多级孔Fe/ZSM-5分子筛催化降解有机胺废水条件优化
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摘要
用CH3COONa溶液处理合成多级孔ZSM-5分子筛,对处理前后的样品采用XRD、XRF、BET、SEM进行表征,并分别负载Fe,进行高浓度有机胺废水的催化氧化降解。结果表明,采用CH3COONa溶液处理ZSM-5分子筛,具有碱改性的作用,且显著提高了催化氧化降解有机胺废水性能。在此基础上,运用正交试验对催化氧化降解有机胺废水条件进行优化,确定出试验范围内的最佳评价条件:反应时间为90 min,反应温度为95℃,催化剂用量为30g/L,溶液初始pH为4,氧化剂H2O2用量为45 m L/L,经过3次验证试验证明,该反应条件具有高度的可靠性和重现性,在此条件下,COD去除率高达98.73%。
The microporous and mesoporous ZSM-5 zeolite was synthesized with CH3 COONa solution. The samples before and after treatment were characterized by XRD,XRF,BET and SEM. The ZSM-5 zeolites before and after the treatment were respectively loaded with Fe to perform the oxidative degradation of the organic amine wastewater with high concentration. The results showed that the treatment of ZSM-5 zeolite with CH3 COONa solution had the effect of alkali modification and the catalytic degradation of organic amine wastewater was improved significantly. On this basis,orthogonal test was used to optimize the conditions for catalytic degradation of organic amine wastewater and the best evaluation conditions within the experimental range were determined:reaction time was 90 min,reaction temperature was 95 ℃,catalyst dosage was 30 g/L,initial solution the pH was 4 and the amount of H2 O2 was 45 m L/L. After three verification experiments,the catalytic effect had high reliability and reproducibility under the reaction conditions. Under this conditions,the removal rate of COD was as high as 98.73%.
The microporous and mesoporous ZSM-5 zeolite was synthesized with CH3 COONa solution. The samples before and after treatment were characterized by XRD,XRF,BET and SEM. The ZSM-5 zeolites before and after the treatment were respectively loaded with Fe to perform the oxidative degradation of the organic amine wastewater with high concentration. The results showed that the treatment of ZSM-5 zeolite with CH3 COONa solution had the effect of alkali modification and the catalytic degradation of organic amine wastewater was improved significantly. On this basis,orthogonal test was used to optimize the conditions for catalytic degradation of organic amine wastewater and the best evaluation conditions within the experimental range were determined:reaction time was 90 min,reaction temperature was 95 ℃,catalyst dosage was 30 g/L,initial solution the pH was 4 and the amount of H2 O2 was 45 m L/L. After three verification experiments,the catalytic effect had high reliability and reproducibility under the reaction conditions. Under this conditions,the removal rate of COD was as high as 98.73%.
引文
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[10]赵岑,刘冬梅,魏民,等.多级孔ZSM-5分子筛的制备及催化噻吩烷基化性能研究[J].燃料化学学报,2013,41(10):1256-1261.
[2] Busca G,Berardinelli S,Resini G,et al. Technologies for the removal of phenol from fluid streams:a short review of recent developments[J]. J. Hazard. Mater.,2008,160(2/3):265-288.
[3] El-Cohary F A,Badawy M I,El-Khateeb M A,et al. Integrated treatment of olive mill waste(OMW)by the combination of Fenton’s reaction and anaerobic treatment[J]. J. Hazard. Meter.,2009,162(2/3):1536-1541.
[4]马健,刘冬梅,魏民,等. Na2CO3溶液处理对Ni-Mo/HZSM-5分子筛硫醚化催化性能的影响[J].燃料化学学报,2014,42(9):1128-1134.
[5]韩伟,潘相米,谭亚南,等. Na2CO3处理制备复合孔ZSM-5分子筛及其丙烷脱氢制丙烯的催化性能[J].化工进展,2016,35(2):174-178.
[6] Groen J C,Moulijn J A. Decoupling mesoporosity formation and acidity modification in ZSM-5 zeolites by sequential desilication-dealuminatio[J]. Microporous and Mesoporous Materials,2005,87(2):153-161.
[7]常江伟,付延俊,张洪建,等.碱处理浓度对预脱铝ZSM-5成孔过程及其MTG反应性能的影响[J].无机化学学报,2015,3(11):2119-2127.
[8]王莹莹. Meso-ZSM-5的制备、表征及催化应用[D].北京:中国石油大学,2015.
[9] Groen J C,Peffer L A,Moulijn J A,et al. Mechanism of hierarchical porosity development in MFI zeolites by desilication:the role of aluminium as a pore-directing agent[J]. Chem. Eur. J.,2005,11(17):4983-4994.
[10]赵岑,刘冬梅,魏民,等.多级孔ZSM-5分子筛的制备及催化噻吩烷基化性能研究[J].燃料化学学报,2013,41(10):1256-1261.