消化污泥负载稳定高效非均相光Fenton催化材料的制备及性能优化

doi:10.1016/S1872-2067(15)61066-X

催化学报 ›› 2016, Vol. 37 ›› Issue (5): 735-742.DOI: 10.1016/S1872-2067(15)61066-X

消化污泥负载稳定高效非均相光Fenton催化材料的制备及性能优化

院士杰, 廖年华, 董滨, 戴晓虎

同济大学环境科学与工程学院城市污染控制国家工程研究中心, 上海 200092

收稿日期:2016-01-13 修回日期:2016-02-04 出版日期:2016-04-26 发布日期:2016-04-26
通讯作者: Xiaohu Dai
基金资助:
国家科技支撑计划(2014BAL02B02);国家自然科学基金(51578397).

Optimization of a digested sludge-derived mesoporous material as an efficient and stable heterogeneous catalyst for the photo-Fenton reaction

Shijie Yuan, Nianhua Liao, Bin Dong, Xiaohu Dai

National Engineering Research Center for Urban Pollution Control, School of Environmental Science and Engineering, Tongji University, Shanghai 200092, China

Received:2016-01-13 Revised:2016-02-04 Online:2016-04-26 Published:2016-04-26
Contact: Xiaohu Dai
Supported by:
This work was supported by the National Key Technology Research & Development Program of China (2014BAL02B02) and the National Natural Science Foundation of China (51578397).

摘要/Abstract

摘要：

近年来, 随着我国经济飞速发展和城市人口快速增长, 城市污水排放量不断增加, 市政污泥产生量也随之增大. 市政污泥含有大量有毒有害物质, 如寄生虫卵、致病菌、有机污染物和重金属等, 若不进行妥善处理处置将会对环境造成严重的二次污染. 传统的污泥处理处置方法如卫生填埋、露天堆放和土地利用等已经无法满足日趋严格的污泥处理处置标准, 研发新的污泥资源化利用方法具有重要的环境意义和经济价值.
本课题组前期以铁盐为前驱体通过简单步骤制备了以市政污泥为载体, 污泥中的重金属为可见光光敏剂, 铁氧化物为活性中心的稳定高效非均相光 Fenton 催化剂. 此催化剂在制备过程中虽然已经充分利用了市政污泥中的所有成分, 但是其中部分可生化的有机大分子物质在制备过程中被直接燃烧或碳化, 从而造成能源流失和浪费. 为了更加充分利用市政污泥中的有机物, 在制备稳定高效催化剂的同时尽可能多地回收能源和资源, 本文在前期研究基础上进行了如下改进和优化: (1) 采用市政污泥厌氧消化后的消化污泥为载体, 通过厌氧消化手段将其中可生化的有机物转化为沼气, 相对于直接用市政污泥制备催化剂, 减少了能量流失, 更具有经济效益和环境意义; (2) 通过改变焙烧温度 (250, 350, 450, 550, 650 和 750 ℃)、铁盐类型 ((NH₄)₂Fe(SO₄)₂, FeSO₄, FeCl₃和 Fe(NO₃)₃) 和铁盐添加量 (0, 0.5, 1.0, 1.5, 2.0 和 3.0 mol/L) 对所制得催化材料的性能进行优化.
利用红外光谱、X 射线衍射、扫描电子显微镜和电感耦合等离子体质谱法等手段对所制备光 Fenton 反应催化剂结构进行了表征. 结果表明, 以消化污泥为原料制备的催化材料具有多孔和较高的比表面积, 保证了在反应过程中催化剂与 H₂O₂和被降解物质充分接触. 样品中 Fe 含量较高, 主要是以α -Fe₂O₃或无定形铁化合物形式存在, 并通过 Si-O-Fe 键结合在污泥载体上, 从而保证了催化剂较多的活性位点和较高的稳定性, 因此所制材料可用作稳定高效的光 Fenton 反应催化剂.
以偶氮染料罗丹明 B 为模式污染物评价了所制催化剂对污染物的降解效果. 结果表明, 在焙烧温度和铁盐添加量一定时, 以亚铁盐 (即 (NH₄)₂Fe(SO₄)₂和 FeSO₄) 为前驱体所制催化剂性能明显优于以铁盐 (FeCl₃和 Fe(NO₃)₃) 为前驱体的催化剂; 以 (NH₄)₂Fe(SO₄)₂为前驱体且其添加量为 1 mol/L, 焙烧温度为 350 ℃时所制 FAS-1-350 催化剂具有较高的降解速率 (0.308±0.016 min^-1) 和较低的 Fe2+ 溶出率 (0.94±0.24 mg/L). 在紫外光照射下 FAS-1-350 重复使用 6 次, 其催化性能没有明显降低, 证实该样品结构稳定, 可重复利用, 具有良好的应用前景.

关键词: 消化污泥, 铁基化合物, 介孔材料, 非均相光Fenton反应

Abstract:

The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane-rich biogas. However, digested sludge, the residue produced in that process, still contains high levels of heavy metals and other harmful substances that might make traditional disposal difficult. We have devised a facile method of converting digested sludge into a mesoporous material that acts as an effective and stable heterogeneous catalyst for the photo-Fenton reaction. A comparison of the removal of rhodamine B under different conditions showed that FAS-1-350, which was synthesized by mixing the digested sludge with a 1 mol/L (NH₄)₂Fe(SO₄)₂ solution followed by calcination at 350 ℃, exhibited the best catalytic activity owing to its faster reaction rate and lower degree of Fe leaching. The results indicate that Fe²⁺-loaded catalysts have significant potential to act as stable and efficient heterogeneous promoters for the photo-Fenton reaction, with better performance than Fe³⁺-loaded catalysts because the Fe(II)/Fe(III) compounds formed in the calcination process are necessary to sustain the Fenton reaction. This protocol provides an alternative, environmentally friendly method of reusing digested sludge and demonstrates an easily synthesized mesoporous material that effectively degrades azo dyes.

Key words: Digested sludge, Iron-based compound, Mesoporous material, Heterogeneous photo-Fenton reaction

院士杰, 廖年华, 董滨, 戴晓虎. 消化污泥负载稳定高效非均相光Fenton催化材料的制备及性能优化[J]. 催化学报, 2016, 37(5): 735-742.

Shijie Yuan, Nianhua Liao, Bin Dong, Xiaohu Dai. Optimization of a digested sludge-derived mesoporous material as an efficient and stable heterogeneous catalyst for the photo-Fenton reaction[J]. Chinese Journal of Catalysis, 2016, 37(5): 735-742.

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消化污泥负载稳定高效非均相光Fenton催化材料的制备及性能优化

Optimization of a digested sludge-derived mesoporous material as an efficient and stable heterogeneous catalyst for the photo-Fenton reaction

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