Selective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2

Yajuan Ma, Xiaoxuan Yi, Shaolei Wang, Tao Li, Bien Tan, Chuncheng Chen, Tetsuro Majima, Eric R. Waclawik, Huaiyong Zhu and Jingyu Wang ()
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Yajuan Ma: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
Xiaoxuan Yi: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
Shaolei Wang: Key Laboratory of Polyoxometalate Science of Education Institution, Faculty of Chemistry, Northeast Normal University
Tao Li: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
Bien Tan: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
Chuncheng Chen: Key Laboratory of Photochemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences
Tetsuro Majima: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
Eric R. Waclawik: School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology
Huaiyong Zhu: School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology
Jingyu Wang: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Direct photocatalytic CO2 reduction from primary sources, such as flue gas and air, into fuels, is highly desired, but the thermodynamically favored O2 reduction almost completely impedes this process. Herein, we report on the efficacy of a composite photocatalyst prepared by hyper-crosslinking porphyrin-based polymers on hollow TiO2 surface and subsequent coordinating with Pd(II). Such composite exhibits high resistance against O2 inhibition, leading to 12% conversion yield of CO2 from air after 2-h UV-visible light irradiation. In contrast, the CO2 reduction over Pd/TiO2 without the polymer is severely inhibited by the presence of O2 ( ≥ 0.2 %). This study presents a feasible strategy, building Pd(II) sites into CO2-adsorptive polymers on hollow TiO2 surface, for realizing CO2 reduction with H2O in an aerobic environment by the high CO2/O2 adsorption selectivity of polymers and efficient charge separation for CO2 reduction and H2O oxidation on Pd(II) sites and hollow TiO2, respectively.

Date: 2022
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DOI: 10.1038/s41467-022-29102-0

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