An unprecedented water stable acylamide-functionalized metal-organic framework for highly efficient CH4/CO2 gas storage/separation and acid-base cooperative catalytic activity

被引:73
作者
Zheng, Baishu [1 ]
Luo, Xin [1 ]
Wang, Zhaoxu [1 ]
Zhang, Shaowei [1 ]
Yun, Ruirui [2 ]
Huang, Lu [1 ]
Zeng, Wenjiang [1 ]
Liu, Wenlong [3 ]
机构
[1] Hunan Univ Sci & Technol, Hunan Prov Key Lab Controllable Preparat & Funct, Sch Chem & Chem Engn,Hunan Prov Key Lab Adv Mat N, Key Lab Theoret Organ Chem & Funct Mol,Minist Edu, Xiangtan 411201, Peoples R China
[2] Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China
[3] Yangzhou Univ, Coll Chem & Chem Engn, Yangzhou 225002, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
CARBON-DIOXIDE CAPTURE; SELECTIVE CO2 CAPTURE; ZEOLITIC IMIDAZOLATE FRAMEWORKS; POROUS COORDINATION POLYMERS; STORAGE WORKING CAPACITY; HIGH METHANE UPTAKE; FINELY TUNING MOFS; HYDROGEN STORAGE; HIGH-PERFORMANCE; RETICULAR SYNTHESIS;
D O I
10.1039/c8qi00662h
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The high porosity, excellent water stability and optimized supramolecular host-guest interactions of MOFs are the three key factors for their potential practical applications in many important areas including gas storage/separation, catalysis and so on. In this study, we designed and constructed a highly porous (3, 36)-connected txt-type acylamide-functionalized metal-organic framework (HNUST-8) from a pyridine-based acylamide-linking diisophthalate and dicopper(ii)-paddlewheel clusters. Interestingly, HNUST-8 possesses an exceptionally water-stable framework with a high BET surface area of about 2800 m(2) g(-1). At 298 K, HNUST-8 exhibits a high excess CO2 uptake of 19.7 mmol g(-1) at 40 bar, an excellent total CH4 storage capacity of 223 cm(3)(STP) cm(-3) with a large working capacity of 178 cm(3)(STP) cm(-3) at 80 bar, as well as highly efficient CO2/CH4 and CO2/N-2 separation under dynamic conditions at 1 bar. Moreover, with the Lewis acidic open copper(ii) sites and Lewis basic acylamide groups integrated into the framework, HNUST-8 demonstrates efficient catalytic activity as an acid-base cooperative catalyst in a tandem one-pot deacetalization-Knoevenagel condensation reaction.
引用
收藏
页码:2355 / 2363
页数:9
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