title: New rht-Type Metal-Organic Frameworks Decorated with Acylamide Groups for Efficient Carbon Dioxide Capture and Chemical Fixation from Raw Power Plant Flue Gas.
abstract: The combination of carbon dioxide capture and chemical fixation in a one-pot process is attractive for both chemists and governments. The cycloaddition of carbon dioxide with epoxides to produce cyclic carbonates is an atomic economical reaction without any side products. By incorporating acylamide to enhance the binding affinity toward CO2, new rht-type metal-organic frameworks (MOFs) with (3, 28) and (3, 24) connected units were constructed. Zn-NTTA with two types of dinuclear paddlewheel building blocks-{Zn2(OOC-)4} and {Zn2(OOC-)3}. The high uptake of CO2(115.6 cm3·g-1) and selectivity over N2(30:1) at 273 K indicated that these MOFs are excellent candidates for postcombustion CO2isolation and capture. The MOFs feature high catalytic activity, rapid dynamics of transformation and excellent stability with turnover number (TON) values up to 110 000 per paddlewheel unit after 5 × 6 rounds of recyclability, demonstrating that they are promising heterogeneous catalysts for CO2cyclo-addition to value-added cyclic carbonates. The cycloaddition of epoxides with wet gases demonstrated that the catalyst activity was not affected by moisture, and the indices of the PXRD patterns of the bulk samples filtered from the catalytic reaction revealed that the crystallinities were maintained. The combination of the selective capture and catalytic transformation in one-pot enables the use of a negative-cost feedstock-raw power plant flue gas without any separation and purification-revealing the broad prospects of such MOFs for practical CO2fixation in industry.
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, China.
authors.forename: Xiangyang
authors.initials: X
authors.lastname: Guo
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, China.
authors.forename: Zhen
authors.initials: Z
authors.lastname: Zhou
authors.affiliation: State Key Laboratory of Coordination Chemistry, Nanjing University , Nanjing 210093, China.
authors.forename: Cong
authors.initials: C
authors.lastname: Chen
authors.affiliation: State Key Laboratory of Coordination Chemistry, Nanjing University , Nanjing 210093, China.
authors.forename: Junfeng
authors.initials: J
authors.lastname: Bai
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, China.
authors.forename: Cheng
authors.initials: C
authors.lastname: He
authors.affiliation: State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian 116024, China.
authors.forename: Chunying
authors.initials: C
authors.lastname: Duan
keywords: carbon dioxide capture; chemical fixation; cyclic carbonates; cycloaddition; mixed gas; rht-type metal−organic frameworks