Ti3+ self-doped TiO2−x nanowires for efficient electrocatalytic N2 reduction to NH3

Ti³⁺ self-doped TiO_2−x nanowires for efficient electrocatalytic N₂ reduction to NH₃†

Bingyue Li,‡^ab Xiaojuan Zhu,‡^ac Jianwei Wang,‡^d Ruimin Xing,^b Qian Liu,

^a Xifeng Shi,^e Yonglan Luo,

*^c Shanhu Liu,*^b Xiaobin Niu

*^d and Xuping Sun

Author affiliations

* Corresponding authors

^a Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China

^b Henan Key Laboratory of Polyoxometalate Chemistry, Henan Joint International Research Laboratory of Environmental Pollution Control Materials, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 47504, Henan, China
E-mail: liushanhu@vip.henu.edu.cn

^c Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province, College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, Sichuan, China
E-mail: luoylcwnu@hotmail.com

^d School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
E-mail: xbniu@uestc.edu.cn

^e College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, Shandong, China

Abstract

Electrochemical N₂ reduction is an environmentally friendly and sustainable approach for NH₃ synthesis under mild conditions, while an efficient electrocatalyst is crucial for the N₂ reduction reaction (NRR). Herein, we report Ti³⁺ self-doped TiO_2−x nanowires on Ti mesh (Ti³⁺–TiO_2−x/TM) as an efficient non-noble-metal NRR electrocatalyst with excellent selectivity. In 0.1 M Na₂SO₄, the Ti³⁺–TiO_2−x/TM achieves a high faradaic efficiency of 14.62% with a NH₃ yield of 3.51 × 10⁻¹¹ mol s⁻¹ cm⁻² at −0.55 V vs. the reversible hydrogen electrode. Density functional theory calculations further reveal that introducing Ti³⁺ decreases the reaction energy barrier and increases the number of active sites on the TiO₂ surface for the NRR.

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Ti³⁺ self-doped TiO_2−x nanowires for efficient electrocatalytic N₂ reduction to NH₃†

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Ti³⁺ self-doped TiO_2−x nanowires for efficient electrocatalytic N₂ reduction to NH₃

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