Boosting nitrogen electrocatalytic fixation by three-dimensional TiO2-delta N delta nanowire arrays | |
Mu, Jianjia1; Gao, Xuan-Wen1; Liu, Zhaomeng1; Luo, Wen-Bin1; Sun, Zhenhua2; Gu, Qinfen3; Li, Feng2 | |
通讯作者 | Luo, Wen-Bin(luowenbin@smm.neu.edu.cn) ; Li, Feng(fli@imr.ac.cn) |
2022-12-01 | |
发表期刊 | JOURNAL OF ENERGY CHEMISTRY
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ISSN | 2095-4956 |
卷号 | 75页码:293-300 |
摘要 | Owing to the environmental and inherent advantages, nitrogen reduction reaction (NRR) by electrocatalysts attracts global attention. The surface engineering is widely employed to enhance the electrocatalytic activity by atomic defects and heterostructure effects. A three-dimensional (3D) free-standing integrated electrode was fabricated by numerous nearly-single-crystal TiO2-delta N delta nanowire arrays. Based on the high electronic conductivity network, it exposes numerous active sites as well to facilitate the selective nitrogen adsorption and *H adsorption suppression. The synergistic effects between Ti3+ and oxygen vacancy (O-v) boost the intrinsic catalytic activity, in which Ti3+ acquired electrons via Ov can effectively activate the N N bond and make it easy to bind with protons. The energy barrier of primary protonation process (*N-2+H++e -> *NNH) can be dramatically decreased. The highest ammonia yield rate (14.33 mu g h(-1) mg(cat)(-1)) emerges at -0.2 V, while the optimal ammonia Faradaic efficiency (9.17%) is acquired at -0.1 V. Density functional theory (DFT) calculation reveals that the Ti3+ can be served as the active sites for nitrogen adsorption and activation, while ammonia synthesis is accomplished by the distal pathway. The high electronic conductivity integrated network and synergistic effects can significantly facilitate nitrogen absorption and accelerate electrocatalytic reaction kinetic, which are responsible for the excellent NRR performance at room temperature. (C) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved. |
关键词 | Nanowires TiO2-delta N delta Electrocatalysis NRR DFT |
资助者 | LiaoNing Revitalization Talents Program ; Fundamental Research Funds for the Central Universities |
DOI | 10.1016/j.jechem.2022.08.007 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | LiaoNing Revitalization Talents Program ; Fundamental Research Funds for the Central Universities ; [XLYC2007155] ; [N2025018] ; [N2025009] |
WOS研究方向 | Chemistry ; Energy & Fuels ; Engineering |
WOS类目 | Chemistry, Applied ; Chemistry, Physical ; Energy & Fuels ; Engineering, Chemical |
WOS记录号 | WOS:000870204100002 |
出版者 | ELSEVIER |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/176407 |
专题 | 中国科学院金属研究所 |
通讯作者 | Luo, Wen-Bin; Li, Feng |
作者单位 | 1.Northeastern Univ, Sch Met, Shenyang 110819, Liaoning, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China 3.Australian Synchrotron ANSTO, 800 Blackburn Rd, Clayton, Vic 3168, Australia |
推荐引用方式 GB/T 7714 | Mu, Jianjia,Gao, Xuan-Wen,Liu, Zhaomeng,et al. Boosting nitrogen electrocatalytic fixation by three-dimensional TiO2-delta N delta nanowire arrays[J]. JOURNAL OF ENERGY CHEMISTRY,2022,75:293-300. |
APA | Mu, Jianjia.,Gao, Xuan-Wen.,Liu, Zhaomeng.,Luo, Wen-Bin.,Sun, Zhenhua.,...&Li, Feng.(2022).Boosting nitrogen electrocatalytic fixation by three-dimensional TiO2-delta N delta nanowire arrays.JOURNAL OF ENERGY CHEMISTRY,75,293-300. |
MLA | Mu, Jianjia,et al."Boosting nitrogen electrocatalytic fixation by three-dimensional TiO2-delta N delta nanowire arrays".JOURNAL OF ENERGY CHEMISTRY 75(2022):293-300. |
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