第一作者：Xue Zhao, Liangfei Duan, Mengshan Chen 通讯作者：Xue Zhao 通讯单位：云南师范大学化学与化学工程学院 DOI:10.1016/j.cej.2024.149928 基于过一硫酸盐（PMS）的高级氧化工艺（AOPs）可以为消除持久性有机污染物（POPs）提供强活性氧（ROS），但关键在于输入高活性的环境友好型催化剂。在这里，利用库仑相互作用将封闭钴原位沉积在天然矿物埃洛石纳米管上，进一步实现了在具有大比表面积的掺氮中空碳纳米管中引入原子分散的钴位点。所构建的 CoNC/NHCNTs-900 材料能有效活化 PMS，使四环素探针污染物的去除率接近 100%，矿化率达到创纪录的 89.07%。结合密度泛函理论计算证明，石墨氮的富集有利于调节Co的微环境，促进PMS的吸附和活化。对 ROS 的形成和四环素矿化机理的深入跟踪证明，CoNC/NHCNTs-900 驱动的 AOPs 将持久性有机污染物降解为低毒物种具有可靠性和实用性。
Fig. 1. A schematic diagram of constructing CoCN/NHCNT by combining complexation confinement and spatial confinement.
Fig. 2. (a) SEM image of CoCN/NHCNTs-600, (b) SEM image of CoCN/NHCNTs-750, (c) SEM image of CoCN/NHCNTs-900; (d,f) AC-STEM image of CoCN/NHCNTs-900; (e) Element mapping of CoCN/NHCNTs-900.
Fig. 3. (a) XRD signals of CoCN/NHCNTs-600, CoCN/NHCNTs-600, CoCN/NHCNTs-600; (b) The hysteresis loops of CoNPs/CN, CoCN/NHCNTs-600, CoCN/NHCNTs-600, and CoCN/NHCNTs-600; (c) High-resolution XPS signals of Co elements in CoCN/NHCNTs-600, CoCN/NHCNTs-600, and CoCN/NHCNTs-600; (d) High-resolution XPS signals of N elements in CoCN/NHCNTs-600, CoCN/NHCNTs-600, and CoCN/NHCNTs-600; (e) The raio of different N species; (f) XANES of Co-foil, CoO, and CoCN/NHCNTs-900; (g) EXAFS of Co-foil, CoO, CoPc, and CoCN/NHCNTs-900; (h) The two-dimensional color block diagram of EXAFS signal obtained by wavelet transform.
Fig. 4. (a) The removal rate-time curves of CoNC/NHCNTs-600, CoNC/NHCNTs-750, and CoNC/NHCNTs-900 degraded TC; (b) The effect of the dosage of CoNC/NHCNTs-900 on the degradation of TC was changed; (c) The effect of the dosage of PMS on the degradation of TC was changed; (d-e) The relationship between ln(Ct/C0) and time; (g) The removal of TC by adding only PMS and adding PMS first and then adding CoNC/NHCNTs-900; (h) The changes of current signals when PMS was added to the electrolyte with carbon paper and CoNC/NHCNTs-900 as working electrodes, respectively; (i) The removal rate of total organic carbon after TC degradation by CoNC/NHCNTs-900 activated PMS for 30 min. Generally, PMS dosage is 30 mg, TC concentration is 20 mg/L, solution volume is 100 mL, pH value is 7.0, and catalyst dosage is 20 mg.
Fig. 5. (a) The effect of solution pH on the degradation of TC by CoNC/NHCNTs-900 activated PMS; (b) The performance of CoNC/NHCNTs-900 activated PMS for the degradation of 4-NP, BPA, MO and RhB, respectively; (c) The effect of coexisting ions in the solution on the degradation of TC by CoNC/NHCNTs-900 activated PMS; (d) The performance of TC degradation by CoNC/NHCNTs-900 in the case of repeated use. Generally, PMS dosage is 30 mg, solution volume is 100 mL, pH value is 7.0, and catalyst dosage is 20 mg.
Fig. 6. (a) The effect of light on the degradation of TC by CoNC/NHCNTs-900; (b) The degradation performance of TC by CoNC/NHCNTs-900, CoNPs and CoPc; (c) Electrochemical impedance spectroscopy of CoNC/NHCNTs-900 and CoPc; (d) The temperature-programmed adsorption/desorption curves of CoNC/NHCNTs-900 and CoNPs/CN for nitrogen. Where, PMS dosage is 30 mg, solution volume is 100 mL, pH value is 7.0, and catalyst dosage is 20 mg. Xue Zhao, Liangfei Duan, Mengshan Chen, Peizhi Yang, Qian Liu, Yuelong Liu, Haoran Zhang, Zhuang He, Guangzhi Hu, Yingtang Zhou, Regulating the microenvironment of atomically dispersed cobalt to achieve the record-breaking mineralization and 100% removal of organic pollutant, Chemical Engineering Journal, 2024, https:///10.1016/j.cej.2024.149928  声明：本公众号仅分享前沿学术成果，无商业用途。如涉及侵权，请立刻联系公众号后台或发送邮件，我们将及时修改或删除！ |
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