,which can initiate FRP directly and indirectly,respectively.In other words,TX-NHPIEs absorb one photon and can generate two active radicals,which break through the limitations of common PIs.TX-NHPIE-Cpe demonstrates the highest initiating efficiency,and its application in coatings and 3D printing was also studied,indicating TX-NHPIEs have broad potential applications in photopolymerization processes.
基金the Natural National Science Foundation of China (No. 51973083)the Fundamental Research Funds for the Central Universities (No. JUSRP22027)clinical research and translational medicine program of affiliated hospital of Jiangnan University (No. LCYJ202239).
文摘Carbon dots(CDs)with superior fluorescence properties have attracted a growing number of research interests in anti-counterfeiting.However,the preparation of CDs with thermally turn-on fluorescence and full-color-emitting in visible spectrum is still a big challenge due to the complicated reaction mechanism in the formation of CDs.Here,a simple precursor-oriented strategy for the preparation of multicolor CDs with heat-stimuli turn-on fluorescence is reported.Comprehensive experimental characterizations and theoretical calculations revealed that the emission wavelength of CDs can be readily tuned from 460 nm to 654 nm with selected precursors,which was ascribed to the extent of conjugated sp2-domains(core states)and the amount of oxygen-and nitrogen-containing groups bound to sp2-domains(surface states).After simply mixing two or three kinds of CDs,a full-color range of fluorescence emission was realized,and the CDs-based fluorescence inks were successfully fabricated.Particularly,all the printed patterns from the inkjet exhibited a thermal-induced enhancement in fluorescence.On this basis,combining CDs with heating-induced“turn-off”fluorescence materials can lead to multidimensional and multistage encryption.These results demonstrate that the thermochromic and photochromic CDs with much more enhanced security exhibit promising application in data storage and encryption.
基金financially supported by the National Natural Science Foundation of China(No.22305101)the Natural Science Foundation of Jiangsu Province(No.BK20231032)+2 种基金the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(No.BK20220023)the Fundamental Research Funds for the Central Universities(No.JUSRP123020)the Startup Funding at Jiangnan University(No.1045219032220100)。
文摘Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.
基金the Natural National Science Foundation of China(No.51973083)National First-Class Discipline Program of Food Science and Technology(No.JUFSTR20180301)+1 种基金China Postdoctoral Science Foundation(No.2019M651688)Fundamental Research Funds for the Central Universities(No.JUSRP22027)。
文摘An efficient photo-Fenton catalyst(Fe S_(2)@HTCN)was designed by maximizing the synergistic effect of Fe S_(2)nanoparticles and hollow tubular g-C_(3)N_(4)(HTCN).Molecule self-assembly and molten salts-assisted calcination were used to engineering the hollow structured g-C_(3)N_(4)before anchoring Fe S_(2)nanoparticles on the walls of HTCN via reflux method.Compared to bulk g-C_(3)N_(4),the unique structure of HTCN and heterojunction in the composite endowed FeS_(2)@HTCN with more active sites and abundant channels for electron transfer and charge separation.The enriched electrons can improve the Fe^(3+) recycling and boost Fe^(2+) catalyzed ^(·)OH production via H_(2)O_(2).As-prepared photo-Fenton catalyst was successfully applied to the treatment of industrial paint wastewater.The paint wastewater with its COD as high as 8200 mg/L can be effectively degraded with 0.2 mol/L H_(2)O_(2)in 90 min under visible light irradiation.The photoFenton system was further evaluated according to the process stability and economic benefit,proving that the strategy presented in this work would be applicable to the treatment of real wastewater.
基金National Natural Science Foundation of China,Grant/Award Number:21902009National Key Research and Development Project,Grant/Award Numbers:2018YFB1502401,2018YFA0702002+2 种基金Royal Society and the Newton Fund through the Newton Advanced Fellowship Award,Grant/Award Number:NAF\R1\191294Program for Changjiang Scholars and Innovation Research Team in the University,Grant/Award Number:IRT1205Fundamental Research Funds for the Central Universities,and the longterm subsidy mechanism from the Ministry of Finance and the Ministry of Education of PRC。
文摘Electroreduction of carbon dioxide into fuels and feedstocks with renewable energy is an attractive route to mitigate carbon emission and solve energy crisis.However,how to improve the selectivity of high‐value multicarbon products is still challenging.Here,we demonstrate that the high‐index crystalline surface of copper could be designed and obtained through a simple square‐wave potential treatment on copper nanowires,which is beneficial to improve the selectivity of multi‐carbon products,especially the reaction route towards ethylene.The Faradaic efficiency of C_(2+)products can reach nearly 60%,and hydrogen can be suppressed to below 20%.Density functional theory(DFT)calculations reveal that(311)high‐index facet can activate CO_(2) effectively and promote adsorption of the*COCOH intermediate on copper for ethylene formation,therefore improves the selectivity of ethylene and inhibits the competing hydrogen evolution reaction.This method can be extended to the design of other catalytic systems and has inspirations for other electrochemical catalytic reactions.
