文献类型：期刊文献

英文题名：Selective and Scalable CO2 Electrolysis Enabled by Conductive Zinc Ion-Implanted Zeolite-Supported Cadmium Oxide Nanoclusters

作者：Zhang, Zhen[1];Li, Minzhe[2];Gao, Rui[3];Yang, Shuwen[4,5,6];Ma, Qianyi[1];Feng, Renfei[7];Dou, Haozhen[5,6];Dang, Jianan[4,5,6];Wen, Guobin[1];Bai, Zhengyu[4];Liu, Dianhua[2];Feng, Ming[3];Chen, Zhongwei[1,5,6]

机构：[1]Univ Waterloo, Dept Chem Engn, Waterloo, ON N2L 3G1, Canada;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Jilin Normal Univ, Key Lab Funct Mat Phys & Chem, Minist Educ, Changchun 130103, Peoples R China;[4]Henan Normal Univ, Sch Chem & Chem Engn, Key Lab Green Chem Media & React, Minist Educ, Xinxiang 453007, Henan, Peoples R China;[5]Chinese Acad Sci, Dalian Inst Chem Phys, Power Battery & Syst Res Ctr, Dalian 116023, Peoples R China;[6]Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China;[7]Canadian Light Source, Saskatoon, SK S7N 2V3, Canada

年份：2024

卷号：146

期号：9

起止页码：6397

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20240915663603);WOS:【SCI-EXPANDED(收录号:WOS:001177662200001)】；

基金：The authors appreciate the support from the University of Waterloo, the National Natural Science Foundation of China (Nos. 52171210 and 21978110), the Program for the Development of Science and Technology of Jilin Province (No. 20220201130GX), the Strategic Priority Research Program of the Chinese Academy of Sciences (Nos. XDB0600000, XDB0600100, XDB0600200, XDB0600300, and XDB0600400), Liaoning Binhai Laboratory (No. LILBLB-2023-04), and Dalian Revitalization Talents Program (No. 2022RG01). The authors acknowledge the support for XAS measurements from Dr. Roman Chernikov and Dr. Emilio Heredia with the BioXAS beamline and Dr. Ning Chen and Dr. Weifeng Chen with the HXMA beamline at the Canadian Light Source.

语种：英文

外文关键词：Cadmium compounds - Carbon dioxide - Electrocatalysis - Electrocatalysts - Electrolysis - Nanoclusters

摘要：Catalyst supports play an essential role in catalytic reactions, hinting at pronounced metal-support effects. Zeolites are a propitious support in heterogeneous catalysts, while their use in the electrocatalytic CO2 reduction reaction has been limited as yet because of their electrically insulating nature and serious competing hydrogen evolution reaction (HER). Enlightened by theoretical prediction, herein, we implant zinc ions into the structural skeleton of a zeolite Y to strategically tailor a favorable electrocatalytic platform with remarkably enhanced electronic conduction and strong HER inhibition capability, which incorporates ultrafine cadmium oxide nanoclusters as guest species into the supercages of the tailored 12-ring window framework. The metal d-bandwidth tuning of cadmium by skeletal zinc steers the extent of substrate-molecule orbital mixing, enhancing the stabilization of the key intermediate *COOH while weakening the CO poisoning effect. Furthermore, the strong cadmium-zinc interplay causes a considerable thermodynamic barrier for water dissociation in the conversion of H+ to *H, potently suppressing the competing HER. Therefore, we achieve an industrial-level partial current density of 335 mA cm(-2) and remarkable Faradaic efficiency of 97.1% for CO production and stably maintain Faradaic efficiency above 90% at the industrially relevant current density for over 120 h. This work provides a proof of concept of tailored conductive zeolite as a favorable electrocatalytic support for industrial-level CO2 electrolysis and will significantly enhance the adaptability of conductive zeolite-based electrocatalysts in a variety of electrocatalysis and energy conversion applications.