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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
ISSN2095-4956
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
DOI10.1016/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
被引频次:2[WOS]   [WOS记录]     [WOS相关记录]
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
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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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