Citation: Tian-Ru HAN, Jing-Jing WU, Zi-Xin QU, Xin TANG. Pyrochlore Structure Y_2-xMg_xRu₂O_7-δ (x=0.05, 0.1, 0.15): Preparation and OER Catalytic Performance[J]. Chinese Journal of Inorganic Chemistry, ;2021, 37(2): 285-294. doi: 10.11862/CJIC.2021.043 shu

Pyrochlore Structure Y_2-xMg_xRu₂O_7-δ (x=0.05, 0.1, 0.15): Preparation and OER Catalytic Performance

Tian-Ru HAN ^{1, 2} ,
Jing-Jing WU ^{1, 2} ,
Zi-Xin QU ^{1, 2} ,
Xin TANG ^{1, 2,,}

1.
Key Lab of New Processing Technology for Nonferrous Metal & Materials, Ministry of Education, Guilin University of Technology, Guilin, Guangxi 541004, China
2.
College of Material Science and Engineering, Guilin University of Technology, Guilin, Guangxi 541004, China

Corresponding author: Xin TANG, xtang@glut.edu.cn
Received Date: 30 August 2020
Revised Date: 9 December 2020

Figures(9)

Herein, pyrochlore structure Y_2-xMg_xRu₂O_7-δ (YMRO-x, x=0.05, 0.1, 0.15) catalysts were prepared by solgel method. The X-ray photoelectron spectroscopy was employed to analyze the surface chemical composition and valence state of as-synthesized YMRO. The results showed that oxygen defects were increased when Mg²⁺ partially substituted Y³⁺ of A site in pyrochlore (A₂B₂O_7-δ). Especially, YMRO-0.1 catalyst possessed the most extraordinary performance in oxygen evolution reaction (OER). Reaching current density of 10 mA·cm^-2 only required 265 mV overpotential, outperformed the RuO₂ (358 mV), Y₂Ru₂O_7-δ (294 mV), YMRO-0.05 (282 mV) and YMRO-0.15 (281 mV). The Tafel slope of YMRO-0.1 was 45 mV·dec^-1, much smaller than that of RuO₂ (88 mV·dec^-1), YRO (64 mV·dec^-1), YMRO-0.05 (51 mV·dec^-1) and YMRO-0.15 (52 mV·dec^-1), having the fastest kinetic process. Turning to stability test of YMRO-0.1, the potential moved little in 12 h, compared with Y₂Ru₂O_7-δ which shifted up 30 mV under acidic environment. Moreover, first principle calculation indicated that the substitution atom Mg_Y formed a complex with oxygen vacancies, favored the formation of oxygen vacancies, narrowed the band gap, and lowered the charge-transfer-energy. In addition, the excellent OER reactivity can be partly attributed to the Ru⁵⁺ ions. Due to the introduction of Mg, the Ru⁴⁺ ions at central active site was oxidized to Ru⁵⁺ ions, donating electron to surface and accelerating the process of oxygen evolution reaction. As a result, the active sites also minimized Gibbs free energy of oxygen radical desorption, which promoted the OER. Based on the results, YMRO should be a promising OER catalytic material which can stably work in acid environment.
- catalysis,
- electrochemistry,
- ab initio calculations,
- sol-gel processes
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通讯作者: 陈斌, bchen63@163.com

Pyrochlore Structure Y_2-xMg_xRu₂O_7-δ (x=0.05, 0.1, 0.15): Preparation and OER Catalytic Performance