Spatial, Hysteretic, and Adaptive Host–Guest Chemistry in a Metal–Organic Framework with Open Watson–Crick Sites*
This research is financially supported by the National Basic Research Program of China (973 Program, 2012CB821706 and 2013CB834803) and the National Natural Science Foundation of China (91222202 and 21171114). We are grateful for constructive criticism and suggestions from the reviewers and Prof. Jie‐Peng Zhang (Sun Yat‐Sen University).
Abstract
Biological and artificial molecules and assemblies capable of supramolecular recognition, especially those with nucleobase pairing, usually rely on autonomous or collective binding to function. Advanced site‐specific recognition takes advantage of cooperative spatial effects, as in local folding in protein–DNA binding. Herein, we report a new nucleobase‐tagged metal–organic framework (MOF), namely ZnBTCA (BTC=benzene‐1,3,5‐tricarboxyl, A=adenine), in which the exposed Watson–Crick faces of adenine residues are immobilized periodically on the interior crystalline surface. Systematic control experiments demonstrated the cooperation of the open Watson–Crick sites and spatial effects within the nanopores, and thermodynamic and kinetic studies revealed a hysteretic host–guest interaction attributed to mild chemisorption. We further exploited this behavior for adenine–thymine binding within the constrained pores, and a globally adaptive response of the MOF host was observed.
Number of times cited: 29
- Thomas Wittmann, Arobendo Mondal, Carsten B. L. Tschense, Johannes J. Wittmann, Ottokar Klimm, Renée Siegel, Björn Corzilius, Birgit Weber, Martin Kaupp and Juergen Senker, Probing Interactions of N-Donor Molecules with Open Metal Sites within Paramagnetic Cr-MIL-101: A Solid-State NMR Spectroscopic and Density Functional Theory Study, Journal of the American Chemical Society, (2018).
- Jianguo Jia, Yang Zhang, Min Zheng, Changfu Shan, Huicheng Yan, Wenyu Wu, Xuan Gao, Bo Cheng, Weisheng Liu and Yu Tang, Functionalized Eu(III)-Based Nanoscale Metal–Organic Framework To Achieve Near-IR-Triggered and -Targeted Two-Photon Absorption Photodynamic Therapy, Inorganic Chemistry, 10.1021/acs.inorgchem.7b02475, 57, 1, (300-310), (2017).
- Edwin A. Giles-Mazón, Iván Germán-Ramos, Fernando Romero-Romero, Eric Reinheimer, Rubén A. Toscano, Nazario Lopez, Carlos E. Barrera-Díaz, Víctor Varela-Guerrero and María F. Ballesteros-Rivas, Synthesis and characterization of a Bio-MOF based on mixed adeninate/tricarboxylate ligands and zinc ions, Inorganica Chimica Acta, 10.1016/j.ica.2017.09.047, 469, (306-311), (2018).
- Songmin Shang, Ka‐Lok Chiu and Shouxiang Jiang, Synthesis of immobilized poly(vinyl alcohol)/cyclodextrin eco‐adsorbent and its application for the removal of ibuprofen from pharmaceutical sewage, Journal of Applied Polymer Science, 134, 21, (2017).
- Muhammad Usman, Shruti Mendiratta and Kuang‐Lieh Lu, Semiconductor Metal–Organic Frameworks: Future Low‐Bandgap Materials, Advanced Materials, 29, 6, (2016).
- Yang Li, Hong-Han Yuan, Cheng-Peng Li and Jun Li, A 2D Zn(II) metal-organic framework to show selective removal of Neutral Red (NR) from water, Inorganic Chemistry Communications, 80, (36), (2017).
- Balaram Mohapatra, Pratibha Pratibha and Sandeep Verma, Directed adenine functionalization for creating complex architectures for material and biological applications, Chem. Commun., 10.1039/C7CC00222J, 53, 35, (4748-4758), (2017).
- Lan-Xia Hu, Meiyan Gao, Tian Wen, Yao Kang and Shumei Chen, Synthesis of Halide-Modulated Cuprous(I) Coordination Polymers with Mechanochromic and Photocatalytic Properties, Inorganic Chemistry, 56, 11, (6507), (2017).
- Lu Han, Jie Zhou, Xiao Li, Chun-Yi Sun, Liang Zhao, Yu-Teng Zhang, Man Zhu, Xin-Long Wang and Zhong-Min Su, Recognition of harmful fused aromatic hydrocarbons via a metal-organic framework with hydrophobic pores, Inorganic Chemistry Communications, 10.1016/j.inoche.2017.10.015, 86, (200-203), (2017).
- Jian-Long Du, Ju-Ping Gao, Chao-Ping Li, Xiao-Ying Zhang, Jin-Xin Hou, Xu Jing, Ya-Juan Mu and Li-Jun Li, A stable 3D Cd(ii) metal–organic framework for highly sensitive detection of Cu2+ ions and nitroaromatic explosives, RSC Adv., 7, 78, (49618), (2017).
- Cheng-Peng Li, Hang Zhou, Si Wang, Hong-Han Yuan, Su-Zhen Zhang and Miao Du, A nanoporous Ag(i) coordination polymer for selective adsorption of carcinogenic dye Acid Red 26, Chemical Communications, 53, 35, (4767), (2017).
- S. Rojas, T. Devic and P. Horcajada, Metal organic frameworks based on bioactive components, Journal of Materials Chemistry B, 5, 14, (2560), (2017).
- Tian-Tian Zheng, Jiao Zhao, Zhou-Wen Fang, Meng-Ting Li, Chun-Yi Sun, Xiao Li, Xin-Long Wang and Zhong-Min Su, A luminescent metal organic framework with high sensitivity for detecting and removing copper ions from simulated biological fluids, Dalton Transactions, 46, 8, (2456), (2017).
