杂原子
硫黄
催化作用
化学
碳纤维
钴
无机化学
兴奋剂
电催化剂
光化学
红外光谱学
电化学
材料科学
物理化学
有机化学
电极
复合材料
复合数
光电子学
戒指(化学)
作者
Zhiming Wei,Yuhang Liu,Jie Ding,Qinye He,Qiao Zhang,Yueming Zhai
出处
期刊:Authorea - Authorea
日期:2023-07-18
标识
DOI:10.22541/au.168966885.58328939/v1
摘要
Electrocatalytic reduction of CO2 to fuels and chemicals possesses huge potential to alleviate current environmental crisis. Heteroatom doping in metal-nitrogen-carbon (M-N-C) single-atom catalysts (SACs) has been found capable to promote the electrocatalytic CO2 reduc-tion reaction (CO2RR). However, the origin of the enhanced activity is still elusive. Here, we report that sulfur-doped cobalt-nitrogen-carbon single-atom catalyst (Co1-SNC) exhibits superior CO2RR performance compared to sulfur-free counterpart (Co1-NC). On the basis of in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), kinetic isotope effect (KIE) and theoretical calculation, it is demonstrated that sulfur doping can promote water activation, elevate the d-band center of Co active site, and reduce the free energy of *COOH intermediate formation. This work deepens the understanding of the CO2RR chemistry over heteroatom-doped SACs for designing efficient CO2RR processes.
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