Controllable synthesis of a hollow Cr2O3 electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis

doi:10.1016/j.cjche.2021.11.016

中国化学工程学报 ›› 2022, Vol. 41 ›› Issue (1): 358-365.DOI: 10.1016/j.cjche.2021.11.016

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Controllable synthesis of a hollow Cr₂O₃ electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis

Lei Shi^1,2, Yu Yin³, Hong Wu¹, Rajan Arjan Kalyan Hirani¹, Xinyuan Xu¹, Jinqiang Zhang¹, Nasir Rafique¹, Abdul Hannan Asif¹, Shu Zhang², Hongqi Sun¹

1 School of Engineering, Edith Cowan University, Joondalup, WA 6027, Australia;
2 College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China;
3 School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China

收稿日期:2021-06-28 修回日期:2021-10-10 出版日期:2022-01-28 发布日期:2022-02-25
通讯作者: Lei Shi,E-mail address:l.shi@ecu.edu.au;Hongqi Sun,E-mail address:h.sun@ecu.edu.au
基金资助:
The author (Sun) would like to express his thanks for the support from Vice-Chancellor’s Professorial Research Fellowship. The work was partially supported by Australian Research Council Discovery Projects (DP170104264 and DP190103548).

Controllable synthesis of a hollow Cr₂O₃ electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis

Lei Shi^1,2, Yu Yin³, Hong Wu¹, Rajan Arjan Kalyan Hirani¹, Xinyuan Xu¹, Jinqiang Zhang¹, Nasir Rafique¹, Abdul Hannan Asif¹, Shu Zhang², Hongqi Sun¹

1 School of Engineering, Edith Cowan University, Joondalup, WA 6027, Australia;
2 College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China;
3 School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China

Received:2021-06-28 Revised:2021-10-10 Online:2022-01-28 Published:2022-02-25
Contact: Lei Shi,E-mail address:l.shi@ecu.edu.au;Hongqi Sun,E-mail address:h.sun@ecu.edu.au
Supported by:
The author (Sun) would like to express his thanks for the support from Vice-Chancellor’s Professorial Research Fellowship. The work was partially supported by Australian Research Council Discovery Projects (DP170104264 and DP190103548).

摘要/Abstract

摘要： As a fascinating alternative to the energy-intensive Haber-Bosch process, the electrochemically-driven N₂ reduction reaction (NRR) utilizing the N₂ and H₂O for the production of NH₃ has received enormous attention. The development and preparation of promising electrocatalysts are requisite to realize an efficient N₂ conversion for NH₃ production. In this research, we propose a template-assisted strategy to construct the hollow electrocatalyst with controllable morphology. As a paradigm, the hollow Cr₂O₃ nanocatalyst with a uniform size (~170 nm), small cavity and ultrathin shell (~15 nm) is successfully fabricated with this strategy. This promising hollow structure is favourable to trap N₂ into the cavity, provides abundant active sites to accelerate the three-phase interactions, and facilitates the reactant transfer across the shell. Attributed to these synergetic effects, the designed catalyst displays an outstanding behaviour in N₂ fixation for NH₃ production in ambient condition. In the neutral electrolyte of 0.1 mol·L^-1 Na₂SO₄, an impressive electrocatalytic performance with the NH₃ generation rate of 2.72 μg·h^-1·cm^-2 and a high FE of 5.31% is acquired respectively at -0.85 V with the hollow Cr₂O₃ catalyst. Inspired by this work, it is highly expected that this approach could be applied as a universal strategy and extended to fabricating other promising electrocatalysts for realizing highly efficient nitrogen reduction reaction (NRR).

关键词: Hollow structure, Electrocatalytic N₂ fixation, NH₃ synthesis, Template-assisted strategy, Ambient condition

Abstract: As a fascinating alternative to the energy-intensive Haber-Bosch process, the electrochemically-driven N₂ reduction reaction (NRR) utilizing the N₂ and H₂O for the production of NH₃ has received enormous attention. The development and preparation of promising electrocatalysts are requisite to realize an efficient N₂ conversion for NH₃ production. In this research, we propose a template-assisted strategy to construct the hollow electrocatalyst with controllable morphology. As a paradigm, the hollow Cr₂O₃ nanocatalyst with a uniform size (~170 nm), small cavity and ultrathin shell (~15 nm) is successfully fabricated with this strategy. This promising hollow structure is favourable to trap N₂ into the cavity, provides abundant active sites to accelerate the three-phase interactions, and facilitates the reactant transfer across the shell. Attributed to these synergetic effects, the designed catalyst displays an outstanding behaviour in N₂ fixation for NH₃ production in ambient condition. In the neutral electrolyte of 0.1 mol·L^-1 Na₂SO₄, an impressive electrocatalytic performance with the NH₃ generation rate of 2.72 μg·h^-1·cm^-2 and a high FE of 5.31% is acquired respectively at -0.85 V with the hollow Cr₂O₃ catalyst. Inspired by this work, it is highly expected that this approach could be applied as a universal strategy and extended to fabricating other promising electrocatalysts for realizing highly efficient nitrogen reduction reaction (NRR).

Key words: Hollow structure, Electrocatalytic N₂ fixation, NH₃ synthesis, Template-assisted strategy, Ambient condition

Lei Shi, Yu Yin, Hong Wu, Rajan Arjan Kalyan Hirani, Xinyuan Xu, Jinqiang Zhang, Nasir Rafique, Abdul Hannan Asif, Shu Zhang, Hongqi Sun. Controllable synthesis of a hollow Cr₂O₃ electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis[J]. 中国化学工程学报, 2022, 41(1): 358-365.

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Controllable synthesis of a hollow Cr₂O₃ electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis

Controllable synthesis of a hollow Cr₂O₃ electrocatalyst for enhanced nitrogen reduction toward ammonia synthesis

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