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Article(id=1295065161497333769, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295064874678252123, articleNumber=null, orderNo=null, doi=10.19666/j.rlfd.202505085, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1747152000000, receivedDateStr=2025-05-14, revisedDate=1750176000000, revisedDateStr=2025-06-18, acceptedDate=1750608000000, acceptedDateStr=2025-06-23, onlineDate=1786697195648, onlineDateStr=2026-08-14, pubDate=1774368000000, pubDateStr=2026-03-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1786697195648, onlineIssueDateStr=2026-08-14, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1786697195648, creator=13701087609, updateTime=1786697195648, updator=13701087609, issue=Issue{id=1295064874678252123, tenantId=1146029695717560320, journalId=1210938733613449225, year='2026', volume='55', issue='3', pageStart='1', pageEnd='184', issueExtLink='null', onlineDate='null', pubDate='1774368000000', pubDateStr='2026-03-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1786697127264, creator='13701087609', updateTime=1786698874628, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1295072203708592834, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295064874678252123, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1295072203708592835, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295064874678252123, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=28, endPage=35, ext={EN=ArticleExt(id=1295065161673494539, articleId=1295065161497333769, tenantId=1146029695717560320, journalId=1210938733613449225, language=EN, title=Performance simulation of synergistic CO2 capture and NOx removal by integrated compression-purification for natural gas oxy-fuel combustion flue gas, columnId=1211002405299294959, journalTitle=Thermal Power Generation, columnName=Thermal Energy Science Research, runingTitle=null, highlight=null, articleAbstract=
[Objective]

This study aims to investigate the applicable conditions and key operational parameters for an integrated compression, purification, decarbonization, and denitrification process applied to natural gas oxy-fuel combustion flue gas. The research seeks to clarify the technical feasibility and performance boundaries of this process for achieving efficient carbon dioxide (CO2) capture coupled with deep removal of nitrogen oxides (NOx), providing a practical solution for integrated carbon capture and pollutant control in natural gas oxy-fuel combustion systems.

[Methods]

A steady-state process model for the compression and purification of oxy-fuel combustion flue gas was developed using Aspen Plus, which accurately describes the thermodynamic behavior of the high-pressure, multi-component gas mixture. Through systematic simulation and parametric sensitivity analysis, the study focused on the combined effects of the initial CO2 volume fraction in the flue gas and the system operating pressure on process performance. Key performance indicators evaluated include the CO2 recovery rate, liquid CO2 product purity, NOx removal efficiency, and specific comprehensive power consumption.

[Results]

The simulation results establish a definitive and strong correlation between the CO2 recovery efficiency and the initial concentration of CO2 in the flue gas. A clear technical threshold is identified: to attain a CO2 recovery rate of 80% or higher, the initial CO2 volume fraction must exceed 60%. This finding defines a primary applicability criterion for the compression-purification approach. Subsequent analysis concentrated on flue gas compositions meeting this high-concentration criterion (>60% CO2). Within this domain, the system operating pressure emerges as the most influential parameter governing the synergistic relationship between NOx abatement and CO2 purification efficiency. Detailed parametric optimization reveals a distinct optimal operating pressure of 2.8 MPa. Operating at this pressure enables the process to achieve superior performance across all key metrics: the NOx removal efficiency surpasses 94%, the purified liquid CO2 product attains a purity of 95% or higher, and the target CO2 recovery rate of ≥80% is reliably maintained. Crucially, this operating point corresponds precisely to the minimum in specific power consumption, which is quantified at 120.1 kW·h per ton of CO2 captured. This represents an optimal trade-off, balancing high environmental performance with minimized energy penalty, a critical factor for economic feasibility.

[Conclusion]

The compression and purification technology is suitable for treating oxy-fuel combustion flue gas with a high initial CO2 volume fraction (>60%). By optimizing the system pressure to 2.8 MPa, efficient CO2 capture and deep NOx removal can be achieved simultaneously with low energy consumption. This study clarifies the key performance thresholds and optimal operating parameters for this integrated process, providing a concrete and feasible technical solution for achieving pollution reduction, carbon mitigation, and resource utilization in natural gas oxy-fuel combustion systems.

