Efficient Bifunctional Electrocatalysts for Oxygen Evolution/Reduction Reactions in Two-Dimensional Metal-Organic Frameworks by a Constant Potential Method

Yu Jin; Tianyun Liu; Xuefei Liu; Wei Deng; Wenjun Xiao; Yaqiong Su; Xiaosi Qi; Gang Wang; Degui Wang; Mingqiang Liu; Yan Wu; Abuduwayiti Aierken; Xuan Chen; Xu Wang; Changsong Gao; Hui Xiong; Xiangyu Wu; Jiajin Ge; Jinshun Bi

doi:10.1021/acs.langmuir.4c04034

Efficient Bifunctional Electrocatalysts for Oxygen Evolution/Reduction Reactions in Two-Dimensional Metal-Organic Frameworks by a Constant Potential Method

Langmuir. 2025 Jan 14;41(1):745-754. doi: 10.1021/acs.langmuir.4c04034. Epub 2024 Dec 29.

Authors

Yu Jin^{1

2}, Tianyun Liu³, Xuefei Liu^{1

2}, Wei Deng⁴, Wenjun Xiao^{1

2}, Yaqiong Su⁵, Xiaosi Qi⁶, Gang Wang^{1

2}, Degui Wang^{1

2}, Mingqiang Liu^{1

2}, Yan Wu^{1

2}, Abuduwayiti Aierken^{1

2}, Xuan Chen¹, Xu Wang⁷, Changsong Gao^{1

2}, Hui Xiong^{1

2}, Xiangyu Wu^{1

2}, Jiajin Ge^{1

2}, Jinshun Bi^{1

2}

Affiliations

¹ School of Physics and Electronic Science, Guizhou Normal University, Guiyang 550025, China.
² School of Integrated Circuit, Guizhou Normal University, Guiyang, 550025, China.
³ School of Physical Science and Technology, Soochow University, Suzhou 215000, China.
⁴ College of Big Data Statistics, Guizhou University of Finance and Economics,Guiyang,550000,China.
⁵ School of Chemistry, Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education, National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi'an Jiaotong University, Xi'an, 710049, China.
⁶ College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University, Guiyang City 550025, P.R. China.
⁷ College of Big Data and Information Engineering, Guizhou University, Guiyang, 550025, China.

PMID: 39810363
DOI: 10.1021/acs.langmuir.4c04034

Abstract

The evolution of bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts that are highly active, stable, and conductive is crucial for advancing metal-air batteries and fuel cells. We have here thoroughly explored the OER and ORR performance for a category of two-dimensional (2D) metal-organic frameworks (MOFs) called TM₃(HADQ)₂, and Rh₃(HADQ)₂ exhibits a promising bifunctional OER/ORR activity, with an overpotential of 0.31 V for both OER and ORR. The d-band center (ε_d) and crystal orbital Hamilton populations (COHP) are utilized to study the relationship between OER/ORR activity and the electronic structure of catalysts, and it is found that the elementary d-electron number (Ne) of the central TM for TM₃(HADQ)₂, as well as the electronegativity of the ligand TM-N₄ and the intermediate O atom, are the main reason that affects the catalytic activity of OER/ORR. Additionally, Rh₃(HADQ)₂ can be proven through the constant potential method (CPM) and microkinetics method that it is an acidic OER/ORR bifunctional catalyst. Rh₃(HADQ)₂ has a high toxicity tolerance, making it a potential bifunctional catalyst. Our research contributes to both the rational design of SACs for various catalytic processes and the fabrication of bifunctional, cost-effective oxygen-electric catalysts.