Review on coal and gas co-feed processes for better resource use and lower carbon emission

doi:10.16085/j.issn.1000-6613.2018-1226

Abstract

Abstract:

The low resource efficiency and high carbon emission are severe in coal chemical industries. A great number of co-feed processes of coal and hydrogen-rich gas were proposed to achieve carbon reduction at source. The integrated hydrogen-rich gas includes natural gas, coke-oven gas and shale gas. The representative co-feed processes can be divided into the co-feed process integrated with methane partial oxidation (MPO) and the co-feed process integrated with dry/steam methane reforming (DMR/SMR) according to the differences in process. Tech-economic analysis was conducted for these two processes by means of resource utilization and economic performance, compared with the conventional coal to methanol (CTM) process. The co-feed process with MPO has higher carbon elemental utilization ratios up to 57.9%. It emits 1.50t CO₂ per ton methanol, giving 37.5% reduction. It has a slightly lower production cost. The process integrated with DMR/SMR has the highest carbon utilization ratios of 83.7%. The carbon emission reduction effect is the most obvious. This process emits 0.90t CO₂ per ton methanol, which is 62.5% lower than the traditional process. It has a slightly higher production cost brought by the energy consumption of CO₂ conversion. With the carbon tax higher than 65CNY/t, the advantage of these co-feed processes is emerging on economy due to its carbon reduction.

Key words: coal and gas co-feed, methane partial oxidation, dry/steam methane reforming, techno-economic analysis, element utilization

摘要：

为解决煤化工过程资源利用率低和碳排放高的问题，有研究者提出以天然气、焦炉气、页岩气等富氢资源和煤炭资源联供方案，旨在实现源头碳减排。文章指出依据联供过程技术的差异，较有代表性的方案可分为集成甲烷部分氧化和集成甲烷干/水蒸气重整的气煤联供过程。文章以生产甲醇为例，从资源利用和经济效益等方面对集成甲烷部分氧化和集成甲烷干/水蒸气重整的气煤联供过程进行分析和比较。集成甲烷部分氧化的工艺碳元素利用率达到57.9%，每吨甲醇排放CO₂为1.50t，较传统煤制甲醇工艺排放减少37.5%。甲醇产品成本稍低于传统工艺。集成甲烷干/水蒸气重整工艺的碳元素利用率最高，达到83.7%。减排效果最明显，每吨甲醇排放CO₂为0.90t，较传统工艺排放减少62.5%，但是由于CO₂转化增加能耗，甲醇产品成本有所提升。由于气煤联供过程有利于CO₂减排，当碳税高于65CNY/tCO₂时，两个气煤联供工艺的生产成本低于传统的煤制甲醇工艺。

关键词: 气煤联供, 甲烷部分氧化, 甲烷干/水蒸气重整, 技术-经济分析, 碳氢元素利用

CLC Number:

TQ536.1

Shuoshi LIU, Siyu YANG, Jingfang GU, Yu QIAN. Review on coal and gas co-feed processes for better resource use and lower carbon emission[J]. Chemical Industry and Engineering Progress, 2019, 38(01): 664-671.

刘硕士, 杨思宇, 顾竞芳, 钱宇. 气煤联供实现资源高效利用和碳减排技术进展[J]. 化工进展, 2019, 38(01): 664-671.

