Ligand–Metal Charge Transfer Induced <i>via</i> Adjustment of Textural Properties Controls the Performance of Single-Atom Catalysts during Photocatalytic Degradation
Jiaxu Liu, Yajun Zou, Daniel Cruz, Aleksandr Savateev, Markus Antonietti, Gianvito Vilé
Abstract
. We show that adjustment of materials textural properties and therefore metal single-atom coordination mode enables ligand-to-metal charge transfer (LMCT) or ligand-to-metal-to-ligand charge transfer (LMLCT), properties that were long speculated in single-atom catalysis but never observed. We employ the developed materials in the degradation of organic pollutants under irradiation with visible light. Kinetic investigations under flow conditions show that single atoms of Ag and Cu decrease the number of toxic organic fragmentation products while leading to a higher selectivity toward full degradation. The results correlate with the selected mode of charge transfer in the designed photocatalysts and provide a new understanding of how the local environment of a single-atom catalyst affects the surface structure and reactivity. The concepts can be exploited further to rationally design and optimize other single-atom materials.