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Title: 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 » can be used as recoverable stable heterogeneous catalysts without losing performance.« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [3];  [1];  [1];  [1]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and X-ray Science Division
  3. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemical Engineering and Macromolecules Innovation Inst.
  4. Nanjing Univ. of Technology (China). State Key Lab. of Materials-Oriented Chemical Engineering (MCE) and College of Chemical Engineering
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  6. 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 Lab. (BNL), Upton, NY (United States); Argonne National Lab. (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; SC0012445; 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. 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., & 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 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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    • DOI: 10.1039/c9cc02174d

    Formation of CX Bonds in CO 2 Chemical Fixation Catalyzed by Metal−Organic Frameworks
    journal, June 2019


    A Core-Shell-Structured Silver Nanowire/Nitrogen-Doped Carbon Catalyst for Enhanced and Multifunctional Electrofixation of CO 2
    journal, September 2018


    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
    • DOI: 10.1007/s10847-018-0855-4

    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
    • DOI: 10.1039/c8dt01103f

    Three novel topologically different metal–organic frameworks built from 3-nitro-4-(pyridin-4-yl)benzoic acid
    journal, January 2019

    • Qin, Tao; Zhang, Shunlin; Wang, Yixiong
    • Acta Crystallographica Section C Structural Chemistry, Vol. 75, Issue 2
    • DOI: 10.1107/s2053229618018211

    Hexanuclear 3d–4f complexes as efficient catalysts for converting CO 2 into cyclic carbonates
    journal, January 2019

    • Gao, Guoshu; Wang, Li; Zhang, Ruilian
    • Dalton Transactions, Vol. 48, Issue 12
    • DOI: 10.1039/c8dt05048a

    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
    • DOI: 10.1002/chem.201905194

    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
    • DOI: 10.1039/c8ra10475a

    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
    • DOI: 10.1039/c9ay00371a

    URJC‐1‐MOF as New Heterogeneous Recyclable Catalyst for C‐Heteroatom Coupling Reactions
    journal, June 2019


    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
    • DOI: 10.1002/anie.201803081

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.