Van Der Waals gap-rich BiOCl atomic layers realizing efficient, pure-water CO2-to-CO photocatalysis

Nat Commun. 2021 Oct 11;12(1):5923. doi: 10.1038/s41467-021-26219-6.

ABSTRACT

Photocatalytic CO2 reduction (PCR) is able to convert solar energy into chemicals, fuels, and feedstocks, but limited by the deficiencies of photocatalysts in steering photon-to-electron conversion and activating CO2, especially in pure water. Here we report an efficient, pure water CO2-to-CO conversion photocatalyzed by sub-3-nm-thick BiOCl nanosheets with van der Waals gaps (VDWGs) on the two-dimensional facets, a graphene-analog motif distinct from the majority of previously reported nanosheets usually bearing VDWGs on the lateral facets. Compared with bulk BiOCl, the VDWGs-rich atomic layers possess a weaker excitonic confinement power to decrease exciton binding energy from 137 to 36 meV, consequently yielding a 50-fold enhancement in the bulk charge separation efficiency. Moreover, the VDWGs facilitate the formation of VDWG-Bi-VO••-Bi defect, a highly active site to accelerate the CO2-to-CO transformation via the synchronous optimization of CO2 activation, *COOH splitting, and *CO desorption. The improvements in both exciton-to-electron and CO2-to-CO conversions result in a visible light PCR rate of 188.2 μmol g-1 h-1 in pure water without any co-catalysts, hole scavengers, or organic solvents. These results suggest that increasing VDWG exposure is a way for designing high-performance solar-fuel generation systems.

PMID:34635665 | DOI:10.1038/s41467-021-26219-6

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