Conventional chemical oxidation of aldehydes such as furfural to corresponding acids by molecular oxygen usually needs high pressure to increase the solubility of oxygen in aqueous phase,while electrochemical oxidatio...Conventional chemical oxidation of aldehydes such as furfural to corresponding acids by molecular oxygen usually needs high pressure to increase the solubility of oxygen in aqueous phase,while electrochemical oxidation needs input of external electric energy.Herein,we developed a liquid flow fuel cell(LFFC)system to achieve oxidation of furfural in anode for furoic acid production with co-production of hydrogen gas.By controlling the electron transfer in cathode for reduction of oxygen,efficient generation of electricity or production of H_(2)O_(2)were achieved.Metal oxides especially Ag_(2)O have been screened as the efficient catalyst to promote the oxidation of aldehydes,while liquid redox couples were used for promoting the kinetics of oxygen reduction.A novel alkaline-acidic asymmetric design was also used for anolyte and catholyte,respectively,to promote the efficiency of electron transfer.Such an LFFC system achieves efficient conversion of chemical energy of aldehyde oxidation to electric energy and makes full use the transferred electrons for high-value added products without input of external energy.With(VO_(2))_(2)SO_(4)as the electron carrier in catholyte for four-electron reduction of oxygen,the peak output power density(Pmax)at room temperature reached 261 mW/cm^(2)with furoic acid and H_(2)yields of 90%and 0.10 mol/mol furfural,respectively.With anthraquinone-2-sulfonate(AQS)as the cathodic electron carrier,Pmaxof 60 mW/cm^(2)and furoic acid,H_(2)and H_(2)O_(2)yields of 0.88,0.15 and 0.41 mol/mol furfural were achieved,respectively.A new reaction mechanism on furfural oxidation on Ag_(2)O anode was proposed,referring to one-electron and two-electron reaction pathways depending on the fate of adsorbed hydrogen atom transferred from furfural aldehyde group.展开更多
The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-ba...The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.展开更多
The biotransformation of food waste(FW)to bioenergy has attracted considerable research attention as a means to address the energy crisis and waste disposal problems.To this end,a promising technique is two-stage anae...The biotransformation of food waste(FW)to bioenergy has attracted considerable research attention as a means to address the energy crisis and waste disposal problems.To this end,a promising technique is two-stage anaerobic digestion(TSAD),in which the FW is transformed to biohythane,a gaseous mixture of biomethane and biohydrogen.This review summarises the main characteristics of FW and describes the basic principle of TSAD.Moreover,the factors influencing the TSAD performance are identified,and an overview of the research status;economic aspects;and strategies such as pre-treatment,co-digestion,and regulation of microbial consortia to increase the biohythane yield from TSAD is provided.Additionally,the challenges and future considerations associated with the treatment of FW by TSAD are highlighted.This paper can provide valuable reference for the improvement and widespread implementation of TSAD-based FW treatment.展开更多
Achieving a high carrier migration efficiency by constructing built-in electric field is one of the promising approaches for promoting photocatalytic activity. Herein, we have designed a donor-acceptor(D-A) crystallin...Achieving a high carrier migration efficiency by constructing built-in electric field is one of the promising approaches for promoting photocatalytic activity. Herein, we have designed a donor-acceptor(D-A) crystalline carbon nitride(APMCN) with 4-amino-2,6-dihydroxypyrimidine(AP) as electron donor, in which the pyrimidine ring was well embedded in the heptazine ring via hydrogen-bonding effect during hydrothermal process. The APMCN shows superior charge-transfer due to giant built-in electric field(5.94times higher than pristine carbon nitride), thereby exhibiting excellent photocatalytic H_(2) evolution rate(1350 μmol/h) with a high AQY(62.8%) at 400 nm. Mechanistic analysis based on detailed experimental investigation together with theoretical analysis reveals that the excellent photocatalytic activity is attributed to the promoted charge separation by the giant internal electric field originated from the D–A structure.展开更多
