Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous ...The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous N-doped carb on frameworks with tun able configurati ons and contents of N dopants,by using a secondary doping process via the treatment of N,N-dimethylformamide(DMF)solvent.The obtained mesoporous N-doped carbon(denoted as MNC-D)served as an efficient electrocatalyst for electroreduction of CO2 to CO.A high Faradaic efficiency of^92%and a partial current density for CO of-6.8 mA·cm^-2 were achieved at a potential of-0.58 V vs.RHE.Electrochemical analyses further revealed that the active sites within the N-doped carb on catalysts were the pyridinic N and defects gen erated by the DMF treatme nt,which enhan ced the activati on and adsorpti on CO2 molecules.Our study suggests a new approach to develop efficie nt carb on-based catalysts for potential scalable CO2 reduction reaction(CO2RR)to fuels and chemicals.展开更多
As a promising technology that may solve global environmental challenges and enable intermittent renewable energy storage as well as zero-carbon-emission energy cycling, the carbon dioxide reduction reaction has been ...As a promising technology that may solve global environmental challenges and enable intermittent renewable energy storage as well as zero-carbon-emission energy cycling, the carbon dioxide reduction reaction has been extensively studied in the past several years. Beyond the fruitful progresses and innovations in catalysts, the system engineering-based research on the full carbon dioxide reduction reaction is urgently needed toward the industrial application. In this review, we summarize and discuss recent works on the innovations in the reactor architectures and optimizations based on system engineering in carbon dioxide reduction reaction. Some challenges and future trends in this field are further discussed, especially on the system engineering factors.展开更多
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金We thank the following funding agencies for supporting this work:the National Key Research and Development Program of China(Nos.2017YFA0206901 and 2018YFA0209401)the National Natural Science Foundation of China(No.21773036)+1 种基金the Science and Technology Commission of Shanghai Municipality(Nos.17JC1402000 and 19XD1420400)the Innovation Program of Shanghai Municipal Education Commission(No.2019-01-07-00-07-E00045).
文摘The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous N-doped carb on frameworks with tun able configurati ons and contents of N dopants,by using a secondary doping process via the treatment of N,N-dimethylformamide(DMF)solvent.The obtained mesoporous N-doped carbon(denoted as MNC-D)served as an efficient electrocatalyst for electroreduction of CO2 to CO.A high Faradaic efficiency of^92%and a partial current density for CO of-6.8 mA·cm^-2 were achieved at a potential of-0.58 V vs.RHE.Electrochemical analyses further revealed that the active sites within the N-doped carb on catalysts were the pyridinic N and defects gen erated by the DMF treatme nt,which enhan ced the activati on and adsorpti on CO2 molecules.Our study suggests a new approach to develop efficie nt carb on-based catalysts for potential scalable CO2 reduction reaction(CO2RR)to fuels and chemicals.
基金supported by the National Key Research and Development Program of China (2017YFA0206901,2018YFA0209401)the National Natural Science Foundation of China (21975051,21773036)+2 种基金the Science and Technology Commission of Shanghai Municipality (17JC1402000,19XD1420400)the Innovation Program of Shanghai Municipal Education Commission (2019-01-07-00-07-E00045)the Shanghai Shu-Guang Program (15SG01)
文摘As a promising technology that may solve global environmental challenges and enable intermittent renewable energy storage as well as zero-carbon-emission energy cycling, the carbon dioxide reduction reaction has been extensively studied in the past several years. Beyond the fruitful progresses and innovations in catalysts, the system engineering-based research on the full carbon dioxide reduction reaction is urgently needed toward the industrial application. In this review, we summarize and discuss recent works on the innovations in the reactor architectures and optimizations based on system engineering in carbon dioxide reduction reaction. Some challenges and future trends in this field are further discussed, especially on the system engineering factors.
