Metal Doping Induced Formation and Dynamic Gas Sorption of a Highly Porous Mesoporous MetalOrganic Framework

Zheng Yin
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Abstract

A new high-porosity MOF of [Ni2.3Zn0.7(tzba)3 (H2 O)6 ]·12DMF (NiZn-MOF) processes 2D (3,6)-grid layers constructed from rare [M2 (tz)3 (H2 O)3 ] and [M(COO)3 ] nodes. The metal doping of Ni2+ and Zn2+ are crucial for the formation of the two kinds of metal nodes and subsequent synergistical assembly into the mesoporous MOF, in contrast to the formation of MIL-88-topology resembled compound of {(Me2 NH2 )[Ni3 (μ3 -OH)(tzba)3 (H2 O)3 ]·8DMF (Ni3-MOF) using single Ni2+ as metal source. The regular 2D layers stacked in parallel and ABAB fashion through interlayer hydrogen bonding, leading to a neutral framework with void fraction up to 72.1% and 1D mesoporous hexagonal channels sized at 24.0 Å in diameter. The large gas accessible porosity was revealed by the saturated N2 and CO2 uptake of 720 and 708 cm3 g-1, at 77 K and 195 K, respectively, giving a high Langmuir surface area of 2066 m2 g-1. The varying gas sorption amounts dependent on accommodated solvents and activation temperature, as well as the gate-opening behaviors in sorption isotherms, well confirm the dynamic structure response to guest species of the flexible framework.
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金属掺杂诱导高孔介孔金属有机骨架的形成和动态气体吸附
一种新型的高孔隙率MOF [Ni2.3Zn0.7(tzba)3 (H2 O)6]·12DMF (NiZn-MOF)处理了由稀有的[M2 (tz)3 (H2 O)3]和[M(COO)3]节点构成的2D(3,6)网格层。相对于以单一Ni2+为金属源形成的mil -88结构类似化合物{(Me2 NH2)[Ni3 (μ3 -OH)(tzba)3 (H2 O)3]·8DMF (Ni3-MOF), Ni2+和Zn2+的金属掺杂是形成这两种金属节点并协同组装成介孔MOF的关键。规则的二维层通过层间氢键以平行和ABAB方式堆叠,形成空隙率高达72.1%的中性骨架和直径为24.0 Å的一维介孔六边形通道。在77 K和195 K条件下,饱和N2和CO2吸收量分别为720和708 cm3 g-1, Langmuir表面积为2066 m2 g-1,显示出较大的气体可达孔隙度。吸附量随溶剂和活化温度的变化,以及吸附等温线上的开门行为,很好地证实了柔性骨架对客体物质的动态结构响应。
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