SCI和EI收录∣中国化工学会会刊

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 Shi1,2, Yu Yin3, Hong Wu1, Rajan Arjan Kalyan Hirani1, Xinyuan Xu1, Jinqiang Zhang1, Nasir Rafique1, Abdul Hannan Asif1, Shu Zhang2, Hongqi Sun1   

  1. 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 Shi1,2, Yu Yin3, Hong Wu1, Rajan Arjan Kalyan Hirani1, Xinyuan Xu1, Jinqiang Zhang1, Nasir Rafique1, Abdul Hannan Asif1, Shu Zhang2, Hongqi Sun1   

  1. 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: 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