tWe proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcina-tion method at the temperatures of 850-1000°C,which were used for CO_(2) electrochemical reduction to CO.The p...tWe proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcina-tion method at the temperatures of 850-1000°C,which were used for CO_(2) electrochemical reduction to CO.The porous carbon was prepared by carbonizing cheap and abundant humic acid.The structural characterizations of the as-synthesized catalysts and their electrocatalytic performances were analyzed.The results showed that the single-Ni-atom catalyst activated at 950°C showed an optimum catalytic performance,and it reached a CO Faradaic efficiency of 91.9% with a CO partial current density of 6.9 mAcm^(-2)at-0.9 V vs.reversible hydrogen electrode(RHE).Additionally,the CO Faradaic efficiency and current density of the optimum catalyst changed slightly after 8 h of continuous operation,suggesting that it possessed an excellent stability.The structure-activity relations indicate that the variation in the CO_(2) electroche-mical reduction performance for the as-synthesized catalysts is ascribed to the combined effects of the increase in the content of pyrrolic N,the evaporation of Ni and N,the decrease in pore volume,and the change in graphitization degree.展开更多
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.22308006 and 22278001)the Anhui Province Major Industrial Innovation Plan(Grant No.AHZDCYCXLSDT2023-04)+3 种基金the University Synergy Innovation Program of Anhui Province(Grant No.GXXT-2022-006)the Natural Science Foundation of Anhui Provincial Education Department(Grant No.KJ2021A0407)the Youth Natural Science Foundation of Anhui University of Technology(GrantNt o.QZ202216)UndergraduateInnovation and Entrepreneurship Training Program of Anhui Province(Grant No.S202310360214).
文摘tWe proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcina-tion method at the temperatures of 850-1000°C,which were used for CO_(2) electrochemical reduction to CO.The porous carbon was prepared by carbonizing cheap and abundant humic acid.The structural characterizations of the as-synthesized catalysts and their electrocatalytic performances were analyzed.The results showed that the single-Ni-atom catalyst activated at 950°C showed an optimum catalytic performance,and it reached a CO Faradaic efficiency of 91.9% with a CO partial current density of 6.9 mAcm^(-2)at-0.9 V vs.reversible hydrogen electrode(RHE).Additionally,the CO Faradaic efficiency and current density of the optimum catalyst changed slightly after 8 h of continuous operation,suggesting that it possessed an excellent stability.The structure-activity relations indicate that the variation in the CO_(2) electroche-mical reduction performance for the as-synthesized catalysts is ascribed to the combined effects of the increase in the content of pyrrolic N,the evaporation of Ni and N,the decrease in pore volume,and the change in graphitization degree.
