TY  - JOUR
JF  - Nano Energy
A1  - Cheng, R
A1  - He, X
A1  - Ran, B
A1  - Li, H
A1  - Tang, W
A1  - Sun, F
A1  - Li, K
A1  - Shao, X
A1  - Chen, H
A1  - Fu, C
KW  - High-entropy; metal organic framework; d-orbital; large current density;
overall water splitting
N2  - Water electrolysis provides a promising way for hydrogen production through renewable power sources. The exploration of non-precious metal-based electrocatalysts capable of sustaining high current densities for water electrocatalysis is of critical importance. Herein, we develop a high-entropy Mil53 metal organic framework (denoted as Mil53-HE) bifunctional electrocatalyst with improved performance for overall water splitting at large current densities. The improved activity and stability of Mil53-HE for water electrolysis stem from the optimized electronic configurations of d-orbitals in the metal centers, as the overall d-band center (E?d) is upshifted and the total number of d-orbital electrons in the supercell (?Nd) is decreased of Mil53-HE. Therefore, the reduced reaction energy barriers and enriched unpaired d-electrons promote both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). As a result, the HER and OER activities of Mil53-HE surpass those of their benchmarks Pt/C and RuO2, respectively. Meanwhile, the HER and OER mechanisms on Mil53-HE are revealed by in-situ characterizations and theoretical calculations. Furthermore, the anion exchange membrane water electrolysis cell with Mil53-HE can stably operate at large current densities with small voltages (1.9 V at 0.52 A cm?2 and 2.1 V at 1.48 A cm?2), demonstrating good feasibility for practical application.
ID  - discovery10205497
PB  - ELSEVIER
UR  - https://doi.org/10.1016/j.nanoen.2024.110529
SN  - 2211-2855
N1  - This version is the author accepted manuscript. For information on re-use, please refer to the publisher?s terms and conditions.
TI  - High-entropy optimizing d-orbital electronic configuration of metal organic framework for high-current-density anion exchange membrane water electrolysis
Y1  - 2025/02//
AV  - restricted
VL  - 134
EP  - 13
ER  -