臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究

严永桂; 毛中建; 罗津晶; 杜如鹏; 林家璇

臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究

1.
厦门大学环境与生态学院, 福建厦门 361105
2.
厦门佰瑞福环保科技有限公司, 福建厦门 361105

基金项目:

厦门市科技计划 3502z20173014

详细信息

本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).
中图分类号: X511
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出版历程
- 收稿日期: 2020-09-30
- 修回日期: 2020-10-29
- 刊出日期: 2020-12-10

Simultaneous removal of SO₂, NO_x and Hg⁰ by O₃ oxidation integrated with bio-charcoal adsorption

1.
College of the Environment & Ecology, Xiamen University, Xiamen 361105, China
2.
Xiamen Brave Environmental Protection Technology Co., Ltd, Xiamen 361105, China

Funds:

the Science and Technology Planning Project of Xiamen 3502z20173014

More Information

Corresponding author: LUO Jin-jing, Tel:18959288119, E-mail:luojj27@xmu.edu.cn

摘要

摘要: 以O₃为氧化剂，玉米生物炭和椰壳活性炭为吸附剂，开展同时脱硫脱硝除汞研究。研究考察了温度、O₃/NO和吸附时间对玉米/椰壳炭脱硫脱硝除汞效率的影响，并对玉米/椰壳炭进行表征分析。结果表明，NO和Hg⁰氧化率随O₃/NO升高而升高，SO₂氧化率则先升高后略微降低；温度升高抑制NO氧化但促进Hg⁰和SO₂氧化；在140 ℃下，当O₃/NO为1.4时，NO、Hg⁰和SO₂氧化率分别达99%、78.6%和3.5%，随O₃/NO从0.4升至1.4，玉米炭对NO_x脱除效率从4.6%提升至93%，椰壳炭从4.5%提升至79%。玉米/椰壳炭会还原部分NO₂造成出口NO浓度上升，但玉米炭的NO_x吸附性能较椰壳炭强，而椰壳炭对Hg⁰和SO₂的吸附性能较强。椰壳炭较玉米炭具有更强的物理吸附能力；玉米炭表面含氧官能团C-O和C=O的相对含量较椰壳炭高，而COOH和O=C-O相对含量较椰壳炭低。
- 脱硫脱硝除汞 /
- 臭氧氧化 /
- 生物炭 /
- 活性炭
Abstract: Simultaneous removal of SO₂, NO_x and Hg⁰ by using O₃ and corn bio-charcoal/coconut shell activated carbon was compared in a fixed bed. The effects of temperature, adsorption time and ratio of O₃/NO on the removal efficiency of NO, Hg⁰ and SO₂ by corn/coconut shell charcoal were studied, and the corn/coconut shell charcoal was characterized and analyzed. The results indicated that the oxidation rate of NO and Hg⁰ increases with the increase of O₃/NO ratio, while the oxidation rate of SO₂ first increases and then decreases slightly. The increase of temperature inhibits the oxidation of NO but promotes the oxidation of Hg⁰ and SO₂. At 140 ℃ and O₃/NO ratio of 1.4, the oxidation rate of NO, Hg⁰ and SO₂ is 99%, 78.6% and 3.5%, respectively. As O₃/NO ratio increases from 0.4 to 1.4, the removal efficiency of corn charcoal for NO_x increases from 4.6% to 93%, and coconut shell charcoal increases from 4.5% to 79%. Corn/coconut shell charcoal can reduce part of NO₂ and increase NO concentration at the outlet. NO_x adsorption performance on corn charcoal is relatively better, while those of Hg⁰ and SO₂ on coconut charcoal are relatively stronger. Coconut shell charcoal has stronger physical adsorption capacity than corn charcoal. The relative content of oxygen-containing functional groups C-O and C=O on the surface of corn charcoal is higher than that of coconut shell charcoal, while its relative content of COOH and O=C-O is lower.
- simultaneous removal of SO₂, NO_x and Hg⁰ /
- ozone oxidation /
- bio-charcoal /
- activated carbon
注释:

1) 本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).

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图 1 实验装置示意图

Figure 1 Adsorption experimental apparatus

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图 2 O₃/NO物质的量比对NO、SO₂和Hg⁰氧化率的影响

Figure 2 Influences of O₃/NO molar ratio on the oxidation efficiency of NO, SO₂ and Hg⁰

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图 3 O₃/NO物质的量比对NO_x、SO₂和Hg⁰去除效率的影响

Figure 3 Influence of O₃/NO molar ratio on the removal efficiency of NO_x, SO₂ and Hg⁰

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图 4 不同O₃/NO物质的量比下炭吸附后出口烟烟气中的NO、NO₂质量浓度

Figure 4 Concentrations of NO and NO₂ in flue gas after carbon adsorption at different O₃/NO molar ratios

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图 5 玉米炭对NO_x、SO₂和Hg⁰的吸附

Figure 5 Adsorption curve of NO_x, SO₂ and Hg⁰ on corn charcoal

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图 6 椰壳炭对NO_x、SO₂和Hg⁰的吸附

Figure 6 Adsorption curve of NO_x, SO₂ and Hg⁰ on coconut shell charcoal

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图 7 椰壳炭的SEM照片

Figure 7 SEM image of coconut shell charcoal

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图 8 玉米炭的SEM照片

Figure 8 SEM image of corn charcoal

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图 9 椰壳炭(a)、玉米炭(b)的XPS全谱谱图

Figure 9 XPS full spectrum

(a): the coconut shell charcoal; (b): the corn charcol

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表 1 样品的元素分析

Table 1 Elemental composition of the sample

Sample	Uitimate analysis w/%					O/C	N/C	(O+N)/C
Sample	C	N	H	S	O	O/C	N/C	(O+N)/C
CS	79.984	0.249	1.258	0.667	17.842	0.223	0.003	0.226
CR	63.254	1.582	1.698	0.268	33.198	0.525	0.025	0.549

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表 2 C 1s、O 1s和N 1s含量及比例

Table 2 Content and proportion of C 1s, O 1s and N 1s obtained from XPS

Sample	C 1s	O 1s	N 1s	O/C	N/C
CS	91.38	7.44	0.58	0.081	0.006
CR	81.71	14.53	1.61	0.178	0.019

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表 3 样品的C 1s分峰

Table 3 C 1s peak fitting results of samples

Sample	Peak label	Peak position /eV	Functional group	Content
CS	C1	284.8	C-C	0.554
	C2	286.1	C-O	0.228
	C3	288.5	C=O	0.067
	C4	290.6	COOH	0.151
CR	C1	284.8	C-C	0.599
	C2	286.1	C-O	0.267
	C3	288.5	C=O	0.115
	C4	290.6	COOH	0.100

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表 4 样品的O 1s分峰

Table 4 O 1s peak fitting results of samples

Sample	Peak label	Peak position /eV	Functional group	Content
CS	O1	531.5	C=O	0.171
	O2	532.5	C-O	0.532
	O3	533.3	O=C-O	0.098
	O4	534.2	COOH	0.199
CR	O1	531.5	C=O	0.284
	O2	532.5	C-O	0.621
	O3	533.3	O=C-O	0.039
	O4	534.2	COOH	0.066

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