A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation

Zhu, Jie; Usov, Pavel M.; Xu, Wenqian; Celis-Salazar, Paula J.; Lin, Shaoyang; Kessinger, Matthew C.; Landaverde-Alvarado, Carlos; Cai, Meng; May, Ann M.; Slebodnick, Carla; Zhu, Dunru; Senanayake, Sanjaya D.; Morris, Amanda J.

doi:10.1021/jacs.7b10643

Title: A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO₂ Adsorption and Chemical Fixation

Journal Article · 22 December 2017 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.7b10643 · OSTI ID:1430863

Zhu, Jie ^[1]; Usov, Pavel M. ^[1]; Xu, Wenqian ^[2]; Celis-Salazar, Paula J. ^[1]; Lin, Shaoyang ^[1]; Kessinger, Matthew C. ^[1]; Landaverde-Alvarado, Carlos ^[3]; Cai, Meng ^[1]; May, Ann M. ^[1]; Slebodnick, Carla ^[1];

^[4];

^[5];

^[6]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and X-ray Science Division
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemical Engineering and Macromolecules Innovation Inst.
Nanjing Univ. of Technology (China). State Key Lab. of Materials-Oriented Chemical Engineering (MCE) and College of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemistry and Macromolecules Innovation Inst.

Metal–organic frameworks (MOFs) have shown great promise in catalysis, mainly due to their high content of active centers, large internal surface areas, tunable pore size, and versatile chemical functionalities. However, it is a challenge to rationally design and construct MOFs that can serve as highly stable and reusable heterogeneous catalysts. Here two new robust 3D porous metal-cyclam-based zirconium MOFs, denoted VPI-100 (Cu) and VPI-100 (Ni), have been prepared by a modulated synthetic strategy. The frameworks are assembled by eight-connected Zr₆ clusters and metallocyclams as organic linkers. Importantly, the cyclam core has accessible axial coordination sites for guest interactions and maintains the electronic properties exhibited by the parent cyclam ring. The VPI-100 MOFs exhibit excellent chemical stability in various organic and aqueous solvents over a wide pH range and show high CO₂ uptake capacity (up to ~9.83 wt% adsorption at 273 K under 1 atm). Moreover, VPI-100 MOFs demonstrate some of the highest reported catalytic activity values (turnover frequency and conversion efficiency) among Zr-based MOFs for the chemical fixation of CO₂ with epoxides, including sterically hindered epoxides. Thus, the MOFs, which bear dual catalytic sites (Zr and Cu/Ni), enable chemistry not possible with the cyclam ligand under the same conditions and can be used as recoverable stable heterogeneous catalysts without losing performance.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: SC0012704; SC0012446; AC02-06CH11357; 21476115

