Bo Shufeng, Zhao Xin, An Qingda, Luo Junmei, Xiao Zuoyi, Zhai Shangru
Faculty of Light Industry and Chemical Engineering, Dalian Polytechnic University Dalian 116034 China
RSC Adv. 2019 Feb 11;9(9):5009-5024. doi: 10.1039/c9ra00357f. eCollection 2019 Feb 5.
The rational optimization of catalytic composites with excellent catalytic activities and long-term cycling stabilities for environmental remediation is still maintained as highly desired but is an ongoing challenge. Here, seaweed-derived N-doped versatile carbonaceous beads with Co O (Co-NC-0.25-700 °C) are employed as a novel catalyst to activate peroxymonosulfate (PMS) for methylene blue (MB) degradation. Profiting from the improved structure-activity relationship and the synergistic effects between the "egg-box" structure and the Co O loaded on the N-doped carbonaceous beads, Co-NC-0.25-700 °C exhibited relatively high performance and comparative long-term stability. The universal applicability of Co-NC-0.25-700 °C was investigated by degrading other types of organic pollutants in various systems. For this type of newly fabricated high-performance versatile composites, structure-property relationships were plausibly proposed. Notably, the degradation efficiency and the catalyst structure could be tailored by the amount of polyethyleneimine (PEI) introduced in the preparation process and by the pyrolysis temperature. More favorably, the coupling of the magnetic properties and bead-like shape endows the resultant composites with remarkable reusability and recyclability, as compared to powder state materials. Another interesting finding is that MB degradation over Co-NC-0.25-700 °C is minimally affected by common ions (Cl, NO , SO , ), and holds a certain catalytic activity under the background conditions of two simulated real water conditions (running water and seawater). Of particular interest, a microreactor filled with Co-NC-0.25-700 °C was utilized as a verification model for practical applications of the reaction in continuous-flow. More far-reaching, the simulations of actual water conditions and the design of a continuous-flow reactor represent a giant step towards universal applications for organic pollution treatment.
合理优化具有优异催化活性和长期循环稳定性的催化复合材料用于环境修复，仍然是人们高度期望的，但也是一项持续存在的挑战。在此，以海藻衍生的负载Co₃O₄的N掺杂多功能碳质珠粒（Co-NC-0.25-700 °C）作为新型催化剂，用于活化过一硫酸盐（PMS）以降解亚甲基蓝（MB）。得益于改善的结构-活性关系以及N掺杂碳质珠粒上的“蛋盒”结构与负载的Co₃O₄之间的协同效应，Co-NC-0.25-700 °C表现出相对较高的性能和相当长的长期稳定性。通过在各种体系中降解其他类型的有机污染物，研究了Co-NC-0.25-700 °C的普遍适用性。对于这类新制备的高性能多功能复合材料，合理提出了结构-性能关系。值得注意的是，降解效率和催化剂结构可以通过制备过程中引入的聚乙烯亚胺（PEI）的量以及热解温度来调节。更有利的是，与粉末状材料相比，磁性和珠状形状的结合赋予了所得复合材料显著的可重复使用性和可回收性。另一个有趣的发现是，Co-NC-0.25-700 °C对亚甲基蓝的降解受常见离子（Cl⁻、NO₃⁻、SO₄²⁻）的影响最小，并且在两种模拟实际水条件（自来水和海水）的背景条件下保持一定的催化活性。特别值得关注的是，一个填充有Co-NC-0.25-700 °C的微反应器被用作该反应在连续流中实际应用的验证模型。更具深远意义的是，实际水条件的模拟和连续流反应器的设计代表了有机污染处理通用应用向前迈出的一大步。