Electric discharge has been carried out in LPG using DC high voltage (0.4 - 3 KV) at gas pressure in the range of 1 to 25 torr. The electric and spectroscopic characteristics of the discharge were studied at different...Electric discharge has been carried out in LPG using DC high voltage (0.4 - 3 KV) at gas pressure in the range of 1 to 25 torr. The electric and spectroscopic characteristics of the discharge were studied at different discharge conditions. Deviations from Paschen’s law were observed as a result of the change of the distance between the two the electrodes. Two discharge modes, namely glow discharge and spark discharge modes, has been observed in the discharge current waveforms. The discharge current waveforms indicate a repetitive pulsed behaviour with frequencies of 5 kHz to 5 MHz depending upon the applied voltage and the gas pressure. The emitted spectra from the discharge are also studied near both the cathode and the anode using different electrode materials. Hα line and C2 Swan band system are observed, which confirms the conversion of LPG to hydrogen and carbon clusters.展开更多
为应对当前全球能源危机,提出一种氢能证书交易体系架构以期鼓励对新型清洁能源氢能的应用。该氢证体系建立在碳权交易体系上,将氢能在制备与储运过程中减少1 t CO_(2)排放量的凭证记为1本氢证,氢证价值等价于在碳交易市场中1 t CO_(2)...为应对当前全球能源危机,提出一种氢能证书交易体系架构以期鼓励对新型清洁能源氢能的应用。该氢证体系建立在碳权交易体系上,将氢能在制备与储运过程中减少1 t CO_(2)排放量的凭证记为1本氢证,氢证价值等价于在碳交易市场中1 t CO_(2)排放额的价值,同时该氢证还体现对氢能源生产、储存、运输和应用等领域氢能源技术和应用的专业能力认证。氢证的交易是一次性的,可以直接在氢证市场以拍卖形式或在交易所对氢证进行出售;或是可流入碳交易市场进行交易,氢证与碳交易市场的CO_(2)排放配额具有相同效力,购得1本氢证可获得1 t CO_(2)排放配额。在氢证交易体系下优化风电辅以电网功率制氢加氢一体站运行,达到系统收益最大化。算例结果表明在氢能生命周期评估中考虑碳排放,通过使用氢能证书可以为氢能源在碳交易市场中的参与提供支持和便利。该氢证交易体系具有可行性,通过对氢能产业的经济激励,促进氢能生态链发展以及可再生能源消纳,缓解未来碳市场所面临的由配额紧缩带来的清缴碳排放额压力,为其在电制氢领域的应用提供理论参考。展开更多
基金supported by the National Natural Science Foundation of China(No.2187817622178197)。
文摘Conventional chemical oxidation of aldehydes such as furfural to corresponding acids by molecular oxygen usually needs high pressure to increase the solubility of oxygen in aqueous phase,while electrochemical oxidation needs input of external electric energy.Herein,we developed a liquid flow fuel cell(LFFC)system to achieve oxidation of furfural in anode for furoic acid production with co-production of hydrogen gas.By controlling the electron transfer in cathode for reduction of oxygen,efficient generation of electricity or production of H_(2)O_(2)were achieved.Metal oxides especially Ag_(2)O have been screened as the efficient catalyst to promote the oxidation of aldehydes,while liquid redox couples were used for promoting the kinetics of oxygen reduction.A novel alkaline-acidic asymmetric design was also used for anolyte and catholyte,respectively,to promote the efficiency of electron transfer.Such an LFFC system achieves efficient conversion of chemical energy of aldehyde oxidation to electric energy and makes full use the transferred electrons for high-value added products without input of external energy.With(VO_(2))_(2)SO_(4)as the electron carrier in catholyte for four-electron reduction of oxygen,the peak output power density(Pmax)at room temperature reached 261 mW/cm^(2)with furoic acid and H_(2)yields of 90%and 0.10 mol/mol furfural,respectively.With anthraquinone-2-sulfonate(AQS)as the cathodic electron carrier,Pmaxof 60 mW/cm^(2)and furoic acid,H_(2)and H_(2)O_(2)yields of 0.88,0.15 and 0.41 mol/mol furfural were achieved,respectively.A new reaction mechanism on furfural oxidation on Ag_(2)O anode was proposed,referring to one-electron and two-electron reaction pathways depending on the fate of adsorbed hydrogen atom transferred from furfural aldehyde group.
