eprintid: 10205497
rev_number: 7
eprint_status: archive
userid: 699
dir: disk0/10/20/54/97
datestamp: 2025-03-03 16:12:47
lastmod: 2025-03-03 16:12:47
status_changed: 2025-03-03 16:12:47
type: article
metadata_visibility: show
sword_depositor: 699
creators_name: Cheng, R
creators_name: He, X
creators_name: Ran, B
creators_name: Li, H
creators_name: Tang, W
creators_name: Sun, F
creators_name: Li, K
creators_name: Shao, X
creators_name: Chen, H
creators_name: Fu, C
title: High-entropy optimizing d-orbital electronic configuration of metal organic framework for high-current-density anion exchange membrane water electrolysis
ispublished: pub
divisions: UCL
divisions: B04
divisions: C06
divisions: F43
divisions: F56
keywords: High-entropy; metal organic framework; d-orbital; large current density;
overall water splitting
note: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
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.
date: 2025-02
date_type: published
publisher: ELSEVIER
official_url: https://doi.org/10.1016/j.nanoen.2024.110529
full_text_type: other
language: eng
verified: verified_manual
elements_id: 2343288
doi: 10.1016/j.nanoen.2024.110529
lyricists_name: Li, Kaiqi
lyricists_name: Li, Huanxin
lyricists_id: KLIDX18
lyricists_id: HLIPX63
actors_name: Li, Huanxin
actors_id: HLIPX63
actors_role: owner
funding_acknowledgements: 22ZR1429700 [Natural Science Foundation of Shanghai]; 52274302 [National Natural Science Foundation of China]
full_text_status: restricted
publication: Nano Energy
volume: 134
article_number: 110529
pages: 13
issn: 2211-2855
citation:        Cheng, R;    He, X;    Ran, B;    Li, H;    Tang, W;    Sun, F;    Li, K;             ... Fu, C; + view all <#>        Cheng, R;  He, X;  Ran, B;  Li, H;  Tang, W;  Sun, F;  Li, K;  Shao, X;  Chen, H;  Fu, C;   - view fewer <#>    (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 <https://doi.org/10.1016/j.nanoen.2024.110529>.      
 
document_url: https://discovery.ucl.ac.uk/id/eprint/10205497/1/NE_final.pdf