Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 30, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202203249
Keywords
Carbon Dioxide Photoreduction; Energy Barrier; Noble-Metal Doping; Water Activation
Categories
Funding
- National Key R&D Program of China [2019YFA0210004]
- National Natural Science Foundation of China [22125503, 21975242, U2032212, 21890754]
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB36000000]
- Youth Innovation Promotion Association of CAS [CX2340007003]
- Major Program of Development Foundation of Hefei Center for Physical Science and Technology [2020HSC-CIP003]
- Users with Excellence Program of Hefei Science Center CAS [2020HSC-UE001]
- University Synergy Innovation Program of Anhui Province [GXXT-2020-001]
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In this study, noble-metal-doped two-dimensional metal oxide nanosheets were designed for selective CO2 photoreduction to CH4. The Pd-doped CeO2 nanosheets achieved nearly 100% CH4 selectivity with a CH4 evolution rate of 41.6 mu mol g(-1) h(-1).
Here, noble-metal-doped two-dimensional metal oxide nanosheets are designed to realize selective CO2 photoreduction to CH4. As a prototype, Pd-doped CeO2 nanosheets are fabricated, where the active sites of Pd delta+ (2<4) and Ce3+-O-v are revealed by quasi in situ X-ray photoelectron spectra and in situ electron paramagnetic resonance spectra. Moreover, in situ Fourier-transform infrared spectra of D2O photodissociation and desorption verify the existence of the Pd-OD bond, implying that Pd delta+ sites can participate in water oxidation to deliver H* species for facilitating the protonation of the intermediates. Furthermore, theoretical calculations suggest the Pd doping could regulate the formation energy barrier of the key intermediates CO* and CH3O*, thus making CO2 reduction to CH4 become the favorable process. Accordingly, Pd-doped CeO2 nanosheets achieve nearly 100 % CH4 selectivity of CO2 photoreduction, with the raising CH4 evolution rate of 41.6 mu mol g(-1) h(-1).
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