富氧条件下生物质基活性炭负载钾催化剂高选择性还原氮氧化物

束韫; 张凡; 王凡; 王红梅; 王洪昌

富氧条件下生物质基活性炭负载钾催化剂高选择性还原氮氧化物

中国环境科学研究院大气污染控制技术研究中心, 北京 100012

基金项目:

国家自然科学基金 21507119

青海省科技支撑计划 2012-J-144

详细信息

通讯作者:
束韫, Tel:010-84934516, E-mail:shuyun@craes.org.cn

中图分类号: X51
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- 被引次数: 0
出版历程
- 收稿日期: 2017-01-24
- 修回日期: 2017-03-31
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-06-10

Biomass-derived activated carbon supported potassium catalyst for reduction of NO_x in excess oxygen with higher selectivity

Research Center of Air Pollution Control Technology, Chinese Research Academy of Environmental Sciences, Beijing 100012, China

Funds:

the National Natural Science Foundation of China 21507119

the Key Technology Research and Development Program of Qinghai Province 2012-J-144

摘要

摘要: 研究了富氧环境中生物质基活性炭负载钾催化剂选择性还原氮氧化物的性能。结果表明，与煤基（褐煤）活性炭负载钾催化剂相比，生物质基（木屑）活性炭负载钾催化剂表现出高选择性还原NO能力，在2 h恒温稳态实验过程中能够保持80%的NO还原效率，而C-O₂反应活性仅为18%。X射线衍射、比表面积、X射线光电子能谱以及程序升温脱附实验表征结果显示，生物质基活性炭负载钾催化剂优异的选择性还原NO性能应归因于炭表面钾物种的高度分散性，这与催化剂的高比表面积以及大量的表面氧基团有关。另外，生物质基炭材料还原NO反应产物中具有较高的CO₂选择性。
- NO还原 /
- 生物质炭 /
- 选择性 /
- 催化剂
Abstract: The selective reduction of NO in an oxygen-rich environment with biomass-derived activated carbon supported potassium catalyst was investigated. The. results show that in comparison with coal (lignite) based activated carbon supported potassium catalyst, biomass (sawdust) based activated carbon supported potassium catalyst exhibits a high selectivity for the reduction of NO_x to N₂, keeping a high and stable activity with NO reduction of about 80% during 2 h-isothermal experiment as well as a relatively low activity with the oxygen-carbon reaction of 18%. XRD, BET, XPS and TPD results indicate that the excellent catalytic performance of the biomass-derived activated carbon supported potassium catalyst is associated with the highly dispersion of active potassium species, which might result from the high surface area and the large amount of surface oxygen groups. Furthermore, the selective emission of CO₂ with regard to CO is an additional benefit of using biomass-derived activated carbon as the support for NO reduction.
- NO reduction /
- biomass carbon /
- selective /
- catalyst

HTML全文

图 1 实验装置示意图

Figure 1 Schematic diagram of the experimental setup

1: N₂; 2: NO; 3: O₂; 4: mass flow controller;5: electric furnace; 6: fixed bed reactor; 7: catalyst; 8: temperature controller; 9: gas analyzer

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图 2 400℃时不同样品的恒温稳态脱硝活性

Figure 2 Isothermal NO reduction activity at 400℃ with different samples

■: MAC; ●: DAC; ▲: YAC; ◆: HACreaction conditions: [NO] = 0.1%, [O₂] = 5%, t=400℃, N₂ balance and GHSV = 20000h^-1

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图 3 两种不同催化剂的CO₂-TPD和CO-TPD谱图

Figure 3 CO₂-TPD and CO-TPD profiles on two different catalysts

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图 4 程序升温暂态反应MAC、MAC-K和HAC-K

Figure 4 Temperature programmed reaction with MAC(a), MAC-K(b) and HAC-K(c)

reaction conditions: [NO] = 0.1%, [O₂] = 5%, N₂ balance and GHSV = 20000h^-1■: NO; □: O₂; ●: CO₂; ○: CO

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图 5 350℃时催化剂MAC-K和HAC-K的恒温稳态脱硝活性NO和O₂转化率，CO₂和CO排放

中文注解

Figure 5 Isothermal NO reduction activity at 350℃ with MAC-K and HAC, NO and O₂ conversion (a), CO₂ and CO emission (b)

a: MAC-K-NO; b: HAC-K-NO; c: MAC-K-O₂; d: HAC-K-O₂; e: MAC-K-CO₂; f: HAC-K-CO₂; g: MAC-K-CO; h: HAC-K-COreaction conditions: [NO] = 0.1%, [O₂] = 5%, N₂ balance and GHSV = 20000h^-1

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图 6 不同催化剂的XRD谱图

Figure 6 X-ray diffraction patterns for different catalyst

a: MAC-K; b: HAC-K

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表 1 实验原料的工业分析及元素分析

Table 1 Proximate and ultimate analyses of raw materials for the experiment

表 2 催化剂和活性炭的特性表征

Table 2 Characteristics of catalysts and carbon supporting

表 3 300、325、350℃时测试样品在恒温稳态反应实验中的反应数据与选择性

Table 3 Reaction data and selectivity for tested samples in isothermal reactions at 300, 325 and 350℃

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