10.1021/acs.chemmater.7b05121.s001 Xinghua Guo Xinghua Guo Yin Tian Yin Tian Meicheng Zhang Meicheng Zhang Yang Li Yang Li Rui Wen Rui Wen Xing Li Xing Li Xiaofeng Li Xiaofeng Li Ying Xue Ying Xue Lijian Ma Lijian Ma Chuanqin Xia Chuanqin Xia Shoujian Li Shoujian Li Mechanistic Insight into Hydrogen-Bond-Controlled Crystallinity and Adsorption Property of Covalent Organic Frameworks from Flexible Building Blocks American Chemical Society 2018 monomer sources crystallinity adsorption performance H-bonding interaction lattice sizes application values order degree adsorption properties intralayer hydrogen bonds Flexible Building Blocks as-prepared COFs show adsorption capacities building blocks Covalent Organic Frameworks variation tendency H-bonding effects ultrahigh-capacity iodine adsorbents FBB Mechanistic Insight Hydrogen-Bond-Controlled Crystallinity hydrogen bonds Adsorption Property 2018-03-19 00:00:00 Journal contribution https://acs.figshare.com/articles/journal_contribution/Mechanistic_Insight_into_Hydrogen-Bond-Controlled_Crystallinity_and_Adsorption_Property_of_Covalent_Organic_Frameworks_from_Flexible_Building_Blocks/6024011 The effective control of crystallinity of covalent organic frameworks (COFs) and the optimization of their performances related to the crystallinity have been considered as big challenges. COFs bearing flexible building blocks (FBBs) generally own larger lattice sizes and broader monomer sources, which may endow them with unprecedented application values. Herein, we report the oriented synthesis of a series of two-dimensional (2D) COFs from FBBs with different content of intralayer hydrogen bonds. Studies of H-bonding effects on the crystallinity and adsorption properties indicate that partial structure of the COFs is “locked” by the H-bonding interaction, which consequently improves their microscopic order degree and crystallinity. Thus, the regulation of crystallinity can be effectively realized by controlling the content of hydrogen bonds in COFs. Impressively, the as-prepared COFs show excellent and reversible adsorption performance for volatile iodine with capacities up to 543 wt %, much higher than all previously reported adsorbents, although the variation tendency of adsorption capacities is opposite to their crystallinity. This study provides a general guidance for the design and construction of highly/appropriately crystalline COFs and ultrahigh-capacity iodine adsorbents.