Oxygen-Activated Boron Nitride for Selective Photocatalytic Coupling of Methanol to Ethylene Glycol

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION(2024)

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摘要
The controllable photocatalytic C-C coupling of methanol to produce ethylene glycol (EG) is a highly desirable but challenging objective for replacing the current energy-intensive thermocatalytic process. Here, we develop a metal-free porous boron nitride catalyst that demonstrates exceptional selectivity in the photocatalytic production of EG from methanol under mild conditions. Comprehensive experiments and calculations are conducted to thoroughly investigate the reaction mechanism, revealing that the OB3 unit in the porous BN plays a critical role in the preferential activation of C-H bond in methanol to form & sdot;CH2OH via a concerted proton-electron transfer mechanism. More prominent energy barriers are observed for the further dehydrogenation of the & sdot;CH2OH intermediate on the OB3 unit, inhibiting the formation of some other by-products during the catalytic process. Additionally, a small downhill energy barrier for the coupling of & sdot;CH2OH in the OB3 unit promotes the selective generation of EG. This study provides valuable insights into the underlying mechanisms and can serve as a guide for the design and optimization of photocatalysts for efficient and selective EG production under mild conditions. Oxygen-activated boron nitride fibers (BNH) have been successfully synthesized and applied for the selective photocatalytic coupling of methanol to ethylene glycol (EG) reaction. The OB3 unit in the BNH plays an important role in the selective dehydrogenation and C-C coupling of methanol molecules, leading to excellent activity and selectivity of BNH for EG production.+ image
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关键词
Photocatalysis,oxygen-doped boron nitride,selective dehydrogenation,C-C coupling,high selectivity
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