Protruding Pt single-sites on hexagonal ZnIn2S4 to accelerate photocatalytic hydrogen evolution

• Published in: Nature communications Vol. 13; no. 1; pp. 1287 - 10
• Main Authors: Shi, Xiaowei, Dai, Chao, Wang, Xin, Hu, Jiayue, Zhang, Junying, Zheng, Lingxia, Mao, Liang, Zheng, Huajun, Zhu, Mingshan
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 11.03.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/146; 147/135; 147/143; 147/3; 639/301/299/890; 639/301/357; 639/638/542; Adsorption; Basal plane; Catalysts; Evolution; Holes (electron deficiencies); Humanities and Social Sciences; Hydrogen; Hydrogen evolution; Hydrogen production; Irradiation; Light; Light irradiation; Mass transfer; Metals; multidisciplinary; Nanoparticles; Photocatalysis; Photochemical reactions; Photochemicals; Radiation; Recombination; Science; Science (multidisciplinary); Tetrahedra
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-28995-1

Single-site cocatalysts engineered on supports offer a cost-efficient pathway to utilize precious metals, yet improving the performance further with minimal catalyst loading is still highly desirable. Here we have conducted a photochemical reaction to stabilize ultralow Pt co-catalysts (0.26 wt%) onto the basal plane of hexagonal ZnIn 2 S 4 nanosheets (Pt SS -ZIS) to form a Pt-S 3 protrusion tetrahedron coordination structure. Compared with the traditional defect-trapped Pt single-site counterparts, the protruding Pt single-sites on h -ZIS photocatalyst enhance the H 2 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g −1 h −1 under visible light irradiation. Importantly, through simple drop-casting, a thin Pt SS -ZIS film is prepared, and large amount of observable H 2 bubbles are generated, providing great potential for practical solar-light-driven H 2 production. The protruding single Pt atoms in Pt SS -ZIS could inhibit the recombination of electron-hole pairs and cause a tip effect to optimize the adsorption/desorption behavior of H through effective proton mass transfer, which synergistically promote reaction thermodynamics and kinetics. An alternative approach to defect-trapped Pt single-sites on a semiconductor is reported. Here, protruding Pt sites inhibit charge recombination and cause a tip effect which enhances H 2 evolution yield rates with minimal co-catalyst loading.