不同热解活化条件下制备的污泥炭常温催化氧化NO

周易; 邓文义; 胡明涛; 许铈尧; 苏亚欣

doi:10.1016/S1872-5813(21)60160-3

不同热解活化条件下制备的污泥炭常温催化氧化NO

doi: 10.1016/S1872-5813(21)60160-3

东华大学环境科学与工程学院，上海 201620

基金项目: 上海自然科学基金（19ZR1400700），中央高校基本科研业务费专项资金（2232019D3-24）和上海市科委科研计划（19DZ1204900）资助

详细信息

作者简介:
周易：zhouyi201508@163.com

通讯作者:
Tel：021-67792555，E-mail：dengwy@dhu.edu.cn

中图分类号: X511
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出版历程
- 收稿日期: 2021-06-16
- 修回日期: 2021-08-24
- 网络出版日期: 2021-09-20
- 刊出日期: 2022-03-28

Low temperature catalytic oxidation of NO over sludge char under different pyrolysis activation conditions

School of Environmental Science and Engineering, Donghua University, Shanghai 201620, China

Funds: The project was supported by the Shanghai Natural Science Foundation (19ZR1400700), the Fundamental Research Funds for the Central Universities (2232019D3-24), and the Scientific Research Project from Science and Technology Commission of Shanghai Municipality (19DZ1204900)

摘要

摘要: 以市政污泥为原料制备污泥炭（SC），开展了SC常温催化氧化NO的实验研究。通过对不同热解温度（600 、700 和800 ℃）和不同干基污泥（DS）/KOH混合质量比下（4∶1、3∶1、2∶1和1∶1）的NO脱除特性研究，探究了污泥裂解活化工艺对NO常温催化氧化的影响规律和作用机理。结果表明，热解温度和KOH活化均对SC的催化活性有显著影响，当热解温度由600 ℃升至800 ℃，裂解样的NO转化率由12%升至36%；不同热解温度下，SC的催化活性均随KOH用量增加呈先增大后减小趋势；当热解温度为700 ℃、DS/KOH = 3∶1时，SC的催化活性最优，达到56%；对该样品进一步进行氢气还原处理后，其脱硝效率进一步提升，达到76.5%。研究发现，SC的催化活性与其比表面积有强相关性，其反应机理遵循Eley-Rideal（E-R）模型。
- NO /
- 催化氧化 /
- 污泥炭 /
- KOH活化 /
- 热解
Abstract: Catalytic oxidation of NO (CONO) at ambient temperature over sludge char (SC) prepared from sewage sludge was studied in this paper. The influencing mechanism of sludge pyrolysis/activation parameters on the CONO were investigated for the SC prepared with different pyrolysis temperatures (600, 700, and 800 ℃) and different mass ratios of dried sludge (DS) to KOH (DS/KOH = 4∶1, 3∶1, 2∶1, and 1∶1). The results indicated that both pyrolysis temperature and KOH activation had great influence on the catalytic performance of SC. With the increase of temperature from 600 to 800 ℃, the NO conversion increased from 12% to 36%. However, the catalytic activity of KOH-activated SC increased and then decreased with the increase of KOH content. The SC prepared under the pyrolysis temperature of 700 ℃ and the DS/KOH mass ratio of 3∶1 showed the best catalytic performance with NO conversion of 56%. The NO conversion further increased to 76.5% when the SC was reduced by H₂. It was also found that there was a strong correlation between the catalytic activity and the specific surface area of the SCs. The reaction might follow the Eley-Rideal (E-R) mechanism.
- NO /
- catalytic oxidation /
- sludge char /
- KOH activation /
- pyrolysis

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FIG. 1391. FIG. 1391.

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图 1 常温催化氧化NO反应系统

Figure 1 Reaction system of catalytic oxidation of NO at ambient temperature

1: Mass flow meter; 2: Gas mixer; 3: Switching valve; 4: Quartz tube; 5: Temperature controller; 6: Gas analyzer; 7: Thermocouple; 8: Bypass tube; 9: SC sample; 10: Heating belt

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图 2 不同成品SC的照片

Figure 2 Images of different SCs (a): SC-600 ℃ (1∶1); (b): SC-700 ℃ (2∶1); (c): SC-700 ℃ (1∶1)

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图 3 不同SC样品的XRD谱图

Figure 3 XRD profiles of SCs

(a): SC-600 ℃ (1∶1); (b): SC-700 ℃ (2∶1); (c): SC-700 ℃ (1∶1)

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图 4 SC表面形貌的SEM照片

Figure 4 SEM images of SCs

(a): SC-600 ℃; (b): SC-700 ℃; (c): SC-800 ℃; (d): SC-600 ℃ (2∶1); (e): SC-700 ℃ (3∶1); (f): SC-800 ℃ (4∶1)

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图 5 不同SC的碘值

Figure 5 Iodine value of different SCs

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图 6 不同SC的脱硝曲线

Figure 6 Denitration curves of different SCs

(a): SC without KOH addition; (b) DS/KOH = 4∶1; (c): DS/KOH = 3∶1; (d): DS/KOH = 2∶1; (e): DS/KOH = 1∶1; (f): SC-700(3∶1)-H₂ Reaction temperature of 30 ℃, total flow rate of 0.5 L/min, inlet NO = 450 μL/L, O₂ = 20%

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图 7 不同SC的稳态NO转化率

Figure 7 NO conversion of different SC at stable stage

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图 8 SC的NO转化率与其碘值的联系

Figure 8 Correlation between NO conversions and iodine values of SCs

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图 9 SCs脱硝前后的FT-IR谱图

Figure 9 FT-IR of SCs before and after catalytic oxidation of NO

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表 1 DS及不同工况样品的工业成分分析

Table 1 Proximate analysis of DS and SCs

Sample	Proximate analysis w/%
Sample	A	V	FC
DS	43.24	49.64	7.12
SC-600 ℃	67	22.69	10.31
SC-600 ℃（4∶1）	54.33	17.39	28.27
SC-600 ℃（3∶1）	53.12	20.93	25.95
SC-600 ℃（2∶1）	59.42	22.12	18.46
SC-600 ℃（1∶1）	64.26	24.96	10.78
SC-700 ℃	73.22	14.08	12.7
SC-700 ℃（4∶1）	54.23	18.16	27.61
SC-700 ℃（3∶1）	53.74	20.22	26.04
SC-700 ℃（2∶1）	56.76	22.77	20.47
SC-700 ℃（1∶1）	73.87	16.23	9.9
SC-800 ℃	75.09	10.89	14.02
SC-800 ℃（4∶1）	53.97	17.61	28.42
SC-800 ℃（3∶1）	55.83	18.94	25.23
SC-800 ℃（2∶1）	61.93	19.21	18.86
SC-800 ℃（1∶1）	69.82	19.23	10.95

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表 2 DS的灰分分析

Table 2 Ash components in DS

Content w/%
Fe₂O₃	SiO₂	Al₂O₃	SO₃	P₂O₅	TiO₂	CaO	K₂O
36.64 ± 0.24	28.31 ± 0.23	10.61 ± 0.15	9.58 ± 0.15	7.29 ± 0.13	2.03 ± 0.07	1.82 ± 0.07	1.21 ± 0.05

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