The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity...The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.展开更多
Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble m...Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble metal‐based hybrid catalyst which consists of binary FeNi alloy/nitride nanocrystals with graphitic‐shell and biomass‐derived N‐doped carbon(NC)(FexNiyN@C/NC).This novel nanostructure exhibits superior performance for ORR/OER,which can be attributed to the strong interactions between the graphitic‐shell encapsulated FeNi alloy/nitride nanocrystals and the N‐doped porous carbon substrate.The X‐ray absorption spectroscopy technique was employed to reveal the underlying mechanisms for the excellent performance.The assembled Zn‐air battery device exhibits outstanding charging/discharging performance and cycling stability,indicating the great potential of this type of novel catalysts.展开更多
基金This work is supported financially by the Natural Sciences and Engineering Research Council of Canada(NSERC),the Fonds de Recherche du Québec-Nature et Technologies(FRQNT)Centre Québécois sur les Materiaux Fonctionnels(CQMF),the Canada Foundation for Innovation(CFI)+1 种基金Institut National de la Recherche Scientifique(INRS).The XAS characterizations were performed at the Canadian Light Source(CLS),which is financially supported by NSERC,CFIthe University of Saskatchewan,the Government of Saskatchewan,Western Economic Diversification Canada,the National Research Council of Canada,and the Canadian Institutes of Health Research。
文摘The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.
基金This study was supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)the National Natural Science Foundation of China(21972017)+2 种基金Canada Foundation for Innovation(CFI)Centre Québécois sur les Materiaux Fonctionnels,Fondsde Recherche du Québec‐Nature et TechnologiesInstitut National de la Recherche Scientifique.Mingjie Wu gratefully acknowledges the scholarships from the China Scholarship Council.
文摘Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble metal‐based hybrid catalyst which consists of binary FeNi alloy/nitride nanocrystals with graphitic‐shell and biomass‐derived N‐doped carbon(NC)(FexNiyN@C/NC).This novel nanostructure exhibits superior performance for ORR/OER,which can be attributed to the strong interactions between the graphitic‐shell encapsulated FeNi alloy/nitride nanocrystals and the N‐doped porous carbon substrate.The X‐ray absorption spectroscopy technique was employed to reveal the underlying mechanisms for the excellent performance.The assembled Zn‐air battery device exhibits outstanding charging/discharging performance and cycling stability,indicating the great potential of this type of novel catalysts.