, authors=Shaolong YANG, Aijun FU, Jiawei HE, Xiaoshan LI, Cong LUO, Fan WU, Liqi ZHANG, authorsList=Shaolong YANG, Aijun FU, Jiawei HE, Xiaoshan LI, Cong LUO, Fan WU, Liqi ZHANG, authorCompany=null, correspAuthors=Xiaoshan LI, authorNote=null, correspAuthorsNote=null, copyrightStatement=null, copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, fund=null), CN=ArticleExt(id=1295065165364482088, articleId=1295065161497333769, tenantId=1146029695717560320, journalId=1210938733613449225, language=CN, title=天然气富氧燃烧烟气压缩净化协同脱碳脱硝性能模拟, columnId=1211002405437706993, journalTitle=热力发电, columnName=热能科学研究, runingTitle=null, highlight=null, articleAbstract=
【目的】

为满足减污降碳与低能耗目标，针对天然气富氧燃烧烟气，探究压缩净化协同脱碳脱硝工艺的适用条件与关键操作参数，以实现高效的碳捕集与污染物控制。

【方法】

利用Aspen Plus建立富氧燃烧烟气压缩净化工艺模型，通过模拟分析工艺性能及关键影响因素，重点考察CO2体积分数、系统压力等参数对CO2液化提纯及NOx脱除效果的综合影响。

【结果】

CO2回收率显著依赖于初始烟气中CO2的体积分数，为实现CO2回收率≥80%，CO2体积分数需高于60%；对高体积分数CO2烟气（>60%）的研究表明，系统压力是协同脱硝与CO2提纯的关键参数；在系统压力为2.8 MPa时，NOx脱除率>94%，产品CO2纯度≥95%，CO2回收率≥80%，且单位综合电耗最低，为120.1 kW·h/t CO2。

【结论】

富氧燃烧烟气压缩净化技术适用于初始烟气中CO2体积分数较高的烟气条件。通过优化系统压力，可在低能耗下同步实现高效的碳捕集与NOx深度脱除，为天然气富氧燃烧系统的减污降碳与资源化利用提供可行方案。

, authors=杨少龙, 付爱军, 何佳伟, 李小姗, 罗聪, 邬凡, 张立麒, authorsList=杨少龙, 付爱军, 何佳伟, 李小姗, 罗聪, 邬凡, 张立麒, authorCompany=null, correspAuthors=李小姗, authorNote=

杨少龙（2001），男，硕士研究生，主要研究方向富氧燃烧烟气污染物控制技术，。

, correspAuthorsNote=
李小姗（1990），女，博士，副教授，主要研究方向碳捕集与污染物控制技术，。
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杨少龙（2001），男，硕士研究生，主要研究方向富氧燃烧烟气污染物控制技术，。

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杨少龙（2001），男，硕士研究生，主要研究方向富氧燃烧烟气污染物控制技术，。

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Modelling analysis of NOx and SOx removal from oxygen-enriched combustion flue gas based on high-pressure combined removal in a bubbling reactor[J]. Environmental Engineering, 2019, 37(7): 135-141., articleTitle=Modelling analysis of NOx and SOx removal from oxygen-enriched combustion flue gas based on high-pressure combined removal in a bubbling reactor, refAbstract=null)], funds=[Fund(id=1295065175942516865, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, awardId=51806076, language=EN, fundingSource=National Natural Science Foundation of China(51806076), fundOrder=null, country=null), Fund(id=1295065176018014338, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, awardId=51806076, language=CN, fundingSource=国家自然科学基金项目(51806076), fundOrder=null, country=null)], companyList=[AuthorCompany(id=1295065166182371369, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, xref=null, ext=[AuthorCompanyExt(id=1295065166190759978, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, 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figureFileBig=o4fnH7oF4yYzMTY0RyeAfw==, tableContent=null), ArticleFig(id=1295065175007187061, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=CN, label=图11, caption=二级闪蒸温度对CO2纯度及回收率的影响, figureFileSmall=j3XUZiEklc9GXUm+sS+Mow==, figureFileBig=o4fnH7oF4yYzMTY0RyeAfw==, tableContent=null), ArticleFig(id=1295065175070101622, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=EN, label=Tab.1, caption=

