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从环境空气中捕获和浓缩二氧化碳的可逆氟醇光碱
作者:小柯机器人 发布时间:2025/8/15 17:37:20


近日,美国哈佛大学Liu, Richard Y.团队实现了从环境空气中捕获和浓缩二氧化碳的可逆氟醇光碱。相关论文于2025年8月13日发表在《自然-化学》杂志上。

从点热源和直接从大气中捕获二氧化碳的主要策略面临着热吸附剂再生的高能源成本。由阳光作为唯一的外部刺激驱动的光化学过程提供了一个有前景的替代方案。尽管报道了许多光诱导pH波动的例子,但互补的操作模式,即光切换碱,并没有得到广泛的考虑。这在一定程度上是由于很少有光碱能在水中支持大的、可逆的pH值跳跃。

研究组报道了基于芴醇的Arrhenithem光碱的设计,该光碱利用激发态芳香性和基态反芳香性来产生大的碱度波动和高可逆性。该系统是氧稳定的,可以由自然阳光驱动,并从环境空气中捕获/浓缩二氧化碳。利用瞬态吸收光谱分析了C-O解离的机理,以了解氢氧化物的高效释放。该研究为光可逆水基的设计提供了框架,并为其在太阳能CO2管理中的主题提供了指导原则。

附:英文原文

Title: Reversible fluorenol photobases that perform CO2 capture and concentration from ambient air

Author: Purdy, Michael, Wang, Ariel Y., Drummer, Matthew C., Nocera, Daniel G., Liu, Richard Y.

Issue&Volume: 2025-08-13

Abstract: Leading strategies for the capture of CO2 from point sources and directly from the atmosphere face high energy costs for thermal sorbent regeneration. Photochemical processes, driven by sunlight as the sole external stimulus, offer a promising alternative. Despite many reported examples of light-induced pH swings using metastable photoacids, the complementary mode of operation, using photoswitchable bases, has not been extensively considered. This is due in part to the rarity of photobases that can support large, reversible pH jumps in water. Here we report the design of fluorenol-based Arrhenius photobases that take advantage of excited-state aromaticity and ground-state antiaromaticity to generate large basicity swings with high reversibility. The system is oxygen stable, can be driven by natural sunlight and captures/concentrates CO2 from ambient air. We elucidated the mechanism of C–O dissociation using transient absorption spectroscopy to understand the high efficiency of hydroxide release. This study provides a framework for the design of photoreversible aqueous bases and guiding principles for their use in solar-powered CO2 management.

DOI: 10.1038/s41557-025-01901-0

Source: https://www.nature.com/articles/s41557-025-01901-0

期刊信息

Nature Chemistry:《自然—化学》,创刊于2009年。隶属于施普林格·自然出版集团,最新IF:24.274
官方网址:https://www.nature.com/nchem/
投稿链接:https://mts-nchem.nature.com/cgi-bin/main.plex