Recently, an article entitled “Support work-function dependent Fenton-like catalytic activity of Co single atoms for selective cobalt(IV)=O generation” was published in Science Bulletin by Mingce Long's group from the School of Environmental Science and Engineering, Shanghai Jiao Tong University.
In the study, the reaction of Co-SACs activated PMS for Co IV =O generation was systematically investigated by loading cobalt single atoms on the surfaces of graphene, MnO 2 , ZrO 2 , and TiO 2 with different prior facets using a strong electrostatic adsorption method. The Co IV =O generated on Co-SACs was determined by in-situ Co K-edge XAS, and the steady-state concentration of Co IV =O in Co-SACs/PMS was determined and found to be positively correlated with the work function of supports. The in-situ characterization and theoretical calculations revealed that the supports with a high W F value like anatase-TiO 2 facilitate the binding of PMS-terminal oxo-ligand to Co sites by extracting Co-d electrons, thus decreasing the generation barrier for the critical intermediate (Co-OOSO 3 2− ). The normalized steady-state concentration of Co IV =O in Co-TiO 2 /PMS system was three orders of magnitude higher than that of free radicals, and 1.3- to 11-fold higher than that generated in other Co-SACs/PMS systems. The Co-TiO 2 /PMS continuously and efficiently removed sulfamethoxazole (SMX) from water under continuous flow operation. Overall, these results underscore the significance of support selection for enhanced generation of high-valent metal-oxo species and efficient PMS activation in supported metal SACs.
Science Bulletin