文献类型：期刊文献

英文题名：Aqueous Electroreduction of Nitric Oxide to Ammonia at Low Concentration via Vacancy Engineered FeOCl

作者：Guo, Xiaoxi[1,2];Wang, Pai[3];Wu, Tongwei[3];Wang, Zhiqiang[4,5,6];Li, Jiong[9];Liu, Kang[2,7];Fu, Junwei[2];Wu, Jun[7];Lin, Zhang[7];Chai, Liyuan[7];Bian, Zhenfeng[10,11];Li, Hengfeng[1];Liu, Min[2,2,8]

机构：[1]Cent South Univ, Sch Mat Sci & Engn, Changsha 410083, Hunan, Peoples R China;[2]Cent South Univ, Hunan Joint Int Res Ctr Carbon Dioxide Resource U, Sch Phys, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China;[3]Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Sichuan, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Joint Int Res Lab Precis Chem & Mol Engn, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[7]Cent South Univ, Sch Met & Environm, Changsha 410083, Hunan, Peoples R China;[8]Univ South China, Coll Nucl Sci & Technol, Hengyang 421001, Hunan, Peoples R China;[9]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China;[10]Shanghai Normal Univ, MOE Key Lab Resource Chem, Shanghai 200234, Peoples R China;[11]Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Shanghai 200234, Peoples R China

年份：2024

卷号：63

期号：6

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20240215341309);WOS:【SCI-EXPANDED(收录号:WOS:001143086500001)】；

基金：The authors acknowledge the support of the funding from the National Natural Science Foundation of China (Grant Nos. 22002189, 22376222, 52372253, 52202214 and 52202125), Science and Technology Innovation Program of Hunan Province (Grant No. 2023RC1012), Central South University Research Programme of Advanced Interdisciplinary Studies (Grant No. 2023QYJC012), Central South University Innovation-Driven Research Programme (Grant No. 2023CXQD042), Natural Science Foundation of Sichuan Province (No. 2023NSFSC0954), China National Postdoctoral Program for Innovative Talents (No. BX2021053), and China Postdoctoral Science Foundation (No. 2021M700680). The authors thank BL11B beamline of the Shanghai Synchrotron Radiation Facility (SSRF) for providing the XAFS beamtime. The numerical calculations in this paper have been done on Hefei advanced computing center.

语种：英文

外文关键词：Electrocatalytic NO Reduction Reaction (NORR); Low-Concentration NO; NH3 Synthesis; In Situ Spectroelectrochemical; Cl Vacancy

摘要：Electroreduction of nitric oxide (NO) to NH3 (NORR) has gained extensive attention for the sake of low carbon emission and air pollutant treatment. Unfortunately, NORR is greatly hindered by its sluggish kinetics, especially under low concentrations of NO. Herein, we developed a chlorine (Cl) vacancy strategy to overcome this limitation over FeOCl nanosheets (FeOCl-V-Cl). Density functional theory (DFT) calculations revealed that the Cl vacancy resulted in defective Fe with sharp d-states characteristics in FeOCl-V-Cl to enhance the absorption and activation of NO. In situ X-ray absorption near-edge structure (XANES) and attenuated total reflection-infrared spectroscopy (ATR-IR) verified the lower average oxidation state of defective Fe to enhance the electron transfer for NO adsorption/activation and facilitate the generation of key NHO and NHx intermediates. As a result, the FeOCl-V-Cl exhibited superior NORR activities with the NH3 Faradaic efficiency up to 91.1 % while maintaining a high NH3 yield rate of 455.4 mu g cm(-2) h(-1) under 1.0 vol % NO concentration, competitive with those of previously reported literatures under higher NO concentration. Further, the assembled Zn-NO battery utilizing FeOCl-V-Cl as cathode delivered a record peak power density of 6.2 mW cm(-2), offering a new route for simultaneous NO removal, NH3 production, and energy supply.