%0 Journal Article
%T C<sub>2</sub>N负载的过渡金属三聚体催化剂用于CO<sub>2</sub>电催化还原制CH<sub>4</sub>：第一性原理研究<br>Transition Metals Trimers on C<sub>2</sub>N as Electrochemical Catalysts for CO<sub>2</sub> Reduction to CH<sub>4</sub>: A First-Principles Study
%A 佟立凯
%A 张钰
%A 张博
%J Hans Journal of Nanotechnology
%P 330-339
%@ 2161-0878
%D 2022
%I Hans Publishing
%R 10.12677/NAT.2022.124033
%X 三原子催化剂(TACs)在二氧化碳还原反应(CO<sub>2</sub>RR)中展现了巨大潜力，设计新型三原子催化剂具有重要意义。本工作利用第一性原理，建立了单层多孔氮化石墨烯(C<sub>2</sub>N)负载的过渡金属三聚体(3TM-C<sub>2</sub>N, TM = Mn, Mo, Ru, Ti)催化剂用于将二氧化碳(CO<sub>2</sub>)还原为甲烷(CH<sub>4</sub>)。计算结果表明，3TM-C<sub>2</sub>N催化剂结构稳定，不但能有效吸附和活化CO<sub>2</sub>，而且对析氢反应(HER)有良好的抑制性。吉布斯自由能分布图显示，CO<sub>2</sub>RR在3TM-C<sub>2</sub>N上会以不同的反应路径生成CH<sub>4</sub>。极限电势(UL)分析显示，3Mn-C<sub>2</sub>N表现出了最好的催化性能，对应的U<sub>L</sub>为？0.44 V。这些发现不仅为实验上调控C<sub>2</sub>N基催化剂提供了理论依据，还对开发其他高效的CO<sub>2</sub>RR电催化剂有一定的指导意义。<br />
Triple-Atom Catalysts (TACs) have shown great potential in carbon dioxide reduction reactions (CO<sub>2</sub>RR). It is of great significance to design new Triple-Atom Catalysts. In this work, a monolayer porous nitrogen-doped graphene (C<sub>2</sub>N) supported transition metal trimers (3TM-C<sub>2</sub>N, TM = Mn, Mo, Ru, Ti) catalyst models were established to catalyze the reduction of carbon dioxide (CO<sub>2</sub>) to me-thane (CH<sub>4</sub>) using first-principles. The results show that the structure of the 3TM-C<sub>2</sub>N catalyst is stable, not only can effectively adsorb and activate CO<sub>2</sub>, but also has good inhibition of Hydrogen Evolution Reaction (HER). The Gibbs free energy profiles show that the CO<sub>2</sub>RR produces CH<sub>4</sub> products in different reaction paths on 3TM-C<sub>2</sub>N. The limiting potential (U<sub>L</sub>) analysis showed that 3Mn-C<sub>2</sub>N ex-hibited the best catalytic performance, UL of ？0.44 V. These findings not only provide a theoretical basis for the experimental regulation of C<sub>2</sub>N-based catalysts, but also provide guidance for the development of other efficient CO<sub>2</sub>RR electrocatalysts.
%K C2N，三原子催化剂，二氧化碳还原反应，CH<sub>4</sub>，第一性原理<br>C<sub>2</sub>N
%K Triple-Atom Catalyst
%K Carbon Dioxide Reduction
%K CH<sub>4</sub>
%K First-Principles
%U http://www.hanspub.org/journal/PaperInformation.aspx?PaperID=57815