Confinement of CsPbBr3 Perovskite Nanocrystals into Extra-large-pore Zeolite for Efficient and Stable Photocatalytic Hydrogen Evolution

Shiqin Gao; Bolun Wang; Feijian Chen; Guangyuan He; Tianjun Zhang; Lin Li; Junyan Li; Yida Zhou; Binyao Feng; Donghai Mei; Jihong Yu

doi:10.1002/anie.202319996

Confinement of CsPbBr₃ Perovskite Nanocrystals into Extra-large-pore Zeolite for Efficient and Stable Photocatalytic Hydrogen Evolution

Angew Chem Int Ed Engl. 2024 Apr 8;63(15):e202319996. doi: 10.1002/anie.202319996. Epub 2024 Feb 23.

Authors

Shiqin Gao^{1

2}, Bolun Wang^{1

2}, Feijian Chen^{1

2}, Guangyuan He³, Tianjun Zhang⁴, Lin Li⁵, Junyan Li^{1

6}, Yida Zhou¹, Binyao Feng¹, Donghai Mei³, Jihong Yu^{1

2}

Affiliations

¹ State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, 130012, Changchun, China.
² International Center of Future Science, Jilin University, 130012, Changchun, China.
³ School of Materials Science and Engineering, State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, 300387, Tianjin, China.
⁴ College of Chemistry and Materials Science, Hebei University, 071002, Baoding, China.
⁵ Electron Microscopy Center, Jilin University, 130012, Changchun, China.
⁶ Center for High-resolution Electron Microscopy (CħEM), School of Physical Science and Technology, ShanghaiTech University, 201210, Shanghai, China.

PMID: 38316641
DOI: 10.1002/anie.202319996

Abstract

Metal halide perovskites (MHPs), renowned for their outstanding optoelectronic properties, hold significant promise as photocatalysts for hydrogen evolution reaction (HER). However, the low stability and insufficient exposure of catalytically active sites of bulky MHPs seriously impair their catalytic efficiency. Herein, we utilized an extra-large-pore zeolite ZEO-1 (JZO) as a host to confine and stabilize the CsPbBr₃ nanocrystals (3.4 nm) for boosting hydrogen iodide (HI) splitting. The as-prepared CsPbBr₃@ZEO-1 featured sufficiently exposed active sites, superior stability in acidic media, along with intrinsic extra-large pores of ZEO-1 that were favorable for molecule/ion adsorption and diffusion. Most importantly, the unique nanoconfinement effect of ZEO-1 led to the narrowing of the band gap of CsPbBr₃, allowing for more efficient light utilization. As a result, the photocatalytic HER rate of the as-prepared CsPbBr₃@ZEO-1 photocatalyst was increased to 1734 μmol ⋅ h^-1 ⋅ g^-1 _(CsPbBr3) under visible light irradiation compared with bulk CsPbBr₃ (11 μmol ⋅ h^-1 ⋅ g^-1 _(CsPbBr3)), and the long-term durability (36 h) can be achieved. Furthermore, Pt was incorporated with well-dispersed CsPbBr₃ nanocrystals into ZEO-1, resulting in a significant enhancement in activity (4826 μmol ⋅ h^-1 ⋅ g^-1 _(CsPbBr3)), surpassing most of the Pt-integrated perovskite-based photocatalysts. Density functional theory (DFT) calculations and charge-carrier dynamics investigation revealed that the dramatically boosted photocatalytic performance of Pt/CsPbBr₃@ZEO-1 could be attributed to the promotion of charge separation and transfer, as well as to the substantially lowered energy barrier for HER. This work highlights the advantage of extra-large-pore zeolites as the nanoscale platform to accommodate multiple photoactive components, opening up promising prospects in the design and exploitation of novel zeolite-confined photocatalysts for energy harvesting and storage.

Keywords: H2 evolution; Nanoconfinement; Perovskite; Photocatalysis; Zeolite.

Abstract

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