Photocatalytic aerobic oxidation of C(sp3)-H bonds

Lei Zhang; Run-Han Li; Xiao-Xin Li; Shengyao Wang; Jiang Liu; Xiao-Xuan Hong; Long-Zhang Dong; Shun-Li Li; Ya-Qian Lan

doi:10.1038/s41467-024-44833-y

Photocatalytic aerobic oxidation of C(sp³)-H bonds

Nat Commun. 2024 Jan 15;15(1):537. doi: 10.1038/s41467-024-44833-y.

Authors

Affiliations

¹ School of Chemistry, South China Normal University, Guangzhou, 510006, P. R. China.
² School of Chemistry, South China Normal University, Guangzhou, 510006, P. R. China. xxli@m.scnu.edu.cn.
³ College of Science, Huazhong Agricultural University, Wuhan, 430070, P. R. China.
⁴ School of Chemistry, South China Normal University, Guangzhou, 510006, P. R. China. yqlan@m.scnu.edu.cn.

^# Contributed equally.

Abstract

In modern industries, the aerobic oxidation of C(sp³)-H bonds to achieve the value-added conversion of hydrocarbons requires high temperatures and pressures, which significantly increases energy consumption and capital investment. The development of a light-driven strategy, even under natural sunlight and ambient air, is therefore of great significance. Here we develop a series of hetero-motif molecular junction photocatalysts containing two bifunctional motifs. With these materials, the reduction of O₂ and oxidation of C(sp³)-H bonds can be effectively accomplished, thus realizing efficient aerobic oxidation of C(sp³)-H bonds in e.g., toluene and ethylbenzene. Especially for ethylbenzene oxidation reactions, excellent catalytic capacity (861 mmol g cat^-1) is observed. In addition to the direct oxidation of C(sp³)-H bonds, CeBTTD-A can also be applied to other types of aerobic oxidation reactions highlighting their potential for industrial applications.