Shihao Li, Jiafu Shi, Yu Chen, Xinyu Mao, Shusong Liu, Yang Yang, Hong Wu, Zhongyi Jiang
{"title":"Light-Driven Synthesis of 2-Aminoethanol from Formaldehyde and Ammonia","authors":"Shihao Li, Jiafu Shi, Yu Chen, Xinyu Mao, Shusong Liu, Yang Yang, Hong Wu, Zhongyi Jiang","doi":"10.1021/acscatal.5c00337","DOIUrl":null,"url":null,"abstract":"Amino alcohols are widely used in chemical and pharmaceutical industries, while conventional synthesis methods face drawbacks such as low selectivity and high energy consumption. Multienzyme catalysis combined with light-driven cofactor regeneration affords a platform of light-driven synthesis of chemicals, where the transfer of electrons and protons as well as the route of enzymatic reactions dominates the energy conversion efficiency and atomic economy of carbon utilization. Herein, we construct a light-driven synthesis system comprising an energy-supplying module and a multienzyme catalytic module for 2-aminoethanol synthesis from formaldehyde and ammonia. First, a S-scheme heterojunction photocatalysts with a metal–organic framework core and a bipyridine-based conjugated polymer shell are prepared as an energy-supplying module. Through synergistic intensification of proton transfer and electron transfer, the photocatalysts render cofactor (NADH) regeneration efficiency with a turnover frequency of 30.49 h<sup>–1</sup>. Second, a multienzyme catalytic module is constructed for 2-aminoethanol synthesis in the presence of NADH. Under optimal conditions, this module produces 2-aminoethanol with an average reaction rate of 76.34 μmol L<sup>–1</sup> h<sup>–1</sup> within 24 h. Finally, the energy-supplying module is coupled with the multienzyme catalytic module for continuous synthesis of 2-aminoethanol from formaldehyde and ammonia, generating 0.55 mmol L<sup>–1</sup> 2-aminoethanol after 4 light–dark cycles. In addition, triethanolamine (TEOA) and glucose, a biomass-derived carbon source, are both confirmed as effective electron donors for NADH regeneration and light-driven synthesis system. This work opens a pathway for the synthesis of amino alcohols and demonstrates a paradigm for the intensification of reaction processes.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"44 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.5c00337","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Amino alcohols are widely used in chemical and pharmaceutical industries, while conventional synthesis methods face drawbacks such as low selectivity and high energy consumption. Multienzyme catalysis combined with light-driven cofactor regeneration affords a platform of light-driven synthesis of chemicals, where the transfer of electrons and protons as well as the route of enzymatic reactions dominates the energy conversion efficiency and atomic economy of carbon utilization. Herein, we construct a light-driven synthesis system comprising an energy-supplying module and a multienzyme catalytic module for 2-aminoethanol synthesis from formaldehyde and ammonia. First, a S-scheme heterojunction photocatalysts with a metal–organic framework core and a bipyridine-based conjugated polymer shell are prepared as an energy-supplying module. Through synergistic intensification of proton transfer and electron transfer, the photocatalysts render cofactor (NADH) regeneration efficiency with a turnover frequency of 30.49 h–1. Second, a multienzyme catalytic module is constructed for 2-aminoethanol synthesis in the presence of NADH. Under optimal conditions, this module produces 2-aminoethanol with an average reaction rate of 76.34 μmol L–1 h–1 within 24 h. Finally, the energy-supplying module is coupled with the multienzyme catalytic module for continuous synthesis of 2-aminoethanol from formaldehyde and ammonia, generating 0.55 mmol L–1 2-aminoethanol after 4 light–dark cycles. In addition, triethanolamine (TEOA) and glucose, a biomass-derived carbon source, are both confirmed as effective electron donors for NADH regeneration and light-driven synthesis system. This work opens a pathway for the synthesis of amino alcohols and demonstrates a paradigm for the intensification of reaction processes.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.