Peroxymonosulfate activated with waste battery-based Mn-Fe oxides for pollutant removal: Electron transfer mechanism, selective oxidation and LFER analysis
Peroxymonosulfate activated with waste battery-based Mn-Fe oxides for pollutant removal: Electron transfer mechanism, selective oxidation and LFER analysis
复制标题
用废电池锰铁氧化物活化过一硫酸盐去除污染物：电子转移机制、选择性氧化和 LFER 分析
DOI：
10.1016/j.cej.2020.124864
复制
发表时间：
2020-08
影响因子：
15.1
通讯作者：
Zhang Hui
中科院分区：
文献类型：
--
作者：
Tan Weihua;Ren Wei;Wang Chanjuan;Fan Yuanrou;Deng Bin;Lin Heng;Zhang Hui
Mn2O3-Fe2O3 催化剂由废碱性电池制成，通过活化过一硫酸盐 (PMS) 有效消除对乙酰氨基酚 (APAP)。研究了不同初始pH下APAP的去除、降解途径和催化剂的稳定性。三键Mn(III)被认为是主要活性位点，三键Fe(III)可以通过金属间相互作用提高耐腐蚀性。化学猝灭实验、电子顺磁共振 (EPR) 光谱、溶剂交换、开路电位 (OCP) 和计时电流分析测试表明，APAP 通过高反应性表面吸附 PMS 的电子转移而被氧化。傅里叶变换红外(FTIR)、原位拉曼光谱、X射线光电子能谱(XPS)谱和离子强度实验进一步揭示了催化剂与PMS之间的相互作用。 Mn2O3-Fe2O3/PMS体系对不同的污染物表现出选择性氧化作用，并采用线性自由能关系（LFER）研究污染物的结构和性质对反应动力学的影响。峰值电位（Eop）> 0.91 V的污染物，Mn2O3-Fe2O3/PMS系统中的稳态OCP，具有抗氧化性；而Eop<0.91V的污染物容易被氧化，表观一级速率常数（k1）与Eop之间有很好的相关性。该研究不仅对废碱性电池中环保型锰铁氧化物活化PMS进行了深入研究，而且为非自由基机理、选择性氧化和LFER研究提供了一些新的见解。
Mn2O3-Fe2O3catalyst was fabricated from spent alkaline batteries and used for effective elimination of acetaminophen (APAP) by activating peroxymonosulfate (PMS). APAP removal at various initial pH, its degradation pathway and the stability of catalyst were investigated. The triple bondMn(III) was inferred to be the primary active site and triple bondFe(III) could improve the corrosion resistance through intermetallic interactions. Chemical quenching experiments, electron paramagnetic resonance (EPR) spectroscopy, solvent exchange, open circuit potential (OCP) and chronoamperometry tests imply that APAP is oxidized by electron transfer through highly reactive surface-adsorbed PMS. Fourier transform infrared (FTIR),in situRaman spectroscopy, X-ray photoelectron spectroscopy (XPS) spectra and ionic strength experiments further revealed the interaction between the catalyst and PMS. The Mn2O3-Fe2O3/PMS system exhibits selective oxidation for different contaminants, and linear free energy relationship (LFER) was employed to investigate the effect of structure and properties of pollutant on the reaction kinetics. Pollutant with peak potential (Eop) > 0.91 V, the steady-state OCP in the Mn2O3-Fe2O3/PMS system, is resistant to oxidation; while pollutant withEop< 0.91 V is prone to be oxidized and there is a good correlation between apparent first-order rate constant (k1) andEop. The research not only puts in-depth study into PMS activation through environment-friendly Mn-Fe oxides from spent alkaline batteries, but also provides some new insights for nonradical mechanism, selective oxidation and LFER study.
登录
查看更多内容
影响因子：
2.8
作者：
E. Zahonyi-Budo;L. Simándi
通讯作者：
E. Zahonyi-Budo;L. Simándi
通过嵌入镁/铝层状双氢氧化物来新型活化过硫酸盐：增强非自由基氧化
影响因子：
15.1
作者：
Huang Xin;Su Man;Zhou Jizhi;Shu Weikang;Huang Zhifeng;Gao Naiyun;Qian Guangren
通讯作者：
Qian Guangren
影响因子：
4.6
作者：
J. Ribeiro;T. Moreira;I. L. Santana;Sandra Ferreira;M. Lelis;M. Freitas
通讯作者：
J. Ribeiro;T. Moreira;I. L. Santana;Sandra Ferreira;M. Lelis;M. Freitas
影响因子：
8.8
作者：
E. Saputra;Huayang Zhang;Qiaoran Liu;Hongqi Sun;Shaobin Wang
通讯作者：
E. Saputra;Huayang Zhang;Qiaoran Liu;Hongqi Sun;Shaobin Wang
影响因子：
11.4
作者：
Tao Zhang;Yin Chen;Yuru Wang;Julien Le Roux;Yang Yang-Yang;J. Croué
通讯作者：
Tao Zhang;Yin Chen;Yuru Wang;Julien Le Roux;Yang Yang-Yang;J. Croué