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Tri(pyridinyl)pyridine Viologen-Based Kagome Dual Coordination Polymer with Selective Chromic Response to Soft X-ray and Volatile Organic Amines.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-06-19 , DOI: 10.1021/acs.inorgchem.0c00922 Shi-Li Li 1 , Mei Li 1 , Yan Zhang 1 , Hui-Min Xu 1 , Xian-Ming Zhang 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-06-19 , DOI: 10.1021/acs.inorgchem.0c00922 Shi-Li Li 1 , Mei Li 1 , Yan Zhang 1 , Hui-Min Xu 1 , Xian-Ming Zhang 1
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The development of new responsive smart materials has been highly desirable in the recent decade due to growing demand in our daily life, and extended viologen-based coordination polymers are regarded as proper and promising candidates for stimuli-responsive study. A tri(pyridinyl)pyridine viologen-based Kagome dual (kgd) topological coordination polymer, [Mn3Cl4(tpptb)2]·Cl2·(H2O)2, (tpptb = N,N′,N″-tri(3-carboxybenzyl)-2,4,6-tri(pyridinium-4-yl)pyridine; 1) has been solvothermally synthesized, which can selectively respond to soft X-ray Al–Kα (λ = 8.357 Å) irradiation but not to UV light and hard X-rays of λ < 1.5418 Å at room temperature. Appealingly, 1 is very sensitive and convenient for the visual detection of various volatile amine vapors, especially ethylamine vapors at a low concentration of 100 ppm, and the vapochromic sample can be recovered after exposure in the air at room temperature. The sequence of amines in vapochromism could be rationalized by combined consideration of vapor pressure, the molecular size, and electron-donor ability of various amine molecules as well as the void spaces of 1. In addition, 1 exhibits an obvious hydrochromic transformation upon heating in the air and an anhydrous atmosphere. Combined XPS and EPR confirmed that these physical and chemical stimuli can cause electron transfer from electron-rich groups to quaternary nitrogen atoms of the ligand to generate charge-separated radicals, leading to soft X-ray-induced photochromic and selective vapochromic behavior of 1. Such behavior indicates that it will become a convenient, recyclable, and practical multifunctional material for chemical and environmental sensing. These results provide an effective avenue for the rational design and synthesis of multifunctional chromic materials for potential use in sensing devices.
中文翻译：
三（吡啶基）吡啶基于紫精的Kagome双配位聚合物，对软X射线和挥发性有机胺具有选择性色性。
由于对日常生活的需求不断增长，近十年来人们一直非常希望开发新的响应型智能材料，并且基于长紫精的配位聚合物被认为是刺激响应研究的合适且有希望的候选者。基于三（吡啶基）吡啶的紫精基的Kagome双（kgd）拓扑配位聚合物[Mn 3 Cl 4（tpptb）2 ]·Cl 2 ·（H 2 O）2，（tpptb = N，N'，N''-三（3-羧基苄基）-2,4,6-三（吡啶-4-基）吡啶; 1）是溶剂热合成的，在室温下可以选择性地响应软X射线Al-Kα（λ= 8.357Å）辐射，但不响应紫外光和λ<1.5418Å的硬X射线。有吸引力的是，1对各种挥发性胺蒸气（尤其是低浓度100 ppm的乙胺蒸气）的视觉检测非常灵敏且方便，并且在室温下暴露于空气后可以回收气相色谱样品。可以通过综合考虑蒸气压力，各种胺分子的分子大小和电子给体能力以及1的空隙空间来合理化气相致变色中胺的序列。另外，1在空气和无水气氛中加热时，表现出明显的水致变色转变。结合XPS和EPR证实，这些物理和化学刺激会导致电子从富电子基团转移到配体的季氮原子上，从而产生电荷分离的自由基，从而导致X射线引起的软变色和选择性的vapochromic行为1。这种行为表明它将成为一种方便，可回收且实用的用于化学和环境传感的多功能材料。这些结果为合理设计和合成潜在用于传感设备的多功能铬材料提供了有效途径。
更新日期：2020-07-06
中文翻译：
三（吡啶基）吡啶基于紫精的Kagome双配位聚合物，对软X射线和挥发性有机胺具有选择性色性。
由于对日常生活的需求不断增长，近十年来人们一直非常希望开发新的响应型智能材料，并且基于长紫精的配位聚合物被认为是刺激响应研究的合适且有希望的候选者。基于三（吡啶基）吡啶的紫精基的Kagome双（kgd）拓扑配位聚合物[Mn 3 Cl 4（tpptb）2 ]·Cl 2 ·（H 2 O）2，（tpptb = N，N'，N''-三（3-羧基苄基）-2,4,6-三（吡啶-4-基）吡啶; 1）是溶剂热合成的，在室温下可以选择性地响应软X射线Al-Kα（λ= 8.357Å）辐射，但不响应紫外光和λ<1.5418Å的硬X射线。有吸引力的是，1对各种挥发性胺蒸气（尤其是低浓度100 ppm的乙胺蒸气）的视觉检测非常灵敏且方便，并且在室温下暴露于空气后可以回收气相色谱样品。可以通过综合考虑蒸气压力，各种胺分子的分子大小和电子给体能力以及1的空隙空间来合理化气相致变色中胺的序列。另外，1在空气和无水气氛中加热时，表现出明显的水致变色转变。结合XPS和EPR证实，这些物理和化学刺激会导致电子从富电子基团转移到配体的季氮原子上，从而产生电荷分离的自由基，从而导致X射线引起的软变色和选择性的vapochromic行为1。这种行为表明它将成为一种方便，可回收且实用的用于化学和环境传感的多功能材料。这些结果为合理设计和合成潜在用于传感设备的多功能铬材料提供了有效途径。
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