posted on 2019-04-17, 00:00authored byLan Yuan, Sung-Fu Hung, Zi-Rong Tang, Hao Ming Chen, Yujie Xiong, Yi-Jun Xu
Probing the dynamic evolution of
catalyst structure and chemical
state under operating conditions is highly important for investigating
the reaction mechanism of catalysis more in depth, which in turn advances
the rational design of redox catalysis in using renewable energy to
produce fuels. Herein, the evolution of atomically dispersed Cu species
supported by mesoporous TiO2 (mTiO2) during the in situ photocatalytic reduction of CO2 with H2O to valuable solar fuels has been reported. The
results unveil that the initial atomically dispersed Cu(II) undergoes
reduction to Cu(I) and ultimately to Cu(0); the Cu(I)/Cu(0) mixture
is proposed to be more effective for CH4 formation. In
addition, the enhanced CO2 adsorption ability benefited
from the structural advantage of mTiO2 and the elevated charge carrier transfer synergistically contributes
to the CO2 photoreduction. It is anticipated that this
work would guide the rational design of Cu-based light-harvesting
catalysts for artificial CO2 reduction to value-added feedstocks
and inspire further interest in using in situ techniques to study
the structure–activity interplay of photocatalysts under operating
reaction conditions.