- T. W. Tseng, L. W. Lee, T. T. Luo, P. H. Chien, Y. H. Liu, S. L. Lee, C. M. Wang and K. L. Lu, Gate-opening upon CO 2 adsorption on a metal–organic framework that mimics a natural stimuli-response system , Dalton Transactions, 10.1039/C7DT03119J, 46, 43, (14728-14732), (2017).
- Bei Zhao, Na Li, Xi Wang, Ze Chang and Xian-He Bu, Host–Guest Engineering of Coordination Polymers for Highly Tunable Luminophores Based on Charge Transfer Emissions, ACS Applied Materials & Interfaces, 10.1021/acsami.6b14554, 9, 3, (2662-2668), (2017).
- Hong Cai, Yong-Liang Huang and Dan Li, Biological metal–organic frameworks: Structures, host–guest chemistry and bio-applications, Coordination Chemistry Reviews, 10.1016/j.ccr.2017.12.003, (2017).
- Hong Cai, Li-Li Xu, He-Yun Lai, Jing-Yi Liu, Seik Weng Ng and Dan Li, A highly emissive and stable zinc( ii ) metal–organic framework as a host–guest chemopalette for approaching white-light-emission , Chem. Commun., 10.1039/C7CC03350H, 53, 56, (7917-7920), (2017).
- S. R. Sushrutha, Raghunandan Hota and Srinivasan Natarajan, Adenine‐Based Coordination Polymers: Synthesis, Structure, and Properties, European Journal of Inorganic Chemistry, 2016, 18, (2962-2974), (2016).
- Sringeri Ramesh Sushrutha and Srinivasan Natarajan, Selective Sensing of Nitrophenols by a Inorganic Coordination Polymer: [Cd2(C4H4O5)2(C5H5N5)].H2O. DMA, ChemistrySelect, 1, 10, (2413-2421), (2016).
- Raymond Wai-Yin Sun, Ming Zhang, Dan Li, Mian Li and Alice Sze-Tsai Wong, Enhanced anti-cancer activities of a gold(III) pyrrolidinedithiocarbamato complex incorporated in a biodegradable metal-organic framework, Journal of Inorganic Biochemistry, 163, (1), (2016).
- Yu Shen, Cong-Cong Fan, Yu-Zhen Wei, Jie Du, Hai-Bin Zhu and Yue Zhao, An anionic zeolite-like metal–organic framework (AZMOF) with a Moravia network for organic dye absorption through cation-exchange, Dalton Trans., 10.1039/C6DT01697A, 45, 27, (10909-10915), (2016).
- Ramamoorthy Boomishankar and Anant Kumar Srivastava, Functional metal-organic molecules and materials derived from rigid and flexible P-N scaffolds, Phosphorus, Sulfur, and Silicon and the Related Elements, 191, 4, (618), (2016).
- Dries Jonckheere, Eduardo Coutino-Gonzalez, Wouter Baekelant, Bart Bueken, Helge Reinsch, Ivo Stassen, Oliver Fenwick, Fanny Richard, Paolo Samorì, Rob Ameloot, Johan Hofkens, Maarten B. J. Roeffaers and Dirk E. De Vos, Silver-induced reconstruction of an adeninate-based metal–organic framework for encapsulation of luminescent adenine-stabilized silver clusters, Journal of Materials Chemistry C, 4, 19, (4259), (2016).
- Jun-Sheng Qin, Dong-Ying Du, Mian Li, Xi-Zhen Lian, Long-Zhang Dong, Mathieu Bosch, Zhong-Min Su, Qiang Zhang, Shun-Li Li, Ya-Qian Lan, Shuai Yuan and Hong-Cai Zhou, Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks, Journal of the American Chemical Society, 10.1021/jacs.6b01093, 138, 16, (5299-5307), (2016).
- Tomislav Stolar, Stipe Lukin, Josip Požar, Mirta Rubčić, Graeme M. Day, Ivana Biljan, Dubravka Šišak Jung, Gordan Horvat, Krunoslav Užarević, Ernest Meštrović and Ivan Halasz, Solid-State Chemistry and Polymorphism of the Nucleobase Adenine, Crystal Growth & Design, 10.1021/acs.cgd.6b00243, 16, 6, (3262-3270), (2016).
- Zhi-Qiang Jiang, Fei Wang and Jian Zhang, Adsorption of Iodine Based on a Tetrazolate Framework with Microporous Cages and Mesoporous Cages, Inorganic Chemistry, 55, 24, (13035), (2016).
- Cheng‐Hua Lee , Hung‐Yu Huang , Jey‐Jau Lee, Chia‐Yuan Huang, Ya‐Chuan Kao, Gene‐Hsiang Lee, Shie‐Ming Peng , Jyh‐Chiang Jiang, Ito Chao and Kuang‐Lieh Lu, Amide‐CO2 Interaction Induced Gate‐Opening Behavior for CO2 Adsorption in 2‐Fold Interpenetrating Framework, ChemistrySelect, 1, 11, (2923-2929), (2016).
- Jitendra Kumar, Pratibha and Sandeep Verma, Crystallographic signatures of silver-purine frameworks with an azide functionality, Inorganica Chimica Acta, 10.1016/j.ica.2016.03.016, 452, (214-221), (2016).
- Raymond Wai‐Yin Sun, Ming Zhang, Dan Li, Zhi‐Feng Zhang, Hong Cai, Mian Li, Yue‐Jiao Xian, Seik Weng Ng and Alice Sze‐Tsai Wong, Dinuclear Gold(I) Pyrrolidinedithiocarbamato Complex: Cytotoxic and Antimigratory Activities on Cancer Cells and the Use of Metal–Organic Framework, Chemistry – A European Journal, 21, 51, (18534-18538), (2015).




