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论文类型：期刊论文

发表时间：2016-11-23

发表刊物：ACS Applied Materials & Interfaces

收录刊物：SCIE、PubMed

卷号：8

期号：46

页面范围：31746-31756

ISSN号：1944-8244

关键字：rht-type metal-organic frameworks; carbon dioxide capture; chemical fixation; cycloaddition; mixed gas; cyclic carbonates

摘要：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-{Zn-2(OOC-)(4)} and {Zn-2(OOC-)(3)}. The high uptake of CO2 (115.6 cm(3).g(-1)) and selectivity over N-2 (30:1) at 273 K indicated that these MOFs are excellent candidates for postcombustion CO2 isolation 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 x 6 rounds of recyclability, demonstrating that they are promising heterogeneous catalysts for CO2 cyclo-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 CO2 fixation in industry.