Gao Zhuyan, Montini Tiziano, Mu Junju, Luo Nengchao, Fonda Emiliano, Fornasiero Paolo, Wang Feng
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
J Am Chem Soc. 2024 Sep 4;146(35):24440-24449. doi: 10.1021/jacs.4c06573. Epub 2024 Aug 20.
Supported metal in the form of single atoms, clusters, and particles can individually or jointly affect the activity of supported heterogeneous catalysts. While the individual contribution of the supported metal to the overall activity of supported photocatalysts has been identified, the joint activity of mixed metal species is overlooked because of their different photoelectric properties. Here, atomically dispersed Pd (Pd) and Pd clusters are loaded onto CdS, serving as oxidation and reduction sites for methanol dehydrogenation. The Pd substitutes Cd, forming hole-trapping states for methanol oxidation and assisting the dispersion of photodeposited Pd clusters. Therefore, methanol dehydrogenation on CdS with supported Pd and Pd clusters exhibits the highest turnover frequency of 1.14 s based on the Pd content and affords H and HCHO with a similar apparent quantum yield of 87 ± 1% at 452 nm under optimized reaction conditions. This work highlights the synergistic catalysis of supported metal for improved photocatalytic activity.
以单原子、团簇和颗粒形式存在的负载型金属可以单独或共同影响负载型多相催化剂的活性。虽然已经确定了负载型金属对负载型光催化剂整体活性的单独贡献，但由于混合金属物种具有不同的光电性质，其联合活性被忽视了。在这里，原子分散的钯（Pd）和钯团簇负载在硫化镉上，作为甲醇脱氢的氧化和还原位点。钯取代镉，形成甲醇氧化的空穴捕获态，并有助于光沉积钯团簇的分散。因此，在优化的反应条件下，负载有钯和钯团簇的硫化镉上的甲醇脱氢基于钯含量表现出最高的1.14 s-1的周转频率，并在452 nm处提供氢和甲醛，表观量子产率相似，为87±1%。这项工作突出了负载型金属的协同催化作用，以提高光催化活性。