OSTI ID:: 1430863

Alternate ID(s):: OSTI ID: 1421945

Report Number(s):: BNL-203399-2018-JAAM; TRN: US1802760

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 3; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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URJC‐1‐MOF as New Heterogeneous Recyclable Catalyst for C‐Heteroatom Coupling Reactions Muñoz, Antonio; Leo, Pedro; Orcajo, Gisela ChemCatChem, Vol. 11, Issue 15 https://doi.org/10.1002/cctc.201900906	journal	June 2019
Computational screening of metal-substituted HKUST-1 catalysts for chemical fixation of carbon dioxide into epoxides Hu, Tian-ding; Jiang, Yan; Ding, Yi-hong Journal of Materials Chemistry A, Vol. 7, Issue 24 https://doi.org/10.1039/c9ta02455g	journal	January 2019
Efficient Synthesis of Multifunctional Chelating Agents Based on Tetraazacycloalkanes: Efficient Synthesis of Multifunctional Chelating Agents Based on Tetraazacycloalkanes Sok, Nicolas; Bernhard, Claire; Désogère, Pauline European Journal of Organic Chemistry, Vol. 2018, Issue 34 https://doi.org/10.1002/ejoc.201800801	journal	August 2018
Computational screening, synthesis and testing of metal–organic frameworks with a bithiazole linker for carbon dioxide capture and its green conversion into cyclic carbonates Müller, Philipp; Bucior, Benjamin; Tuci, Giulia Molecular Systems Design & Engineering, Vol. 4, Issue 5 https://doi.org/10.1039/c9me00062c	journal	January 2019
A tri-functional metal–organic framework heterogeneous catalyst for efficient conversion of CO ₂ under mild and co-catalyst free conditions Ma, Dingxuan; Zhang, Yaowen; Jiao, Shaoshao Chemical Communications, Vol. 55, Issue 95 https://doi.org/10.1039/c9cc08236k	journal	January 2019
A Flexible Aromatic Tetracarboxylate as a New Linker for Coordination Polymers Gu, Wenjun; Gu, Jinzhong; Kirillov, Alexander M. Crystals, Vol. 10, Issue 2 https://doi.org/10.3390/cryst10020084	journal	February 2020
Structural diversity of metal–organic frameworks via employment of azamacrocycles as a building block Lee, Jae Hwa; Moon, Hoi Ri Journal of Inclusion Phenomena and Macrocyclic Chemistry, Vol. 92, Issue 3-4 https://doi.org/10.1007/s10847-018-0855-4	journal	November 2018
Solvent-dependent variations of both structure and catalytic performance in three manganese coordination polymers Kang, Xiao-Min; Wang, Wen-Min; Yao, Lin-Hong Dalton Transactions, Vol. 47, Issue 20 https://doi.org/10.1039/c8dt01103f	journal	January 2018
Experimental and theoretical study for CO ₂ activation and chemical fixation with epoxides Gao, Jinwei; Li, Liuyi; Cui, Caiyan RSC Advances, Vol. 9, Issue 23 https://doi.org/10.1039/c8ra10475a	journal	January 2019
Colorimetric sensor arrays for the detection and identification of antibiotics Abedalwafa, Mohammed Awad; Li, Yan; Ni, Chunfang Analytical Methods, Vol. 11, Issue 22 https://doi.org/10.1039/c9ay00371a	journal	January 2019
Lower Activation Energy for Catalytic Reactions through Host-Guest Cooperation within Metal-Organic Frameworks Aguila, Briana; Sun, Qi; Wang, Xiaoliang Angewandte Chemie International Edition, Vol. 57, Issue 32 https://doi.org/10.1002/anie.201803081	journal	June 2018
Diversity-Oriented Metal Decoration on UiO-Type Metal–Organic Frameworks: an Efficient Approach to Increase CO₂ Uptake and Catalytic Conversion to Cyclic Carbonates Norouzi, Fataneh; Khavasi, Hamid Reza ACS Omega, Vol. 4, Issue 21 https://doi.org/10.1021/acsomega.9b02035	journal	November 2019
Three Novel Zn-Based Coordination Polymers: Synthesis, Structure, and Effective Detection of Al3+ and S2− Ions Wang, Yuna; Zhang, Xiaofeng; Zhao, Yanru Molecules, Vol. 25, Issue 2 https://doi.org/10.3390/molecules25020382	journal	January 2020

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Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
MOFs
zirconium
metal-cyclam
CO2 fixation

CCDC 1576953: Experimental Crystal Structure Determination: YESTAU : catena-[tetrakis(μ-oxo)-bis(μ-1,4,8,11-tetraazacyclotetradecane-6,13-dicarboxylato)-di-copper-tri-zirconium tetrachloride icosahydrate] Zhu, Jie; Usov, Pavel; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pxyg0 The current record is supplemented by this dataset	dataset	October 2017
CCDC 1572992: Experimental Crystal Structure Determination: YESQIZ : (1,4,8,11-tetraazacyclotetradecane-6,13-dicarboxylic acid)-nickel(ii) diperchlorate dihydrate Zhu, Jie; Usov, Pavel; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pstpz The current record is supplemented by this dataset	dataset	September 2017
CCDC 1572994: Experimental Crystal Structure Determination: YESQUL : dichloro-(1,4,8,11-tetraazacyclotetradecane-6,13-dicarboxylic acid)-nickel N,N-dimethylformamide solvate Zhu, Jie; Usov, Pavel; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pstr1 The current record is supplemented by this dataset	dataset	September 2017
CCDC 1572993: Experimental Crystal Structure Determination Zhu, Jie; Usov, Pavel M.; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pstq0 The current record is supplemented by this dataset	dataset	June 2017
CCDC 1572991: Experimental Crystal Structure Determination: HAWKAR01 : bis(perchlorato)-(1,4,8,11-tetraazacyclotetradecane-6,13-dicarboxylic acid)-copper(ii) Zhu, Jie; Usov, Pavel; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pstny The current record is supplemented by this dataset	dataset	September 2017
CCDC 1576954: Experimental Crystal Structure Determination Zhu, Jie; Usov, Pavel M.; Xu, Wenqian https://doi.org/10.5517/ccdc.csd.cc1pxyh1 The current record is supplemented by this dataset	dataset	March 2017

Title: A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation

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