我国石化储罐VOCs安全高效深度减排、回收和热氧化技术进展

doi:10.16085/j.issn.1000-6613.2023-0623

摘要/Abstract

摘要：

全面总结了石化储罐VOCs产排机理、排放特征以及VOCs减排、回收和热氧化技术进展，并提出了意见和建议，希望对我国石化储罐VOCs深度减排有所裨益。石化储罐除大小呼吸产气外，还有高温重油储存热裂解等产气现象。在计算储罐排气中可燃物浓度时不应忽视硫化氢、甲烷、氢气、氨等组分。目前，中美储罐VOCs管控都以选择浮顶罐等源头减排为主，以储罐使用过程控制和排放气末端治理为辅，我国应适时修订现行标准，以适应越来越严的环保要求。核算得出2019年我国有机液体储罐VOCs排放量为(39.2~90.4)×10⁴t，主要来自石化企业，建议将粗柴油、粗汽油、粗航煤、蜡油、燃料油、渣油等中间产品罐或重油罐与苯、甲苯、二甲苯、甲醇等储罐一起列为优先管控对象。建议我国开展石化储罐VOCs深度减排，包括源头减排、过程控制和末端治理，内浮顶罐内置气袋有可能成为继浮盘之后又一重要的源头减排技术；低温柴油吸收与吸附、冷凝相比，在处理含硫量较高的粗汽油、粗柴油、高温重油等储罐废气上具有优势。总体上，我国石化储罐外排VOCs治理正在从回收向回收+热氧化（催化氧化、蓄热氧化、焚烧炉、工艺加热炉、锅炉）转变，控制热氧化单元出口非甲烷总烃小于20mg/m³。

关键词: 石化储罐, 挥发性有机物, 产气机理, 减排, 回收, 氧化, 安全

Abstract:

This review summarized the VOCs generation and emission mechanisms, emission characteristics, as well as the progress in VOCs reduction, recovery and thermal oxidation technologies for the petrochemical storage tanks. It proposes opinions and suggestions, aiming to contribute to the deep reduction of VOCs emissions from petrochemical storage tanks in China. Besides the gas generation from the large and small breathing of storage tanks, there are also gas generation phenomena such as high temperature heavy oil thermal cracking. When calculating the combustible gas concentration in tank emissions, components such as hydrogen sulfide, methane, hydrogen and ammonia should not be overlooked. The current VOCs control for storage tanks in China and the United States mainly focuses on source reduction through the use of floating roof tanks, with process control during tank operation and end-of-pipe treatment as supplementary measures. However, it is difficult to meet increasingly strict environmental requirements. It is suggested that China should revise the current standards in a timely manner. According to calculations, the VOCs emissions from organic liquid storage tanks in China in 2019 were estimated to be approximately 392000t to 904000t, mainly from petrochemical enterprises. It is recommended to prioritize control emissions from intermediate product tanks such as crude diesel, crude gasoline, crude aviation kerosene, wax oil, fuel oil, and residual oil, together with tanks containing benzene, toluene, xylene, methanol, and other substances. It is proposed that China should carry out deep reduction of VOCs emissions from petrochemical storage tanks, including source reduction, process control and end-of-pipe treatment. The internal floating roof tanks with built-in gas bag could become another important source reduction technology following floating roofs. It is also emphasized that compared to absorption and condensation, low-temperature diesel absorption have advantages in treating exhaust gases from tanks with high sulfur content, such as crude gasoline, crude diesel, and high-temperature heavy oil. Furthermore, it is noted that overall VOCs control for external emissions from petrochemical storage tanks in China is transitioning from recovery to combined recovery and thermal oxidation (catalytic oxidation, regenerative thermal oxidation, incinerators, process heating furnaces, boilers). The control target for non-methane total hydrocarbons at the outlet of thermal oxidation units is set to be less than 20mg/m³.

Key words: petrochemical storage tank, volatile organic compounds (VOCs), gas production mechanism, emission reduction, recovery, oxidation, safety

中图分类号:

TE991

刘世达, 王海燕, 侯栓弟, 刘忠生, 廖昌建, 王宽岭. 我国石化储罐VOCs安全高效深度减排、回收和热氧化技术进展[J]. 化工进展, 2024, 43(4): 2063-2076.

LIU Shida, WANG Haiyan, HOU Shuandi, LIU Zhongsheng, LIAO Changjian, WANG Kuanling. Recent advances in safely efficient deep emission reduction, recovery and thermal oxidation of VOCs from petrochemical storage tanks in China[J]. Chemical Industry and Engineering Progress, 2024, 43(4): 2063-2076.

