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通过金钯/氮化镓实现从一氧化碳到甲醇的氧原子接枝来进行甲醇的光合作用。

Photosynthesis of CHOH via oxygen-atom-grafting from CO to CH enabled by AuPd/GaN.

作者信息

Su Hui, Han Jing-Tan, Miao Botong, Salehi Mahdi, Li Chao-Jun

机构信息

Department of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC, H3A 0B8, Canada.

Department of Chemical Engineering, McGill University, Montreal, QC, H3A 0C5, Canada.

出版信息

Nat Commun. 2024 Jul 31;15(1):6435. doi: 10.1038/s41467-024-50801-3.

Abstract

The direct co-conversion of methane and carbon dioxide into valuable chemicals has been a longstanding scientific pursuit for carbon neutrality and combating climate change. Herein, we present a photo-driven chemical process that reforms these two major greenhouse gases together to generate green methanol and CO, two high-valued industrial chemicals. Isotopic labeling and control experiments indicate an oxygen-atom-graft occurs, wherein CO transfers one O into the C-H bond of CH via photo-activated interfacial catalysis with AuPd nanoparticles supported on GaN. The photoexcited AuPd/GaN interface effectively orchestrates the CH oxidation and the CO reduction producing 13.66 mmol g of CHOH yield over 10 h. This design provides a solid scientific basis for the photo-driven oxygen-atom-grafting process to be further extended to visible light region.

摘要

将甲烷和二氧化碳直接转化为有价值的化学品,一直是实现碳中和和应对气候变化的长期科学追求。在此,我们展示了一种光驱动化学过程,该过程将这两种主要温室气体一起进行重整,以生成绿色甲醇和一氧化碳这两种高价值工业化学品。同位素标记和对照实验表明发生了氧原子接枝,其中一氧化碳通过负载在氮化镓上的金钯纳米颗粒的光活化界面催化将一个氧转移到甲烷的碳氢键中。光激发的金钯/氮化镓界面有效地协调了甲烷氧化和一氧化碳还原,在10小时内产生了13.66 mmol g的甲醇产率。该设计为光驱动氧原子接枝过程进一步扩展到可见光区域提供了坚实的科学基础。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/50d6/11291648/475ceb7b8696/41467_2024_50801_Fig1_HTML.jpg

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