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固态物质体系的维度与化学反应
Dimensions of Solid-State Material Systems and Their Chemical Reactions
【摘要】 随着研究手段的不断进步和完善,结构化学应该从传统地探讨“反应物-产物与化学反应的关系”逐步发展到揭示和利用“凝聚态中物质的动态结构与化学反应的关系”这一高度。当我们在凝聚态体系当中讨论化学反应时,就不能抛却体系结构动态变化及多因素耦合所带来的显著影响。为了便于指明固体物质体系的空间维度与化学反应之间的关联,我们从Bloch理论出发介绍晶体材料体系的空间维度。通过对晶体表面构型特点、低维体系及其异质结构的调控,可以显著改变材料体系的物性,进而影响体系所参与的化学反应,甚至改变反应路径。本文通过碳纳米管在催化丙酸乙酯不对称氢化反应中的表现介绍空间限域效应对催化反应所能产生的多种作用方式。在反应条件下,固体表面自身结构以及其上分布的缺陷、催化剂颗粒等都处于动态变化过程中。除了温度和压强以外,反应体系所处的环境氛围(包括pH值、外电/磁场、光场等等)都会对缺陷和催化活性位点的几何与电子构型产生动态的影响。通过对上述凝聚态化学实例的综合介绍,我们期待能够简单、明了地展示出固体材料结构的维度与动态变化对化学反应的影响,提高对凝聚态结构化学研究的重视。
【Abstract】 With the continuous advancement and refinement of research methodologies, structural chemistry should evolve from the traditional exploration of “the relationship between reactants-products and chemical reactions” to the higher level of revealing and utilizing “the relationship between the dynamic structure of matter in condensed states and its chemical reactions”. When discussing chemical reactions within condensed matter systems, we cannot disregard the significant influences of the dynamic evolutions in their structures and the coupling of environmental factors. To elucidate the connection between the spatial dimensions of solid material systems and chemical reactions, we introduce the spatial dimension of crystal materials by starting from Bloch theory. Changes in spatial dimensions, surface configurations, and heterostructures can significantly alter their physical properties, thereby affecting the related chemical reactions, and even modifying the reaction pathways. In this review, we will discuss the ways in which spatial confinement effects can influence catalytic reactions, as demonstrated by the performance of carbon nanotubes in the asymmetric hydrogenation of ethyl propionate. Under reaction conditions, the intrinsic structure of solid surfaces, as well as the defects and catalyst particles distributed on them, undergo a series of dynamic changes. Beyond temperature and pressure, the environmental conditions of the reaction system(including pH-values, external electric/magnetic fields, optical fields, etc.) can also dynamically influence the geometric and electronic configurations of defects and catalytically active sites. Through a comprehensive introduction to these examples, we aim to clearly and concisely demonstrate how the dimensionality and dynamic changes in solid material structures affect chemical reactions, thereby emphasizing the importance and essentiality of research in condensed matter structural chemistry.
【Key words】 spatial dimensions; local microenvironment effects; spatial confinement effects; defects; dynamic structures;
- 【文献出处】 化学进展 ,Progress in Chemistry , 编辑部邮箱 ,2026年01期
- 【分类号】O621.251
- 【下载频次】8