Shi Xiaowei, Dai Chao, Wang Xin, Hu Jiayue, Zhang Junying, Zheng Lingxia, Mao Liang, Zheng Huajun, Zhu Mingshan
Department of Applied Chemistry, Zhejiang University of Technology, 310032, Hangzhou, P.R. China.
Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, 511443, Guangzhou, P.R. China.
Nat Commun. 2022 Mar 11;13(1):1287. 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 ZnInS nanosheets (Pt-ZIS) to form a Pt-S 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 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g h under visible light irradiation. Importantly, through simple drop-casting, a thin Pt-ZIS film is prepared, and large amount of observable H bubbles are generated, providing great potential for practical solar-light-driven H production. The protruding single Pt atoms in Pt-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.
在载体上设计的单位点助催化剂提供了一种经济高效的利用贵金属的途径,然而,以最小的催化剂负载进一步提高性能仍然是非常可取的。在这里,我们进行了光化学反应,将超低Pt助催化剂(0.26 wt%)稳定在六方ZnInS纳米片(Pt-ZIS)的基面上,形成Pt-S突出四面体配位结构。与传统的缺陷捕获Pt单位点对应物相比,h-ZIS光催化剂上突出的Pt单位点将析氢产率提高了2.2倍,在可见光照射下可达17.5 mmol g h。重要的是,通过简单的滴铸法制备了薄的Pt-ZIS薄膜,并产生了大量可观察到的H气泡,为实际的太阳能驱动制氢提供了巨大潜力。Pt-ZIS中突出的单个Pt原子可以抑制电子-空穴对的复合,并通过有效的质子传质产生尖端效应,以优化H的吸附/解吸行为,从而协同促进反应的热力学和动力学。