Chen Jingjing, Zhang Guoping, Bai Yi, Xiong Yan, Liu Xing
School of Geography and Resources, Guizhou Education University, Guiyang, China.
State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, China.
PLoS One. 2025 Sep 4;20(9):e0331138. doi: 10.1371/journal.pone.0331138. eCollection 2025.
Antimony (Sb) is extensively utilized in industrial activities, but most of its compounds exhibit human toxicity and are classified as priority-controlled pollutants. Unlike traditional electrochemical methods that remove metallic pollutants via coagulation or precipitation, electrochemical hydride generation technology converts antimony (Sb) in wastewater into stibine gas (SbH3) for efficient removal. Furthermore, the generated SbH₃ can be decomposed thermally to partially recover metallic antimony. In synthetic wastewater treatment (Sb = 5 mg/L), the proton exchange membrane (Nafion117) electrolysis device achieved an antimony removal efficiency of 72.8 ± 2.2%, outperforming traditional cation-exchange membranes. This enhancement is attributed to the membrane's proton-selective transport and high H conductivity. Increasing the temperature enhanced the generation and release of SbH3, with the higher removal efficiency of 87.3 ± 2.6% achieved at approximately 30 °C. However, temperatures exceeding 30 °C could lead to the partial decomposition of SbH3 back into the solution, thereby affecting removal efficiency. Ultrasonic stirring in the cathode chamber significantly enhanced Sb removal from high-concentration solutions (5 mg/L), while magnetic stirring was more suitable for lower-concentration solutions. Orthogonal experiments revealed that due to the competitive relationship between hydrogen generation and SbH3 generation, as well as the gas-blocking effect, current intensity and electrode area both had a significant impact on Sb removal. Under appropriate current intensity and electrode area conditions (0.5 A, 20 cm²), a high removal rate of 78.5 ± 4.6% can be achieved. Consequently, employing a Nafion membrane coupled with ultrasonic agitation under optimized conditions (30°C, 25 mA/cm²) effectively accelerates antimony removal kinetics and enhances elimination efficiency. However, the substantial reduction in current efficiency and elevated energy consumption induced by competitive hydrogen evolution represent critical challenges requiring urgent resolution. This treatment approach provides a technical reference for shifting from mere contaminant removal to resource recovery. The integration of removal and recovery processes holds substantial potential for implementing circular economy models in mining and metallurgical industries.
锑(Sb)在工业活动中被广泛使用,但其大多数化合物具有人体毒性,被列为优先控制污染物。与通过混凝或沉淀去除金属污染物的传统电化学方法不同,电化学氢化物发生技术将废水中的锑(Sb)转化为锑化氢气体(SbH₃)以实现高效去除。此外,生成的SbH₃可以通过热分解来部分回收金属锑。在合成废水处理(Sb = 5 mg/L)中,质子交换膜(Nafion117)电解装置实现了72.8±2.2%的锑去除效率,优于传统阳离子交换膜。这种提高归因于该膜的质子选择性传输和高H⁺传导率。升高温度增强了SbH₃的生成和释放,在约30°C时实现了更高的87.3±2.6%的去除效率。然而,温度超过30°C可能导致SbH₃部分分解回到溶液中,从而影响去除效率。阴极室中的超声搅拌显著提高了高浓度溶液(5 mg/L)中锑的去除率,而磁力搅拌更适合低浓度溶液。正交实验表明,由于析氢与SbH₃生成之间的竞争关系以及气体阻塞效应,电流强度和电极面积对锑的去除都有显著影响。在适当的电流强度和电极面积条件(0.5 A,20 cm²)下,可以实现78.5±4.6%的高去除率。因此,在优化条件(30°C,25 mA/cm²)下采用Nafion膜并结合超声搅拌可有效加速锑的去除动力学并提高去除效率。然而,竞争性析氢导致的电流效率大幅降低和能耗升高是亟待解决的关键挑战。这种处理方法为从单纯的污染物去除转向资源回收提供了技术参考。去除和回收过程的整合在采矿和冶金行业实施循环经济模式方面具有巨大潜力。