In recent times, the theoretical prediction of catalytic efficiency is of utmost urgency. With the advent of density functional theory (DFT), reliable computations can delineate a quantitative aspect of the study. To this state-of-the art approach, valuable incorporation would be a tool that can acknowledge the efficiency of a catalyst. In the current work, we developed the efficiency conceptualization model (ECM) method that utilizes the quantum mechanical tool to achieve efficiency in terms of turnover frequency (TOF). Twenty-six experimentally designed transition metal (TM) water oxidation catalysts were chosen under similar experimental conditions of temperature, pressure, and pH to execute the same. The computations conclude that the Fe based [Fe(OTf)2(Me2Pytacn)] (MWOC-17) is a highly active catalyst and, therefore, can endure for more time in the catalytic cycle. Our results conclude that the Ir-based catalysts [Cp∗Ir(κ2-N,O)X] with MWOC-23: X = Cl; and MWOC-24: X = NO3 report the highest computed turnover numbers (TONs), Γ0computed TON of 406 and 490 against the highest experimental TONs, Γ0 experimental TON of 2000 and 1200 respectively, whereas the Co-based [Co(12-TMC)]2+ (MWOC-19) has the lowest TONs (Γ0computed TON = 19, Γ0 experimental TON= 16) among the chosen catalysts and thereby successful in corroborating the previous experimental results.
Keywords: Catalysis; Density Functional Theory (DFT); Efficiency Conceptualization Model (ECM); Turnover Frequency (TOF); water splitting.
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