Bao Zongbi, Wang Jiawei, Zhang Zhiguo, Xing Huabin, Yang Qiwei, Yang Yiwen, Wu Hui, Krishna Rajamani, Zhou Wei, Chen Banglin, Ren Qilong
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD, 20899-6102, USA.
Angew Chem Int Ed Engl. 2018 Dec 3;57(49):16020-16025. doi: 10.1002/anie.201808716. Epub 2018 Nov 11.
Purification of C H from an C H /C H mixture, one of the most important while challenging industrial separation processes, is mainly through energy-intensive cryogenic distillation. Now a family of gallate-based metal-organic framework (MOF) materials is presented, M-gallate (M=Ni, Mg, Co), featuring 3D interconnected zigzag channels, the aperture sizes of which (3.47-3.69 Å) are ideally suitable for molecular sieving of ethylene (3.28×4.18×4.84 Å ) and ethane (3.81×4.08×4.82 Å ) through molecular cross-section size differentiation. Co-gallate shows an unprecedented IAST selectivity of 52 for C H over C H with a C H uptake of 3.37 mmol g at 298 K and 1 bar, outperforming the state-of-the-art MOF material NOTT-300. Direct breakthrough experiments with equimolar C H /C H mixtures confirmed that M-gallate is highly selective for ethylene. The adsorption structure and mechanism of ethylene in the M-gallate was further studied through neutron diffraction experiments.
从乙烯/乙烷混合物中提纯乙烯是最重要但极具挑战性的工业分离过程之一,主要通过能耗高的低温蒸馏进行。现在报道了一类基于没食子酸盐的金属有机框架(MOF)材料,即M-没食子酸盐(M = Ni、Mg、Co),其具有三维相互连接的之字形通道,通道孔径大小(3.47 - 3.69 Å)非常适合通过分子横截面尺寸差异对乙烯(3.28×4.18×4.84 Å)和乙烷(3.81×4.08×4.82 Å)进行分子筛分离。在298 K和1 bar下,Co-没食子酸盐对乙烯相对于乙烷表现出前所未有的IAST选择性52,乙烯吸附量为3.37 mmol g,性能优于最先进的MOF材料NOTT-300。用等摩尔乙烯/乙烷混合物进行的直接突破实验证实,M-没食子酸盐对乙烯具有高度选择性。通过中子衍射实验进一步研究了乙烯在M-没食子酸盐中的吸附结构和机理。