Water Oxidation Electrocatalysis with a Cobalt‐Borate‐Based Hybrid System under Neutral Conditions

Abstract The development of new water oxidation electrocatalysts that are both stable and efficient, particularly in neutral conditions, holds great promise for overall water splitting. In this study, the electrocatalytic water oxidation performance of a new cobalt‐based catalyst, Co 3 (BO 3 ) 2 , with a Kotoite‐type crystal structure is investigated under neutral conditions. The catalyst is also hybridized with CNTs to enhance its electrocatalytic properties. A remarkable increase in catalytic current along with a significant shift in the onset overpotential is observed in Co 3 (BO 3 ) 2 @CNT. Additionally, CNT addition also greatly influences the surface concentration of the catalyst: 12.7 nmol cm −2 for Co 3 (BO 3 ) 2 @CNT compared with 3.9 nmol cm −2 for Co 3 (BO 3 ) 2 . Co 3 (BO 3 ) 2 @CNT demands overpotentials of 303 and 487 mV to attain current densities of 1 and 10 mA cm −2 , respectively, at pH 7. Electrochemical and characterization studies performed over varying pH conditions reveal that the catalyst retains its stability over a pH range of 3–14. Multi‐reference quantum chemical calculations are performed to study the nature of the active cobalt sites and the effect of boron atoms on the activity of the cobalt ions.