Nitrogen-Neighbored Single-Cobalt Sites Enable Heterogeneous Oxidase-Type Catalysis
Qi Zhang, Mi Peng, Zirui Gao, Wendi Guo, Zehui Sun, Yi Zhao, Wu Zhou, Meng Wang, Bingbao Mei, Xian‐Long Du, Zheng Jiang, Wei Sun, Chao Liu, Yifeng Zhu, Yongmei Liu, Heyong He, Zhen Hua Li, Ding Ma, Yong Cao
Abstract
The development of biomimetic catalytic systems that can imitate or even surpass natural enzymes remains an ongoing challenge, especially for bioinspired syntheses that can access non-natural reactions. Here, we show how an all-inorganic biomimetic system bearing robust nitrogen-neighbored single-cobalt site/pyridinic-N site (Co–N 4 /Py-N) pairs can act cooperatively as an oxidase mimic, which renders an engaged coupling of oxygen (O 2 ) reduction with synthetically beneficial chemical transformations. By developing this broadly applicable platform, the scalable synthesis of greater than 100 industrially and pharmaceutically appealing O-silylated compounds including silanols, borasiloxanes, and silyl ethers via the unprecedented aerobic oxidation of hydrosilane under ambient conditions is demonstrated. Moreover, this heterogeneous oxidase mimic also offers the potential for expanding the catalytic scope of enzymatic synthesis. We anticipate that the strategy demonstrated here will pave a new avenue for understanding the underlying nature of redox enzymes and open up a new class of material systems for artificial biomimetics.