A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation
Abstract
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 andmore »
- Authors:
-
[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.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1430863
- Alternate Identifier(s):
- OSTI ID: 1421945
- Report Number(s):
- BNL-203399-2018-JAAM
Journal ID: ISSN 0002-7863; TRN: US1802760
- Grant/Contract Number:
- SC0012704; SC0012446; AC02-06CH11357; 21476115
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 3; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; MOFs; zirconium; metal-cyclam; CO2 fixation
Citation Formats
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., and Morris, Amanda J.. A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b10643.
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.. A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation. United States. https://doi.org/10.1021/jacs.7b10643
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., and Morris, Amanda J.. Fri .
"A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation". United States. https://doi.org/10.1021/jacs.7b10643. https://www.osti.gov/servlets/purl/1430863.
@article{osti_1430863,
title = {A New Class of Metal-Cyclam-Based Zirconium Metal–Organic Frameworks for CO2 Adsorption and Chemical Fixation},
author = {Zhu, Jie and Usov, Pavel M. and Xu, Wenqian and Celis-Salazar, Paula J. and Lin, Shaoyang and Kessinger, Matthew C. and Landaverde-Alvarado, Carlos and Cai, Meng and May, Ann M. and Slebodnick, Carla and Zhu, Dunru and Senanayake, Sanjaya D. and Morris, Amanda J.},
abstractNote = {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.},
doi = {10.1021/jacs.7b10643},
journal = {Journal of the American Chemical Society},
number = 3,
volume = 140,
place = {United States},
year = {2017},
month = {12}
}
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Figures / Tables:
Figure 1: Anisotropic displacement ellipsoid drawing (30%) of (a) [CuL(ClO4)2] (1), (b) [NiL](ClO4)2 (3), (c) [CuLCl2] (4) and (d) [NiLCl2]·2DMF (5). Hydrogen atoms were omitted for clarity. Color scheme: C, grey; O, red; N, blue; Ni, light green; Cu, yellow; Cl, green.
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- Acta Crystallographica Section C Structural Chemistry, Vol. 75, Issue 2
Rational Stepwise Construction of Different Heterometallic–Organic Frameworks (HMOFs) for Highly Efficient CO 2 Conversion
journal, March 2020
- Liu, Jiao; Wu, Dan; Yang, Guo‐Ping
- Chemistry – A European Journal, Vol. 26, Issue 24
URJC‐1‐MOF as New Heterogeneous Recyclable Catalyst for C‐Heteroatom Coupling Reactions
journal, June 2019
- Muñoz, Antonio; Leo, Pedro; Orcajo, Gisela
- ChemCatChem, Vol. 11, Issue 15
Computational screening of metal-substituted HKUST-1 catalysts for chemical fixation of carbon dioxide into epoxides
journal, January 2019
- Hu, Tian-ding; Jiang, Yan; Ding, Yi-hong
- Journal of Materials Chemistry A, Vol. 7, Issue 24
Efficient Synthesis of Multifunctional Chelating Agents Based on Tetraazacycloalkanes: Efficient Synthesis of Multifunctional Chelating Agents Based on Tetraazacycloalkanes
journal, August 2018
- Sok, Nicolas; Bernhard, Claire; Désogère, Pauline
- European Journal of Organic Chemistry, Vol. 2018, Issue 34
Computational screening, synthesis and testing of metal–organic frameworks with a bithiazole linker for carbon dioxide capture and its green conversion into cyclic carbonates
journal, January 2019
- Müller, Philipp; Bucior, Benjamin; Tuci, Giulia
- Molecular Systems Design & Engineering, Vol. 4, Issue 5
A tri-functional metal–organic framework heterogeneous catalyst for efficient conversion of CO 2 under mild and co-catalyst free conditions
journal, January 2019
- Ma, Dingxuan; Zhang, Yaowen; Jiao, Shaoshao
- Chemical Communications, Vol. 55, Issue 95
A Flexible Aromatic Tetracarboxylate as a New Linker for Coordination Polymers
journal, February 2020
- Gu, Wenjun; Gu, Jinzhong; Kirillov, Alexander M.
- Crystals, Vol. 10, Issue 2
An exceptionally stable core–shell MOF/COF bifunctional catalyst for a highly efficient cascade deacetalization–Knoevenagel condensation reaction
journal, January 2019
- Gao, Ming-Liang; Qi, Mei-Hong; Liu, Lin
- Chemical Communications, Vol. 55, Issue 45
Structural diversity of metal–organic frameworks via employment of azamacrocycles as a building block
journal, November 2018
- Lee, Jae Hwa; Moon, Hoi Ri
- Journal of Inclusion Phenomena and Macrocyclic Chemistry, Vol. 92, Issue 3-4
Solvent-dependent variations of both structure and catalytic performance in three manganese coordination polymers
journal, January 2018
- Kang, Xiao-Min; Wang, Wen-Min; Yao, Lin-Hong
- Dalton Transactions, Vol. 47, Issue 20
Experimental and theoretical study for CO 2 activation and chemical fixation with epoxides
journal, January 2019
- Gao, Jinwei; Li, Liuyi; Cui, Caiyan
- RSC Advances, Vol. 9, Issue 23
Colorimetric sensor arrays for the detection and identification of antibiotics
journal, January 2019
- Abedalwafa, Mohammed Awad; Li, Yan; Ni, Chunfang
- Analytical Methods, Vol. 11, Issue 22
Lower Activation Energy for Catalytic Reactions through Host-Guest Cooperation within Metal-Organic Frameworks
journal, June 2018
- Aguila, Briana; Sun, Qi; Wang, Xiaoliang
- Angewandte Chemie International Edition, Vol. 57, Issue 32
Diversity-Oriented Metal Decoration on UiO-Type Metal–Organic Frameworks: an Efficient Approach to Increase CO2 Uptake and Catalytic Conversion to Cyclic Carbonates
journal, November 2019
- Norouzi, Fataneh; Khavasi, Hamid Reza
- ACS Omega, Vol. 4, Issue 21
Three Novel Zn-Based Coordination Polymers: Synthesis, Structure, and Effective Detection of Al3+ and S2− Ions
journal, January 2020
- Wang, Yuna; Zhang, Xiaofeng; Zhao, Yanru
- Molecules, Vol. 25, Issue 2
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