Magnetic Mn-Incorporated Cs₃Cu₂Br₅ Nanocrystals for Spin-Polarized Enhanced Photocatalytic Biomass Conversion Coupled with H₂O₂ Evolution

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dc.contributor.authorGuo, M.
dc.contributor.authorTalebian-Kiakalaieh, A.
dc.contributor.authorHashem, E.M.
dc.contributor.authorXia, B.
dc.contributor.authorRan, J.
dc.contributor.authorQiao, S.Z.
dc.date.issued2024
dc.descriptionPublished online: June 8, 2024
dc.description.abstractCopper-based halide perovskite, as an ideal alternative to lead-based halide perovskite, has attracted much attention in many applications owing to its earth-abundant element, non-toxicity, and excellent optical properties. In this report, magnetic Mn-incorporated lead-free copper halide perovskite (Cs₃Cu₂Br₅) nanocrystal (NC) is for the first time designed and prepared using a one-pot hot-injection route, resulting in a new emission band at ≈540 nm accompanied with self-trapped exciton (STE) emission centered at ≈445 nm from Cs₃Cu₂Br₅ NC. In situ X-ray photoelectron spectroscopy and in situ kelvin probe force microscopy (KPFM) confirm that the Mn²⁺ incorporation causes efficient electron–hole separation and extended charge lifetime in Mn-doped Cs₃Cu₂Br₅ NC, which exhibits significantly raised selectively photocatalytic biomass conversion coupled with obviously enhanced H₂O₂ evolution. With an external magnetic field, the spin-polarized electrons in Mn-doped Cs₃Cu₂Br₅ NC arouses reduced charge recombination and more available electrons/holes for surface redox reaction, further raising the photocatalytic performance. This is confirmed by in situ steady-state/transient-state photoluminescence (PL) spectroscopy, in situ transient photocurrent measurement, and in situ electrochemical impedance spectroscopy with external magnetic field. In situ electron paramagnetic resonance (EPR) spectra reveal the radical-involved reaction pathway for biomass conversion. This research exhibits the great potential of spin-polarization-enhanced photocatalysis by an external magnetic field without additional energy consumption.
dc.description.statementofresponsibilityMeijun Guo, Amin Talebian-Kiakalaieh, Elhussein M. Hashem, Bingquan Xia, Jingrun Ran, and Shi-Zhang Qiao
dc.identifier.citationAdvanced Functional Materials, 2024; 34(45):2406356-1-2406356-10
dc.identifier.doi10.1002/adfm.202406356
dc.identifier.issn1616-301X
dc.identifier.issn1616-3028
dc.identifier.orcidGuo, M. [0000-0002-7974-5165]
dc.identifier.orcidHashem, E.M. [0000-0001-7656-2358]
dc.identifier.orcidXia, B. [0000-0003-0909-7788]
dc.identifier.orcidRan, J. [0009-0009-1588-6215]
dc.identifier.orcidQiao, S.Z. [0000-0002-1220-1761] [0000-0002-4568-8422]
dc.identifier.urihttps://hdl.handle.net/2440/142922
dc.language.isoen
dc.publisherWiley
dc.relation.granthttp://purl.org/au-research/grants/arc/DE200100629
dc.relation.granthttp://purl.org/au-research/grants/arc/DP230102027
dc.relation.granthttp://purl.org/au-research/grants/arc/FT230100192
dc.relation.granthttp://purl.org/au-research/grants/arc/LP210301397
dc.relation.granthttp://purl.org/au-research/grants/arc/CE230100032
dc.rights© 2024 The Author(s). Advanced Functional Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
dc.source.urihttp://dx.doi.org/10.1002/adfm.202406356
dc.subjectexternal magnetic field; in situ characterization; Mn-incorporated Cs₃Cu₂Br₅; photocatalysis; spin-polarized electron
dc.titleMagnetic Mn-Incorporated Cs₃Cu₂Br₅ Nanocrystals for Spin-Polarized Enhanced Photocatalytic Biomass Conversion Coupled with H₂O₂ Evolution
dc.title.alternativeMagnetic Mn-Incorporated Cs(3)Cu(2)Br(5) Nanocrystals for Spin-Polarized Enhanced Photocatalytic Biomass Conversion Coupled with H(2)O(2) Evolution
dc.typeJournal article
pubs.publication-statusPublished

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