化学
石墨烯
催化作用
电催化剂
电化学
异质结
密度泛函理论
过渡金属
电子转移
氧化还原
化学物理
无机化学
纳米技术
物理化学
计算化学
电极
材料科学
生物化学
光电子学
作者
Yun Yang,Zhijun Yang,Canyu Zhang,Jiao Zhou,Shixi Liu,Qiue Cao
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2022-07-21
卷期号:61 (30): 12012-12022
被引量:14
标识
DOI:10.1021/acs.inorgchem.2c02020
摘要
Electrochemical reduction of CO2 to high-energy chemicals is a promising strategy for achieving carbon-neutral energy circulation. However, designing high-performance electrocatalysts for the CO2 reduction reaction (CO2RR) remains a great challenge. In this work, by means of density functional theory calculations, we systematically investigate the transition metal (TM) anchored on the nitrogen-doped graphene/graphdiyne heterostructure (TM-N4@GRA/GDY) as a single-atom catalyst for CO2 electroreduction applications. The computational results show that Co-N4@GRA/GDY exhibits remarkable activity with a low limiting potential of -0.567 V for the reduction of CO2 to CH4. When the charged Co-N4@GRA/GDY system is immersed in a continuum solvent, the reaction barrier decreases to 0.366 eV, which is ascribed to stronger electron transfer between GDY and transition metal atoms in the GRA/GDY heterostructure. In addition, the GRA/GDY heterostructure system significantly weakens the linear scaling relationship between the adsorption free energy of key CO2 reduction intermediates, which leads to a catalytic activity that is higher than that of the single-GRA system and thus greatly accelerates the CO2RR. The electronic structure analysis reveals that the appropriate d-π interaction will affect the d orbital electron distribution, which is directly relevant to the selectivity and activity of catalysis. We hope these computational results not only provide a potential electrocatalyst candidate but also open up an avenue for improving the catalytic performance for efficient electrochemical CO2RR.
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