图/表 9

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罐型	相对排放系数
固定顶罐	1
外浮顶罐	0.1~0.15
内浮顶罐	0.05~0.1
低压罐+排气处理	<0.01
压力罐	约为0

罐型	相对排放系数
固定顶罐	1
外浮顶罐	0.1~0.15
内浮顶罐	0.05~0.1
低压罐+排气处理	<0.01
压力罐	约为0

类型	序号	标准/政令
美国主要标准	1	40 CFR-60-K^①：1973年6月11日后至1978年5月19日前新建、重建或改造的石油液体储罐的性能标准
	2	40 CFR-60-Ka：1978年5月18日后至1984年7月23日前新建、重建或改造的石油液体储罐的性能标准
	3	40 CFR-60-Kb：1984年7月23日后新建、重建或改造的挥发性有机液体储罐（包括石油液体储罐）的性能标准
	4	40 CFR-61-Y^②：苯储存容器的苯排放国家标准
	5	40 CFR-63-CC^③：石油炼制工业有害空气污染物（HAPs）排放国家标准
	6	40 CFR-63-F：合成有机化学品制造业HAPs排放国家标准
	7	40 CFR-63-G：合成有机化学品制造工艺排气口、储罐、输送作业和废水的有机HAPs排放国家标准
	8	40 CFR-65-C^④：储存容器
	9	OSHA No.1910.95^⑤：职业健康和环境控制标准
中国标准	1	GB 31570—2015《石油炼制工业污染物排放标准》
	2	GB 31571—2015《石油化学工业污染物排放标准》
	3	GB 31572—2015《合成树脂工业污染物排放标准》
	4	GB 37822—2019《挥发性有机物无组织排放控制标准》
	5	GB 37823—2019《制药工业大气污染物排放标准》
	6	GB 39728—2020《陆上石油天然气开采工业大气污染物排放标准》
	7	GB 20950—2020《储油库大气污染物排放标准》
	8	GB 14554—1993《恶臭污染物排放标准》
	9	GBZ 2.1—2019《工作场所有害因素职业接触限值第1部分：化学有害因素》
	10	HJ 1094—2020《石油炼制工业废气治理工程技术规范》
	11	北京市DB11/447—2015《炼油与石油化学工业大气污染物排放标准》
	12	北京市DB11/1385—2017《有机化学品制造业大气污染物排放标准》
	13	天津市DB12/524—2020《工业企业挥发性有机物排放控制标准》
	14	河北省 DB13/2322—2016《工业企业挥发性有机物排放控制标准》
	15	山东省 DB37/2801.6—2018《挥发性有机物排放标准第6部分：有机化工行业》
中国政府和企业政令	1	环境保护部《石化行业挥发性有机物综合整治方案》（环发〔2014〕177号）
	2	生态环境部《重点行业挥发性有机物综合治理方案》（环大气〔2019〕53号）
	3	生态环境部《2020年挥发性有机物治理攻坚方案》（环大气〔2020〕33号）
	4	生态环境部《重污染天气重点行业应急减排措施制定技术指南(2020年修订版)》（环办大气函〔2020〕340号）
	5	生态环境部《关于加快解决当前挥发性有机物治理突出问题的通知》（环大气〔2021〕65号）
	6	生态环境部《2021—2022年秋冬季大气污染综合治理攻坚方案》（环大气〔2021〕104号）
	7	中国石化2020年总经理1号令《臭氧污染防治专项行动方案》
	8	中国石化能环部关于印发《内浮顶储罐VOCs治理环保技术要求（试行）》的通知（2021.9.9）

