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Journal Article
Concentrated solar CO2 reduction in H2O vapour with >1% energy conversion efficiency
2024
Overview
H
2
O dissociation plays a crucial role in solar-driven catalytic CO
2
methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V
o
) rich CeO
2
catalyst with single-atom Ni anchored around its surface V
o
sites by replacing Ce atoms to promote H
2
O dissociation and achieve effective photothermal CO
2
reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH
4
production and prevents V
o
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 H
2
O activation. The catalyst presents a CH
4
yield of 192.75 µmol/cm
2
/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 H
2
O-activating catalysts for CO
2
reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
This work reports a single-atom Ni incorporated CeO
2
catalyst that boosts the efficiency of solar CO
2
reduction under concentrated light irradiation.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
