Accelerated discovery of superoxide-dismutase nanozymes via high-throughput computational screening

Zhenzhen Wang,Hui Wei,Yuliang Zhao,Jia-Jia Zheng,Liang Yan,Xiaomei Shen,Jiangjiexing Wu,Xingfa Gao

doi:10.1038/s41467-021-27194-8

Abstract

The activity of nanomaterials (NMs) in catalytically scavenging superoxide anions mimics that of superoxide dismutase (SOD). Although dozens of NMs have been demonstrated to possess such activity, the underlying principles are unclear, hindering the discovery of NMs as the novel SOD mimics. In this work, we use density functional theory calculations to study the thermodynamics and kinetics of the catalytic processes, and we develop two principles, namely, an energy level principle and an adsorption energy principle, for the activity. The first principle quantitatively describes the role of the intermediate frontier molecular orbital in transferring electrons for catalysis. The second one quantitatively describes the competition between the desired catalytic reaction and undesired side reactions. The ability of the principles to predict the SOD-like activities of metal-organic frameworks were verified by experiments. Both principles can be easily implemented in computer programs to computationally screen NMs with the intrinsic SOD-like activity.

Highlights

The activity of nanomaterials (NMs) in catalytically scavenging superoxide anions mimics that of superoxide dismutase (SOD)
To protect cells from O2−, biosystems have evolved a specific family of metalloenzyme called superoxide dismutases (SOD), which catalyze the dismutation of O2− to form biologically less harmful species, hydrogen peroxide (H2O2) and O2 (Fig. 1a)
Using density functional theory (DFT) calculations, we computationally studied the rearrangements of HO2 radicals on the surfaces of nanoceria[32] and noble metals[33] in the gas phase, which suggested that the catalyst surfaces influence the catalytic activity by tuning the kinetic stability of the intermediate structures involved in the rearrangements[32,33]

Summary

Introduction

The activity of nanomaterials (NMs) in catalytically scavenging superoxide anions mimics that of superoxide dismutase (SOD). To verify the energy level principle, we have calculated the electronic density of states (DOSs) for all materials listed, whose SOD-like catalytic activities have been experimentally confirmed before. The energy level principle provides the criterion to screen out NMs as potential catalysts and new insight into the catalysis mechanism.

Results

Conclusion