Twisted BiOCl Moire\nSuperlattices for Photocatalytic\nChloride Reforming of Methane

Solar-driven conversion of CH<sub>4</sub> into value-added\nmethyl\nchlorides and H<sub>2</sub> with abundant chloride ions offers a sustainable\nCH<sub>4</sub> reforming strategy but suffers from inefficient Cl<sup>–</sup> activation and severe e<sup>–</sup>–h<sup>+</sup> recombination in traditional photocatalysts. Herein, we demonstrate\nthat BiOCl moiré superlattices with a 11.1° twist angle\nare highly efficient for photocatalytic CH<sub>4</sub> reforming into\nCH<sub>3</sub>Cl and H<sub>2</sub> with NaCl. These moiré superlattices,\nfeaturing misalignment-induced tensile strains, destabilize surface\nBi–Cl bonds, facilitating a hole-mediated MvK-analogous process\nto activate lattice Cl into reactive <sup>•</sup>Cl for CH<sub>4</sub> chlorination. Meanwhile, their twisted stacking configurations\nreinforce interlayer electronic coupling and thus accelerate out-of-plane\ncarrier transfer. Along with surface anchoring of single-atom Pt sites\nfor H<sub>2</sub> evolution, the resulting Pt<sub>1</sub>/BiOCl moiré\nsuperlattices deliver a CH<sub>3</sub>Cl yield of 53.4 μmol\ng<sup>–1</sup> h<sup>–1</sup> with an impressive selectivity\nof 96% under visible light. This study highlights the potential of\nlattice engineering in two-dimensional photocatalysts to regulate\nstructural strains and carrier dynamics for the decentralized reforming\nof CH<sub>4</sub>.

Publication Details

Journal
Figshare
Published
2024-11-12
DOI
https://doi.org/10.1021/jacs.4c13254.s001
Primary Topic
Advanced Photocatalysis Techniques
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article
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article

Twisted BiOCl Moire\nSuperlattices for Photocatalytic\nChloride Reforming of Methane

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Advanced Photocatalysis Techniques
article

Twisted BiOCl Moire\nSuperlattices for Photocatalytic\nChloride Reforming of Methane

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Abstract

Solar-driven conversion of CH<sub>4</sub> into value-added\nmethyl\nchlorides and H<sub>2</sub> with abundant chloride ions offers a sustainable\nCH<sub>4</sub> reforming strategy but suffers from inefficient Cl<sup>–</sup> activation and severe e<sup>–</sup>–h<sup>+</sup> recombination in traditional photocatalysts. Herein, we demonstrate\nthat BiOCl moiré superlattices with a 11.1° twist angle\nare highly efficient for photocatalytic CH<sub>4</sub> reforming into\nCH<sub>3</sub>Cl and H<sub>2</sub> with NaCl. These moiré superlattices,\nfeaturing misalignment-induced tensile strains, destabilize surface\nBi–Cl bonds, facilitating a hole-mediated MvK-analogous process\nto activate lattice Cl into reactive <sup>•</sup>Cl for CH<sub>4</sub> chlorination. Meanwhile, their twisted stacking configurations\nreinforce interlayer electronic coupling and thus accelerate out-of-plane\ncarrier transfer. Along with surface anchoring of single-atom Pt sites\nfor H<sub>2</sub> evolution, the resulting Pt<sub>1</sub>/BiOCl moiré\nsuperlattices deliver a CH<sub>3</sub>Cl yield of 53.4 μmol\ng<sup>–1</sup> h<sup>–1</sup> with an impressive selectivity\nof 96% under visible light. This study highlights the potential of\nlattice engineering in two-dimensional photocatalysts to regulate\nstructural strains and carrier dynamics for the decentralized reforming\nof CH<sub>4</sub>.

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