Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO2

能源化学(英文版) ›› 2019, Vol. 39 ›› Issue (12): 144-151.

Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO₂

Shan Cheng, Yi-Jing Gao, Yi-Long Yan, Xu Gao, Shao-Hua Zhang, Gui-Lin Zhuang, Sheng-Wei Deng, Zhong-Zhe Wei, Xing Zhong, Jian-Guo Wang

Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China

收稿日期:2018-11-26 修回日期:2019-01-16 出版日期:2019-12-15 发布日期:2020-12-18
通讯作者: Gui-Lin Zhuang, glzhuang@zjut.edu.cn; Jian-Guo Wang, jgw@zjut.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (Nos. 21671172, 21625604, 21776251, 21706229 and Z86101001) and Zhejiang Provincial Natural Science Foundation (No. LR19B010001).

Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO₂

Shan Cheng, Yi-Jing Gao, Yi-Long Yan, Xu Gao, Shao-Hua Zhang, Gui-Lin Zhuang, Sheng-Wei Deng, Zhong-Zhe Wei, Xing Zhong, Jian-Guo Wang

Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China

Received:2018-11-26 Revised:2019-01-16 Online:2019-12-15 Published:2020-12-18
Contact: Gui-Lin Zhuang, glzhuang@zjut.edu.cn; Jian-Guo Wang, jgw@zjut.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (Nos. 21671172, 21625604, 21776251, 21706229 and Z86101001) and Zhejiang Provincial Natural Science Foundation (No. LR19B010001).

摘要/Abstract

摘要： To search the new effective nitrogen reduction reaction (NRR) electrocatalyst is very important for the ammonia-based industry. Herein, we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-vacancy TiO₂ (Ru/TiO₂-Vo). Structural characterizations revealed that oxygen vacancy was loaded in the matrix of Ru/TiO₂-Vo. Electrocatalytic results indicated that Ru/TiO₂-Vo showed good NRR performance (2.11 μg h^-1 cm^-2). Contrast tests showed that NRR property of Ru/TiO₂-Vo was much better than those of Ru/TiO₂(B) (0.53 μg h^-1 cm^-2) and Ru/P25 (0.42 μg h^-1 cm^-2). Furthermore, density functional theory calculation results indicated catalytic mechanism of NRR and rate-determining step (^*N₂ + 1/2H₂ → ^*N+^*NH) was the potential-determining step with the overpotential requirement of 0.21 V. A combination of electronic structure analysis and catalytic measurement shed light on the synergistic effect of Ru and oxygen vacancy on the NRR performance.

关键词: Nitrogen reduction reaction, Electrocatalysis, Oxygen vacancy, DFT

Abstract: To search the new effective nitrogen reduction reaction (NRR) electrocatalyst is very important for the ammonia-based industry. Herein, we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-vacancy TiO₂ (Ru/TiO₂-Vo). Structural characterizations revealed that oxygen vacancy was loaded in the matrix of Ru/TiO₂-Vo. Electrocatalytic results indicated that Ru/TiO₂-Vo showed good NRR performance (2.11 μg h^-1 cm^-2). Contrast tests showed that NRR property of Ru/TiO₂-Vo was much better than those of Ru/TiO₂(B) (0.53 μg h^-1 cm^-2) and Ru/P25 (0.42 μg h^-1 cm^-2). Furthermore, density functional theory calculation results indicated catalytic mechanism of NRR and rate-determining step (^*N₂ + 1/2H₂ → ^*N+^*NH) was the potential-determining step with the overpotential requirement of 0.21 V. A combination of electronic structure analysis and catalytic measurement shed light on the synergistic effect of Ru and oxygen vacancy on the NRR performance.

Key words: Nitrogen reduction reaction, Electrocatalysis, Oxygen vacancy, DFT

Shan Cheng, Yi-Jing Gao, Yi-Long Yan, Xu Gao, Shao-Hua Zhang, Gui-Lin Zhuang, Sheng-Wei Deng, Zhong-Zhe Wei, Xing Zhong, Jian-Guo Wang. Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO₂[J]. 能源化学(英文版), 2019, 39(12): 144-151.

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Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO₂

Oxygen vacancy enhancing mechanism of nitrogen reduction reaction property in Ru/TiO₂

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