Initial composition of the flue gas under different circulation Cases

, figureFileSmall=null, figureFileBig=null, tableContent=
工况流量/m3CO2体积分数/%O2体积分数/%N2体积分数/%H2O体积分数/%NOx体积分数/（×10–6）
工况156 11322.09.067.02.095.17
工况255 01632.04.358.05.5137.72
工况342 10235.08.050.06.5149.32
工况440 99060.53.130.36.1261.51
工况538 96766.03.124.66.3284.72
工况635 83476.33.313.86.6329.60
工况734 32082.42.58.36.8355.90
), ArticleFig(id=1295065175145599097, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=CN, label=表1, caption=

不同烟气循环工况下烟气初始组分

, figureFileSmall=null, figureFileBig=null, tableContent=
工况流量/m3CO2体积分数/%O2体积分数/%N2体积分数/%H2O体积分数/%NOx体积分数/（×10–6）
工况156 11322.09.067.02.095.17
工况255 01632.04.358.05.5137.72
工况342 10235.08.050.06.5149.32
工况440 99060.53.130.36.1261.51
工况538 96766.03.124.66.3284.72
工况635 83476.33.313.86.6329.60
工况734 32082.42.58.36.8355.90
), ArticleFig(id=1295065175216902266, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=EN, label=Tab.2, caption=

The simplified results of NOx removal mechanism for natural gas oxyfuel combustion flue gas

, figureFileSmall=null, figureFileBig=null, tableContent=
序号反应相态
12NO+O2→2NO2气相
2NO+NO2+H2O→2HNO2气相
3N2O3+H2O→2HNO2液相
4N2O4+H2O→HNO3+HNO2液相
52NO2+H2O→HNO3+HNO2液相
), ArticleFig(id=1295065175439200379, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=CN, label=表2, caption=

天然气富氧燃烧烟气NOx 脱除机理简化结果

, figureFileSmall=null, figureFileBig=null, tableContent=
序号反应相态
12NO+O2→2NO2气相
2NO+NO2+H2O→2HNO2气相
3N2O3+H2O→2HNO2液相
4N2O4+H2O→HNO3+HNO2液相
52NO2+H2O→HNO3+HNO2液相
), ArticleFig(id=1295065175502114940, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=EN, label=Tab.3, caption=

Simulation results of compression purification process

, figureFileSmall=null, figureFileBig=null, tableContent=
项目模拟结果Callide Oxyfuel Project[25]
NOx脱除率%99.5699.69
出口NO体积分数/（×10–6）5.22<2.5
), ArticleFig(id=1295065175569223805, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=CN, label=表3, caption=

压缩净化工艺流程模拟结果

, figureFileSmall=null, figureFileBig=null, tableContent=
项目模拟结果Callide Oxyfuel Project[25]
NOx脱除率%99.5699.69
出口NO体积分数/（×10–6）5.22<2.5
), ArticleFig(id=1295065175762161790, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=EN, label=Tab.4, caption=

Simulation results under different Cases

, figureFileSmall=null, figureFileBig=null, tableContent=
工况CO2体积分数/%CO2回收率/%CO2纯度/%水耗/（t·h–1）液化能耗/（kW·h·t–1）烟气压缩能耗/（kW·h·t–1）总能耗/（kW·h·t–1）
工况122.0——————
工况232.035.6595.6979.747.6557.8605.4
工况335.045.7595.31102.747.6386.5434.1
工况460.582.7596.14183.751.5135.5187.0
工况566.087.1596.29189.346.2106.1152.3
工况676.393.6996.56201.045.784.2129.9
工况782.496.7896.75206.645.474.7120.1
), ArticleFig(id=1295065175833464959, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295065161497333769, language=CN, label=表4, caption=

