Abstract

Photocatalytic hydrogen evolution (PHE) is a sustainable alternative for generating green and clean energy. However, it requires the use of nanoscale photocatalysts, whose applicability is limited by their poor reusability and proton release from water molecules. Herein, a porous two-dimensional lamellar membrane (2DLM) photocatalyst was fabricated from bismuth oxychloride (BiOCl) nanosheets (BNs) and cellulose nanofibers (CNFs) via layer-by-layer self-assembly. The hybridization of the CNFs with the BNs improved the PHE rate of the resulting BiOCl/CNFs membrane (BCM). The optimal PHE rate was observed for a CNF content of 3.2 wt% and was 4.7-times that of raw BNs dispersed in an aqueous solution alone and 1.85-times that of the BiOCl membrane (BM). Moreover, the PHE rate remained unchanged even after 10 discontinuous cycles for a total time of 60 h. Comprehensive experimental characterization and molecular dynamics simulations confirmed that the introduction of the CNFs effectively regulated the hydrogen bond network of the confined water molecules, thus improving the efficiency of the conversion of H2O into H2. Meanwhile, the optimization of the nanochannel sizes of the BNs by the hybridized CNFs accelerated water transport within the nanochannels. The 2DLM also showed excellent mechanical strength, flexibility, and translucence. This strategy of fabricating 2DLMs using a nanosheet photocatalyst and CNFs not only results in improved PHE performance but also should also aid the development of stable and reusable photocatalysts for other industrial applications.

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