Interfacial-engineered cobalt@carbon hybrids for synergistically boosted evolution of sulfate radicals toward green oxidation

Efficient water remediation relies on robust and capable catalysts to drive the cutting-edge purification technologies. In this work, Prussian blue analogues (PBA) are engaged as the starting materials to fabricate various transition metal (TM)@carbon composites for water decontamination. The encapsulated metallic cobalt is unveiled to be more favorable to deliver electrons to the adjacent carbons than CoP and Co₃O₄, due to the low work function, high conductivity and formation of multiple Co-C bonds for electron tunnelling. Such a hybrid structure significantly tailors the electron density of the carbon lattice, which is the decisive factor influencing activating peroxymonosulfate (PMS) to generate highly reactive sulfate radicals for degradation of contaminants, meanwhile achieving outstanding long-term stability. Deliberate material design and theoretical computations unveil the structure-activity regimes of the composite materials in promoted carbocatalysis. This proof-of-concept study dedicates to elucidating the principles in developing fine-tuned and high-performance TM@carbon hybrids for advanced catalytic oxidation.