Abstract

H2O dissociation plays a crucial role in solar-driven catalytic CO2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (Vo) rich CeO2 catalyst with single-atom Ni anchored around its surface Vo sites by replacing Ce atoms to promote H2O dissociation and achieve effective photothermal CO2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH4 production and prevents Vo from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d-impurity orbitals, thereby inducing more effective H2O activation. The catalyst presents a CH4 yield of 192.75 µmol/cm2/h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H2O-activating catalysts for CO2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.

This work reports a single-atom Ni incorporated CeO2 catalyst that boosts the efficiency of solar CO2 reduction under concentrated light irradiation.

Details

Title
Concentrated solar CO2 reduction in H2O vapour with >1% energy conversion efficiency
Author
Ren, Yuqi 1 ; Fu, Yiwei 2 ; Li, Naixu 1 ; You, Changjun 1 ; Huang, Jie 2 ; Huang, Kai 1   VIAFID ORCID Logo  ; Sun, Zhenkun 3 ; Zhou, Jiancheng 1 ; Si, Yitao 1 ; Zhu, Yuanhao 1   VIAFID ORCID Logo  ; Chen, Wenshuai 4   VIAFID ORCID Logo  ; Duan, Lunbo 5 ; Liu, Maochang 2   VIAFID ORCID Logo 

 Southeast University, School of Chemistry and Chemical Engineering, Nanjing, PR China (GRID:grid.263826.b) (ISNI:0000 0004 1761 0489) 
 Xi’an Jiaotong University, International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an, PR China (GRID:grid.43169.39) (ISNI:0000 0001 0599 1243) 
 School of Energy and Environment, Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Nanjing, PR China (GRID:grid.263826.b) 
 Northeast Forestry University, Key Laboratory of Bio-Based Material Science and Technology, Ministry of Education, Harbin, PR China (GRID:grid.412246.7) (ISNI:0000 0004 1789 9091) 
 School of Energy and Environment, Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Nanjing, PR China (GRID:grid.412246.7) 
Pages
4675
Publication year
2024
Publication date
2024
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
3062955936
Copyright
© The Author(s) 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.