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通过使用巯基功能化金属有机框架,利用硫氧化还原机制从电子垃圾浸出液中选择性提取金。

Selective gold extraction from e-waste leachate via sulfur-redox mechanisms using sulfhydryl-functionalized MOFs.

作者信息

Qin Jialong, Liu Hengzhi, Fang Zhuoya, Pei Junjun, Yin Kai, Fu Kaixing, Luo Jinming

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha, Hunan Province 410082, PR China; State Environmental Protection Key Laboratory of Environmental Health Impact Assessment of Emerging Contaminants, School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, PR China.

Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen 518055, Guangdong, PR China.

出版信息

Water Res. 2025 May 1;275:123170. doi: 10.1016/j.watres.2025.123170. Epub 2025 Jan 21.

Abstract

Urban mining of precious metals from electronic waste (e-waste) offers a dual advantage by addressing solid waste management challenges and supplying high-value metals for diverse applications. However, traditional extraction methods generally suffer from poor selectivity and limited capacity in complex acidic leachate. Herein, we present a sulfhydryl-functionalized zirconium-based metal-organic framework (Zr-MSA-AA) as a recyclable and highly selective adsorbent for efficient gold recovery. Specifically, the Zr-MSA-AA exhibits high recovery capacity (1021 mg g), remarkable pH-universal, and superb selectivity (K of 2.2 × 10 mL g) for gold ions across wide pH range and competitive conditions. Comprehensive mechanistic investigations highlight the pivotal role of sulfhydryl groups in selectively capturing gold ions. The redox-transformation of sulfhydryl and sulfonic acid groups mediated the reduction of Au(III) to Au(0) through the nucleation of chlorine-stabilized gold clusters. This unique mechanism, driven by the redox activity of designed sulfhydryl sites, not only mitigates interference from competing cations but also facilitates rapid adsorption kinetics (k of 1.17 × 10 m s) for gold ions, surpassing the performance of previous adsorbents. Consequently, Zr-MSA-AA demonstrates exceptional practical applicability, achieving high-purity gold recovery (23.8 Karat) from real e-waste leachate through straightforward physical separation methods. This study introduces an alternative practical strategy for utilizing sulfur's redox activity in adsorbent design, advancing the sustainable recycling of non-renewable metal resources while contributing to environmental conservation.

摘要

从电子废物(电子垃圾)中进行城市贵金属开采具有双重优势,既能应对固体废物管理挑战,又能为各种应用提供高价值金属。然而,传统提取方法在复杂酸性浸出液中通常选择性差且容量有限。在此,我们提出一种巯基功能化的锆基金属有机框架(Zr-MSA-AA)作为一种可回收且具有高选择性的吸附剂,用于高效回收金。具体而言,Zr-MSA-AA在宽pH范围和竞争条件下对金离子表现出高回收容量(1021 mg/g)、显著的pH通用性和卓越的选择性(K为2.2×10 mL/g)。全面的机理研究突出了巯基在选择性捕获金离子中的关键作用。巯基和磺酸基团的氧化还原转化通过氯稳定的金簇的成核介导了Au(III)还原为Au(0)。这种由设计的巯基位点的氧化还原活性驱动的独特机制,不仅减轻了竞争性阳离子的干扰,还促进了金离子的快速吸附动力学(k为1.17×10 m/s),超过了先前吸附剂的性能。因此,Zr-MSA-AA展示了卓越的实际适用性,通过简单的物理分离方法从实际电子垃圾浸出液中实现了高纯度金回收(23.8克拉)。本研究引入了一种在吸附剂设计中利用硫的氧化还原活性的替代实用策略,推动不可再生金属资源的可持续回收,同时有助于环境保护。

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