American Chemical Society
am8b15540_si_001.pdf (1.59 MB)

Fe–N–C Artificial Enzyme: Activation of Oxygen for Dehydrogenation and Monoxygenation of Organic Substrates under Mild Condition and Cancer Therapeutic Application

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journal contribution
posted on 2018-09-24, 00:00 authored by Fei He, Li Mi, Yanfei Shen, Toshiyuki Mori, Songqin Liu, Yuanjian Zhang
Developing highly efficient biomimetic catalysts that directly use O2 as the terminal oxidant to dehydrogenate and monoxygenate substrates with high selectivity under mild conditions has long been pursued but rarely achieved yet. Herein, we report that heterogeneous Fe–N–C, which is commonly used as an electrocatalyst for oxygen reduction reaction, had unusual biomimetic catalytic activity in both dehydrogenation and monoxygenation of a series of organic molecules (∼100% selectivity) by directly using O2. The Fe–Nx center was verified to be the active site that reductively activated O2 by spontaneously generating specific reactive oxygen species (ROS) (1O2, O2•–, and H2O2). Aided by these ROS, under physiological conditions, the Fe–N–C was further successfully exampled to kill proliferative lung cancer cells. Fe–N–C had several striking superior features with respect to natural enzymes, classical heterogeneous nanozymes, and homogeneous artificial enzymes incapable of working under harsh conditions (extreme pH and high temperature), ease of separation and recycling, and direct use of O2. It would open up a new vista of Fe–N–C as an artificial enzyme in biomimetic catalysis, ranging from fundamental simulation of oxidase/oxygenase metabolism to industrial oxidation processes and to disease treatment.