All-Inorganic CsPbBr3 nanocrystals: gram-scale mechanochemical synthesis and selective photocatalytic CO2 reduction to methane
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Accepted version
Supporting information
Author(s)
Kumar, Santosh
Regue, Miriam
Isaacs, Mark
Freeman, Emma
Eslava, Salvador
Type
Journal Article
Abstract
Halide perovskite CsPbBr3 has recently gained wide interest for its application in solar cells, optoelectronics and artificial photosynthesis, but further progress is needed to develop greener and more scalable synthesis procedures and for their application in humid environments. Herein, we report a fast and convenient mechanochemical synthesis of CsPbBr3 perovskite nanocrystals with scale-up capability and control over crystal size and morphology. These perovskite nanocrystals show excellent crystallinity and tunable morphologies, from nanorods to nanospheres and nanosheets, simply changing the mechanochemical reaction conditions such as ball milling time, ball size and Cs precursor. Furthermore, we explore their use for gas-phase photocatalytic CO2 reduction using water vapor as proton source. A photocatalytic conversion of CO2 and H2O(g) to 0.43 (0.03) μmol CH4 g-1 h-1, 2.25 (0.09) μmol CO g-1 h-1 and 0.08 (0.02) μmol H2 g-1 h-1 was for example achieved with CsPbBr3 nanosheets and simulated sunlight, keeping 30% of this activity over three consecutive cycles. When these CsPbBr3 nanosheets were mechanochemically prepared together with Cu-loaded reduced graphene oxide (Cu-RGO), the photocatalytic activity significantly improved to 12.7 (0.95) μmol CH4 g-1 h-1, 0.46 (0.11) μmol CO g-1 h-1 and 0.27 (0.02) μmol H2 g-1 h-1, and a 90% of this activity was retained over three consecutive cycles. The selectivity for CH4 increased to 98.5(0.93)% on an electron basis and a remarkable apparent quantum efficiency of 1.10(0.15)% at 523 nm was achieved. This enhanced activity, selectivity and stability were assigned to the better charge separation, visible light absorption, CO2 adsorption & activation, and hydrophobic character of the obtained composites. These results will contribute to the rational design and application of halide perovskites for CO2 photocatalytic reduction.
Date Issued
2020-05-26
Date Acceptance
2020-04-01
Citation
ACS Applied Energy Materials, 2020, 3 (5), pp.4509-4522
ISSN
2574-0962
Publisher
American Chemical Society (ACS)
Start Page
4509
End Page
4522
Journal / Book Title
ACS Applied Energy Materials
Volume
3
Issue
5
Copyright Statement
© 2020 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Energy Materials, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsaem.0c00195
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Identifier
https://pubs.acs.org/doi/10.1021/acsaem.0c00195
Grant Number
EP/R035407/2
Publication Status
Published
Article Number
acsaem.0c00195
Date Publish Online
2020-04-16