F127辅助制备介孔Fe/TiO<sub>2</sub>催化剂用于中温NH<sub>3</sub>选择性催化还原反应

引用本文: 李昱琳, 韩小金, 侯亚芹, 郭耀萍, 刘勇进, 向宁, 崔燕, 黄张根. F127辅助制备介孔Fe/TiO₂催化剂用于中温NH₃选择性催化还原反应[J]. 催化学报, 2017, 38(11): 1831-1841. doi: 10.1016/S1872-2067(17)62897-3 shu

Citation: Yulin Li, Xiaojin Han, Yaqin Hou, Yaoping Guo, Yongjin Liu, Ning Xiang, Yan Cui, Zhanggen Huang. In situ preparation of mesoporous Fe/TiO₂ catalyst using Pluronic F127-assisted sol-gel process for mid-temperature NH₃ selective catalytic reduction[J]. Chinese Journal of Catalysis, 2017, 38(11): 1831-1841. doi: 10.1016/S1872-2067(17)62897-3 shu

F127辅助制备介孔Fe/TiO₂催化剂用于中温NH₃选择性催化还原反应

a 中国科学院山西煤炭化学研究所煤炭转化国家重点实验室, 山西太原 030001;
b 中国科学院大学, 北京 100049
基金项目:
中国科学院战略性先导科技专项（XDA07030300）.

摘要: NO_x是大气污染物的重要组成部分，能够造成酸雨、光化学烟雾和臭氧层破坏等一系列环境问题，严重危害人类健康.选择性催化还原（SCR）是控制NO_x排放的主要技术，当前工业上普遍采用的是钒钛催化剂，然而该催化剂活性温度窗口较窄（300-400 ℃），N₂选择性较低，而且钒物种本身有毒.因此开发新型SCR催化剂成为研究热点.
Fe/TiO₂催化剂具有稳定的化学性质，环境污染少且价格低廉，近年来受到广泛关注.为了提高Fe/TiO₂催化活性，人们采用了各种不同的制备方法.本文以F127作为结构导向剂，结合溶胶-凝胶法原位合成了具有介孔结构、工作温度在150-300 ℃的Fe/TiO₂脱硝催化剂，并与普通浸渍法和共沉淀法制备的催化剂进行了对比.利用N₂吸附脱附、紫外-可见光谱、X射线电子能谱、NH₃程序升温脱附和原位红外光谱等技术研究了制备方法对Fe/TiO₂催化剂物理结构及脱硝性能的影响.结果表明，相较于浸渍法和共沉淀法，模板法制备的催化剂具有较高的脱硝效率和抗H₂O和SO₂性能.作为结构导向剂，F127能够诱导催化剂形成均匀的介孔结构，有利于提高催化剂比表面积，促进反应物分子的扩散和转移，从而提高催化剂脱硝效率.
进一步研究发现，模板法能够明显促进活性组分Fe物种的分散和NH₃吸附，载体与活性组分具有较强的相互作用，因而有利于催化剂产生较多的活性位.结合XPS结果，较多的活性位点有利于表面吸附氧（O_α）在催化剂表面的吸附.O_α有利于NO到NO₂的转化，从而促进快速SCR反应：NO+NO₂+2NH₃→2N₂+3H₂O.通过原位红外机理分析证明，吸附在模板法制备的催化剂表面的NO物种具有较强的稳定性，当温度超过200 ℃时，仍然保持一定的吸附强度；吸附NH₃红外结果表明，Lewis酸性位比Brønsted酸性位具有更强的稳定性，当温度超过150 ℃仍然具有较强的Lewis酸吸附.催化剂表面稳定的NO物种和Lewis酸位上强的NH₃吸附是催化剂催化活性增加的重要原因.

关键词:

English

In situ preparation of mesoporous Fe/TiO₂ catalyst using Pluronic F127-assisted sol-gel process for mid-temperature NH₃ selective catalytic reduction

a State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China;
b University of Chinese Academy of Sciences, Beijing 100049, China
Received Date: 12 June 2017
Revised Date: 29 July 2017
Fund Project:
This work was supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA07030300).

Abstract: An Fe/TiO₂ catalyst with uniform mesopores was synthesized using Pluronic F127 as a struc-ture-directing agent. This catalyst was used for selective catalytic reduction of NO with NH₃. The catalytic activity and resistance to H₂O and SO₂ of Fe/TiO₂ prepared by a template method were better than those of catalysts synthesized using impregnation and coprecipitation. The samples were characterized using N₂-physisorption, transmission electron microscopy, ultraviolet-visible spectroscopy, X-ray photoelectron spectroscopy, and in situ diffuse reflectance infrared Fouri-er-transform spectroscopy. The results showed that Pluronic F127 acted as a structural and chemi-cal promoter; it not only promoted the formation of a uniform mesoporous structure, leading to a higher surface area, but also improved dispersion of the active phase. In addition, the larger number of Lewis acidic sites, indicated by the presence of coordinated NH₃ species (1188 cm^-1) and the N-H stretching modes of coordinated NH₃ (3242 and 3388 cm^-1), were beneficial to mid-temperature selective catalytic reduction reactions.

Key words:

Fe/TiO₂
/ Mesopore structure
/ Interaction
/ Mid-temperature NH₃ selective catalytic reduction

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F127辅助制备介孔Fe/TiO₂催化剂用于中温NH₃选择性催化还原反应

English

In situ preparation of mesoporous Fe/TiO₂ catalyst using Pluronic F127-assisted sol-gel process for mid-temperature NH₃ selective catalytic reduction

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中国化学会秘书处

F127辅助制备介孔Fe/TiO2催化剂用于中温NH3选择性催化还原反应

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In situ preparation of mesoporous Fe/TiO2 catalyst using Pluronic F127-assisted sol-gel process for mid-temperature NH3 selective catalytic reduction

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通讯作者: 陈斌, bchen63@163.com

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F127辅助制备介孔Fe/TiO₂催化剂用于中温NH₃选择性催化还原反应

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