过电位
材料科学
法拉第效率
催化作用
二氧化碳电化学还原
碳纤维
掺杂剂
X射线光电子能谱
石墨烯
选择性
活动站点
化学工程
无机化学
吉布斯自由能
氮气
兴奋剂
纳米技术
物理化学
有机化学
一氧化碳
复合材料
光电子学
电化学
电极
复合数
工程类
化学
物理
量子力学
作者
Song Liu,Hongbin Yang,Xiang Huang,Linghui Liu,Weizheng Cai,Jiajian Gao,Xuning Li,Tao Zhang,Yanqiang Huang,Bin Liu
标识
DOI:10.1002/adfm.201800499
摘要
Abstract Nitrogen‐doped carbon materials are proposed as promising electrocatalysts for the carbon dioxide reduction reaction (CRR), which is essential for renewable energy conversion and environmental remediation. Unfortunately, the unclear cognition on the CRR active site (or sites) hinders further development of high‐performance electrocatalysts. Herein, a series of 3D nitrogen‐doped graphene nanoribbon networks (N‐GRW) with tunable nitrogen dopants are designed to unravel the site‐dependent CRR activity/selectivity. The N‐GRW catalyst exhibits superior CO 2 electrochemical reduction activity, reaching a specific current of 15.4 A g catalyst −1 with CO Faradaic efficiency of 87.6% at a mild overpotential of 0.49 V. Based on X‐ray photoelectron spectroscopy measurements, it is experimentally demonstrated that the pyridinic N site in N‐GRW serves as the active site for CRR. In addition, the Gibbs free energy calculated by density functional theory further illustrates the pyridinic N as a more favorable site for the CO 2 adsorption, *COOH formation, and *CO removal in CO 2 reduction.
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