Ultrafast Luminescence Detection with Selective Adsorption of Carbon Disulfide in a Gold(I) Metal−Organic Framework

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-11-27 DOI:10.1002/anie.202413830
Haruka Yoshino, Masaki Saigo, Takumi Ehara, Kiyoshi Miyata, Ken Onda, Jenny Pirillo, Yuh Hijikata, Shinya Takaishi, Wataru Kosaka, Keni-ichi Otake, Susumu Kitagawa, Hitoshi Miyasaka
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Abstract

Although a widely used and important industrial chemical, carbon disulfide (CS2) also poses a number of hazards due to its volatility and toxicity. As such, the development of multifunctional materials for the selective capture and easy recognition of CS2 is one of the crucial issues. Herein, we demonstrate completely selective CS2 adsorption among trials involving H2O, alcohols, volatile organic compounds (including thiol derivatives), N2, H2, O2, CH4, CO, NO, and CO2. We also showcase its fine detection using remarkable luminescent response in an Au(I)‐based metal−organic framework (MOF) of {ZnII(pz)[AuI(CN)2]2} (pz = pyrazine; 1) with a two‐fold interpenetration network. Ex situ single crystal X‐ray diffraction for 1 and CS2 accommodated 1 suggested that the Au···Au atoms are not only luminescent centers but also act as interaction sites for CS2 modulating the Au···Au contacts. These experiments revealed the specificity of CS2 and how changes in the CS2‐induced structure. Based on the obtained structural formation, 1 exhibited a sensitive detecting ability for CS2 with an ultrafast response time of less than 10 s. Ex situ time‐resolved photoluminescence analyses developed in this work implied that CS2 varied the energetic relaxation at the excited states related to the luminescent efficiency of the resultant MOF system.
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利用金(I)金属有机框架对二硫化碳的选择性吸附进行超快发光检测
二硫化碳(CS2)虽然是一种广泛使用的重要工业化学品,但由于其挥发性和毒性,也会带来一些危害。因此,开发用于选择性捕获和轻松识别 CS2 的多功能材料是关键问题之一。在此,我们展示了在涉及 H2O、醇类、挥发性有机化合物(包括硫醇衍生物)、N2、H2、O2、CH4、CO、NO 和 CO2 的试验中对 CS2 的完全选择性吸附。我们还利用具有两倍互穿网络的基于金(I)的金属有机框架(MOF){ZnII(pz)[AuI(CN)2]2}(pz = 吡嗪;1)中的显著发光反应,展示了其精细检测能力。1 和含有 CS2 的 1 的原位单晶 X 射线衍射表明,金-金原子不仅是发光中心,而且还是 CS2 调节金-金接触的相互作用位点。这些实验揭示了 CS2 的特异性以及 CS2 诱导的结构变化。这项工作中开发的原位时间分辨光致发光分析表明,CS2 改变了激发态的能量弛豫,这与生成的 MOF 系统的发光效率有关。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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