Research progress of wet process synergistic desulfurization and decarbonization technology for coal-fired flue gas

doi:10.16085/j.issn.1000-6613.2023-1945

Abstract

Abstract:

Treatment of the SO₂ and CO₂ in coal-fired flue gas is gradually developing to remove them simultaneously, and combined technologies based on the wet process of desulfurization and decarbonization have thus gained wide attention. Firstly, this paper systematically reviewed the main research directions of the stepwise (sequential) SO₂ and CO₂ removal technology. It was found that amine degradation caused by SO₂ is the core problem for this technology, but the mechanism was still in debate. The roles of desulfurization intensification and amine degradation inhibitors in alleviating the negative effects of SO₂ were analyzed from the perspectives of emission control and degradation prevention, respectively. Compared with stepwise treatment, the simultaneous SO₂ and CO₂ removal technology could achieve cyclic absorption and desorption based on a single solvent. Therefore, the latest progress of the simultaneous SO₂ and CO₂ removal technology was then summarized, including those using calcium-based, ammonia-based, and amine-based solvents. The principles and process design of each type of absorption system were sorted out and compared, and the most developed one was the ammonia-based combined processes. This paper also briefly described the advantages, disadvantages and development prospects of the two types of synergistic removal technologies. Finally, this paper suggested that future attention for the stepwise SO₂ and CO₂ removal technology should be focused on the mechanism of SO₂caused_{amine degradation and its role in the development of degradation prevention measures, while for the combined removal technology, studies on reaction theory and integrated process modeling should be pursued.}

Key words: coal combustion, flue gas, CO₂ capture, desulfurization, integration

摘要：

燃煤烟气中SO₂和CO₂的处理逐渐向协同脱除方向发展，基于湿法脱硫和脱碳的组合技术因此获得了广泛关注。本文首先系统梳理了梯级（依次）脱硫脱碳技术的重点研究方向，认为SO₂的胺降解作用是该类技术面对的核心问题，但其影响机理尚未形成统一共识。从控制排放和预防降解两个角度出发，分析了强化脱硫技术和胺降解抑制剂对缓解SO₂不利影响的作用。与梯级处理相比，联合（同步）脱硫脱碳技术可基于单一溶剂实现循环吸收-解吸。然后总结了钙法、氨法、胺法等联合脱硫脱碳（联脱）技术的最新进展，梳理并对比了各类吸收体系的原理和工艺设计，其中基于氨水的联脱工艺研究最为成熟。还简述了两类协同脱除技术的优缺点和发展前景。最后，建议对于梯级脱硫脱碳技术未来应重点关注SO₂的胺降解机理及其在开发预防降解措施中的作用，对于联脱技术应加强反应理论和集成工艺建模研究等。

关键词: 煤燃烧, 烟气, 二氧化碳捕集, 脱硫, 集成

CLC Number:

X511

GAO Fanxiang, LIU Yang, ZHANG Guiquan, QIN Feng, YAO Jiantao, JIN Hui, SHI Jinwen. Research progress of wet process synergistic desulfurization and decarbonization technology for coal-fired flue gas[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2324-2342.

高凡翔, 刘阳, 张贵泉, 秦锋, 姚建涛, 金辉, 师进文. 燃煤烟气湿法协同脱硫脱碳技术研究进展[J]. 化工进展, 2024, 43(5): 2324-2342.

