化工学报
化工學報
화공학보
JOURNAL OF CHEMICAL INDUSY AND ENGINEERING (CHINA)
2014年
5期
1696-1705
,共10页
王可可%李亮莎%黄宏亮%阳庆元%张轶%王少华%吴平易%兰玲%刘大欢%仲崇立
王可可%李亮莎%黃宏亮%暘慶元%張軼%王少華%吳平易%蘭玲%劉大歡%仲崇立
왕가가%리량사%황굉량%양경원%장질%왕소화%오평역%란령%류대환%중숭립
金属-有机骨架材料%铪%孔尺寸调控%稳定性%吸附%二氧化碳捕集
金屬-有機骨架材料%鉿%孔呎吋調控%穩定性%吸附%二氧化碳捕集
금속-유궤골가재료%협%공척촌조공%은정성%흡부%이양화탄포집
metal-organic frameworks%hafnium%pore-size regulation%stability%adsorption%CO2 capture
利用三种不同长度的有机配体--反丁烯二酸（H2FUM）、对苯二甲酸（H2BDC）和联苯二甲酸（H2BPDC），合成了一系列具有不同孔尺寸的新型铪（Hf）金属-有机骨架（MOF）材料（Hf-FUM、Hf-BDC 和 Hf-BPDC），并考察了 CO2、N2和 CH4三种气体在这些材料中吸附分离行为。研究结果表明，这三种材料具有和 UiO-66(Zr)相同的拓扑结构，且具有很好的热稳定性。Hf-FUM和Hf-BDC的结构在水中能够保持稳定，而Hf-BPDC在水中会发生降解。同时，具有最小孔尺寸的Hf-FUM材料对CO2/N2以及CO2/CH4体系具有最好的分离性能。这为以后设计用于CO2分离的新型纳微结构材料提供了参考依据。separation of CO2/N2and CO2/CH4 systems were also investigated. It is found that Hf-FUM with the smallest pore size possesses the highest adsorption selectivity for CO2 over N2and CH4. This is the first study on the performance of Hf-based MOFs for gas separation, and the knowledge obtained in this work provides a foundation for the design of new nanoporous materials towards CO2 capture from various gas mixtures.
利用三種不同長度的有機配體--反丁烯二痠（H2FUM）、對苯二甲痠（H2BDC）和聯苯二甲痠（H2BPDC），閤成瞭一繫列具有不同孔呎吋的新型鉿（Hf）金屬-有機骨架（MOF）材料（Hf-FUM、Hf-BDC 和 Hf-BPDC），併攷察瞭 CO2、N2和 CH4三種氣體在這些材料中吸附分離行為。研究結果錶明，這三種材料具有和 UiO-66(Zr)相同的拓撲結構，且具有很好的熱穩定性。Hf-FUM和Hf-BDC的結構在水中能夠保持穩定，而Hf-BPDC在水中會髮生降解。同時，具有最小孔呎吋的Hf-FUM材料對CO2/N2以及CO2/CH4體繫具有最好的分離性能。這為以後設計用于CO2分離的新型納微結構材料提供瞭參攷依據。separation of CO2/N2and CO2/CH4 systems were also investigated. It is found that Hf-FUM with the smallest pore size possesses the highest adsorption selectivity for CO2 over N2and CH4. This is the first study on the performance of Hf-based MOFs for gas separation, and the knowledge obtained in this work provides a foundation for the design of new nanoporous materials towards CO2 capture from various gas mixtures.
이용삼충불동장도적유궤배체--반정희이산（H2FUM）、대분이갑산（H2BDC）화련분이갑산（H2BPDC），합성료일계렬구유불동공척촌적신형협（Hf）금속-유궤골가（MOF）재료（Hf-FUM、Hf-BDC 화 Hf-BPDC），병고찰료 CO2、N2화 CH4삼충기체재저사재료중흡부분리행위。연구결과표명，저삼충재료구유화 UiO-66(Zr)상동적탁복결구，차구유흔호적열은정성。Hf-FUM화Hf-BDC적결구재수중능구보지은정，이Hf-BPDC재수중회발생강해。동시，구유최소공척촌적Hf-FUM재료대CO2/N2이급CO2/CH4체계구유최호적분리성능。저위이후설계용우CO2분리적신형납미결구재료제공료삼고의거。separation of CO2/N2and CO2/CH4 systems were also investigated. It is found that Hf-FUM with the smallest pore size possesses the highest adsorption selectivity for CO2 over N2and CH4. This is the first study on the performance of Hf-based MOFs for gas separation, and the knowledge obtained in this work provides a foundation for the design of new nanoporous materials towards CO2 capture from various gas mixtures.
By incorporating three organic carboxylic acids with different lengths, fumaric (FUM), 1,4-benzene- dicarboxylate (BDC) and 4,4′-biphenyl-dicarboxylate (BPDC) acids, three novel Hf-based metal-organic frameworks (MOFs), Hf-FUM, Hf-BDC and Hf-BPDC, were synthesized using a solvothermal method combined with conventional electric heating. These MOFs were characterized by various experimental techniques including PXRD, N2 adsorption, TG and SEM. Moreover, the stabilities of these materials were examined by soaking the samples in water. The PXRD results reveal that all of these Hf-based MOFs have a topology similar to that of UiO-66(Zr), and Hf-FUM is stable up to 400°C while Hf-BDC and Hf-BPDC remain stable at 500°C. The structures of Hf-FUM and Hf-BDC are water-resistant, while that of Hf-BPDC will decompose after water treatment. On the basis of the adsorption isotherms of CO2, N2 and CH4 at 298 K, the effect of pore size on the separation of CO2/N2 and CO2/CH4 systems were also investigated. It is found that Hf-FUM with the smallest pore size possesses the highest adsorption selectivity for CO2 over N2 and CH4. This is the first study on the performance of Hf-based MOFs for gas separation, and the knowledge obtained in this work provides a foundation for the design of new nanoporous materials towards CO2 capture from various gas mixtures.
