为推进实现碳达峰、碳中和的目标,煤炭作为我国能源结构的基础原料,其利用的清洁化、高效化需要持续深化内涵。量子化学作为解释微观结构及作用机制的重要理论,目前已被广泛应用于煤化学领域,为煤炭研究提供更多微观信息,以促进煤炭清洁高效利用技术的发展。基于此,概述了量子化学计算在优化煤炭模型分子结构、探讨煤炭清洁高效转化反应机理和明确反应影响因素作用机制3方面的应用,重点对煤热解、燃烧、气化及液化过程中存在的微观问题进行分析、梳理,涉及煤的热解和燃烧过程中的氮元素迁移转化机理、煤基特征官能团与CO2的气化特性、煤液化微观机理中的氢转移反应,以及气氛和催化剂等因素的作用机制等,最后就匹配煤炭变质程度的演变模型、煤炭反应过程中的多因素作用影响机制、完整转化机理、催化剂优化、创新集成工艺等问题,对量子化学在煤炭清洁高效转化领域中有待深入挖掘的科学问题进行了总结与展望,力图为煤炭清洁转化利用技术的研究和应用提供启示。

In the pursuit of carbon peak and neutrality targets, China′s significant reliance on coal as a primary energy source requires ongoing focus on its clean and efficient utilization. Quantum chemistry, a theoretical method used to analyze microstructure and mechanisms,has played a crucial role in coal chemistry research. By providing microscopic information, quantum chemistry has facilitated the development of clean and efficient coal utilization technology. This review aimed to summarize the application of quantum chemistry in optimizingthe molecular structure of coal models, studying reaction mechanisms, and analyzing factors affecting reactions. It also highlighted the microscopic challenges encountered in coal pyrolysis, combustion, gasification, and liquefaction, includingthe migration and transformation mechanism of nitrogen during coal pyrolysis and combustion, the gasification characteristics between functional groups and CO2, thehydrogen transfer mechanism of coal liquefaction, and the mechanism of influencing factors, such as atmosphere and catalyst. Lastly, itprovided an overview of scientific challenges faced by quantum chemistry in the field of clean and efficient coal transformation, which involvedin the evolution model of coal metamorphism, the mechanism of multi-factor effect in coal reaction, the complete transformation mechanism, catalyst optimization, and innovative integration process, offering insights for the advancement and application of clean coal technology.

0 引言

1 煤炭清洁利用存在的微观问题

   1.1 煤炭分子结构优化

   1.2 煤炭清洁高效转化反应机理

   1.3 反应影响因素作用机制

2 煤炭清洁利用的量子化学计算

   2.1 煤的热解

   2.2 煤的燃烧

   2.3 煤的气化

   2.4 煤的液化

3 结语及展望