材料科学
电催化剂
法拉第效率
催化作用
Atom(片上系统)
密度泛函理论
吸附
氧气
氧化还原
氧原子
金属
纳米技术
化学工程
物理化学
电化学
电极
计算化学
分子
化学
冶金
嵌入式系统
工程类
生物化学
有机化学
计算机科学
作者
Yubo Liang,Cailing Wu,Songjie Meng,Zhansheng Lu,Runyao Zhao,Huiyong Wang,Zhimin Liu,Jianji Wang
标识
DOI:10.1021/acsami.3c04556
摘要
Ag single-atom catalysts (SACs) have great potential in selective electrocatalysis of the CO2 reduction reaction (CO2RR) to CO, while it is still a challenge to achieve high current density and high atom efficiency simultaneously. Here, we present a new and simple in situ adsorption-reduction method to prepare Ag SACs supported on CeO2 (Ag1/CeO2). It is found that Ag single atoms are anchored on CeO2 through strong metal-support interaction (SMSI), and each Ag atom is accompanied with three interfacial oxygen vacancies. This Ag1/CeO2 exhibits high performance in the electrocatalytic CO2RR with a high CO faradaic efficiency (FE) of >95% under a wide potential range. The turnover frequency (TOF) value can reach 50,310 h-1 at FECO = 99.5% in H-cells. Notably, Ag1/CeO2 achieves an industrial-grade current density of 403 mA cm-2 with a high FECO of 97.2% in flow cells. Experimental results combined with density functional theory calculation revealed that this superior performance was mainly ascribed to the existence of interfacial oxygen vacancies, which lead to the formation of Ag-O-Ce3+ atomic interfaces, and activates the Ce3+-O structures as the synergistic active center of Ag, thus promoting CO2 adsorption and activation and reducing the reaction potential barrier of *COOH-to-*CO.
科研通智能强力驱动
Strongly Powered by AbleSci AI