Insight into the molecular structure construction and pyrolysis mechanism simulation of typical carbonaceous feedstocks for the rapid design and preparation of porous carbon-based materials

Illustration of the development prospects of theoretical studies for typical carbonaceous feedstocks. [Display omitted] •Provide a theoretical perspective towards diverse molecular structures.•Offer a thorough understanding of recent theoretical progress in pyrolysis mechanisms.•Delve into basic molecular dynamics principles for accurate and reliable results.•Evaluate the prospects for the rational design of carbon-based porous materials. Typical carbonaceous feedstocks, such as coal, asphalt, biomass, and resin polymers, serve as precursors for the production of high-performance porous carbon materials due to their abundance and cost-effectiveness. However, the distinct chemical composition and physical structural variations among these feedstocks lead to diverse pyrolysis reactions during carbonization and activation, causing varied microstructures and properties in the produced carbon materials. Therefore, employing computational simulation strategies to elucidate the relationship between microscopic topography and macroscopic performance is beneficial for the design and preparation of high-performance porous carbon-based materials to meet various application demands. This paper presents a review of the modeling construction and pyrolysis simulation of typical carbonaceous feedstocks utilizing reactive molecular dynamics (ReaxFF MD) simulation strategy. It specifically delves into the fundamental principles and software tools currently employed, outlining the methodologies for constructing typical molecular structures along with associated validation techniques. The advancements in thermolysis mechanisms and carbon formation principles are also summarized, as well as the anticipated changes and development trends. Moreover, the challenges and perspectives in this field are addressed, including diversifying the carbonaceous feedstocks, enhancing the theoretical principles and simulation ability, and advancing the artificial intelligence functionality. This review is anticipated to provide detailed theoretical insights into the microstructure morphology and pyrolysis mechanism of carbonaceous feedstocks, while establishing a robust theoretical basis for the rapid screening and preparation of high-performance porous carbon-based materials.