Advances in atmospheric gas-phase reactions initiated by amine absorbent escape

doi:10.16085/j.issn.1000-6613.2023-1765

Abstract

Abstract:

Carbon capture chemical absorption (CCA) is currently the most promising technology for reducing CO₂ emissions from power plants and other fossil fuel-using industries, but fugitive emissions of amine absorbents from CCA systems can trigger a range of atmospheric chemical reactions. During the operation of CCS, the amine absorbent is emitted into the atmosphere in the form of liquid droplets, gaseous and aerosol particles, and thus triggering atmospheric gas-phase reactions. The reaction between amine absorbent and OH radical mainly involves —CH₂ group and H-extraction reaction between C—H bonds. A small amount occurs between N—H bonds, and a very small portion occurs between —OH groups, generating imines, aldehydes, etc. The reaction with Cl radical involves —CH₂ group, —NH₂ group and —OH group, generating nitrogen oxides, HCl, etc. The reaction with NO _x includes the extraction of amino or alkyl groups. Hydrogen reaction, and the addition reaction with unsaturated compounds to generate nitric acid, nitramine, nitrosamines, etc. The reaction between amines and ozone mainly produces amides, isocyanates, nitroso compounds and so on. These compounds are potentially harmful to both the atmospheric environment and human health, and may cause serious impacts on air quality and ecosystems, and even health problems such as cancer. There are domestic and international regulations on carbon capture emission limits and few total amine emission limits. Although some progress has been made in the control of amine emissions, the problems of low removal efficiency, limited applicability, process complexity and high energy consumption of small particle aerosols need to be solved.

Key words: carbon capture, chemical absorption, amine absorbents, atmospheric reactions, photochemistry

摘要：

碳捕集化学吸收技术是目前最具潜力的减少发电厂及其他使用化石燃料行业CO₂排放的技术，但碳捕集化学吸收系统带来的胺吸收剂逃逸排放会引发一系列大气化学反应。碳捕集化学系统运行中胺吸收剂会以液滴、气态、气溶胶颗粒形式排向大气进而引发大气气相反应。胺吸收剂与OH自由基反应主要涉及—CH₂基团、C—H键之间的H-抽提反应，少量在N—H键之间发生，极少部分在—OH基团之间发生，生成亚胺、醛类等；与Cl自由基反应涉及—CH₂基团、—NH₂基团、—OH基团，生成氮氧化物、HCl等；与NO _x 反应包含氨基或烷基的抽氢反应，与不饱和化合物的加成反应生成硝酸、硝胺、亚硝胺等。胺与臭氧的反应主要产生酰胺、异氰酸、亚硝基化合物等。这些化合物对大气环境和人体健康都具有潜在的危害，可能对空气质量和生态系统造成严重影响，甚至引发癌症等健康问题。国内外对碳捕集排放限值皆有规定，但对总胺排放限定缺乏标准。尽管胺排放控制取得一些进展，但小颗粒气溶胶的脱除效率低、适用局限、工艺复杂、能耗高等问题亟待解决。

关键词: 碳捕集, 化学吸收, 胺吸收剂, 大气反应, 光化学

CLC Number:

X701

LU Shijian, ZHU Wenju, LIU Ling, KANG Guojun, CHEN Siming. Advances in atmospheric gas-phase reactions initiated by amine absorbent escape[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6397-6411.

陆诗建, 祝文举, 刘玲, 康国俊, 陈思铭. 胺吸收剂逃逸引发的大气气相反应进展[J]. 化工进展, 2024, 43(11): 6397-6411.

