期刊論文

學年 113
學期 2
出版(發表)日期 2025-04-09
作品名稱 Electrosynthesis of Urea on High-Density Ga─Y Dual-Atom Catalyst via Cross-Tuning
作品名稱(其他語言)
著者 Dechao Chen; Yimeng Cai; Yi Xiao; Chengqiang Wang; Yong Li; Ke Ma; Dongdong Xiao; Hsiao-Tsu Wang; Chi-Feng Lee; Linjie Zhang; Hirofumi Ishii; Yu-Cheng Shao; Nozomu Hiraoka; Lili Han; Xueming Liu; Huolin L. Xin
單位
出版者
著錄名稱、卷期、頁數 Advanced Materials 37(14), 2420593
摘要 Electrochemically converting carbon dioxide (CO2) and nitrate (NO3−) into urea via the C─N coupling route offers a sustainable alternative to the traditional industrial urea production technology, but it is still limited by poor yield rate, low Faradaic efficiency, and insufficient coupling kinetics. Herein, a high-density Ga─Y dual-atom catalyst is developed with loading up to 14.1 wt.% of Ga and Y supported on N, P-co-doped carbon substrate (Ga/Y-CNP) for urea electrosynthesis. The catalyst facilitates efficient C─N coupling through co-reduction of CO2 and NO3−, resulting in a high urea yield rate of 41.9 mmol h−1 g−1 and a Faradaic efficiency of 22.1% at −1.4 V versus the reversible hydrogen electrode. In situ spectroscopy and theoretical calculations reveal that the superior performance is attributed to the cross-tuning between adjacent pair Ga─Y sites, which can mutually optimize their electronic states for facilitating CO2 reduction to *CO at Ga sites and promoting NO3− conversion to hydroxylamine (*NH2OH) at Y sites, followed by spontaneous coupling of *CO and *NH2OH intermediates at Ga─Y sites to form C─N bonds. This work offers a pioneering strategy to manipulate C─N coupling pathways by cross-tuning active sites to produce high-value-added chemicals.
關鍵字
語言 en
ISSN 0935-9648; 1521-4095
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度
國別 USA
公開徵稿
出版型式 ,電子版,紙本
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機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/129453 )