Journal
NATURE CATALYSIS
Volume 3, Issue 8, Pages 649-655Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-020-0476-3
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Funding
- National Key R&D Program of China [2018YFA0209301]
- National Natural Science Foundation of China [U1905214, 21961142019, 21425309, 21761132002, 21861130353, 21802021, 21973014, 51701170, 51871058]
- Chang Jiang Scholars Program of China [T2016147]
- project of science and technology plan of Fujian Province [2018J01520]
- 111 Project [D16008]
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Unraveling how reactive facets promote photocatalysis at the molecular level remains a grand challenge, while identification of the reactive facets can provide guidelines for designing highly efficient photocatalysts and unravelling the microscopic mechanisms behind them. Recently, a series of polytriazine imides (PTIs) was reported with highly crystalline structures; all had a relatively low photocatalytic activity for overall water splitting. Here, high-angle annular dark-field scanning transmission electron microscopy, energy dispersive spectroscopy mapping, and aberration-corrected integrated differential phase contrast imaging were used to study PTI/Li+Cl- single crystals before and after in situ photodeposition of co-catalysts, showing that the prismatic {10 (1) over bar0} planes are more photocatalytically reactive than the basal {0001} planes. Theoretical calculations confirmed that the electrons are energetically favourable to transfer toward the {10 (1) over bar0} planes. Upon this discovery, PTI/Li+Cl- crystals with different aspect ratios were prepared, and the overall water splitting performance followed a linear correlation with the relative surface areas of the {10 (1) over bar0} and {0001} planes. Our controlling of the reactive facets directly instructs the development of highly efficient polymer photocatalysts for overall water splitting.
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