eprintid: 10187773
rev_number: 11
eprint_status: archive
userid: 699
dir: disk0/10/18/77/73
datestamp: 2024-02-27 12:56:49
lastmod: 2024-02-27 12:56:49
status_changed: 2024-02-27 12:56:49
type: article
metadata_visibility: show
sword_depositor: 699
creators_name: Wang, Q
creators_name: Wang, Z
creators_name: Zhao, J
creators_name: Li, J
creators_name: Shen, D
creators_name: Xu, LH
creators_name: Wu, C
creators_name: Hong Luo, K
title: Enhancing d-band center modulation in Carbon-Supported CoP via exogenous nitrogen Dopants: A strategy for boosting Ampere-Level hydrogen evolution reaction
ispublished: pub
divisions: UCL
divisions: B04
divisions: C05
divisions: F45
keywords: Cobalt phosphide, d-band center, work function, ginkgo leaves-based carbon, hydrogen evolution reaction (HER), exogenous nitrogen doping
note: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
abstract: The incorporation of exogenous heteroatoms presents a promising avenue for enhancing the ampere-level hydrogen evolution reaction (HER) by modulating the d-band center of carbon-supported CoP electrocatalysts derived from biomass. In this study, we synthesized carbon-supported CoP electrocatalysts through a simple carbothermal reduction method, using ginkgo leaves as the carbon source. The composition of nitrogen (N) species in the carbon supports was finely tuned by adjusting melamine (MA) addition, optimizing the valence band structure of resulting CoP@N-glC-m (m = 1, 2, 3, 4, and 5) catalysts through electronic metal-support interactions (EMSIs) with CoP nanoparticles (NPs). By correlating the d-band center, work function, N species contents, and η1000 value, we observed a close correlation between the variation of the (pyrrolic N + Co-N)/(pyridinic N + graphitic N) ratio, work function, d-band center, and η1000 value. Notably, CoP@N-glC-3, with the highest ratio of (pyrrolic N + Co-N)/(pyridinic N + graphitic N), exhibited an optimal work function and d-band center, striking a balance between Volmer and Heyrovsky processes, resulting in the highest HER activity among the catalysts. CoP@N-glC-3 demonstrated a 844 mV overpotential, driving the current density to 1000 mA cm−2, more approaching to commercial 20 % Pt/C compared with CoP@glC and CoP@N-glC-m (m = 1, 2, 3 and 5). This research provides crucial insights into electrocatalyst design, connecting chemical properties, valence band structures, and catalytic performance, with profound implications for large-scale HER electrocatalyst production.
date: 2024-02
date_type: published
publisher: Elsevier BV
official_url: https://doi.org/10.1016/j.jcat.2024.115310
full_text_type: other
language: eng
verified: verified_manual
elements_id: 2247531
doi: 10.1016/j.jcat.2024.115310
lyricists_name: Luo, Kai
lyricists_id: KLUOX54
actors_name: Luo, Kai
actors_id: KLUOX54
actors_role: owner
full_text_status: restricted
publication: Journal of Catalysis
volume: 430
article_number: 115310
issn: 0021-9517
citation:        Wang, Q;    Wang, Z;    Zhao, J;    Li, J;    Shen, D;    Xu, LH;    Wu, C;           Wang, Q;  Wang, Z;  Zhao, J;  Li, J;  Shen, D;  Xu, LH;  Wu, C;  Hong Luo, K;   - view fewer <#>    (2024)    Enhancing d-band center modulation in Carbon-Supported CoP via exogenous nitrogen Dopants: A strategy for boosting Ampere-Level hydrogen evolution reaction.                   Journal of Catalysis , 430     , Article 115310.  10.1016/j.jcat.2024.115310 <https://doi.org/10.1016/j.jcat.2024.115310>.      
 
document_url: https://discovery.ucl.ac.uk/id/eprint/10187773/2/Luo%202024%20JCatalysis%20CoP%20accepted.pdf