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標題:Modification of the Coordination Environment of Active Sites on MoC for High-Efficiency CH4 Production
學年109
學期2
出版(發表)日期2021/04/15
作品名稱Modification of the Coordination Environment of Active Sites on MoC for High-Efficiency CH4 Production
作品名稱(其他語言)
著者Lili Han; Xijun Liu; Jia He; Zhixiu Liang; Hsiao-Tsu Wang; Seong-Min Bak; Jingmin Zhang; Adrian Hunt; Iradwikanari Waluyo; W. F. Pong; Jun Luo; Yi Ding; Radoslav R. Adzic; Huolin L. Xin
單位
出版者
著錄名稱、卷期、頁數Advanced Energy Materials 11(24), 2100044
摘要Modulating the coordination environment of active sites on catalyst surfaces is crucial to developing effective catalysts and controlling catalysis. However, this may be a highly challenging procedure. Guided by the first-principles calculations, the modification of the coordination environment of active sites on MoC nanoparticle surfaces is experimentally accomplished by anchoring pyridinic N atom rings of holey graphene on Mo atoms. The rings produce electrostatic forces that enable the tuning of the Mo sites′ affinity to reaction intermediates, which passivates Mo hollow sites, activates Mo top sites, and reduces the overadsorption of OH on the Mo active sites, as predicted by calculations. The atomic-level modification is well confirmed by atomic-resolution imaging, high-resolution electron tomography, synchrotron soft X-ray spectroscopy, and operando electrochemical infrared spectroscopy. Consequently, the Faradaic efficiency for CO2 reduction to CH4 is enhanced from 16% to 89%, a record high efficiency so far, in aqueous electrolytes. It also exhibits a negligible activity loss over 50 h.
關鍵字active sites; CH 4; coordination-environment modification; electrocatalytic CO 2 reduction; OH overadsorption
語言英文
ISSN1614-6840; 1614-6832
期刊性質國外
收錄於SCI;
產學合作
通訊作者
審稿制度
國別德國
公開徵稿
出版型式,電子版,紙本
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