Yi Hong, Huo Xiaowei, Gu Jinhong, Wei Lei, Sun Zhenping, Du Fuxiang, Dai Chao, Wu Xiongfei, Liu Zhiguang, Ren Jian
China Construction Third Engineering Bureau Group Co., Ltd Wuhan 430074 PR China
College of Architecture & Environment, Sichuan University Chengdu 610065 PR China.
RSC Adv. 2022 Aug 8;12(34):21780-21792. doi: 10.1039/d2ra02703h. eCollection 2022 Aug 4.
Boron-doped carbon materials (BCs), low-cost and environmentally friendly carbocatalysts, were prepared for the activation of persulfate (PS) for the removal of bisphenol A (BPA). Compared with B-free carbon materials (Cs), the adsorption and catalytic activity were significantly enhanced by the boron modification. Fast and efficient removal of BPA was achieved using the BCs/PS system. The BPA removal rate constant increased linearly with the adsorption capacity of BCs. Electron paramagnetic resonance (EPR) spectroscopy and radical quenching experiments indicated that the degradation mechanisms in the BCs/PS system were different from conventional radical-based oxidation pathways. On the contrary, nonradical pathways were demonstrated to dominate the oxidation processes in the removal of BPA using the BCs/PS system. Herein, a mechanism is proposed where PS is activated by the carbon material to form a reactive electron-deficient carbocatalyst ([BCs]) complex with a high redox potential, driving a nonradical oxidation pathway to achieve BPA removal. Through experimental investigation and the use of electrochemical techniques (cyclic voltammetry, Tafel corrosion analysis and open circuit voltages), B-doped carbon materials for the activation of PS elevate the potential of the derived nonradical [BCs] complexes, and then accelerate the BPA removal efficiency an electron transfer process. Utilizing adsorption and nonradical oxidation processes, the BCs/PS system possesses great potential for the removal of BPA in practical applications such as wastewater treatment.
硼掺杂碳材料（BCs）是一种低成本且环保的碳催化剂，用于活化过硫酸盐（PS）以去除双酚A（BPA）。与无硼碳材料（Cs）相比，硼改性显著提高了其吸附和催化活性。使用BCs/PS体系可快速高效地去除BPA。BPA去除速率常数随BCs的吸附容量呈线性增加。电子顺磁共振（EPR）光谱和自由基猝灭实验表明，BCs/PS体系中的降解机制不同于传统的基于自由基的氧化途径。相反，非自由基途径在使用BCs/PS体系去除BPA的氧化过程中起主导作用。在此，提出了一种机制，即PS被碳材料活化，形成具有高氧化还原电位的缺电子活性碳催化剂（[BCs]*）络合物，驱动非自由基氧化途径实现BPA的去除。通过实验研究和使用电化学技术（循环伏安法、塔菲尔腐蚀分析和开路电压），用于活化PS的硼掺杂碳材料提高了衍生的非自由基[BCs]*络合物的电位，进而加速了BPA的去除效率——一个电子转移过程。利用吸附和非自由基氧化过程，BCs/PS体系在废水处理等实际应用中具有去除BPA的巨大潜力。
