从分子筛上纳尺度离散行为控制到宏观煤化工过程

doi:10.11949/0438-1157.20200366

摘要/Abstract

摘要：

化学工业基于对化学反应和化学键的操纵，在横跨超12个数量级的空间和时间尺度上解决传递问题，为人类社会创造和生产新物质。石油的发现和利用将化学工业带入了一个全新的时代，支撑了现代社会的运行，但对中国而言，“富煤贫油少气”的资源特点决定了发展煤化工在中国有独特的战略意义。与石化行业常见的烃类裂化过程不同，现代新型煤化工依赖于小分子原料的自组装，依靠择形分子筛的控制作用高选择性制备燃料和化学品。因此，在亚纳米尺度下，即小分子在择形分子筛上的反应和传递行为不能再被视为连续，而是离散的，这导致了宏观上的拟相变失活等一系列现象。因此，需建立新的方法论理解分子筛上的离散反应和传递行为，用以认识离散尺度在十几个数量级空间和时间尺度延展后对宏观化学过程的影响。本文以纳尺度下分子筛内的离散传递现象为基础，综述了运用图论、小世界网络和先进表征手段分析分子筛内失活与传递现象的研究及发现的一系列新现象，并介绍了基于此进行的分子筛原子级精准结构调变及其对宏观煤化工过程带来的革新。面向未来，本文建立的分析分子筛内离散行为的范式将对精确调变分子筛结构、开发下一代煤化工工艺流程提供全新的思路。

关键词: 分子筛, 离散行为, 煤化工, 图论, 小世界网络

Abstract:

Based on the manipulation of chemical reactions and chemical bonds, the chemical industry solves transport problems on a spatial and temporal scale that exceeds 12 orders of magnitude, creating and producing new substances for human society. The discovery and use of crude oil have brought the chemical industry into a new era and supported the operation of modern society. However, for China, the resource endowment determines that the development of the coal chemical industry has unique strategic significance. Unlike the hydrocarbon cracking process, the modern new coal chemical industry relies on the self-assembly of small molecular from raw materials and the shape-selective effect of zeolites to produce fuels and chemicals with high selectivity. Therefore, at the sub-nanometer scale, that is, the reaction and transfer behavior of small molecules on shape-selective zeolites can no longer be regarded as continuous, but discrete, which leads to a series of phenomena such as deactivation with pseudo-phase transitions on the macroscale. Based on the discrete transfer phenomena in zeolites at the nanoscale, this paper reviews the research and discovery of a series of new phenomena using graph theory, small-world networks, and advanced characterization methods to analyze the deactivation and transfer phenomena. The atomic-level precise structural modification of the zeolite and the innovation it brings to the macro coal chemical process is introduced. Towards the future, the paradigm for analyzing the discrete behavior in zeolites established in this article will provide a new way of thinking for precisely adjusting the zeolite structure and developing the next generation coal chemical process.

Key words: zeolite, discrete behavior, coal chemical industry, graph theory, small-world network

中图分类号:

TQ 201

蔡达理, 熊昊, 张晨曦, 魏飞. 从分子筛上纳尺度离散行为控制到宏观煤化工过程[J]. 化工学报, 2020, 71(9): 3849-3865.

Dali CAI, Hao XIONG, Chenxi ZHANG, Fei WEI. From nanoscale discrete diffusion behavior control to macroscale coal chemical process[J]. CIESC Journal, 2020, 71(9): 3849-3865.

图/表 4

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