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甲酸光驱动产氢及其在酶促氢化反应中的应用研究进展

State-of-the-Art Light-Driven Hydrogen Generation from Formic Acid and Utilization in Enzymatic Hydrogenations.

作者信息

Peng Yong, Sakoleva Thaleia, Rockstroh Nils, Bartling Stephan, Schoenmakers Pierre, Lim Guiyeoul, Wei Duo, Bayer Thomas, Dörr Mark, Böttcher Dominique, Lauterbach Lars, Junge Henrik, Bornscheuer Uwe T, Beller Matthias

机构信息

Leibniz-Institut für Katalyse e. V. (LIKAT Rostock), Albert-Einstein-Str. 29a, 18059, Rostock, Germany.

Dept. of Biotechnology & Enzyme Catalysis, Institute of Biochemistry, University of Greifswald, Felix-Hausdorff-Str. 4, 17487, Greifswald, Germany.

出版信息

ChemSusChem. 2025 Feb 16;18(4):e202401811. doi: 10.1002/cssc.202401811. Epub 2024 Nov 9.

Abstract

A concept of combining photocatalytically generated hydrogen with green enzymatic reductions is demonstrated. The developed photocatalytic formic acid (FA) dehydrogenation setup based on Pt(x)@TiO shows stable hydrogen generation activity, which is two orders of magnitude higher than reported values of state-of-the-art systems. Mechanistic studies confirm that hydrogen generation proceeds via a photocatalytic pathway, which is entirely different from purely thermal reaction mechanisms previously reported. The viability of the presented approach is demonstrated by the synthesis of value-added compounds 3-phenylpropanal and (2R, 5S)-dihydrocarvone at ambient pressure and room temperature, which should be applicable for many other hydrogenation processes, e. g., for the preparation of flavours and fragrance compounds, as well as pharmaceuticals.

摘要

展示了一种将光催化产生的氢气与绿色酶促还原相结合的概念。基于Pt(x)@TiO开发的光催化甲酸(FA)脱氢装置表现出稳定的产氢活性,比现有最先进系统的报道值高两个数量级。机理研究证实,产氢通过光催化途径进行,这与先前报道的纯热反应机理完全不同。在常压和室温下合成增值化合物3-苯基丙醛和(2R, 5S)-二氢香芹酮证明了所提出方法的可行性,该方法应适用于许多其他氢化过程,例如用于制备香料和香精化合物以及药物。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/92c0/11826123/687b0a280041/CSSC-18-e202401811-g002.jpg

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