Single-Atom Ru Catalyst-Decorated CNF(ZnO) Nanocages for Efficient H<sub>2</sub> Evolution and CH<sub>3</sub>OH Production
Chandra Shobha Vennapoosa, Sagar Varangane, B. Moses Abraham, Vidha Bhasin, Santanu Bhattacharyya, Xuefeng Wang, Ujjwal Pal, Debabrata Chatterjee
Abstract
The presence of transition-metal single-atom catalysts effectively enhances the interaction between the substrate and reactant molecules, thus exhibiting extraordinary catalytic performance. In this work, we for the first time report a facile synthetic procedure for placing highly dispersed Ru single atoms on stable CNF(ZnO) nanocages. We unravel the atomistic nature of the Ru single atoms in CNF(ZnO)/Ru systems using advanced HAADF-STEM, HRTEM, and XANES analytical methods. Density functional theory calculations further support the presence of ruthenium single-atom sites in the CNF(ZnO)/Ru system. Our work further demonstrates the excellent photocatalytic ability of the CNF(ZnO)/Ru system with respect to H 2 production (5.8 mmol g –1 h –1 ) and reduction of CO 2 to CH 3 OH [249 μmol (g of catalyst) −1 ] with apparent quantum efficiencies of 3.8% and 1.4% for H 2 and CH 3 OH generation, respectively. Our studies unambiguously demonstrate the presence of atomically dispersed ruthenium sites in CNF(ZnO)/Ru catalysts, which greatly enhance charge transfer, thus facilitating the aforementioned photocatalytic redox reactions.