Due to structural tunability, high surface area, abundant pore structures, and abundant active sites, covalent heptazine frameworks (CHFs) constructed from heptazine and other molecular blocks are especially prominent. Here, we proposed a reaction-dependent strategy for designing two dimensional CHFs including high-throughput precursors screening, structure generation, and performance evaluation. Assuming that oxamide-like precursors can undergo the same thermal polymerization reaction as producing C₆N₇, seven precursors were screened from more than 10⁹ molecules in the ZINC20 database in terms of molecular weight, number of substructures, shape index, and symmetry. Furthermore, CHF-L1 to CHF-L7 were constructed from urea and the seven precursors according to the topologically assembling scheme in thermal polymerization. The designed CHFs had band gaps ranging from 1.89 to 3.10 eV. Among them, CHF-L3 assembled structurally by urea and 1,2,4,5-tetrazine-3,6-dicarboxamide with the smallest bandgap and an oxidative potential bias of 1.38 V for oxygen evolution reaction was screened as the candidate with high oxidative ability. The negative formation energy based on the synthesis route indicated the synthetic feasibility of CHF-L3, and negative cohesive energy as well as the stable structure under ab initio molecular dynamics simulations confirmed the stability of CHF-L3. The present work is expected to provide a powerful design strategy for two-dimensional CHFs design and is broadly applicable to various computational covalent organic framework design systems and experimental studies.

由于结构可调性、高表面积、丰富的孔隙结构和丰富的活性位点，由庚嗪和其他分子嵌段构建的共价庚嗪框架 (CHF) 尤为突出。在这里，我们提出了一种用于设计二维 CHF 的反应依赖策略，包括高通量前体筛选、结构生成和性能评估。假设草酰胺类前体可以进行与生成 C ₆ N ₇相同的热聚合反应，则从超过 10 ^{9个中筛选出 7 个前体}ZINC20 数据库中分子的分子量、子结构数、形状指数和对称性。此外，根据热聚合中的拓扑组装方案，CHF-L1 至 CHF-L7 由尿素和七种前体构成。设计的 CHF 的带隙范围为 1.89 至 3.10 eV。其中，CHF-L3由尿素和1,2,4,5-四嗪-3,6-二甲酰胺结构组装而成，带隙最小，析氧反应的氧化电位偏压为1.38 V，被筛选为具有高氧化性的候选物。能力。基于合成路线的负形成能表明CHF-L3的合成可行性，负内聚能以及从头算分子动力学模拟下的稳定结构证实了CHF-L3的稳定性。