不同工况烟气模拟计算结果

, figureFileSmall=null, figureFileBig=null, tableContent=
工况CO2体积分数/%CO2回收率/%CO2纯度/%水耗/（t·h–1）液化能耗/（kW·h·t–1）烟气压缩能耗/（kW·h·t–1）总能耗/（kW·h·t–1）
工况122.0——————
工况232.035.6595.6979.747.6557.8605.4
工况335.045.7595.31102.747.6386.5434.1
工况460.582.7596.14183.751.5135.5187.0
工况566.087.1596.29189.346.2106.1152.3
工况676.393.6996.56201.045.784.2129.9
工况782.496.7896.75206.645.474.7120.1
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天然气富氧燃烧烟气压缩净化协同脱碳脱硝性能模拟
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杨少龙 , 付爱军 , 何佳伟 , 李小姗 , 罗聪 , 邬凡 , 张立麒
热力发电 | 热能科学研究 2026,55(3): 28-35
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热力发电 |热能科学研究 2026 , 55 (3) : 28 -35
天然气富氧燃烧烟气压缩净化协同脱碳脱硝性能模拟
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杨少龙 , 付爱军, 何佳伟, 李小姗 , 罗聪, 邬凡, 张立麒
作者信息
  • 华中科技大学煤燃烧与低碳利用全国重点实验室，湖北 武汉 430074
通讯作者:
李小姗（1990），女，博士，副教授，主要研究方向碳捕集与污染物控制技术，。
作者简介:

杨少龙（2001），男，硕士研究生，主要研究方向富氧燃烧烟气污染物控制技术，。

Performance simulation of synergistic CO2 capture and NOx removal by integrated compression-purification for natural gas oxy-fuel combustion flue gas
Shaolong YANG , Aijun FU, Jiawei HE, Xiaoshan LI , Cong LUO, Fan WU, Liqi ZHANG
Affiliations
  • State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China
出版时间: 2026-03-25 doi: 10.19666/j.rlfd.202505085
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摘要
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【目的】

为满足减污降碳与低能耗目标，针对天然气富氧燃烧烟气，探究压缩净化协同脱碳脱硝工艺的适用条件与关键操作参数，以实现高效的碳捕集与污染物控制。

【方法】

利用Aspen Plus建立富氧燃烧烟气压缩净化工艺模型，通过模拟分析工艺性能及关键影响因素，重点考察CO2体积分数、系统压力等参数对CO2液化提纯及NOx脱除效果的综合影响。

【结果】

CO2回收率显著依赖于初始烟气中CO2的体积分数，为实现CO2回收率≥80%，CO2体积分数需高于60%；对高体积分数CO2烟气（>60%）的研究表明，系统压力是协同脱硝与CO2提纯的关键参数；在系统压力为2.8 MPa时，NOx脱除率>94%，产品CO2纯度≥95%，CO2回收率≥80%，且单位综合电耗最低，为120.1 kW·h/t CO2。

【结论】

富氧燃烧烟气压缩净化技术适用于初始烟气中CO2体积分数较高的烟气条件。通过优化系统压力，可在低能耗下同步实现高效的碳捕集与NOx深度脱除，为天然气富氧燃烧系统的减污降碳与资源化利用提供可行方案。

富CO2烟气  /  压缩纯化  /  脱硝  /  提纯
[Objective]

This study aims to investigate the applicable conditions and key operational parameters for an integrated compression, purification, decarbonization, and denitrification process applied to natural gas oxy-fuel combustion flue gas. The research seeks to clarify the technical feasibility and performance boundaries of this process for achieving efficient carbon dioxide (CO2) capture coupled with deep removal of nitrogen oxides (NOx), providing a practical solution for integrated carbon capture and pollutant control in natural gas oxy-fuel combustion systems.

[Methods]

A steady-state process model for the compression and purification of oxy-fuel combustion flue gas was developed using Aspen Plus, which accurately describes the thermodynamic behavior of the high-pressure, multi-component gas mixture. Through systematic simulation and parametric sensitivity analysis, the study focused on the combined effects of the initial CO2 volume fraction in the flue gas and the system operating pressure on process performance. Key performance indicators evaluated include the CO2 recovery rate, liquid CO2 product purity, NOx removal efficiency, and specific comprehensive power consumption.

