Cheng, R;
He, X;
Ran, B;
Li, H;
Tang, W;
Sun, F;
Li, K;
... Fu, C; + view all
(2025)
High-entropy optimizing d-orbital electronic configuration of metal organic framework for high-current-density anion exchange membrane water electrolysis.
Nano Energy
, 134
, Article 110529. 10.1016/j.nanoen.2024.110529.
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Abstract
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 (E̅d) 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.
| Type: | Article |
|---|---|
| Title: | High-entropy optimizing d-orbital electronic configuration of metal organic framework for high-current-density anion exchange membrane water electrolysis |
| DOI: | 10.1016/j.nanoen.2024.110529 |
| Publisher version: | https://doi.org/10.1016/j.nanoen.2024.110529 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | High-entropy; metal organic framework; d-orbital; large current density; overall water splitting |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10205497 |
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