文献类型：期刊文献

英文题名：Size Effect of Surface Defects Dictates Reactivity for Nitrogen Electrofixation

作者：Sun, Yuntong[1] Lu, Gonggong[2] Wang, Zhiqi[3] Li, Xuheng[4] Li, Yinghao[1] Sui, Nicole L. D.[1] Fan, Wenjun[5] Wang, Ao[1,6] Yuan, Bo[2] Wang, Junjie[3] Lee, Jong-Min[1]

第一作者：Sun, Yuntong

通信作者：Lee, JM[1];Yuan, B[2];Wang, JJ[3];Fan, WJ[4]

机构：[1]Nanyang Technol Univ, Sch Chem Chem Engn & Biotechnol, 62 Nanyang Dr, Nanyang 637459, Singapore;[2]Sichuan Univ, Natl Engn Res Ctr Biomat, 29 Wangjiang Rd, Chengdu 610064, Peoples R China;[3]Northwestern Polytech Univ, Sch Mat Sci & Engn, State Key Lab Solidificat Proc, Xian 710072, Shaanxi, Peoples R China;[4]Northwestern Polytech Univ, Sch Chem & Chem Engn, Xian 710072, Shaanxi, Peoples R China;[5]Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis,iChEM, Dalian 116023, Peoples R China;[6]Chinese Acad Forestry, Inst Chem Ind Forest Prod, 16 Suojin 5th Village, Nanjing 210042, Peoples R China

年份：2025

卷号：64

期号：19

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20251418185840);Scopus(收录号：2-s2.0-105001877695);WOS:【SCI-EXPANDED(收录号:WOS:001481198300049)】；

基金：Y.S., G.L., Z.W., and X.L. contributed equally to this work. This work was supported by the AcRF Tier 1 (grant RG105/19) provided by the Ministry of Education in Singapore and the Forestry Technology Projects of Zhejiang Province (2023SY04). The authors thank the Shanghai Synchrotron Radiation Facility (beamline BL 1W1B) for providing beam time.

语种：英文

外文关键词：Ammonia production; Defect engineering; Electrocatalysis; Nitrogen reduction reaction; Size effect

摘要：Electrocatalytic nitrogen reduction reaction (eNRR) offers a sustainable pathway for ammonia (NH3) production. Defect engineering enhances eNRR activity but can concurrently amplify the competing hydrogen evolution reaction (HER), posing challenges for achieving high selectivity. Herein, VOx with systematically tuned defect sizes is engineered to establish a structure-activity relationship between defect size and eNRR performance. In situ spectroscopy and theoretical calculations reveal that medium-sized defects (VOx-MD, 1-2 nm) provide an optimal electronic environment for enhanced N2 adsorption and activation while maintaining spatial flexibility to facilitate efficient hydrogenation. Consequently, VOx-MD exhibits outstanding eNRR performance, achieving an NH3 yield rate of 81.94 +/- 1.45 mu g h-1 mg-1 and a Faradaic efficiency of 31.97 +/- 0.75 % at -0.5 V (vs RHE). These findings highlight the critical role of defect size in governing eNRR activity, offering a scalable strategy for designing advanced catalysts for competitve electrocatalytic reactions.