Identifying Active Sites of Nitrogen‐Doped Carbon Materials for the CO2 Reduction Reaction,Advanced Functional Materials

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Identifying Active Sites of Nitrogen‐Doped Carbon Materials for the CO2 Reduction Reaction
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2018-04-14 , DOI: 10.1002/adfm.201800499
Song Liu _{1,

2,

3} , Hongbin Yang ₃ , Xiang Huang ₃ , Linghui Liu _{1,

4} , Weizheng Cai ₃ , Jiajian Gao ₃ , Xuning Li ₃ , Tao Zhang ₁ , Yanqiang Huang ₁ , Bin Liu ₃

Affiliation

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 CO₂ 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 CO₂ adsorption, *COOH formation, and *CO removal in CO₂ reduction.

中文翻译：

确定氮掺杂碳材料用于CO2还原反应的活性位点

提出了氮掺杂碳材料作为二氧化碳还原反应（CRR）的有前途的电催化剂，这对于可再生能源转化和环境修复至关重要。不幸的是，对一个或多个CRR活性位点的不清楚认识阻碍了高性能电催化剂的进一步发展。在本文中，设计了一系列带有可调氮掺杂剂的3D氮掺杂石墨烯纳米带网络（N-GRW），以揭示依赖于位点的CRR活性/选择性。N‐GRW催化剂具有出色的CO ₂电化学还原活性，比电流达到15.4 A g_催化剂^-1在0.49 V的轻度过电势下，CO法拉第效率为87.6％。根据X射线光电子能谱测量，实验证明N-GRW中的吡啶N位是CRR的活性位。另外，通过密度泛函理论计算的吉布斯自由能进一步说明了吡啶二氮是更有利于CO ₂吸附，* COOH形成和* CO ₂还原中* CO去除的部位。

更新日期：2018-04-14

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