While the configuration of most metal oxides hollow structures is well established, the synthesis of multinary metal sulfides with complex multi-shelled hollow structures remains in its infancy. Herein, we have developed a facile method to synthesize superhydrophilic CaZnInS double-shelled hollow structures (DSHSs) with the assistance of trisodium citrate bilamellar vesicles, which manifests higher photocatalytic hydrogen generation rate compared with normal CaZnInS single-shelled hollow structures and solid microflowers. Further construction of CdS/CaZnInS S-scheme heterostructures by in situ photodeposition of CdS ultrafine nanoparticles on CaZnInS DSHSs creates an intimate interface coupling and expansive contact region for fast interfacial charge transfer. Consequently, CdS/CaZnInS-5.0 composite exhibits a boosted photocatalytic H evolution of 30.08 mmol h g, which is 2.7 times higher than CaZnInS DSHSs (11.52 mmol h g). Besides, the apparent quantum efficiency of CdS/CaZnInS-5.0 at 370 nm can reach 66.04 %. Moreover, CdS/CaZnInS-5.0 shows good stability for the hydrogen generation reaction. This elaborate design of CdS/CaZnInS-5.0 sheds light on the potential of integrating morphology modulation and S-scheme heterostructures construction with efficient solar energy utilization and optimized charge transfer for catalysis and optoelectronic applications.
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