Ensemble-Exciting Effect in Pd/alk-Ti 3 C 2 on the Activity for Efficient Hydrogen Production

作者：Yao Feng, Shuyan Guan, Linyan Bian, Yanping Fan, Xianyun Liu, Huanhuan Zhang, Baojun Li, Baozhong Liu · 发表于：ACS Sustainable Chemistry & Engineering · 年份：2021 · DOI：10.1021/acssuschemeng.1c04249 · 被引用次数：73 · 研究领域：MXene and MAX Phase Materials、Hydrogen Storage and Materials、Advanced Photocatalysis Techniques

Creating active sites to improve the mass activity and durability of metal catalysts by elucidating the relationship between the metal and the support is a major challenge. In this study, ultrafine palladium nanoparticles (Pd NPs) were supported on alkalized Ti 3 C 2 (alk-Ti 3 C 2 ) to obtain a catalytically active interfacial ensemble. The catalyst Pd/alk-Ti 3 C 2 with a Pd loading of 1.0 wt % exhibited the highest activity in ammonia borane (AB) hydrolysis reaction, with an initial turnover frequency of 230.6 min –1 . A comprehensive analysis revealed that an ensemble-exciting effect originated from the Pd and the alk-Ti 3 C 2 . The hydroxylation of alk-Ti 3 C 2 regulated the local coordination environment of Pd. Water and AB were effortlessly activated by the −OH group and Pd atom aggregates composed of electron-deficient support alk-Ti 3 C 2 and electron-rich Pd, respectively. The efficient generation of hydrogen at the interface of Pd/alk-Ti 3 C 2 was further guaranteed by the interfacial activation. This work on precision active sites opens new avenues for developing high-activity noble-metal catalysts for AB hydrolysis.