Journal of Environmental Radioactivity ( IF 1.9 ) Pub Date : 2020-08-06 , DOI: 10.1016/j.jenvrad.2020.106372 Dien Li 1 , Natalia B Shustova 2 , Corey R Martin 2 , Kathryn Taylor-Pashow 1 , John C Seaman 3 , Daniel I Kaplan 1 , Jake W Amoroso 1 , Roman Chernikov 4
There are few effective technologies for the sequestration of highly water-soluble pertechnetate (TcO4−) from contaminated water despite the urgency of environmental and public health concerns. In this work, anion exchanged and cetyltrimethylammonium bromide (CTAB) functionalized MIL-101-Cr-NO3 were investigated for perrhenate (ReO4−), a surrogate of TcO4−, sequestration from artificial groundwater. Cl−, I−, and CF3SO3− exchanged MIL-101-Cr proved more effective at ReO4− removal than the parent MIL-101-Cr-F. Compared to the parent framework, CTAB functionalized MIL-101-Cr-NO3 increased ReO4− removal capacity from 39 to 139 mg/g, improved the reaction kinetics from ~30 to <10 min to reach full adsorption capacity and the selectivity for ReO4− over competing NO3−, CO32−, SO42−, and Cl−. Spectroscopic data indicated that the chemical speciation of Re in the exchanged MIL-101-Cr remained ReO4−, indicating synergistic sequestration through both anion exchange and non-ion exchange binding with the positively charged ligand of CTAB. These studies foreshadow potential applications of MOFs for the remediation of 99TcO4− from contaminated environments.
中文翻译:
阴离子交换和季铵官能化的MIL-101-Cr金属有机骨架(MOF),用于隔离地下水中的ReO4- / TcO4-。
很少有有效的技术为高水溶性高锝酸盐的封存(TCO 4 - )从受污染的水,尽管对环境和公众健康问题的紧迫性。在这项工作中,阴离子交换和十六烷基三甲基铵(CTAB)官能MIL-101-Cr系NO 3进行了调查高铼酸盐(REO 4 - ),TCO的替代4 - ,从人工地下水封存。氯-,我-,和CF 3 SO 3 -交换MIL-101-的Cr在REO证明更有效的4 -去除率高于母体MIL-101-Cr-F。相比于亲本框架内,CTAB官能MIL-101-Cr系NO 3增加REO 4 -去除能力从39至139毫克/克,改善从〜30中的反应动力学至<10分钟以达到充分的吸附能力和选择性REO 4 -优于竞争NO 3 -,CO 3 2-,SO 4 2-和Cl - 。光谱数据表明,再在化学形态交换MIL-101-铬保持REO 4 -,表明通过阴离子交换和非离子交换与CTAB带正电荷的配体的结合而进行的螯合。这些研究预示了整治MOFs材料的潜在应用99 TCO 4 -从污染的环境。