Figures/Tables 11

References 36

1	王明华, 李政, 倪维斗 . “双气头”多联产中试装置的流程设计研究[J]. 煤炭转化，2007，30(2): 48-52.
	WANG Minghua ， LI Zheng ， NI Weidou . Research on flowsheet design of medium scale double gas polygeneration device[J]. Coal Conversion，2007，30(2): 48-52.
2	王灵梅, 李政, 倪维斗, 等 . “双气头”多联产系统的能值评估[J]. 动力工程学报, 2010，30(10): 798-803.
	WANG Lingmei ， LI Zheng ， NI Weidou ，et al . Energy evaluation of double gas polygeneration systems[J]. Journal of Chinese Society of Power Engineering，2010，30(10): 798-803.
3	谢克昌, 张永发, 赵炜 . “双气头”多联产系统基础研究——焦炉煤气制备合成气[J]. 能源与节能, 2008(2): 10-12.
	XIE Kechang , ZHANG Yongfa , ZHAO Wei . Basic research on the "double head" polygeneration system—Preparation of syngas from coke oven gas[J]. Energy and Energy Conservation, 2008(2): 10-12.
4	LIN H , JIN H G , GAO L , et al . A polygeneration system for methanol and power production based on coke oven gas and coal gas with CO₂ recovery[J]. Energy, 2014, 74(2): 174-180.
5	YI Q , GONG M H , HUANG Y , et al . Process development of coke oven gas to methanol integrated with CO₂, recycle for satisfactory techno-economic performance[J]. Energy, 2016, 112：618-628.
6	MAN Y , YANG S Y , QIAN Y , et al . Conceptual design of coke-oven gas assisted coal to olefins process for high energy efficiency and low CO₂ emission[J]. Applied Energy, 2014, 133：197-205.
7	HUANG H , YANG S , CUI P . Design concept for coal-based polygeneration processes of chemicals and power with the lowest energy consumption for CO₂ capture[J]. Energy Conversion & Management, 2018, 157：186-194.
8	GHODOOSI F , KHOSRAVI-NIKOU M R , SHARIATI A . Mathematical modeling of reverse water-gas shift reaction in a fixed‐bed reactor[J]. Chemical Engineering & Technology, 2017, 40(3): 598-607.
9	刘霞 . 煤制甲醇过程的低温余热利用与碳减排工艺研究[D]. 广州: 华南理工大学, 2016.
	LIU Xia . The study on low temperature waste heat utilization and carbon reduction of coal-based methanol process[D]. Guangzhou: South China University of Technology, 2016
10	彭丽娟 . 焦炉气辅助煤气化制甲醇系统概念设计[D]. 广州: 华南理工大学, 2014.
	PENG Lijuan . Conceptual design of coke-oven gas assisted coal gasification to methanol process[D]. Guangzhou: South China University of Technology, 2014.
11	葛志颖, 郭炜 . 焦炉气催化部分氧化制甲醇氢碳比优化与CO₂减排[J]. 化工设计通讯, 2011, 37(2): 72-74.
	GE Zhiying , GUO Wei . Optimization of hydrogen-carbon ratio in methanol production from COG catalytic partial oxidation and CO₂ emission reduction[J]. Chemical Engineering Design Communications, 2011, 37(2): 72-74.
12	ZHAN M C , WANG W D , TIAN T F , et al . Catalytic partial oxidation of methane over perovskite La₄Sr₈Ti₁₂O_38- _δ solid oxide fuel cell (SOFC) anode material in an oxygen-permeable membrane reactor[J]. Energy & Fuels, 2010(24): 764-771.
13	BERMÚDEZ J M , FERRERA-LORENZO N , LUQUE S , et al . New process for producing methanol from coke oven gas by means of CO₂ reforming. Comparison with conventional process[J]. Fuel Processing Technology, 2013, 115(11): 215-221.
14	COURSON C , MAKAGA E , PETIT C , et al . Development of Ni catalysts for gas production from biomass gasification. Reactivity in steam-and dry -reforming[J]. Catalysis Today, 2000, 63(2): 427-437.
15	ABASHAR M E E . Coupling of steam and dry reforming of methane in catalytic fluidized bed membrane reactors[J]. International Journal of Hydrogen Energy, 2004, 29(8): 799-808.
16	BHAVSAR S , NAJERA M , VESER G . Chemical looping dry reforming as novel, intensified process for CO₂ activation[J]. Chemical Engineering & Technology, 2012, 35(7): 1281-1290.
17	NAJERA M , GRACE H , BHAVSAR S , et al . CO₂ activation via chemical Looping dry reforming[C]//23rd North American Catalysis Society Meeting, 2013.
