Efficient chemical fixation of CO2 from direct air under environment-friendly co-catalyst and solvent-free ambient conditions

被引:70
作者
Das, Rajesh [1 ]
Ezhil, Thirumavalavan [1 ]
Palakkal, Athulya S. [2 ]
Muthukumar, D. [2 ]
Pillai, Renjith S. [2 ,3 ]
Nagaraja, C. M. [1 ]
机构
[1] Indian Inst Technol Ropar, Dept Chem, Rupnagar 140001, Punjab, India
[2] SRM Inst Sci & Technol, Fac Engn & Technol, Dept Chem, Chennai 603203, Tamil Nadu, India
[3] Christ Univ, Dept Chem, Bangalore 560023, Karnataka, India
关键词
METAL-ORGANIC FRAMEWORK; CARBON-DIOXIDE; CYCLIC CARBONATES; RATIONAL DESIGN; FLUE-GAS; CAPTURE; CONVERSION; MOF; CYCLOADDITION; TRANSFORMATION;
D O I
10.1039/d1ta05138e
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The capture and conversion of CO2 from direct air into value-added products under mild conditions represents a promising step towards environmental remediation and energy sustainability. Consequently, herein, we report the first example of a Mg(ii)-based MOF exhibiting highly efficient fixation of CO2 from direct air into value-added cyclic carbonates under eco-friendly co-catalyst and solvent-free mild conditions. The bifunctional MOF catalyst was rationally constructed by utilizing an eco-friendly Lewis acidic metal ion, Mg(ii), and a nitrogen-rich tripodal linker, TATAB. The MOF possesses a high BET surface area of 2606.13 m(2) g(-1) and highly polar 1D channels decorated with a high density of CO2-philic sites which promote a remarkably high CO2 uptake of 50.2 wt% at 273 K with a high heat of adsorption value of 55.13 kJ mol(-1). The high CO2-affinity combined with the presence of a high density of nucleophilic and Lewis acidic sites conferred efficient catalytic properties to the Mg-MOF for chemical fixation of CO2 from direct air under environment-friendly mild conditions. The remarkable performance of the Mg-MOF for the fixation of CO2 from direct air was further supported by in-depth theoretical calculations. Moreover, the computational studies provided an insight into the mechanistic details of the catalytic process in the absence of any co-catalyst and solvent. Overall, this work represents a rare demonstration of carbon capture and utilization (CCU) from direct air under eco-friendly mild conditions.
引用
收藏
页码:23127 / 23139
页数:13
相关论文
共 50 条
  • [41] Xylan/DBU as an efficient and green catalyst for chemical fixation of CO2
    Zhou, Qiu-sheng
    Peng, Xin-wen
    Zhong, Lin-Xin
    Li, Xue-hui
    Chua, Wei-tian
    Sun, Run-cang
    FUEL PROCESSING TECHNOLOGY, 2018, 176 : 146 - 152
  • [42] Green synthesized cobalt-bipyridine constructed conjugated microporous polymer: An efficient heterogeneous catalyst for cycloaddition of epoxides via CO2 fixation under ambient conditions
    Zhang, Xiaofeng
    Qiu, Bo
    Zou, Yu
    Wang, Shimin
    Mai, Wenpeng
    Cao, Yi
    Wang, Yanwei
    Chen, Jian
    Li, Tao
    MICROPOROUS AND MESOPOROUS MATERIALS, 2021, 319
  • [43] Solvent-free conversion of CO2 in carbonates through a sustainable macroporous catalyst
    Dattilo, Sandro
    Zagni, Chiara
    Mecca, Tommaso
    Patamia, Vincenzo
    Floresta, Giuseppe
    Nicotra, Pietro
    Carroccio, Sabrina C.
    Rescifina, Antonio
    GIANT, 2024, 18
  • [44] Synthesis of Methanol and Diols from CO2 via Cyclic Carbonates under Metal-Free, Ambient Pressure, and Solvent-Free Conditions
    Bobbink, Felix D.
    Menoud, Florent
    Dyson, Paul J.
    ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2018, 6 (09): : 12119 - 12123
  • [45] A Cationic Zinc-Organic Framework with Lewis Acidic and Basic Bifunctional Sites as an Efficient Solvent-Free Catalyst: CO2 Fixation and Knoevenagel Condensation Reaction
    Yao, Cheng
    Zhou, Shaolin
    Kang, Xiaojing
    Zhao, Yang
    Yan, Rui
    Zhang, Yan
    Wen, Lili
    INORGANIC CHEMISTRY, 2018, 57 (17) : 11157 - 11164
  • [46] Ionic liquid post-modified carboxylate-rich MOFs for efficient catalytic CO2 cycloaddition under solvent-free conditions
    Bao, Wen-Li
    Kuai, Jie
    Gao, Hai-Yang
    Zheng, Meng-Qi
    Sun, Zhong-Hua
    He, Ming-Yang
    Chen, Qun
    Zhang, Zhi-Hui
    DALTON TRANSACTIONS, 2024, 53 (14) : 6215 - 6223
  • [47] Crystal Engineering of an nbo Topology Metal-Organic Framework for Chemical Fixation of CO2 under Ambient Conditions
    Gao, Wen-Yang
    Chen, Yao
    Niu, Youhong
    Williams, Kia
    Cash, Lindsay
    Perez, Pastor J.
    Wojtas, Lukasz
    Cai, Jianfeng
    Chen, Yu-Sheng
    Ma, Shengqian
    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (10) : 2615 - 2619
  • [48] Efficient Acid-Base Bifunctional Catalysts for the Fixation of CO2 with Epoxides under Metal- and Solvent-Free Conditions
    Sun, Jian
    Han, Lijun
    Cheng, Weiguo
    Wang, Jinquan
    Zhang, Xiangping
    Zhang, Suojiang
    CHEMSUSCHEM, 2011, 4 (04) : 502 - 507
  • [49] Engineering noble-metal-free metal-organic framework composite catalyst for efficient CO2 conversion under ambient conditions
    Cui, Hui-Ya
    Zhang, Ya-Xin
    Cao, Chun-Shuai
    Hu, Tian-Ding
    Wu, Zhi-Lei
    CHEMICAL ENGINEERING JOURNAL, 2023, 451
  • [50] Functional Porous Ionic Polymers as Efficient Heterogeneous Catalysts for the Chemical Fixation of CO2 under Mild Conditions
    Dai, Zhifeng
    Long, Yang
    Liu, Jianliang
    Bao, Yuanfei
    Zheng, Liping
    Ma, Jiacong
    Liu, Jiayi
    Zhang, Fei
    Xiong, Yubing
    Lu, Ji-Qing
    POLYMERS, 2022, 14 (13)