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层状金属硫化物 (KInSnS) 从酸性放射性废水中高效分离三价微量锕系元素。

Highly Efficient Separation of Trivalent Minor Actinides by a Layered Metal Sulfide (KInSnS) from Acidic Radioactive Waste.

机构信息

School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , Suzhou 215123, China.

Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States.

出版信息

J Am Chem Soc. 2017 Nov 22;139(46):16494-16497. doi: 10.1021/jacs.7b10464. Epub 2017 Nov 10.

Abstract

The elimination of trivalent minor actinides (Am, Cm) is of great concern for the safe management and operation of nuclear waste geological repository and environmental remediation. However, because of the effects of protonation, most of the present sorbents exhibit inferior removal properties toward minor actinides at low pH values. Finding stable ion-exchangers with high sorption capacities, fast kinetics, and good removal toward minor actinides from highly acidic solution remains a great challenge. This work reports a new family member of KMS materials with a robust acid-stable layered metal sulfide structure (KInSnS, KMS-5) bearing strong affinity toward trivalent minor actinides. KMS-5 can simultaneously separate trivalent Am and Eu from acidic solutions below pH 2 with high efficiency (>98%). The ion-exchange kinetics is extremely fast (<10 min) and the largest distribution coefficient is as high as 5.91 × 10 mL/g. KMS-5 is also capable of efficiently removing Am from acidic solution containing various competitive cations in large excess. In addition, the ion exchange process of Am by KMS-5 is reversible and the loaded material can be easily eluted by high concentration of potassium chloride. This work represents the first case for efficient minor actinides removal from highly acidic solution using layered metal sulfide materials.

摘要

消除三价次锕系元素(Am、Cm)是安全管理和运行核废料地质处置库和环境修复的关键问题。然而,由于质子化的影响,大多数现有的吸附剂在低 pH 值下对次锕系元素的去除性能较差。寻找具有高吸附容量、快速动力学和良好去除能力的稳定离子交换剂,从高酸度溶液中去除次锕系元素仍然是一个巨大的挑战。本工作报道了一种具有强三价次锕系元素亲和力的新型 KMS 材料家族成员,具有坚固的耐酸稳定层状金属硫化物结构(KInSnS,KMS-5)。KMS-5 可以在 pH 值低于 2 的酸性溶液中同时高效(>98%)分离三价 Am 和 Eu。离子交换动力学非常快(<10 分钟),最大分配系数高达 5.91×10 mL/g。KMS-5 还能够有效地从含有大量过剩竞争阳离子的酸性溶液中去除 Am。此外,KMS-5 对 Am 的离子交换过程是可逆的,负载的材料可以很容易地用高浓度的氯化钾洗脱。本工作代表了首次使用层状金属硫化物材料从高酸度溶液中高效去除次锕系元素的情况。

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