Figures/Tables 20

排放类型	形态	产生原因	吸收塔后胺排放数量级/μL·L^-1
物理夹带	液滴D≥100μm	气液接触时部分吸收剂被气流携带	<1
气体	气态	吸收剂及其降解产物挥发	0~10²
气溶胶	气溶胶颗粒100μm>D>1nm	吸收塔内非均相成核、均相成核、气泡破裂等	0~10³

来源	报道的排放浓度/mg·m^-3	组分
IEAGHG技术报告试验厂^[13]	0.5~3	MEA
Niederaussem中试工厂^[14]	0.02~0.03	MEA
CESAR中试工厂^[15]	<0.3	MEA
ENEL中试工厂^[16]	1.2~1.5	MEA（WESP运行与否）
Maasvlakte火电站CO₂捕集中试厂，1500m³/h^[10]	0.97~4	MEA（除雾器后）
	206	MEA（水洗塔后）
	336~460	MEA（吸收塔后）
Loy Yang中试工厂^[17]	2.4	MEA
KIT中试火电厂CO₂捕集系统，180m³/h^[18]	3000	MEA
TNO微型移动捕集试验厂，4m³/h^[19]	100~200	MEA（进口烟气含有烟尘）
TNO微型移动捕集试验厂，4m³/h^[19]	600~1100	MEA（进口烟气含有SO₃）
TNO微型移动捕集试验厂，4m³/h^[9]	1000~1900	MEA（贫液温度40~80℃)）
	100~2940	AMP（贫液pH=9.4~11.0，硫酸气溶胶浓度变化）
	0~416	PZ（CO₂体积分数0.7%~13%，硫酸气溶胶浓度变化）
TNO微型移动捕集试验厂，4m³/h^[20]	383 1051	MEA（进口烟气无SO₃） MEA（进口烟气SO₃浓度5.25μL/L）

胺吸收剂种类	结构	k_OH/cm³·mol^-1·s^-1
MEA		(7.61±0.76)×10^-11[24] (9.2±1.1)×10^-11[25] (7.02±0.46)×10^-11[26]
DMEA		(9.0±2.0)×10^-11[27] (4.7±1.2)×10^-11[28] (7.29±0.72)×10^-11[29]
AMP		(2.8±0.5)×10^-11[28]
PZ		(2.8±0.6)×10^-10[30]
MMEA		(8.26±0.82)×10^-11[29]

胺吸收剂种类	结构	k $O 3$ /cm³·mol^-1·s^-1
MEA		(1.09±0.05)×10^-18[35]
AMP		1.9×10^-19[36]
DMAE		(6.76±0.83)×10^-18[37]

胺吸收剂种类	结构	k $O 3$ /cm³·mol^-1·s^-1
MEA		(1.09±0.05)×10^-18[35]
AMP		1.9×10^-19[36]
DMAE		(6.76±0.83)×10^-18[37]

化学名称/种类	缩写名称	是否鉴定
2-氨基-2-甲基-1-丙醇（碱胺）	AMP	是
AMP的氨基	AMPN	否（未观察到自由基）
AMP的过氧基团	AMPR	否（未观察到自由基）
AMP硝酸气溶胶	AMPNTR	通过SMPS测量间接观察到
AMP亚硝胺	AMPNO	否（亚硝胺很难观察到）
AMP硝胺	AMPNO₂	通过SIFT-MS观察到，但很难量化
甲烯丙醇等产品	ISPD	否

污染物	最高允许排放浓度/mg·m^-3	最高允许排放速率/kg·h^-1			无组织排放监控浓度限值
污染物	最高允许排放浓度/mg·m^-3	排放气筒高度/m	二级	三级	监控点	浓度/mg·m^-3
苯胺类	20	15	0.52	0.78	周界外最高浓度点	0.40
		20	0.87	7.3
		30	2.9	4.4
		40	5.0	7.6
		50	7.7	12
		60	11	17
氮氧化物	240（硝酸使用和其他）	15	0.77	1.2	周界外最高浓度点	0.12
		20	1.3	2.0
		30	4.4	6.6
		40	7.5	11
		50	12	18
		60	16	25
		70	23	35
		80	31	47
		90	40	61
		100	52	78
甲醛	25	15	0.26	0.39	周界外最高浓度点	0.20
		20	0.43	0.65
		30	1.4	2.2
		40	2.6	3.8
		50	3.8	5.9
		60	5.4	8.3

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