类型	序号	标准/政令
美国主要标准	1	40 CFR-60-K^①：1973年6月11日后至1978年5月19日前新建、重建或改造的石油液体储罐的性能标准
	2	40 CFR-60-Ka：1978年5月18日后至1984年7月23日前新建、重建或改造的石油液体储罐的性能标准
	3	40 CFR-60-Kb：1984年7月23日后新建、重建或改造的挥发性有机液体储罐（包括石油液体储罐）的性能标准
	4	40 CFR-61-Y^②：苯储存容器的苯排放国家标准
	5	40 CFR-63-CC^③：石油炼制工业有害空气污染物（HAPs）排放国家标准
	6	40 CFR-63-F：合成有机化学品制造业HAPs排放国家标准
	7	40 CFR-63-G：合成有机化学品制造工艺排气口、储罐、输送作业和废水的有机HAPs排放国家标准
	8	40 CFR-65-C^④：储存容器
	9	OSHA No.1910.95^⑤：职业健康和环境控制标准
中国标准	1	GB 31570—2015《石油炼制工业污染物排放标准》
	2	GB 31571—2015《石油化学工业污染物排放标准》
	3	GB 31572—2015《合成树脂工业污染物排放标准》
	4	GB 37822—2019《挥发性有机物无组织排放控制标准》
	5	GB 37823—2019《制药工业大气污染物排放标准》
	6	GB 39728—2020《陆上石油天然气开采工业大气污染物排放标准》
	7	GB 20950—2020《储油库大气污染物排放标准》
	8	GB 14554—1993《恶臭污染物排放标准》
	9	GBZ 2.1—2019《工作场所有害因素职业接触限值第1部分：化学有害因素》
	10	HJ 1094—2020《石油炼制工业废气治理工程技术规范》
	11	北京市DB11/447—2015《炼油与石油化学工业大气污染物排放标准》
	12	北京市DB11/1385—2017《有机化学品制造业大气污染物排放标准》
	13	天津市DB12/524—2020《工业企业挥发性有机物排放控制标准》
	14	河北省 DB13/2322—2016《工业企业挥发性有机物排放控制标准》
	15	山东省 DB37/2801.6—2018《挥发性有机物排放标准第6部分：有机化工行业》
中国政府和企业政令	1	环境保护部《石化行业挥发性有机物综合整治方案》（环发〔2014〕177号）
	2	生态环境部《重点行业挥发性有机物综合治理方案》（环大气〔2019〕53号）
	3	生态环境部《2020年挥发性有机物治理攻坚方案》（环大气〔2020〕33号）
	4	生态环境部《重污染天气重点行业应急减排措施制定技术指南(2020年修订版)》（环办大气函〔2020〕340号）
	5	生态环境部《关于加快解决当前挥发性有机物治理突出问题的通知》（环大气〔2021〕65号）
	6	生态环境部《2021—2022年秋冬季大气污染综合治理攻坚方案》（环大气〔2021〕104号）
	7	中国石化2020年总经理1号令《臭氧污染防治专项行动方案》
	8	中国石化能环部关于印发《内浮顶储罐VOCs治理环保技术要求（试行）》的通知（2021.9.9）

排序	储存油品/温度/蒸气压	储罐类型	液体储存量/10⁴t·a^-1	VOCs排放量/t·a^-1
合计				389317.3（901269.4）
1	粗柴油/22（40）℃/3.7（8.14）kPa^①	固定顶	16638.3	84798.2（172440）
2	柴油/22（40）℃/3.7（8.14）kPa	固定顶	14618.4	74530.6（151505）
3	原油/22（45）℃/30.8（62）kPa	外浮顶	69592	71416（75351.7）
4	汽油/22℃/52kPa	内浮顶(双封)	13162	40256
5	粗汽油/22（38）℃/44（91.8）kPa	内浮顶(双封)	14120.7	32986（117342）
6	粗航煤/22（40）℃/3.7（8.1）kPa	固定顶	5252	26858.2（54522.9）
7	航煤/22（40）℃/3.7（8.14）kPa	固定顶	3869.6	19788.7（40171.7）
8	蜡油/120℃/0.25kPa	固定顶	20877.6	11151.4
9	燃料油/90℃/2.38kPa	固定顶	2838	7792.4
10	渣油/120℃/0.18kPa	固定顶	13918.4	6044.5
11	乙醇/22℃/8.0kPa	固定顶	986.45	3935.5
12	正、异丙醇/20℃/4.4kPa	内浮顶(双封)	57.2	3105.2
13	乙苯/25.9℃/1.33kPa	固定顶	954.23	1659.5
14	醋酸/22℃/2.06kPa	固定顶	743.93	1330.4
15	石脑油/22（36.9）℃/63.1（102）kPa	内浮顶(双封)	4598.52	1264.7（212321.2）
16	异丙苯/25.9℃/2.48kPa	固定顶	150	667.7
17	甲醇/22℃/12.3kPa	内浮顶(双封)	7288	602.7
18	环己酮/38.5℃/1.33kPa	固定顶	338	564.2
19	丙烯酸/40℃/1.33kPa	固定顶	250	340
20	对二甲苯/22℃/0.98kPa	内浮顶(双封)	2957.6	225.4