Two-Electron or Four-Electron Nanocatalysis for Aerobic Glucose Oxidation: A Mechanism-Driven Prediction Model
Xiaoli Wang, Qiao-Zhi Li, Jia‐Jia Zheng, Xingfa Gao
Abstract
The nanomaterial-catalyzed oxidation of glucose can produce H 2 O 2 or H 2 O as the oxygen reduction products. However, the theoretical model predicting the selection between H 2 O 2 and H 2 O products is still lacking, which limits the rational design of aerobic glucose oxidation nanocatalysts for H 2 O 2 -targeted applications in disease diagnoses and therapies. In this work, a mechanism-driven prediction model that can predict whether a nanocatalyst preferably undergoes the 2e-catalysis to produce H 2 O 2 or the 4e-catalysis to produce H 2 O is developed. The development of the model is first based on the reaction thermodynamics, and then a correction constant is introduced in conjunction with experimental reports to compensate to some extent for the lack of consideration of other influencing factors such as the reaction kinetics. The predictive power of the model is verified by density functional theory investigations on the mechanisms and kinetics of the experimentally reported noble metal nanocatalysts. Using the model, binary alloy nanomaterials, which preferably undergo 2e-catalysis to produce H 2 O 2, have been predicted. This work provides theoretical guidelines for the rational design of aerobic glucose oxidation nanocatalysts capable of producing H 2 O 2 and facilitates their application in H 2 O 2 -targeted biomedicine.