过渡金属
催化作用
限制
石墨烯
选择性
化学
Atom(片上系统)
电化学
金属
材料科学
纳米技术
化学物理
物理化学
电极
计算机科学
机械工程
有机化学
工程类
嵌入式系统
生物化学
作者
Xiting Wang,Huan Niu,Xuhao Wan,Jun Wang,Chunguang Kuai,Zhaofu Zhang,Yuzheng Guo
标识
DOI:10.1016/j.apsusc.2022.152470
摘要
Electrochemical CO2 reduction reaction (CO2RR) to generate CH4 is more desirable than CO. Herein, we investigate the potential of CO2-to-CH4 conversion on the representative single-atom catalysts (SACs), single transition metal atom with four coordinated nitrogen atoms embedded in graphene (TM-N4) by first-principle calculations. Interestingly, the CH4 product can be formed more favorably on TM-N4 through the key intermediate of *HCOOH instead of the traditional *CO. Among all TM-N4 candidates, Mn-, Fe-, and Ru-N4 stand out with the low limiting potentials of −0.31, −0.42, and −0.30 V, respectively. The analysis of electronic structures and charge variation shed light on the CO2RR activity origin. Moreover, it is suggested that Mn-N4 and Ru-N4 possess high CH4 selectivity owing to the suppressed hydrogen evolution reaction (HER), while the dominant HER prohibits the CH4 formation on Fe-N4. This work will provide more insights into the underlying mechanism of CO2RR and promote the explorations of TM-N4 for CO2-to-CH4 conversion.
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