甲烷化
选择性
催化作用
活动中心
钴
水煤气变换反应
化学
光化学
无机化学
有机化学
作者
Shuangxi Lin,Qiang Wang,Maoshuai Li,Ziwen Hao,Yutong Pan,Xiaoyu Han,Xuefeng Chang,Shouying Huang,Zhenhua Li,Xinbin Ma
标识
DOI:10.1021/acscatal.1c05582
摘要
Controlling the selectivity of CO2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO2 hydrogenation. The alloying of Ni with Zn to charged (Niσ––Znσ+) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H2, and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO2 species in a η2(C, O) bridge configuration, directly dissociate the C═O bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.
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