基金the Natural Science research project of Universities in Anhui Province(No.KJ2021ZD0001)the Natural Science Foundation of Anhui Province(No.2208085MB20)the National Natural Science Foundation of China(No.22101001).
文摘The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.
基金supported by the National Natural Science Foundation of China(Nos.51978498 and 52131002)the National Key R&D Program of China(No.2019YFC1906301)。
文摘The biotransformation of food waste(FW)to bioenergy has attracted considerable research attention as a means to address the energy crisis and waste disposal problems.To this end,a promising technique is two-stage anaerobic digestion(TSAD),in which the FW is transformed to biohythane,a gaseous mixture of biomethane and biohydrogen.This review summarises the main characteristics of FW and describes the basic principle of TSAD.Moreover,the factors influencing the TSAD performance are identified,and an overview of the research status;economic aspects;and strategies such as pre-treatment,co-digestion,and regulation of microbial consortia to increase the biohythane yield from TSAD is provided.Additionally,the challenges and future considerations associated with the treatment of FW by TSAD are highlighted.This paper can provide valuable reference for the improvement and widespread implementation of TSAD-based FW treatment.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China (No.51888103)the National Natural Science Foundation of China (Nos.52376209 and 52172248)+1 种基金China Postdoctoral Science Foundation (Nos.2020M673386 and 2020T130503)China Fundamental Research Funds for the Central Universities。
文摘Achieving a high carrier migration efficiency by constructing built-in electric field is one of the promising approaches for promoting photocatalytic activity. Herein, we have designed a donor-acceptor(D-A) crystalline carbon nitride(APMCN) with 4-amino-2,6-dihydroxypyrimidine(AP) as electron donor, in which the pyrimidine ring was well embedded in the heptazine ring via hydrogen-bonding effect during hydrothermal process. The APMCN shows superior charge-transfer due to giant built-in electric field(5.94times higher than pristine carbon nitride), thereby exhibiting excellent photocatalytic H_(2) evolution rate(1350 μmol/h) with a high AQY(62.8%) at 400 nm. Mechanistic analysis based on detailed experimental investigation together with theoretical analysis reveals that the excellent photocatalytic activity is attributed to the promoted charge separation by the giant internal electric field originated from the D–A structure.
文摘Electric discharge has been carried out in LPG using DC high voltage (0.4 - 3 KV) at gas pressure in the range of 1 to 25 torr. The electric and spectroscopic characteristics of the discharge were studied at different discharge conditions. Deviations from Paschen’s law were observed as a result of the change of the distance between the two the electrodes. Two discharge modes, namely glow discharge and spark discharge modes, has been observed in the discharge current waveforms. The discharge current waveforms indicate a repetitive pulsed behaviour with frequencies of 5 kHz to 5 MHz depending upon the applied voltage and the gas pressure. The emitted spectra from the discharge are also studied near both the cathode and the anode using different electrode materials. Hα line and C2 Swan band system are observed, which confirms the conversion of LPG to hydrogen and carbon clusters.
文摘为应对当前全球能源危机,提出一种氢能证书交易体系架构以期鼓励对新型清洁能源氢能的应用。该氢证体系建立在碳权交易体系上,将氢能在制备与储运过程中减少1 t CO_(2)排放量的凭证记为1本氢证,氢证价值等价于在碳交易市场中1 t CO_(2)排放额的价值,同时该氢证还体现对氢能源生产、储存、运输和应用等领域氢能源技术和应用的专业能力认证。氢证的交易是一次性的,可以直接在氢证市场以拍卖形式或在交易所对氢证进行出售;或是可流入碳交易市场进行交易,氢证与碳交易市场的CO_(2)排放配额具有相同效力,购得1本氢证可获得1 t CO_(2)排放配额。在氢证交易体系下优化风电辅以电网功率制氢加氢一体站运行,达到系统收益最大化。算例结果表明在氢能生命周期评估中考虑碳排放,通过使用氢能证书可以为氢能源在碳交易市场中的参与提供支持和便利。该氢证交易体系具有可行性,通过对氢能产业的经济激励,促进氢能生态链发展以及可再生能源消纳,缓解未来碳市场所面临的由配额紧缩带来的清缴碳排放额压力,为其在电制氢领域的应用提供理论参考。
