High-Throughput Model-building And Screening Of Zeolitic Imidazolate Frameworks For CO₂ Capture From Flue Gas

The continuous emission of carbon dioxide has caused many climate problems such as global warming.It is imperative to evolve new carbon capture materials to remove greenhouse gases from the atmosphere.Flue gas emissions from power plants are a major source of carbon dioxide in the atmosphere,and the capture of carbon dioxide by flue gas separation can reduce greenhouse gas emissions.Methods for capturing and separating carbon dioxide in flue gas include solvent absorption,cryogenic distillation,adsorption separation,and membrane-based separation,but they have the disadvantages of high pollution,high cost,and high energy consumption.Metal organic frameworks（MOFs）materials have good adsorption separation properties but poor stability,and are difficult to apply under practical industrial conditions.The zeolitic imidazolate frameworks（ZIFs）materials are a class of MOFs with zeolite topologies that exhibit thermal and chemical stability.The ZIFs materials still have the characteristics of MOFs materials,like large surface area and volume,rich and diverse topology,and adjustable functional groups,so ZIFs materials are considered as potential excellent adsorbents for carbon dioxide capture.Existing synthetic ZIFs cannot meet the actual industrial needs,and it is becoming more and more urgent to find new ZIFs materials that are truly suitable for industrial carbon capture applications.It is time-consuming and laborious to design and develop new materials using traditional experimental methods.Computer prediction and molecular simulation provide us a new idea for designing materials.Computer simulations can predict new structures that have not yet been discovered,and molecular simulation techniques can assess the potential of new materials and provide some targets for experimental synthesis.To this end,we carried out two parts of research work,including designing and constructing a large number of hypothetical ZIF models,as well as evaluating carbon capture capabilities for these ZIF models,and finally screening CO₂ capture materials with potential applications.In the first part of the work,we use the top-down topology construction method,using the hypothetical zeolite topology as the blueprint,automatically constructing169,898 hypothetical ZIF models.Then we did the structural optimization and energy calculation for all hypothetical ZIF models.On this basis,we judge the stability of all hypothetical ZIFs based on the already-realised ZIF structures,and retain 83,398hypothetical ZIF models that can exist stably in nature.In the second part of the work,we have evaluated and screened the carbon capture capabilities of 83,398 hypothetical ZIF models and 29 already-realised ZIFs using a fast and efficient high-throughput screening process,and finally we got 49 promising models.The carbon capture properties of these structures are superior to the already-realised ZIFs structures of the same type.This paper developed a model for building ZIFs structures using hypothetical zeolite topology,and realised high-throughput automatic construction of a large number of ZIF models with different topologies.A screening strategy is used to achieve high-throughput carbon capture performance screening of ZIF models.Due to high efficiency and reliability,our high-throughput model-building and screening strategies can be applied to functionally oriented structural design and screening processes.These strategies can not only realise the batch design of porous materials such as ZIFs and MOFs,but also realise the rapid evaluation and screening of the adsorption properties of porous materials,and provide the target products for experimental synthesis finally.In addition,our method also supports the introduction of different functional groups into the porous material,thereby further enhancing the gas adsorption and separation properties of the porous materials.