基金This research was supported by the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(BK20220023)National Natural Science Foun-dation of China(21902009)Startup Funding at Jiangnan University.
文摘Microenvironments of the catalytic center,which play a vital role in adjusting electrocatalytic CO_(2) reduction reaction(ECO_(2) RR)activity,have received increasing attention during the past few years.However,controllable microenvironment construction and the effects of multi-microenvironment variations for improving ECO_(2) RR performance remain unclear.Herein,we summarize the representative strategies for tuning the catalyst and local microenvironments to enhance ECO_(2) RR selectivity and activity.The multifactor synergetic effects of microen-vironment regulation for enhancing CO_(2) accessibility,stabilizing key intermediates,and improving the performance of ECO_(2) RR catalysts are discussed in detail,as well as perspectives on the challenges when investigating ECO_(2) RR microenvironments.We anticipate that the discussions in this review will inspire further research in microenvironment engineering to accelerate the development of the ECO 2 RR for practical application.
基金the National Natural Science Foundation of China(Nos.21975106 and 21403232)MOE&SAFEA,111 Project(B13025)for financial support.
文摘The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable low-cost electrocatalysts with high activity,high selectivity,and long-term stability by a facile and simple method.Herein,we construct this scalable Cu-based nanoarray with muti-oxidation states grown directly on nickel foam(NF)substrate(Cu_(2+1)O@Cu/NF)using a facile molten salt method combined in-situ electrochemical reduction.The as-prepared Cu_(2+1)O@Cu/NF nanoarrays reveal a high NH_(3) yield of 20.14 mg h^(−1) cm^(−2) at−0.95 V vs.a reversible hydrogen electrode(vs.RHE),Faradaic efficiency of 99.38%at−0.55 V vs.RHE in the neutral potassium phosphate(PBS)buffer solution with 50 mM NaNO_(3),which is ascribed to its electron redistribution with abundant oxygen vacancies and favorable charge/mass transfer.
基金financially supported by the National Natural Science Foundation of China(Nos.21908079,21872145 and U21A20326)Jiangsu Specially-Appointed Professor Fund(No.1046010241211400)+4 种基金Natural Science Foundation of Jiangsu Province(Nos.BK20211239,BK20221541 and BK20201345)the State Key Laboratory of Fine ChemicalsDalian University of Technology(No.KF2005)Dalian Institute of Chemical Physics(No.DICP 1201943)the Central Laboratory,School of Chemical and Material Engineering,Jiangnan University。
文摘Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto the edges of two-dimensional(2D)1Tphase MoS_(2)(Pt1/1T-MOS_(2)SAC)as a proof-of-concept catalyst can efficiently convert biomass-derived MAH to SA with 100%conversion and 100%selectivity under mild conditions.The kinetic data and characterization results suggest that the catalytic performance of the edge-anchored Pt1/1T-MoS_(2)SAC originates from the facile H_(2)dissociation induced by the electron-deficient Pt1atoms and the pocket-like configuration of Pt1active site confines the adsorption configuration of MAH by the steric effect.The strategy of fabricating edge-confined catalysts offers a new direction to design novel SACs for biomass-derived transformations.
基金supported by the Freshwater Aquaculture Inno-vative Team Construction Project of Modern Agricultural Industrial Technology System of Hebei Province(HBCT2018180206)the Key Research and Development Plan Project of Hebei Province(21327107D).
文摘Fishy odor has been a major limiting factor for the production and commercialization of loach.Herein,this study aims to develop an efficient deodorization process using single-factor experiments and Design-Expert response surface methodology.The deodorization capability is evaluated using gas chromatography-ion mobility spec-troscopy(GS-IMS).As a result,the trehalose-sweet wine koji method was selected and the final optimal deodorization conditions were shown as follows:the compound ratio of trehalose to sweet wine koji was 51:1,the content of sweet wine koji was 0.10%,and the deodorization time was 33 min at 17℃.Under the conditions,the final trimethylamine content of loach was reduced by 89%.A total of 29 volatile compounds in loach samples before and after deodorization were identified by GC-IMS,including 11 aldehydes,8 alcohol,7 ketones,1 ester,and 2 olefins.Volatile compounds responsible for fish-like odor,such as hexanal,pentanal,heptanal,benzal-dehyde,octanal,nonanal,n-butanol,pentanol,and acetone,were decreased in intensity.Principal component and fingerprint analysis confirmed the deodorization effect of this process on loach was significant(p<0.05).Collectively,the study developed an efficient loach deodorization method,which will improve the quality of loach production.