18	ZENG Y , LIU S , MEI D , et al . Plasma-catalytic dry reforming of methane over Al₂O₃ supported metal catalysts[C]//IEEE International Conference on Plasma Sciences, 2015：80-87.
19	CHEN L , GANGADHARAN P , LOU H H . Sustainability assessment of combined steam and dry reforming versus tri-reforming of methane for syngas production[J]. Asia-Pacific Journal of Chemical Engineering, 2018. DOI:13.10.1002/apj.2168. DOI URL
20	YANG S , YANG Q , YI M , et al . Conceptual design and analysis of a natural gas assisted coal-to-olefins process for CO₂ reuse[J]. Industrial & Engineering Chemistry Research, 2013, 52(40): 14406-14414.
21	LUYBEN W L . Design and control of the dry methane reforming process[J]. Industrial & Engineering Chemistry Research, 2014, 53(37): 14423-14439.
22	GANGADHARAN P , KANCHI K C , LOU H H . Evaluation of the economic and environmental impact of combining dry reforming with steam reforming of methane[J]. Chemical Engineering Research & Design, 2012, 90(11): 1956-1968.
23	BARELLI L , BIDINI G , GALLORINI F , et al . Hydrogen production through sorption-enhanced steam methane reforming and membrane technology: a review[J]. Energy, 2008, 33(4): 554-570.
24	XU J , FROMENT G F . Methane steam reforming, methanation and water-gas shift: I. Intrinsic kinetics[J]. AIChE Journal, 1989, 35：88-96.
25	ROSTRUP-NIELSEN T . Process for the catalytic steam reforming of a hydrocarbon feedstock: AU200048635B2[P]. 2004-02-05.
26	MAN Y , YANG S Y , QIAN Y . Integrated process for synthetic natural gas production from coal and coke-oven gas with high energy efficiency and low emission[J]. Energy Conversion and Management, 2016, 117：162-170.
27	RUIZMERCADO G J , SMITH R L , GONZALEZ M A . Sustainability indicators for chemical processes：Ⅰ. Taxonomy[J]. Industrial & Engineering Chemistry Research, 2012, 51(5): 2309-2328.
28	ZHU Y , BIDDY M J , JONES S B , et al . Techno-economic analysis of liquid fuel production from woody biomass via hydrothermal liquefaction (HTL) and upgrading[J]. Applied Energy, 2014, 129(5): 384-394.
29	ORHAN M F , DINCER I , NATERER G F . Cost analysis of a thermochemical Cu-Cl pilot plant for nuclear-based hydrogen production[J]. International Journal of Hydrogen Energy, 2008, 33(21): 6006-6020.
30	LI Z , HU S , CHEN D , et al . Study on systems based on coal and natural gas for producing dimethyl ether[J]. Industrial & Engineering Chemistry Research, 2009, 48(8): 4101-4108.
31	YANG S , YANG Q , LI H , et al . An integrated framework for modeling, synthesis, analysis, and optimization of coal gasification-based energy and chemical processes[J]. Industrial & Engineering Chemistry Research, 2012, 51(48): 15763-15777.
32	XIANG D , YANG S Y , QIAN Y , et al . Techno-economic performance of the coal-to-olefins process with CCS[J]. Chemical Engineering Journal, 2014, 240(6): 45-54.
33	MANTRIPRAGADA H C , RUBIN E S . Techno-economic evaluation of coal-to-liquids (CTL) plants with carbon capture and sequestration[J]. Energy Policy, 2011, 39(5): 2808-2816.
34	姜睿 . 碳交易与中国碳市场展望[J]. 中国经济报告, 2017(5): 52-56.
	JIANG Rui . Carbon trading and China's carbon market outlook [J]. China Policy Review, 2017(5): 52-56.
35	张亮 . 欧洲国家环境税制度对中国碳税政策的借鉴与启示[J]. 环境与发展, 2017, 29(4): 27-29.
	ZHANG Liang . European countries’ environmental tax system and its inspiration to China’s carbon tax policies[J]. Environment and Development, 2017, 29(4): 27-29.
36	YUAN M , METCALF G E , REILLY J , et al . The revenue implications of a carbon tax[R/OL]. 2017. .