[Results]

The simulation results establish a definitive and strong correlation between the CO2 recovery efficiency and the initial concentration of CO2 in the flue gas. A clear technical threshold is identified: to attain a CO2 recovery rate of 80% or higher, the initial CO2 volume fraction must exceed 60%. This finding defines a primary applicability criterion for the compression-purification approach. Subsequent analysis concentrated on flue gas compositions meeting this high-concentration criterion (>60% CO2). Within this domain, the system operating pressure emerges as the most influential parameter governing the synergistic relationship between NOx abatement and CO2 purification efficiency. Detailed parametric optimization reveals a distinct optimal operating pressure of 2.8 MPa. Operating at this pressure enables the process to achieve superior performance across all key metrics: the NOx removal efficiency surpasses 94%, the purified liquid CO2 product attains a purity of 95% or higher, and the target CO2 recovery rate of ≥80% is reliably maintained. Crucially, this operating point corresponds precisely to the minimum in specific power consumption, which is quantified at 120.1 kW·h per ton of CO2 captured. This represents an optimal trade-off, balancing high environmental performance with minimized energy penalty, a critical factor for economic feasibility.

[Conclusion]

The compression and purification technology is suitable for treating oxy-fuel combustion flue gas with a high initial CO2 volume fraction (>60%). By optimizing the system pressure to 2.8 MPa, efficient CO2 capture and deep NOx removal can be achieved simultaneously with low energy consumption. This study clarifies the key performance thresholds and optimal operating parameters for this integrated process, providing a concrete and feasible technical solution for achieving pollution reduction, carbon mitigation, and resource utilization in natural gas oxy-fuel combustion systems.