Figures/Tables 13

改造类型	改造项目或地点	改造方案	SO₂排放浓度（标准）/mg·m^-3		脱硫效率/%		完工时间 /年
改造类型	改造项目或地点	改造方案	改造前	改造后	改造前	改造后	完工时间 /年
喷淋层	攀枝花某企业小型锅炉^[51]	增设一层冲洗水层，缩短喷嘴与除雾器间距，优化冲洗水管及相关配套设施等	$≤$ 600	78~126	$≥$ 90	98.5~99.0	2016
喷淋层	魏家峁电厂^[50]	采用一层旋流和三层喷淋，增加每层喷淋喷嘴数等	130	<23	>95	>99	2017
托盘塔	某660MW超临界燃煤机组^[53]	采用双托盘，拆除回转式烟气换热器（GGH），增加液气比等	111	<35	91.5~92.5	$≤$ 99	2012
托盘塔	华能集团滇东电厂3号和4号机组^[54]	采用双托盘，增设喷淋层，拆除GGH，布置3级高效屋脊式除雾器及冲洗水系统等	—	<35	—	—	2018
单塔双区	某公司二期630MW电厂^[55]	对吸收塔两段环切加高，优化改进配套设备等	100	$≤$ 32	96	$≥$ 98.9	2018
单塔双循环	山西某超低排放项目^[57]	升级原塔，新建塔外循环塔和配套的浆液循环泵等	$≤$ 200	<35	$≥$ 95.2	$≥$ 99.2	2015
单塔双循环	某1000MW燃煤电厂^[58]	拆除原塔并建新塔和一座循环浆液槽	100~175	$≤$ 35	95	$≥$ 99	2016
双塔双循环	大唐集团河北某600MW发电厂^[59]	新建一级吸收塔与原吸收塔（二级）串联	110~170	<35	95	>99	2014
	国电谏壁发电厂8号机组^[60]	利用7号机组旧塔与8号机组旧塔组合形成双塔双循环	>50	22.43	95	>99.3	2014
	任丘2×300MW燃煤电厂^[61]	新建二级吸收塔与原吸收塔（一级）串联	163.49	20.65	93.07	99.47	2018
	某350MW燃煤电厂^[62]	新建二级吸收塔与原吸收塔（一级）串联	107	27	96.5	99.3	2018
	华能集团滇东电厂1号和2号机组^[54]	新建二级吸收塔与原吸收塔（一级）串联	$≤$ 600	<35	—	99.53	2018
其他	宁夏某2×350MW燃煤电厂^[63]	增大塔壁板高度，增加喷淋层，扩大浆池容积等	>50	35	>98.675	>99.08	2020
	某3×50MW抽凝式发电机组^[64]	新建塔形成“一炉一塔”，原塔新增脱硫增效协同除尘设置，改用三级屋脊式高效除雾器及冲洗水系统等	89.6	9.7	—	98.8~99.7	2022
	某2×600MW燃煤电厂^[65]	新增浆液再循环装置，差异化布置喷嘴，升级除雾器等	> 45	<35	—	>95	2022
	兰州石化公司燃煤锅炉^[66]	新建塔形成“一炉一塔”，原塔喷淋层增设湍流器和偏转环	$≤$ 50	$≤$ 30	—	99	2023

