Linker-Guided Growth of Single-Crystal Covalent Organic Frameworks

Zhou，Zhipeng1,2; Xiong，Xiao Hong3; Zhang，Lei4; Li，Yuyao1; Yang，Yonghang1; Dong，Xin1; Lou，Dongyang5; Wei，Zhangwen3; Liu，Wei5; Su，Cheng Yong3; Sun，Junliang2; Zheng，Zhikun1,6,7

2023

10.1021/jacs.3c13069

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

The core features of covalent organic frameworks (COFs) are crystallinity and porosity. However, the synthesis of single-crystal COFs with monomers of diverse reactivity and adjustment of their pore structures remain challenging. Here, we show that linkers that can react with a node to form single-crystal COFs can guide other linkers that form either COFs or amorphous polymers with the node to gain single-crystal COFs with mixed components, which are homogeneous on the unit cell scale with controlled ratios. With the linker-guided crystal growth method, we created nine types of single-crystal COFs with up to nine different components, which are more complex than any known crystal. The structure of the crystal adapted approximately to that of the main component, and its pore volume could be expanded up to 8.8%. Different components lead to complex and diverse pore structures and offer the possibilities to gain positive synergies, as exemplified by a bicomponent COF with 2200 and 733% SO uptake capacity of that of the two pure-component counterparts at 298 K and 0.002 bar. The selectivity for separation of SO/CO ranges from 1230 to 4247 for flue gas based on ideal adsorbed solution theory, recording porous crystals. The bicomponent COF also exhibits a 1300% retention time of its pure-component counterparts for SO in a dynamic column breakthrough experiment for deep desulfurization.

EI ; SCI

英语

其他

20240715558947

Crystal structure ; Crystallinity ; Lead compounds ; Pore structure

Physical Properties of Gases, Liquids and Solids:931.2 ; Crystalline Solids:933.1 ; Crystal Lattice:933.1.1

2-s2.0-85184519283

Scopus

1.Key Laboratory for Polymeric Composite and Functional Materials,Ministry of Education,School of Chemistry,State Key Laboratory of Optoelectronic Materials and Technologies,Sun Yat-sen University,Guangzhou,510000,China
2.College of Chemistry and Molecular Engineering,Beijing National Laboratory for Molecular Sciences,Peking University,Beijing,100000,China
3.MOE,Laboratory of Bioinorganic and Synthetic Chemistry,LIFM,IGCME,School of Chemistry,Sun Yat-Sen University,Guangzhou,510000,China
4.Cryo-Electron Microscopy Center,Southern University of Science and Technology,Shenzhen,518000,China
5.Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province,Key Laboratory for Polymeric Composite and Functional Materials,Ministry of Education,School of Materials Science and Engineering,State Key Laboratory of Optoelectronic Materials and Technologies,Sun Yat-sen University,Guangzhou,510000,China
6.School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou,510000,China
7.Jieyang Branch,Chemistry and Chemical Engineering Guangdong Laboratory,Jieyang,522000,China

Zhou，Zhipeng,Xiong，Xiao Hong,Zhang，Lei,et al. Linker-Guided Growth of Single-Crystal Covalent Organic Frameworks[J]. Journal of the American Chemical Society,2023.

Zhou，Zhipeng.,Xiong，Xiao Hong.,Zhang，Lei.,Li，Yuyao.,Yang，Yonghang.,...&Zheng，Zhikun.(2023).Linker-Guided Growth of Single-Crystal Covalent Organic Frameworks.Journal of the American Chemical Society.

Zhou，Zhipeng,et al."Linker-Guided Growth of Single-Crystal Covalent Organic Frameworks".Journal of the American Chemical Society (2023).