CO2-enriched flue gas  /  compression-purification  /  NOx abatement  /  CO2 purification
杨少龙, 付爱军, 何佳伟, 李小姗, 罗聪, 邬凡, 张立麒. 天然气富氧燃烧烟气压缩净化协同脱碳脱硝性能模拟. 热力发电, 2026 , 55 (3) : 28 -35 . DOI: 10.19666/j.rlfd.202505085
Shaolong YANG, Aijun FU, Jiawei HE, Xiaoshan LI, Cong LUO, Fan WU, Liqi ZHANG. Performance simulation of synergistic CO2 capture and NOx removal by integrated compression-purification for natural gas oxy-fuel combustion flue gas[J]. Thermal Power Generation, 2026 , 55 (3) : 28 -35 . DOI: 10.19666/j.rlfd.202505085
正文
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碳捕集、利用与封存（carbon capture, utilization and storage, CCUS）技术是我国“双碳”战略下化石能源低碳利用的重要技术选择[1]。目前，工业上CO2捕集主要为燃烧前、富氧燃烧和燃烧后3种技术路径。富氧燃烧技术利用氧气代替空气，结合大比例烟气循环，可实现烟气中CO2高浓度富集（CO2体积分数80%以上）。相较于其他碳捕集技术，该技术具有捕集效率高、操作过程简单、易规模化及成本低的优势，被认为是能够大规模减少CO2排放的主流碳捕集技术之一[2-3]，在电站锅炉[4]、水泥窑炉[5]、高炉炼铁[6]等领域具有广阔的应用前景。
传统富氧燃烧烟气处理工艺包括选择性催化还原（selective catalytic reduction, SCR）脱硝、电除尘（electrostatic precipitator，ESP）、烟气脱硫（flue gas desulfurization，FGD）和直接接触烟气冷凝器（direct contact cooler，DCC）。当烟气污染物浓度满足超低排放标准后，将其送入压缩纯化单元（compression and purification unit，CPU）进行CO2提纯，可得到满足要求的液态CO2产品。一种新的途径是利用富氧燃烧系统特有的压缩纯化单元协同进行污染物脱除，也称富氧烟气压缩净化技术，即利用CO2压缩液化过程中的高压、低温条件，基于铅室法原理，将烟气中的SO2、NOx分别转化成H2SO4和HNO3来实现SO2和NOx的脱除，其反应过程主要为气相NO被氧化为NO2以及NO2的液相吸收。
针对富氧燃烧压缩净化技术，国外包括加拿大CANMET[7]、德国Linde[8]、法国Air Liquide[9]、美国Air Products[10-12]、华盛顿大学[13]等机构，以及国内包括华中科技大学[14-15]、华北电力大学[16]、神华国华电力研究院[17]、四川空分设备有限公司[18]等机构均开展了相关实验研究、机理分析及工艺动力学模拟等工作。但现有富氧燃烧CO2捕集技术主要基于燃煤烟气，针对天然气富氧燃烧烟气的相关技术尚无深入研究。天然气成分纯净，杂质含量极低（无硫、几乎无灰分），与煤不同，在同样使用富氧燃烧技术的基础上，两者在烟气组分上存在较大差异。因此，天然气富氧燃烧对后续污染物脱除及CO2的压缩纯化提出了新的适应性需求。
综上，针对天然气富氧燃烧烟气组分中的“无硫无汞”特点，本文构建了对应的NOx脱除机理，并以此为基础评估了各类工艺参数对NOx脱除的影响。同时，考虑到压力在污染物脱除[19]及压缩纯化中的重要作用，以压力为“枢纽”构建了针对天然气富氧燃烧污染物脱除及CO2提纯的耦合系统，即压缩净化协同脱碳脱硝单元。在该系统中，烟气压缩净化工艺中产生的高压烟气直接进入CO2提纯单元，脱碳脱硝压力一致，极大减少了CO2提纯过程的烟气压缩能耗。相较于传统烟气处理工艺，即烟气依次经过SCR脱硝、ESP除尘、FGD脱硫和DCC烟气冷凝器，待污染物浓度满足超低排放标准后再进入压缩纯化单元CPU装置进行CO2提纯的方式，该方式既实现了NOx的高效脱除，又节约了重复的压缩机能耗，使得烟气全流程富氧燃烧压缩纯化工艺的总运行成本降低，较大提升了富氧燃烧系统的经济性，在发电行业极具应用潜力。
1　研究方法
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1.1　模拟方法
