Unusual and Highly Tunable Missing-Linker Defects in Zirconium Metal-Organic Framework UiO-66 and Their Important Effects on Gas Adsorption | |
Wu, Hui1,2; Chua, Yong Shen1,3; Krungleviciute, Vaiva1,4; Tyagi, Madhusudan1,2; Chen, Ping3; Yildirim, Taner1,4; Zhou, Wei1,2 | |
刊名 | journal of the american chemical society |
2013-07-17 | |
卷号 | 135期号:28页码:10525-10532 |
通讯作者 | wei zhou |
产权排序 | 待补充 |
合作状况 | 英 |
英文摘要 | uio-66 is a highly important prototypical zirconium metal-organic framework (mof) compound because of its excellent stabilities not typically found in common porous mofs. in its perfect crystal structure, each zr metal center is fully coordinated by 12 organic linkers to form a highly connected framework. using high-resolution neutron power diffraction technique, we found the first direct structural evidence showing that real uio-66 material contains significant amount of missing-linker defects, an unusual phenomenon for mofs. the concentration of the missing-linker defects is surprisingly high, similar to 10% in our sample, effectively reducing the framework connection from 12 to similar to 11. we show that by varying the concentration of the acetic acid modulator and the synthesis time, the linker vacancies can be tuned systematically, leading to dramatically enhanced porosity. we obtained samples with pore volumes ranging from 0.44 to 1.0 cm(3)/g and brunauer-emmett-teller surface areas ranging from 1000 to 1600 m(2)/g, the largest values of which are similar to 150% and similar to 60% higher than the theoretical values of defect-free uio-66 crystal, respectively. the linker vacancies also have profound effects on the gas adsorption behaviors of uio-66, in particular co2. finally, comparing the gas adsorption of hydroxylated and dehydroxylated uio-66, we found that the former performs systematically better than the latter (particularly for co2) suggesting the beneficial effect of the -oh groups. this finding is of great importance because hydroxylated uio-66 is the practically more relevant, non-air-sensitive form of this mof. the preferred gas adsorption on the metal center was confirmed by neutron diffraction measurements, and the gas binding strength enhancement by the -oh group was further supported by our first-principles calculations. |
学科主题 | 物理化学 |
WOS标题词 | science & technology ; physical sciences |
类目[WOS] | chemistry, multidisciplinary |
研究领域[WOS] | chemistry |
关键词[WOS] | porous coordination polymer ; neutron-scattering ; methane storage ; ligand ; stabilization ; stability ; hydrogen ; future |
收录类别 | SCI |
资助信息 | 3,2 |
原文出处 | 10532 |
语种 | 英语 |
WOS记录号 | WOS:000322103000064 |
公开日期 | 2014-09-11 |
内容类型 | 期刊论文 |
源URL | [http://159.226.238.44/handle/321008/119371] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
作者单位 | 1.NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA 2.Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA 3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 4.Univ Penn, Dept Mat Sci & Engn, Philadelphia, PA 19104 USA |
推荐引用方式 GB/T 7714 | Wu, Hui,Chua, Yong Shen,Krungleviciute, Vaiva,et al. Unusual and Highly Tunable Missing-Linker Defects in Zirconium Metal-Organic Framework UiO-66 and Their Important Effects on Gas Adsorption[J]. journal of the american chemical society,2013,135(28):10525-10532. |
APA | Wu, Hui.,Chua, Yong Shen.,Krungleviciute, Vaiva.,Tyagi, Madhusudan.,Chen, Ping.,...&Zhou, Wei.(2013).Unusual and Highly Tunable Missing-Linker Defects in Zirconium Metal-Organic Framework UiO-66 and Their Important Effects on Gas Adsorption.journal of the american chemical society,135(28),10525-10532. |
MLA | Wu, Hui,et al."Unusual and Highly Tunable Missing-Linker Defects in Zirconium Metal-Organic Framework UiO-66 and Their Important Effects on Gas Adsorption".journal of the american chemical society 135.28(2013):10525-10532. |
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