Activation of peroxymonosulfate by Fe-N complexes embedded within SBA-15 for removal of organic contaminants via production of singlet oxygen
Activation of peroxymonosulfate by Fe-N complexes embedded within SBA-15 for removal of organic contaminants via production of singlet oxygen
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通过嵌入 SBA-15 中的 Fe-N 络合物活化过一硫酸盐，通过产生单线态氧去除有机污染物
DOI：
10.1007/s11356-018-3323-1
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发表时间：
2018
影响因子：
5.8
通讯作者：
Wen Yuezhong
中科院分区：
文献类型：
--
作者：
Yang Qunfeng;Jia Nanzhengfang;Shen Chensi;Ma Jianqing;Wen Yuezhong
过硫酸盐被认为是一种很有前途的氧化剂，可以替代芬顿反应用于水处理。然而，现有的激活方法限制了其实际应用。本文首次探讨了Fe-N配合物作为过硫酸盐活化催化剂的可能性。以氯化铁、咪唑和SBA-15为原料，在高温下合成了Fe-Im-SBA催化剂。Fe-Im-SBA的内部孔隙结构保持良好；Fe、N、C元素在催化剂上均匀分布。该催化剂在PMS活化下对Rh B的去除率达到97.0%，表现出优异的催化活性，在前5分钟内对Rh B的去除率达到97.0%。在较宽的pH范围内也表现良好，在0.5 ~ 10的pH范围内完全去除Rh B，表明该催化剂在酸性和碱性条件下都具有稳定性。此外，Fe-Im-SBA对不同类型的污染物具有较强的降解能力，这为其在环境保护方面的应用提供了有利条件。通过x射线吸收光谱分析表明，Fe-Im-SBA的活性位点由fe - n4位点和fe2 - n2位点组成。在Fe-Im-SBA/PMS体系中被证明产生了122，并作为主要的活性氧。同时，石墨碳可以加速电子的转移，这也可能是其催化性能高的原因。
Persulfates are recognized as promising oxidants and an alternative to Fenton reaction for water treatment. However, activation methods in hand restrict the practical application. Herein, we explore the possibility of Fe-N complexes being a catalyst for persulfate activation for the first time. The catalyst denoted as Fe-Im-SBA was synthesized from ferric chloride, imidazole, and SBA-15 at high temperature. The internal pore structure of Fe-Im-SBA was maintained well; Fe, N and C elements are evenly distributed on the catalyst. This catalyst presents an extraordinarily catalytic activity for Rh B removal by PMS activation with a removal rate of Rh B that reached up to 97.0% in the first 5 min. It also performed well in a wide pH range with complete removal of Rh B in pH ranged from 0.5 to 10, suggesting the stability of this catalyst in both acidic and alkaline conditions. It also showed high adaptability to degrade different kinds of pollutants, which could give an attractive advantage of Fe-Im-SBA for environmental implications. Through X-ray absorption spectroscopies analysis, it shows that the active sites of Fe-Im-SBA are composed of Fe-N4sites and Fe2–N2sites.1O2were proved to generate in the Fe-Im-SBA/PMS system and serve as the major ROS. Meanwhile, graphitic carbon can accelerate the transfer of electrons, which may also be the reason for its high catalytic performance.