受生物启发的同核双原子铁活性位点调节实现高效防污渗透能量转换

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhe Li, Donghai Wu, Qingchen Wang, Qixiang Zhang, Peng Xu, Fangning Liu, Shibo Xi, Dongwei Ma, Yizhong Lu, Lei Jiang, Zhen Zhang
{"title":"受生物启发的同核双原子铁活性位点调节实现高效防污渗透能量转换","authors":"Zhe Li,&nbsp;Donghai Wu,&nbsp;Qingchen Wang,&nbsp;Qixiang Zhang,&nbsp;Peng Xu,&nbsp;Fangning Liu,&nbsp;Shibo Xi,&nbsp;Dongwei Ma,&nbsp;Yizhong Lu,&nbsp;Lei Jiang,&nbsp;Zhen Zhang","doi":"10.1002/adma.202408364","DOIUrl":null,"url":null,"abstract":"<p>Membrane-based reverse electrodialysis is globally recognized as a promising technology for harnessing osmotic energy. However, its practical application is greatly restricted by the poor anti-fouling ability of existing membrane materials. Inspired by the structural and functional models of natural cytochrome <i>c</i> oxidases (C<i>c</i>O), the first use of atomically precise homonuclear diatomic iron composites as high-performance osmotic energy conversion membranes with excellent anti-fouling ability is demonstrated. Through rational tuning of the atomic configuration of the diatomic iron sites, the oxidase-like activity can be precisely tailored, leading to the augmentation of ion throughput and anti-fouling capacity. Composite membranes featuring direct Fe-Fe motif configurations embedded within cellulose nanofibers (CNF/Fe-DACs-P) surpass state-of-the-art CNF-based membranes with power densities of ca. 6.7 W m<sup>−2</sup> and a 44.5-fold enhancement in antimicrobial performance. Combined, experimental characterization and density functional theory simulations reveal that homonuclear diatomic iron sites with metal-metal interactions can achieve ideally balanced adsorption and desorption of intermediates, thus realizing superior oxidase-like activity, enhanced ionic flux, and excellent antibacterial activity.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"36 46","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion\",\"authors\":\"Zhe Li,&nbsp;Donghai Wu,&nbsp;Qingchen Wang,&nbsp;Qixiang Zhang,&nbsp;Peng Xu,&nbsp;Fangning Liu,&nbsp;Shibo Xi,&nbsp;Dongwei Ma,&nbsp;Yizhong Lu,&nbsp;Lei Jiang,&nbsp;Zhen Zhang\",\"doi\":\"10.1002/adma.202408364\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Membrane-based reverse electrodialysis is globally recognized as a promising technology for harnessing osmotic energy. However, its practical application is greatly restricted by the poor anti-fouling ability of existing membrane materials. Inspired by the structural and functional models of natural cytochrome <i>c</i> oxidases (C<i>c</i>O), the first use of atomically precise homonuclear diatomic iron composites as high-performance osmotic energy conversion membranes with excellent anti-fouling ability is demonstrated. Through rational tuning of the atomic configuration of the diatomic iron sites, the oxidase-like activity can be precisely tailored, leading to the augmentation of ion throughput and anti-fouling capacity. Composite membranes featuring direct Fe-Fe motif configurations embedded within cellulose nanofibers (CNF/Fe-DACs-P) surpass state-of-the-art CNF-based membranes with power densities of ca. 6.7 W m<sup>−2</sup> and a 44.5-fold enhancement in antimicrobial performance. Combined, experimental characterization and density functional theory simulations reveal that homonuclear diatomic iron sites with metal-metal interactions can achieve ideally balanced adsorption and desorption of intermediates, thus realizing superior oxidase-like activity, enhanced ionic flux, and excellent antibacterial activity.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":\"36 46\",\"pages\":\"\"},\"PeriodicalIF\":27.4000,\"publicationDate\":\"2024-09-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/adma.202408364\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.202408364","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

基于膜的反向电渗析技术是全球公认的利用渗透能的前景广阔的技术。然而,由于现有膜材料的防污能力较差,其实际应用受到很大限制。受天然细胞色素 c 氧化酶(CcO)结构和功能模型的启发,研究人员首次将原子精确的同核双原子铁复合材料用作具有优异抗污能力的高性能渗透能转换膜。通过合理调整二原子铁位点的原子构型,可以精确定制类似氧化酶的活性,从而提高离子吞吐量和防污能力。在纤维素纳米纤维(CNF/Fe-DACs-P)中直接嵌入铁-铁图案构型的复合膜超越了最先进的基于 CNF 的膜,其功率密度约为 6.7 W m-2,抗菌性能提高了 44.5 倍。实验表征和密度泛函理论模拟相结合,揭示了具有金属-金属相互作用的同核二原子铁位点可实现理想的中间产物吸附和解吸平衡,从而实现卓越的氧化酶样活性、增强的离子通量和出色的抗菌活性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion

Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion

Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion

Membrane-based reverse electrodialysis is globally recognized as a promising technology for harnessing osmotic energy. However, its practical application is greatly restricted by the poor anti-fouling ability of existing membrane materials. Inspired by the structural and functional models of natural cytochrome c oxidases (CcO), the first use of atomically precise homonuclear diatomic iron composites as high-performance osmotic energy conversion membranes with excellent anti-fouling ability is demonstrated. Through rational tuning of the atomic configuration of the diatomic iron sites, the oxidase-like activity can be precisely tailored, leading to the augmentation of ion throughput and anti-fouling capacity. Composite membranes featuring direct Fe-Fe motif configurations embedded within cellulose nanofibers (CNF/Fe-DACs-P) surpass state-of-the-art CNF-based membranes with power densities of ca. 6.7 W m−2 and a 44.5-fold enhancement in antimicrobial performance. Combined, experimental characterization and density functional theory simulations reveal that homonuclear diatomic iron sites with metal-metal interactions can achieve ideally balanced adsorption and desorption of intermediates, thus realizing superior oxidase-like activity, enhanced ionic flux, and excellent antibacterial activity.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
×
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
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
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 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信