一个原子可以使所有的区别:气体诱导的相变化在Bisimidazole-Linked Diamondoid协调网络
Kyriaki Koupepidou1, Varvara I Nikolayenko1, Debobroto Sensharma1
1Bernal Institute, Department of Chemical Sciences, University of Limerick, Limerick V94 T9PX, Republic of Ireland.
Journal of the American Chemical Society
|April 26, 2023
概括
具有微妙连接器差异的两个协调网络 (CN) 呈现出不同的气体诱导切换行为来储存二氧化碳. 这项研究详细介绍了它们独特的孔隙化学和机制,进步了可控制的气体吸附材料.
科学领域:
- 材料科学
- 化学学
- 纳米技术
背景情况:
- 气体储存应用需要从封闭结构转变为多孔结构的协调网络 (CN).
- 控制这些转型的转换机制和压力仍然是一个重大挑战.
- 现有的CN通常缺乏可调节的孔隙化学,以优化气体吸附.
研究的目的:
- 合成和描述两种新型CN,X-dia-4-Co和X-dia-5-Co,具有不同的链接功能.
- 研究两种CN之间的气体诱导转化机制和毛孔化学差异.
- 探索它们的气体储存应用潜力,特别是二氧化碳的吸收.
主要方法:
- 协调网络的综合 (X-dia-4-Co) 和 (X-dia-5-Co)
- 在不同压力和温度下进行气体吸附分析 (CO2吸收).
- 使用单晶X射线衍射和现场粉末XRD进行结构性表征.
- 通过现场IR进行光谱分析.
- 计算模型包括密度函数理论 (DFT) 和蒙特卡洛模拟.
主要成果:
- 无论是X-dia-4-Co还是X-dia-5-Co,都会从闭合转化为同结构开放阶段,细胞体积增加>27%.
- 在低压下,X-dia-4-Co 呈现逐渐的二氧化碳吸收,而X-dia-5-Co 呈现急剧的阶段性吸收 (类型IV 异温).
- 在N-捐赠者链接剂 (皮里丁与) 的差异导致不同的孔隙化学和切换行为.
- 现场研究和建模阐明了切换机制,并将吸附差异与孔隙化学联系起来.
结论:
- 在CN中,连接器结构的微妙变化会对气体吸附特性和转化机制产生重大影响.
- X-dia-4-Co和X-dia-5-Co的独特孔隙化学和切换行为为设计可控制的气体存储材料提供了洞察力.
- 这些发现为开发具有定制气体吸附能力的先进协调网络铺平了道路.
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