Enantioselective synthesis of amino acids by photocatalytic reduction of CO2 on chiral mesostructured ZnS

IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Chem Pub Date : 2025-05-08 Epub Date: 2025-01-27 DOI:10.1016/j.chempr.2024.102390
Yongping Cui , Jing Ai , Yingying Duan , Menghui Jia , Tianwei Ouyang , Aokun Liu , Lu Yu , Junhong Liu , Xi Liu , Chaoyang Chu , Yuanbo Li , Yanhang Ma , Liwei Chen , Lu Han , Jinquan Chen , Changlin Tian , Shunai Che , Yuxi Fang
{"title":"Enantioselective synthesis of amino acids by photocatalytic reduction of CO2 on chiral mesostructured ZnS","authors":"Yongping Cui ,&nbsp;Jing Ai ,&nbsp;Yingying Duan ,&nbsp;Menghui Jia ,&nbsp;Tianwei Ouyang ,&nbsp;Aokun Liu ,&nbsp;Lu Yu ,&nbsp;Junhong Liu ,&nbsp;Xi Liu ,&nbsp;Chaoyang Chu ,&nbsp;Yuanbo Li ,&nbsp;Yanhang Ma ,&nbsp;Liwei Chen ,&nbsp;Lu Han ,&nbsp;Jinquan Chen ,&nbsp;Changlin Tian ,&nbsp;Shunai Che ,&nbsp;Yuxi Fang","doi":"10.1016/j.chempr.2024.102390","DOIUrl":null,"url":null,"abstract":"<div><div>Reduction and fixation of CO<sub>2</sub> in natural systems via solar energy generate diverse products, ranging from small molecules to biomolecules. To date, only a few multicarbon species have been obtained by artificial CO<sub>2</sub> photoreduction, especially abiotic photosynthesis of biomolecules with various functional groups, which is a challenging issue. Herein, we report the photocatalytic synthesis of amino acids from CO<sub>2</sub> and NH<sub>3</sub> on a chiral mesostructured ZnS (CMZ). Serine is the main component of various amino acids, with an enantiomeric excess (<em>ee</em>) greater than 96% and a total yield of over 30 μmol g<sub>cat</sub><sup>−1</sup>. We propose that the chirality-induced spin polarization of CMZ boosts the creation of triplet OCCO by aligning its parallel electron spins, and the helical lattice distortion reduces the free energy of <sup>∗</sup>OCCO. Enantiospecific activation energies of reactions driven by the spin-polarized electrons in CMZ lead to the formation of enantiomeric amino acids.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 5","pages":"Article 102390"},"PeriodicalIF":19.6000,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chem","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2451929424006351","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/1/27 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

Reduction and fixation of CO2 in natural systems via solar energy generate diverse products, ranging from small molecules to biomolecules. To date, only a few multicarbon species have been obtained by artificial CO2 photoreduction, especially abiotic photosynthesis of biomolecules with various functional groups, which is a challenging issue. Herein, we report the photocatalytic synthesis of amino acids from CO2 and NH3 on a chiral mesostructured ZnS (CMZ). Serine is the main component of various amino acids, with an enantiomeric excess (ee) greater than 96% and a total yield of over 30 μmol gcat−1. We propose that the chirality-induced spin polarization of CMZ boosts the creation of triplet OCCO by aligning its parallel electron spins, and the helical lattice distortion reduces the free energy of OCCO. Enantiospecific activation energies of reactions driven by the spin-polarized electrons in CMZ lead to the formation of enantiomeric amino acids.

Abstract Image

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
手性介观结构ZnS上CO2光催化还原氨基酸的对映选择性合成
通过太阳能在自然系统中减少和固定二氧化碳产生各种各样的产品,从小分子到生物分子。迄今为止,通过人工CO2光还原获得的多碳物种很少,特别是具有各种官能团的生物分子的非生物光合作用,这是一个具有挑战性的问题。本文报道了手性介孔结构ZnS (CMZ)上CO2和NH3光催化合成氨基酸。丝氨酸是各种氨基酸的主要成分,其对映体过剩量(ee)大于96%,总产率大于30 μmol gcat−1。我们提出CMZ的手性诱导自旋极化通过排列其平行电子自旋来促进三重态OCCO的产生,并且螺旋晶格畸变降低了∗OCCO的自由能。由CMZ中自旋极化电子驱动的反应的对映体激活能导致对映体氨基酸的形成。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
Chem
Chem Environmental Science-Environmental Chemistry
CiteScore
32.40
自引率
1.30%
发文量
281
期刊介绍: Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.
期刊最新文献
Aqueous-phase organic photochemistry: Distinct modes and interfaces Trace-water-mediated formamidinium cation anchoring to regulate crystallization of tin-lead perovskite for efficient and stable photovoltaics Hyperspace mapping and iterative dimensionality reduction reveal radical cascade networks controlled by perovskite-type catalysts A new class of nickel precatalysts for cross-coupling: Nickel(I) isocyanide complexes A metal-ion-linked self-assembled molecular layer as a robust hole-selective contact for perovskite solar cells
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1