eprintid: 10177377
rev_number: 8
eprint_status: archive
userid: 699
dir: disk0/10/17/73/77
datestamp: 2023-09-25 11:24:37
lastmod: 2023-09-25 11:24:37
status_changed: 2023-09-25 11:24:37
type: article
metadata_visibility: show
sword_depositor: 699
creators_name: Zhang, Jiajun
creators_name: Feng, Kai
creators_name: Li, Zhengwen
creators_name: Yang, Bin
creators_name: Yan, Binhang
creators_name: Luo, Kai Hong
title: Defect-Driven Efficient Selective CO2 Hydrogenation with Mo-Based Clusters
ispublished: inpress
divisions: UCL
divisions: B04
divisions: C05
divisions: F45
keywords: Mo2C nanoparticle, synthesized fuels, RWGS reaction, atomic magnetism, selective hydrogenation
note: This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
abstract: Synthetic fuels produced from CO2 show promise in combating climate change. The reverse water gas shift (RWGS) reaction is the key to opening the CO2 molecule, and CO serves as a versatile intermediate for creating various hydrocarbons. Mo-based catalysts are of great interest for RWGS reactions featured for their stability and strong metal–oxygen interactions. Our study identified Mo defects as the intrinsic origin of the high activity of cluster Mo2C for CO2-selective hydrogenation. Specifically, we found that defected Mo2C clusters supported on nitrogen-doped graphene exhibited exceptional catalytic performance, attaining a reaction rate of 6.3 gCO/gcat/h at 400 °C with over 99% CO selectivity and good stability. Such a catalyst outperformed other Mo-based catalysts and noble metal-based catalysts in terms of facile dissociation of CO2, highly selective hydrogenation, and nonbarrier liberation of CO. Our study revealed that as a potential descriptor, the atomic magnetism linearly correlates to the liberation capacity of CO, and Mo defects facilitated product desorption by reducing the magnetization of the adsorption site. On the other hand, the defects were effective in neutralizing the negative charges of surface hydrogen, which is crucial for selective hydrogenation. Finally, we have successfully demonstrated that the combination of a carbon support and the carbonization process synergistically serves as a feasible strategy for creating rich Mo defects, and biochar can be a low-cost alternative option for large-scale applications.
date: 2023-09-15
date_type: published
publisher: American Chemical Society (ACS)
official_url: https://doi.org/10.1021/jacsau.3c00206
oa_status: green
full_text_type: pub
language: eng
primo: open
primo_central: open_green
verified: verified_manual
elements_id: 2088283
doi: 10.1021/jacsau.3c00206
lyricists_name: Luo, Kai
lyricists_id: KLUOX54
actors_name: Flynn, Bernadette
actors_id: BFFLY94
actors_role: owner
full_text_status: public
publication: JACS Au
issn: 2691-3704
citation:        Zhang, Jiajun;    Feng, Kai;    Li, Zhengwen;    Yang, Bin;    Yan, Binhang;    Luo, Kai Hong;      (2023)    Defect-Driven Efficient Selective CO2 Hydrogenation with Mo-Based Clusters.                   JACS Au        10.1021/jacsau.3c00206 <https://doi.org/10.1021/jacsau.3c00206>.    (In press).    Green open access   
 
document_url: https://discovery.ucl.ac.uk/id/eprint/10177377/1/jacsau.3c00206.pdf