【摘要】 针对含碳加压氧化渣中金的高效回收难题，本文提出一种两段三氯异氰尿酸（TCCA）高效浸出工艺。通过单因素实验优化浸出条件，并基于未反应收缩核模型揭示其浸出动力学机制。结果表明：TCCA浸出含碳加压氧化渣的最佳条件为：TCCA浓度为0.02 mol·L^-1, NaCl质量浓度为30 g·L^-1，浸出温度为30℃，固-液比为1∶6，浸出时间为3 h。在该条件下，一段浸出的浸金率达86.24%。浸出液经D301树脂靶向吸附后进行二段浸出实验，二段浸出的浸金率为56.72%，总浸出率提升至93.98%。动力学分析表明，浸出前期（0～1 h）和浸出中期（1～2 h）均受固体产物层扩散模型控制，其表观活化能分别为4.552和8.794 kJ·mol^-1。浸出后期（2～3 h）则转变为界面化学反应模型控制，活化能为45.515 kJ·mol^-1。研究结果为含碳难处理金矿的绿色高效提取提供了新的技术思路与理论依据。更多还原

【Abstract】 Carbonaceous refractory gold ores, accounting for over 35% of China’s gold resource reserves, arecharacterized by their complex mineralogy and present intricate challenges stemming from two mechanisms: one is microencapsulation of gold particles within sulfide minerals, such as pyrite and arsenopyrite. And the other is the preg-robbing effect of carbonaceous matters via competitive adsorption of gold-cyanide complexes.In addition, the conventional cyanidation process struggles to achieve efficient gold recovery from such ores, primarily due to low gold recovery and excessive reagent consumption. In China, where such ores account for a substantial proportion of unmined gold resources, their efficient exploitation is critical to ensure domestic gold source security and reduce reliance on imported gold resources. As free-milling gold ore resources continue to deplete, the development and efficient utilization of carbonaceous gold ores are pivotal for sustaining domestic gold production. Currently, the advancements in pretreatment technologies, including roasting oxidation, pressure oxidation, bio-oxidation, and chemical oxidation, have demonstrated efficacy in liberating the encapsulationof gold and mitigatingthe interference of carbonaceous matters, achieving efficient gold leaching.However, these methods face limitations such as high energy consumption, environmental risks, and complex slurry components.According to the limitations of these techniques, this study introduced a novel two-stage leaching process utilizing trichloroisocyanuric acid（TCCA） as an environmentally lixiviant alternative to traditional cyanide-based systems, especially targeting carbonaceous pressure-oxidized ore. TCCA, a chlorinated heterocyclic compound with a triazine ring structure, was renowned for its high effective chlorine content and stable, slow-release property in aqueous solution. As a solid oxidizing agent, TCCA dissociated in aqueous solutions to generate isocyanuric acid and hypochlorous acid, maintaining pH range of 6.5～7.5 while releasing ClO^-. This unique chemical behavior enabled its multifunctional applications across multiple industries, such as water treatment, agriculture and food safety, organic chemical synthesis, pharmaceutical industry, hydrometallurgy, and other fields. In this study, aiming at the efficient recovery of gold from carbonaceous pressure-oxidized ore, an innovative approach for the sustainable and efficient recovery of gold from carbonaceous pressure-oxidized ore by introducing a two-stage leaching process utilizing TCCA as a green lixiviant was proposed. In order to optimize the gold leaching efficiency, systematic one-factor experiments were conducted to investigate the effects of critical parameters, including TCCA concentration, NaCl mass concentration, leaching temperature, solid-liquid ratio, and leaching time. The optimal leaching conditions were determined as follows: TCCA concentration of 0.02 mol·L^-1, NaCl mass concentration of 30 g·L^-1, leaching temperature of 30 ℃, solid-liquid ratio of 1∶6, and a leaching time of 3 h. Under these conditions, the first-stage leaching achieved a gold leaching efficiency of 86.24%. To further enhance recovery, the pregnant leach solution was subjected to D301 resin to adsorb gold-chloride complexes, enabling a subsequent second-stage gold leaching. This secondary process contributed an additional 56.72% gold leaching efficiency, culminating in a remarkable cumulative gold recovery of 93.98%, representing a significant improvement over the conventional single-stage method. Moreover, kinetic investigations based on the unreacted shrinkage core model revealed the gold leaching mechanism by using TCCA. The kinetic analysis of TCCA leaching of carbonaceous pressureoxidized ore was conducted at different temperatures, establishing solid product layer diffusion control and interface chemical reaction control. The results indicated that, in the initial phase（0～1 h）, gold dissolution was governed by a solid product layer diffusion model, as evidenced by a low activation energy of 4.552 kJ·mol^-1. This mechanism persisted during the intermediate stage（1～2 h）, with a slightly increased activation energy of 8.794 kJ·mol^-1, suggesting intensified diffusion limitations. Remarkably, the final leaching stage（2～3 h） exhibited a shift to interfacial chemical reaction control, characterized by a substantially higher activation energy of 45.515 kJ·mol^-1, indicative of surface-bound oxidative reactions dominating the rate-limiting step.During the initial and intermediate leaching stages, TCCA and its hydrolysis products adsorbed onto the surface of gold particles through the diffusion layer, allowing effective contact between effective chlorine and gold. As the leaching reaction progresses, chemical reactions occurred between effective chlorine and gold to form a stable gold-chloride complex, where the reaction rate was controlled by the rate-limiting step for the carbonaceous pressureoxidized ore in TCCA leaching system. The integration of resin adsorption with sequential leaching stages not only demonstrated superior extraction performance but also aligned with environmentally conscious metallurgy by minimizing reagent consumption and enhancing process sustainability. After the two-stage TCCA leaching, the effective chlorine content in TCCA leaching solution decreased to 1.49%. The leaching solution could be repurposed for water treatment or disinfectant preparation, achieving closed-loop recycling of resources. Such utilization aligned with the sustainable development goals of green metallurgy by minimizing waste and promoting circular economy practices. Therefore, this work established a novel paradigm for addressing the challenges of carbonaceous refractory gold ores, offering a technically viable and eco-friendly alternative to conventional cyanidation methods. The findings provided critical insights into reaction dynamics and operational optimization, providing the way for industrial implementation of TCCA-based hydrometallurgical systems, andfurther contributing to the sustainable exploitation of China’s strategic gold resources in green mining technologies.更多还原