Using solar energy and photocatalysts to convert CO2 into high value-added chemicals can simultaneously alleviate the greenhouse effect and energy shortage, being recognized to be a promising alternative to achieve sustainable social development. Single atom cocatalysts decoration has been demonstrated to be effective strategy to improve the CO2 photocatalytic reduction efficiency. Unfortunately, when unraveling the mechanism behind performance promotion, most studies mainly focused on clarifying the superior physicochemical and photoelectrical properties of SACs in comparison with the substrate, the critical role of the sing-atomic state distinguished from those oxide and elemental states was often neglected and remains a mystery hitherto.
Recently, a research team led by Prof. Zhongbiao Wu and Haiqiang Wang from Zhejiang University, China, comprehensively investigated the effect of Pd chemical states on CO2 photocatalytic reduction of g-C3N4 (CN) under visible light irradiation, especially the critical role of Pd-SA in boosting CH4 production. The results were published in Chinese Journal of Catalysis (https://doi.org/10.1016/S1872-2067(22)64199-8).
Performance tests showed Pd species decoration improved the CH4 production of CN, with Pd/CN-SA exhibiting the optimum yields (2.25 μmol g-1), markedly higher than that of PdOx/CN (1.08 μmol g-1) and Pd/CN-NP (0.44 μmol g-1). After comprehensive mechanism analysis with various characterization techniques, in-situ FTIR spectra and DFT calculations, it was found that the conducive activation of CO2, negative conduction band potentials, and excellent •H utilization efficiency, collaboratively the superior CO2 reduction performance of Pd/CN-SA, especially the remarkably boosted CH4 production. Besides, despite the larger electron density of Pd/CN-NP and PdOx/CN, the moderate reduction ability of their photogenerated electrons restricted the further reduction of adsorbed CO2 species and CO intermediate, limiting the enhancement of CO2 reduction activity. Furthermore, the CH4 evolutions of Pd/CN-NP and PdOx/CN were also limited by the poor •H supply and inferior •H utilization efficiency, respectively. The new insights may advance the understanding of CO2 reduction process and inspire the design of efficient photocatalysts for CO2 photocatalytic conversion.
This research was financially supported by National Natural Science Foundation of China (NSFC-51978603, NSFC-51878598), Zhejiang Provincial “151” Talents Program, Program for Zhejiang Leading Team of S&T Innovation (Grant No. 2013TD07) and Changjiang Scholar Incentive Program (Ministry of Education, China, 2009).
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Chinese Journal of Catalysis is co-sponsored by Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Chinese Chemical Society, and it is currently published by Elsevier group. This monthly journal publishes in English timely contributions of original and rigorously reviewed manuscripts covering all areas of catalysis. The journal publishes Reviews, Accounts, Communications, Articles, Highlights, Perspectives, and Viewpoints of highly scientific values that help understanding and defining of new concepts in both fundamental issues and practical applications of catalysis. Chinese Journal of Catalysis ranks among the top two journals in Applied Chemistry with a current SCI impact factor of 12.92. The Editors-in-Chief are Profs. Can Li and Tao Zhang.
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