Photochromic single atom Ag/TiO2 catalysts for selective CO2 reduction to CH4

Literature Information

Publication Date 2023-12-07
DOI 10.1039/D3EE02800C
Impact Factor 38.532
Authors

Chaogang Ban, Yang Wang, Yajie Feng, Zhouhao Zhu, Youyu Duan, Jiangping Ma, Xu Zhang, Xue Liu, Kai Zhou, Hanjun Zou


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Abstract

Photocatalytic production of CH4 from CO2 and H2O is recognized as one of the most sustainable approaches to address the environmental and energy crises. However, this strategy is severely plagued by the poor activity and low selectivity due to the inefficient electron production, inadequate proton supply and insufficient stabilization of the key intermediates. Herein, a new design concept of photochromic single atom photocatalysis is proposed to overcome these issues simultaneously. As a prototype, single Ag atoms anchored TiO2 nanoparticles reveal rapid and macroscopic photochromic behavior upon light irradiation, which is attributed to the trapping of photogenerated electrons. The generated colored state effectively suppresses the combination of photogenerated carriers and improves their migration. Further mechanistic analyses suggest that the isolated Ag atoms act as the dominant active sites to capture CO2 and stabilize the key C1 intermediate, while the adjacent Ti sites promote the activation of H2O for the generation of more protons, thereby together providing highly active sites to boost the production of CH4 instead of CO. As a result, an extraordinary activity of 46.0 μmol g−1 h−1 and an ultrahigh electron selectivity of ∼91% for CH4 production are achieved. The proposed all-in-one design concept, especially the macroscopic electron-trapping photochromism, opens a new avenue to substantially enhance the yield efficiency of photogenerated electrons to accelerate various photocatalytic reduction reactions.

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Source Journal

Energy & Environmental Science

Energy & Environmental Science
CiteScore: 32.34
Self-citation Rate: 3.4%
Articles per Year: 481

Energy & Environmental Science is an international journal dedicated to publishing exceptionally important and high quality, agenda-setting research tackling the key global and societal challenges of ensuring the provision of energy and protecting our environment for the future. The scope is intentionally broad and the journal recognises the complexity of issues and challenges relating to energy conversion and storage, alternative fuel technologies and environmental science. For work to be published it must be linked to the energy-environment nexus and be of significant general interest to our community-spanning readership. All scales of studies and analysis, from impactful fundamental advances, to interdisciplinary research across the (bio)chemical, (bio/geo)physical sciences and chemical engineering disciplines are welcomed. Topics include, but are not limited to, the following: Solar energy conversion and photovoltaics Solar fuels and artificial photosynthesis Fuel cells Hydrogen storage and (bio) hydrogen production Materials for energy systems Capture, storage and fate of CO2, including chemicals and fuels from CO2 Catalysis for a variety of feedstocks (for example, oil, gas, coal, biomass and synthesis gas) Biofuels and biorefineries Materials in extreme environments Environmental impacts of energy technologies Global atmospheric chemistry and climate change as related to energy systems Water-energy nexus Energy systems and networks Globally applicable principles of energy policy and techno-economics

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