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使用葫芦[6]脲进行高效金回收

High-Efficiency Gold Recovery Using Cucurbit[6]uril.

作者信息

Wu Huang, Jones Leighton O, Wang Yu, Shen Dengke, Liu Zhichang, Zhang Long, Cai Kang, Jiao Yang, Stern Charlotte L, Schatz George C, Stoddart J Fraser

机构信息

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

School of Science, Westlake University, 18 Shilongshan Road, Hangzhou 310024, China.

出版信息

ACS Appl Mater Interfaces. 2020 Aug 26;12(34):38768-38777. doi: 10.1021/acsami.0c09673. Epub 2020 Aug 15.

Abstract

Developing an extremely efficient and highly selective process for gold recovery is urgently desired for maintaining a sustainable ecological environment. Herein, we report a highly efficient gold-recovery protocol on the basis of the instantaneous assembly between cucurbit[6]uril (CB[6]) and [AuX] (X = Cl/Br) anions. Upon mixing CB[6] with the four gold-bearing salts MAuX (M = H/K, X = Cl/Br) in aqueous solutions, yellow or brown coprecipitates form immediately, as a result of multiple weak [Au-X···H-C] (X = Cl/Br) hydrogen-bonding and [Au-X···C=O] (X = Cl/Br) ion-dipole interactions. The gold-recovery efficiency, based on · coprecipitation, reaches 99.2% under optimized conditions. In the X-ray crystal superstructures, [AuCl] anions and CB[6] molecules adopt an alternating arrangement to form doubly connected supramolecular polymers, while [AuBr] anions are accommodated in the lattice between two-dimensional layered nanostructures composed of CB[6] molecules. DFT calculations have revealed that the binding energy (34.8 kcal mol) between CB[6] molecules and [AuCl] anions is higher than that (11.3-31.3 kcal mol) between CB[6] molecules and [AuBr] anions, leading to improved crystallinity and higher yields of · (M = H/K) coprecipitates. Additionally, a laboratory-scale gold-recovery protocol, aligned with an attractive strategy for the practical recovery of gold, was established based on the highly efficient coprecipitation of ·. The use of CB[6] as a gold extractant provides us with a new opportunity to develop more efficient processes for gold recovery.

摘要

为了维持可持续的生态环境,迫切需要开发一种极其高效且高度选择性的金回收工艺。在此,我们报告了一种基于葫芦[6]脲(CB[6])与[AuX](X = Cl/Br)阴离子之间的瞬时组装的高效金回收方案。在水溶液中将CB[6]与四种含金盐MAuX(M = H/K,X = Cl/Br)混合时,由于多个弱的[Au-X···H-C](X = Cl/Br)氢键和[Au-X···C=O](X = Cl/Br)离子-偶极相互作用,会立即形成黄色或棕色共沉淀。基于共沉淀的金回收效率在优化条件下达到99.2%。在X射线晶体超结构中,[AuCl]阴离子和CB[6]分子采用交替排列形成双连接超分子聚合物,而[AuBr]阴离子则容纳在由CB[6]分子组成的二维层状纳米结构之间的晶格中。密度泛函理论计算表明,CB[6]分子与[AuCl]阴离子之间的结合能(34.8 kcal mol)高于CB[6]分子与[AuBr]阴离子之间的结合能(11.3 - 31.3 kcal mol),从而导致更高的结晶度和更高产率的·(M = H/K)共沉淀。此外,基于·的高效共沉淀,建立了一种与实用的金回收有吸引力的策略相一致的实验室规模的金回收方案。使用CB[6]作为金萃取剂为我们开发更高效的金回收工艺提供了新机会。

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