Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs,Chemistry of Materials

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Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-01-10 00:00:00 , DOI: 10.1021/acs.chemmater.7b04619
Riki J. Drout , Kenichi Otake , Ashlee J. Howarth , Timur Islamoglu , Lin Zhu _{1,

2} , Chengliang Xiao _{1,

2} , Shuao Wang _{1,

2} , Omar K. Farha ₃

Affiliation

At the Hanford Site in southeastern Washington state, the U.S. Department of Energy intends to treat 56 million gallons of legacy nuclear waste by encasing it in borosilicate glass via vitrification. This process ineffectively captures radioactive pertechnetate (TcO₄^–) because of the ion’s volatility, thereby requiring a different remediation method for this long-lived (t_1/2 = 2.1 × 10⁵ years), environmentally mobile species. Currently available sorbents lack the desired combination of high uptake capacity, fast kinetics, and selectivity. Here, we evaluate the ability of the chemically and thermally robust Zr₆-based metal–organic framework (MOF), NU-1000, to capture perrhenate (ReO₄^–), a pertechnetate simulant, and pertechnetate. Our material exhibits an excellent perrhenate uptake capacity of 210 mg/g, reaches saturation within 5 min, and maintains perrhenate uptake in the presence of competing anions. Additionally, experiments with pertechnetate confirm perrhenate is a suitable surrogate. Single-crystal X-ray diffraction indicates both chelating and nonchelating perrhenate binding motifs are present in both the small pore and the mesopore of NU-1000. Postadsorption diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) further elucidates the uptake mechanism and powder X-ray diffraction (PXRD) and Brunauer–Emmett–Teller (BET) surface area analysis confirm the retention of crystallinity and porosity of NU-1000 throughout adsorption.

中文翻译：

介孔Zr金属-有机骨架有效捕获高r酸盐和高net酸盐和检测阴离子结合基序

美国能源部打算在华盛顿州东南部的汉福德基地，通过玻璃化将其包裹在硼硅酸盐玻璃中，以处理5600万加仑的遗留核废料。由于离子的挥发性，该过程无法有效捕获放射性高tech酸盐（TcO ₄^–），因此需要针对这种长寿命（t _1/2 = 2.1×10 ⁵年），环境可移动的物种采用不同的补救方法。当前可用的吸附剂缺乏高吸收能力，快速动力学和选择性的期望组合。在这里，我们评估了基于化学和耐热性Zr ₆的金属-有机骨架（MOF）NU-1000捕获高r酸盐（ReO ₄^–），高tech模拟物和高tech。我们的材料显示出极好的高r酸盐摄取能力，为210 mg / g，在5分钟内达到饱和，并在存在竞争性阴离子的情况下保持高r酸盐的摄取。此外，高tech酸盐的实验证实高r酸盐是一种合适的替代品。X射线单晶衍射表明，NU-1000的小孔和中孔中均存在螯合和非螯合的高ate酸盐结合基序。吸附后的漫反射红外傅里叶变换光谱（DRIFTS）进一步阐明了吸收机理，粉末X射线衍射（PXRD）和Brunauer-Emmett-Teller（BET）表面积分析证实了NU-1000在整个吸附过程中都保持了结晶度和孔隙率。

更新日期：2018-01-10

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