Polyoxometalate‐Based Single‐Atom Catalyst with Precise Structure and Extremely Exposed Active Site for Efficient H 2 Evolution

• Published in: Angewandte Chemie International Edition
• Main Authors: Zhang, Zhuo‐Ran, Sui, He‐Yu, Shi, Wen‐Xiong, Ren, Jing, Yao, Shuang, Lu, Tong‐Bu, Zhang, Zhi‐Ming
• Format: Journal Article
• Language: English
• Published: 31.10.2024
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202416711

Abstract Single‐atom catalysts with precise structure and extremely high catalytic efficiency remain a fervent focus in the fields of materials chemistry and catalytic science. Herein, a nickel‐substituted polyoxometalate (POM) {NiSb 6 O 4 (H 2 O) 3 [β‐Ni(hmta)SbW 8 O 31 ] 3 } 15− (NiPOM) with one extremely exposed nickel site [NiO 3 (H 2 O) 3 ] was synthesized using the conventional aqueous method. The uniform dispersion of single nickel center with well‐defined structure was facilely achieved by anchoring nanosized NiPOM on graphene oxide (GO). The resulting NiPOM/GO can couple with CdS photoabsorber for the construction of low‐cost and ultra‐efficient hydrogen evolution system. The H 2 yield can reach to 2753.27 mmol g POM −1 h −1 , which represents a record value among all the POM‐based photocatalytic systems. Remarkablely, an extremely high hydrogen yield of 3647.28 mmol g POM −1 h −1 was achieved with simultaneous photooxidation of commercial waste plastic, representing the first POM‐based photocatalytic system for H 2 evolution and waste plastic conversion. This work highlights a straightforward strategy for constructing extremely exposed single‐metal site with precise microenvironment by facilely manipulating nanosized molecular cluster to control individual atom.