当前位置: X-MOL 学术Inorg. Chem. Front. › 论文详情
Construction of a bifunctional Zn(ii)–organic framework containing a basic amine functionality for selective capture and room temperature fixation of CO2†
Inorganic Chemistry Frontiers ( IF 5.934 ) Pub Date : 2019-09-20 , DOI: 10.1039/c9qi01058k
Rajesh Das; Sandeep Singh Dhankhar; C. M. Nagaraja

Selective carbon capture and utilization (CCU) as a C1 feedstock for the synthesis of value-added chemicals under ambient conditions catalyzed by porous MOFs constitutes one of the most promising solutions to mitigate the growing CO2 concentration in the atmosphere. Consequently, the synthesis of a novel 3D, microporous, bifunctional Zn(II)–organic framework, {[Zn2(TDC)2(DATRZ)]·(3H2O)·(DMF)}n (Zn-DAT) (where TDC = 2,5-thiophene dicarboxylate ion and DATRZ = 3,5-diamino-1,2,4-triazole), was achieved using a mixed ligand strategy. Single crystal X-ray structural analysis of the MOF revealed the presence of a 3D microporous structure with two types of 1D channels of dimensions 12.5 × 8.7 Å2 and 7.0 × 4.8 Å2 along the crystallographic c- and b-axes, respectively. The presence of basic –NH2 functionalized pores in Zn-DAT induces a selective adsorption property of CO2 with a high heat of adsorption (Qst) value of 39.5 kJ mol−1 which is supported by a theoretically computed binding energy (BE) of 40.9 kJ mol−1. Interestingly, the Qst value observed for Zn-DAT is about 8 kJ mol−1 higher than that of the analogous MOF {[Zn2(TDC)(TRZ)2]·(DMA)·(MeOH)}n (Zn-TAZ) containing the 1,2,4-triazole (TAZ) linker, which highlights the critical role of –NH2 groups in enhancing the interaction energy for CO2. The significantly high value of Qst can be attributed to the stronger interaction of the acidic CO2 molecule with the basic –NH2 groups present in the 1D channels of the Zn-DAT MOF. Furthermore, the presence of both Lewis acidic Zn2+ ions and basic –NH2 groups resulted in the Zn-DAT MOF as an efficient heterogeneous catalyst for chemical fixation of CO2 into cyclic carbonates under mild conditions at RT. Herein, we report a rare example of porous MOFs for the capture and utilization of CO2 at RT and the influence of basic –NH2 groups on the high value of Qst and catalytic conversion of carbon dioxide.
更新日期:2020-01-14

 

全部期刊列表>>
Springer Nature 2019高下载量文章和章节
化学/材料学中国作者研究精选
《科学报告》最新环境科学研究
ACS材料视界
自然科研论文编辑服务
中南大学国家杰青杨华明
南开大学陈弓课题组招聘启事
中南大学
材料化学和生物传感方向博士后招聘
课题组网站
X-MOL
北京大学分子工程苏南研究院
华东师范大学分子机器及功能材料
中山大学化学工程与技术学院
试剂库存
天合科研
down
wechat
bug