流程	技术规范参数	CTM^[9,10]	MPO^[5,13]	DMR/SMR^[6,20,23]
煤气化（Texaco）	气化压力/MPa	4.2	4.2	4.2
	气化温度/℃	1300	1300	1300
	碳转化率/%	98	98	98
空分	高压/MPa	0.6	0.6	0.6
	低压/MPa	0.13	0.13	0.13
水煤气变换（Co-Mo）	高温段入口温度/℃	400
	低温段入口温度/℃	210
酸性气体脱除（Rectisol）	CO₂吸收温度/℃	-33		-33
	H₂S吸收温度/℃	-23		-23
变压吸附	氢气收率			>90%
甲烷部分氧化	反应压力/MPa		3.0
	反应温度/℃		1000
	碳转化率/%		>88
甲烷干重整	反应压力/MPa			0.1
	反应温度/℃			800
	碳转化率/%			99.9
甲烷水蒸气重整	反应压力/MPa			0.1
	反应温度/℃			900
	碳转化率/%			99.9
甲醇合成	反应压力/MPa	5.0	5.0	5.0
	反应温度/℃	240	250	240
	循环比	4.5	4.0	4.5

流程	技术规范参数	CTM^[9,10]	MPO^[5,13]	DMR/SMR^[6,20,23]
煤气化（Texaco）	气化压力/MPa	4.2	4.2	4.2
	气化温度/℃	1300	1300	1300
	碳转化率/%	98	98	98
空分	高压/MPa	0.6	0.6	0.6
	低压/MPa	0.13	0.13	0.13
水煤气变换（Co-Mo）	高温段入口温度/℃	400
	低温段入口温度/℃	210
酸性气体脱除（Rectisol）	CO₂吸收温度/℃	-33		-33
	H₂S吸收温度/℃	-23		-23
变压吸附	氢气收率			>90%
甲烷部分氧化	反应压力/MPa		3.0
	反应温度/℃		1000
	碳转化率/%		>88
甲烷干重整	反应压力/MPa			0.1
	反应温度/℃			800
	碳转化率/%			99.9
甲烷水蒸气重整	反应压力/MPa			0.1
	反应温度/℃			900
	碳转化率/%			99.9
甲醇合成	反应压力/MPa	5.0	5.0	5.0
	反应温度/℃	240	250	240
	循环比	4.5	4.0	4.5

参数	流程
参数	CTM	MPO	DMR/SMR
规模/kt·a^-1	1200	1200	1200
总投资/×10⁹ CNY	5.8	2.5	4.0
物料和能量消耗
煤/t·(t甲醇) ^-1	1.32	0.21	0.36
焦炉气/m³·(t甲醇) ^-1	N/A	1600	1217
氧气/m³·(t甲醇) ^-1	858	560	234
蒸汽/MJ·(t甲醇) ^-1	5403	0	5093
电力/KW·h·(t甲醇) ^-1	548	651	612
产品成本/CNY·t ^-1	1840	1732	1936

参数	流程
参数	CTM	MPO	DMR/SMR
规模/kt·a^-1	1200	1200	1200
总投资/×10⁹ CNY	5.8	2.5	4.0
物料和能量消耗
煤/t·(t甲醇) ^-1	1.32	0.21	0.36
焦炉气/m³·(t甲醇) ^-1	N/A	1600	1217
氧气/m³·(t甲醇) ^-1	858	560	234
蒸汽/MJ·(t甲醇) ^-1	5403	0	5093
电力/KW·h·(t甲醇) ^-1	548	651	612
产品成本/CNY·t ^-1	1840	1732	1936

[1]	LIU Yang, WU Xiuzhang, LIU Yongjian, WANG Bo. Global heat integration and optimization of coal to natural gas process [J]. Chemical Industry and Engineering Progress, 2021, 40(7): 3719-3727.
[2]	YANG Qingchun, YANG Qing, ZHANG Jinliang, GAO Minglin, MEI Shumei, ZHANG Dawei. Development and system assessment of a coal-to-ethylene glycol process coupled with SOEC [J]. Chemical Industry and Engineering Progress, 2021, 40(11): 6061-6070.
[3]	Yongjian LIU, Xiuzhang WU, Heming WANG, Junbing XIA, Bo WANG. Investigation and analysis of coal-based co-production process of synthetic natural gas and chemicals [J]. Chemical Industry and Engineering Progress, 2019, 38(07): 3111-3116.
[4]	XIAO Honghua, LIU Yang, HUANG Hong, YANG Siyu. Modeling and heat integration for water gas shift unit of coal to SNG process [J]. Chemical Industry and Engineering Progress, 2018, 37(02): 554-560.
[5]	MA Youfu, YANG Lijuan. Techno-economic comparison of the thermodynamic system at lignite-fired boiler's cold-end for recovering waste heat of exhaust gases [J]. Chemical Industry and Engineering Progree, 2016, 35(12): 4088-4095.
[6]	HE Wenjun, FEI Taikang, WANG Jiahua, YANG Weimin. Economic investigation of direct catalytic hydration of ethylene oxide to ethylene glycol [J]. Chemical Industry and Engineering Progree, 2016, 35(07): 2268-2273.
[7]	ZHOU Huairong, YANG Qingchun, YANG Siyu. Techno-economic analysis and comparison of oil shale-to-liquid fuels and coal-to-liquid fuels processes [J]. Chemical Industry and Engineering Progress, 2016, 35(05): 1404-1409.
[8]	ZHOU Huairong, ZHANG Jun, YANG Siyu. Techno-economic analysis of oil shale retorting process [J]. Chemical Industry and Engineering Progree, 2015, 34(3): 684-688.