改造类型	改造项目或地点	改造方案	SO₂排放浓度（标准）/mg·m^-3		脱硫效率/%		完工时间 /年
改造类型	改造项目或地点	改造方案	改造前	改造后	改造前	改造后	完工时间 /年
喷淋层	攀枝花某企业小型锅炉^[51]	增设一层冲洗水层，缩短喷嘴与除雾器间距，优化冲洗水管及相关配套设施等	$≤$ 600	78~126	$≥$ 90	98.5~99.0	2016
喷淋层	魏家峁电厂^[50]	采用一层旋流和三层喷淋，增加每层喷淋喷嘴数等	130	<23	>95	>99	2017
托盘塔	某660MW超临界燃煤机组^[53]	采用双托盘，拆除回转式烟气换热器（GGH），增加液气比等	111	<35	91.5~92.5	$≤$ 99	2012
托盘塔	华能集团滇东电厂3号和4号机组^[54]	采用双托盘，增设喷淋层，拆除GGH，布置3级高效屋脊式除雾器及冲洗水系统等	—	<35	—	—	2018
单塔双区	某公司二期630MW电厂^[55]	对吸收塔两段环切加高，优化改进配套设备等	100	$≤$ 32	96	$≥$ 98.9	2018
单塔双循环	山西某超低排放项目^[57]	升级原塔，新建塔外循环塔和配套的浆液循环泵等	$≤$ 200	<35	$≥$ 95.2	$≥$ 99.2	2015
单塔双循环	某1000MW燃煤电厂^[58]	拆除原塔并建新塔和一座循环浆液槽	100~175	$≤$ 35	95	$≥$ 99	2016
双塔双循环	大唐集团河北某600MW发电厂^[59]	新建一级吸收塔与原吸收塔（二级）串联	110~170	<35	95	>99	2014
	国电谏壁发电厂8号机组^[60]	利用7号机组旧塔与8号机组旧塔组合形成双塔双循环	>50	22.43	95	>99.3	2014
	任丘2×300MW燃煤电厂^[61]	新建二级吸收塔与原吸收塔（一级）串联	163.49	20.65	93.07	99.47	2018
	某350MW燃煤电厂^[62]	新建二级吸收塔与原吸收塔（一级）串联	107	27	96.5	99.3	2018
	华能集团滇东电厂1号和2号机组^[54]	新建二级吸收塔与原吸收塔（一级）串联	$≤$ 600	<35	—	99.53	2018
其他	宁夏某2×350MW燃煤电厂^[63]	增大塔壁板高度，增加喷淋层，扩大浆池容积等	>50	35	>98.675	>99.08	2020
	某3×50MW抽凝式发电机组^[64]	新建塔形成“一炉一塔”，原塔新增脱硫增效协同除尘设置，改用三级屋脊式高效除雾器及冲洗水系统等	89.6	9.7	—	98.8~99.7	2022
	某2×600MW燃煤电厂^[65]	新增浆液再循环装置，差异化布置喷嘴，升级除雾器等	> 45	<35	—	>95	2022
	兰州石化公司燃煤锅炉^[66]	新建塔形成“一炉一塔”，原塔喷淋层增设湍流器和偏转环	$≤$ 50	$≤$ 30	—	99	2023

地点	名称	规模	溶剂类型	能耗/GJ·t^-1	时间/年
美国	Warrior Run示范项目	150t/d	MEA	—	2000
美国	Petro Nova碳捕集项目	1.4×10⁶t/a	KS-1	2.4	2017
德国	Staudinger电站中试项目	—	氨基酸	2.7	2009
德国	Wilhelmshaven电站中试项目	70t/d	二甘醇胺	2.7	2012
加拿大	Boundary Dam项目	1×10⁶t/a	MEA	—	2014
澳大利亚	Hazelwood电站中试项目	1t/d	碳酸钾	2.5	2011
中国	华能北京热电厂中试项目	3000t/a	MEA	—	2008
	华能上海石洞口示范项目	1.2×10⁵t/a	MEA	3	2009
	胜利发电厂100t/a CO₂捕集纯化工程	100t/d	新型MSA复合吸收剂	5.95	2012
	长春热电厂相变型碳捕集工业装置	1000t/a	相变吸收剂	2.3	2020
	国能锦界1.5×10⁵t/a CCUS示范项目	1.5×10⁵t/a	复合胺（多氨基胺及位阻胺）	2.4	2021
	齐鲁石化-胜利油田百万吨级CCUS项目	1t/a	新型MSA复合吸收剂	—	2022

技术类型	优点	缺点
梯级脱硫脱碳技术	1.技术成熟，工程经验丰富	1.占地空间大，不易维护
	2.易于在已有电站改造（无论是否有FGD系统）	2.能耗高
	3.脱硫和脱碳系统便于各自调控实现高脱除率	3.烟气成分对脱碳剂的影响大
联合脱硫脱碳技术	1.节能潜力大	1.技术不成熟，工程经验极少
	2.占地空间小，运行维护方便	2.不适合已有FGD系统的电站改造
		3.单一吸收剂的用量更大，使吸收效率受影响，设备更易腐蚀、胺损耗更严重等

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