化工进展 ›› 2021, Vol. 40 ›› Issue (7): 4027-4035.DOI: 10.16085/j.issn.1000-6613.2020-1542

• 资源与环境化工 • 上一篇    下一篇

稻壳白炭黑负载Fe2O3的气相芬顿反应NO预氧化

闫文杰(), 熊源泉(), 杨思源, 何珊珊   

  1. 东南大学能源热转换及其过程测控教育部重点实验室,江苏 南京 210096
  • 收稿日期:2020-08-05 修回日期:2020-09-29 出版日期:2021-07-06 发布日期:2021-07-19
  • 通讯作者: 熊源泉
  • 作者简介:闫文杰(1994—),男,硕士研究生,研究方向为烟气脱硫脱硝。E-mail:18361226586@163.com
  • 基金资助:
    国家自然科学基金(51376047)

NO preoxidation by gas phase Fenton reaction with Fe2O3 over rice husk-based silica carrier

YAN Wenjie(), XIONG Yuanquan(), YANG Siyuan, HE Shanshan   

  1. Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Southeast University, Nanjing 210096, Jiangsu, China
  • Received:2020-08-05 Revised:2020-09-29 Online:2021-07-06 Published:2021-07-19
  • Contact: XIONG Yuanquan

摘要:

以稻壳为硅源,采用直接煅烧法制备白炭黑,以其为载体,采用共浸渍法制备Fe2O3/SiO2催化剂;并采用同样方法以商用二氧化硅为载体制备Fe2O3/C-SiO2催化剂,将二者用于催化H2O2预氧化NO的实验。探究不同工况(负载量、催化温度、H2O2汽化温度、H2O2流量和水汽浓度)对NO预氧化的影响,并对催化剂进行表征,分析其物理化学性质对催化性能的影响。结果表明,在负载量为50%、催化温度为140℃、H2O2汽化温度为120℃、H2O2流量为2.5mL/h时,达到最佳工况,NO氧化度能达到73%;在相同实验条件下Fe2O3/SiO2催化剂的预氧化效果要比Fe2O3/C-SiO2催化剂高20%左右。TPR结果表明载体可以降低活性组分的还原温度,减少活性组分的团聚;催化剂的晶相结构稳定,机械强度及热稳定性良好;ESR和XPS结果显示Fe2O3/SiO2催化剂的催化性能优于Fe2O3/C-SiO2催化剂,能够更好地催化分解H2O2产生·OH。

关键词: 稻壳, 二氧化硅, 铁基催化剂, 气相双氧水, 脱硝

Abstract:

With rice husk as silicon source, silica was firstly prepared by the direct calcination method, and then the Fe2O3/SiO2 catalyst was prepared by co-impregnation method with the silica as the carrier. As a comparison, the Fe2O3/C-SiO2 catalyst supported on commercial silica was prepared by the same method. Both catalysts were used in catalyzing H2O2 to pre-oxidize NO. The effects of different operating conditions (loading, catalysis temperature, vaporization temperature of H2O2, flow rate of H2O2 and vapor concentration) on the pre-oxidation of NO were systematically investigated. In addition, the physicochemical properties of the catalysts were characterized and attempts were made to correlate them with their catalytic performance. The experimental results indicated that a NO oxidation efficiency of 73% could be achieved when the loading was 50%, catalysis temperature was 140℃, vaporization temperature of H2O2 was 120℃, and the flow rate of H2O2 was 2.5mL/h. Under the same experiment conditions, the NO pre-oxidation efficiency of Fe2O3/SiO2 catalyst was about 20% higher than that of Fe2O3/C-SiO2 catalyst. TPR result showed that the carrier could lower the reduction temperature of active components and further reduce their agglomeration. The catalyst has a stable crystal structure, and good mechanical strength and thermal stability. ESR and XPS results indicated that the catalytic performance of Fe2O3/SiO2 catalyst was better than that of Fe2O3/C-SiO2 catalyst, which better catalyzed the decomposition of H2O2 to produce ·OH.

Key words: rice husk, silica, iron-based catalyst, gas phase H2O2, denitrification

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