TY - JOUR
T1 - Efficient Bifunctional Electrocatalysts for Oxygen Evolution/Reduction Reactions in Two-Dimensional Metal-Organic Frameworks by a Constant Potential Method
AU - Jin, Yu
AU - Liu, Tianyun
AU - Liu, Xuefei
AU - Deng, Wei
AU - Xiao, Wenjun
AU - Su, Yaqiong
AU - Qi, Xiaosi
AU - Wang, Gang
AU - Wang, Degui
AU - Liu, Mingqiang
AU - Wu, Yan
AU - Aierken, Abuduwayiti
AU - Chen, Xuan
AU - Wang, Xu
AU - Gao, Changsong
AU - Xiong, Hui
AU - Wu, Xiangyu
AU - Ge, Jiajin
AU - Bi, Jinshun
N1 - Publisher Copyright:
© 2024 American Chemical Society.
PY - 2025/1/14
Y1 - 2025/1/14
N2 - 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 (ϵd) 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.
AB - 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 (ϵd) 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.
UR - https://www.scopus.com/pages/publications/85213535849
U2 - 10.1021/acs.langmuir.4c04034
DO - 10.1021/acs.langmuir.4c04034
M3 - 文章
C2 - 39810363
AN - SCOPUS:85213535849
SN - 0743-7463
VL - 41
SP - 745
EP - 754
JO - Langmuir
JF - Langmuir
IS - 1
ER -