Liu Yucan, Zhang Guangming, Fang Shunyan, Chong Shan, Zhu Jia
School of Environment & Natural Resource, Renmin University of China, Beijing, 100872, PR China.
School of Environment & Natural Resource, Renmin University of China, Beijing, 100872, PR China.
J Environ Manage. 2016 Nov 1;182:367-373. doi: 10.1016/j.jenvman.2016.07.084. Epub 2016 Aug 4.
A Ni-Fe oxalate complex catalyst was synthesized and characterized by means of Brunauer-Emmet-Teller (BET) method, scanning electron microscope (SEM) and X-ray photo-electron spectroscopy (XPS). The catalyst showed good catalytic activity for aniline degradation by heterogeneous Fenton's reaction, in which the synergetic index was 9.3. The effects of reaction temperature, catalyst dosage, hydrogen peroxide concentration and initial pH were investigated. Under the optimum conditions (T = 293 K, catalyst dosage = 0.2 g/L, H2O2 concentration = 4 mmol/L and initial pH = 5.4), 100% aniline could be removed within 35 min, and approximately 88% deamination efficiency was achieved in 60 min. The aniline degradation process followed the pseudo-first-order kinetic (k = 0.177 min(-1)) with activation energy (Ea) of 49.4 kJ mol(-1). Aniline could be removed in a broad initial pH (3-8) due to the excellent pH-tolerance property of the catalyst. The detected ammonium ion indicated that deamination occurred during aniline degradation. It was proposed that deamination synchronized with aniline removal, and aniline was attacked by free radicals to generate benzoquinonimine and phenol. This system is promising for the removal of aniline from water.
合成了一种草酸镍铁复合催化剂，并通过布鲁诺尔-埃米特-特勒（BET）法、扫描电子显微镜（SEM）和X射线光电子能谱（XPS）对其进行了表征。该催化剂在非均相芬顿反应中对苯胺降解表现出良好的催化活性，其中协同指数为9.3。研究了反应温度、催化剂用量、过氧化氢浓度和初始pH的影响。在最佳条件下（T = 293 K，催化剂用量 = 0.2 g/L，H2O2浓度 = 4 mmol/L，初始pH = 5.4），35分钟内可去除100%的苯胺，60分钟内脱氨效率达到约88%。苯胺降解过程遵循准一级动力学（k = 0.177 min(-1)），活化能（Ea）为49.4 kJ mol(-1)。由于催化剂具有优异的耐pH性能，在较宽的初始pH范围（3 - 至8）内均可去除苯胺。检测到的铵离子表明苯胺降解过程中发生了脱氨反应。提出脱氨与苯胺去除同步进行，苯胺受到自由基攻击生成苯醌亚胺和苯酚。该体系在从水中去除苯胺方面具有广阔前景。