使用Aspen Plus软件中的电解质模型对烟气压缩净化流程单元进行模拟计算，使用ELENRTL计算吉布斯自由能和化学平衡过程[20]，采用Redlich-Kwang-Soave状态方程和Boston-Mathias α函数预测气相性质和模拟气液相平衡[21]。NOx的反应动力学数据则采用对Laribi[22]完整反应中NOx子系统进行优化后的机理。自产冷量闪蒸分离工艺流程模型使用Peng-Robinson物性方法（基于Posch等人[23]提出的方法），混合参数来自Egger等人[24]的工作。
烟气数据参考采用富氧燃烧技术的某石灰窑（产量500 t/d），不同烟气循环工况下，烟气成分及相关参数如表1所示。
1.2　评价指标定义及计算
1.2.1　NOx脱除率计算方法
η(NOx)=Cin(NO)−Cout(NO)−Cout(NO2)Cin(NO)×100
式中：η（NOx）为NOx脱除率，%；Cin（NO）为反应前所配置模拟烟气中NO的初始体积分数，10–6；Cout（NO）、Cout（NO2）分别为反应后采集烟气中NO、NO2的体积分数，10–6。
1.2.2　CO2回收率η（CO2）
CO2回收率η（CO2）的计算以工艺前、后烟气和液态产品中关键组分的质量流量为基准：
η(CO2)=Qm,in(CO2)Qm,out(CO2)
式中：η（CO2）为CO2回收率，%；Qm，in（CO2）为初始烟气中CO2的质量流量，t/h；Qm，out（CO2）为液体CO2产品的质量流量，t/h。
1.2.3　CO2单位能耗E（CO2）
CO2单位能耗E（CO2）的计算公式为：
E(CO2)=EQm,out(CO2)
式中：E为系统总能耗，kW，包括烟气压缩能耗、液化提纯系统压缩能耗及制冷机组能耗。
1.3　模型建立及验证
天然气富氧燃烧烟气在除尘后经干燥冷却直接进入压缩净化协同脱碳脱硝系统，最后得到满足工艺要求的液化CO2。烟气压缩净化协同脱碳脱硝模型（图1）主要包含污染物压缩净化及CO2提纯2个单元。鉴于污染物脱除单元与CO2提纯单元的模拟侧重点不同，本文采用分区建模策略。其中，污染物脱除单元侧重于高压反应过程的精确计算，其模拟聚焦于气相及气-液相化学平衡的预测；而CO2压缩纯化单元则着重于工艺模块配置及其物理变化过程的模拟。此独立建模框架旨在确保各单元模拟精度，进而实现系统整体运行效率的优化。
1.3.1　压缩净化单元模型
污染物净化工艺流程示意如图2所示。模型使用FSplit模块对烟气进行除水处理，之后使用MCompr模块模拟多级压缩机对烟气进行加压，设置级间冷却对压缩后气体进行降温，之后将烟气通入填料塔模块进行污染物的脱除模拟，填料塔的模拟使用Radfrac模块。酸水的分离使用FSplit模块进行模拟，循环酸水重新泵入塔内由Pump模块进行模拟。
针对天然气富氧燃烧烟气组分中的“无硫无汞”特点构建对应的NOx脱除机理，如表2所示。
模型验证采用Callide Oxyfuel Project[25]在脱除SO2后的烟气组分，即烟气经过LP Scrubber脱硫工艺后的组分，此时烟气中SO2体积分数<10–6，符合天然气富氧燃烧后产生的无硫烟气组分情况。模拟结果（表3）与项目结果绝对误差<1%，可以认为该特定机理可用于脱硝单元的模拟。
1.3.2　CO2提纯单元模型
CO2提纯部分采用自产冷量闪蒸分离工艺，如图3所示：烟气经填料塔上端出来后直接脱水，经多流股换热器1冷却；然后通过闪蒸罐进行2次绝热节流膨胀，闪蒸罐1、2的底部液相产物混合在一起，在一定温度、压力下形成高纯度CO2流；高纯度CO2流经过多级压缩机被压缩至8 MPa，最后经氨冰机冷却液化，最终得到高纯度CO2产品。
针对CO2提纯单元，根据文献[26]的烟气条件，基于建立的流程模型对CO2液化提纯过程进行模拟，得到CO2回收率和纯度分别为91.77%、96.58%，与文献[26]结果（92.00%、96.61%）的绝对误差均小于1%，表明该模型可用于压缩纯化单元的模拟。
2　结果与讨论
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2.1　不同烟气循环方案CO2提纯工艺性能分析
将采用不同烟气循环方案得到的烟气成分及相关参数作为系统输入烟气，计算CO2回收率、CO2纯度、水耗及能耗等性能指标，结果如表4所示。其中液化能耗指制冷能耗和CO2产品压缩能耗，总能耗并未包括脱硝工艺的部分能耗。
由表4可知，不同工况下产品CO2纯度保持在96%左右，变化范围不大，当初始烟气CO2体积分数为82.4%（工况7）时，产品CO2纯度可达96.75%，此处产品纯度由闪蒸分离工艺决定，受初始烟气条件影响较小。工况1—工况3（初始烟气中CO2体积分数<35.0%）的CO2回收率较低（小于50%）。为避免CO2在液化提纯过程中凝固结冰从而对设备运行造成干扰，系统工艺规定流股温度不应低于CO2的三相点温度，即–56.55 ℃。初始烟气中CO2体积分数为22.0%（工况1）时，烟气中CO2分压过低，在规定温度条件下已经无法进行液化分离。
系统总能耗包括液化能耗与烟气压缩能耗，其随不同初始烟气中CO2体积分数的增加而减少；提高初始烟气中CO2体积分数，产品CO2纯度增加，系统制冷能耗减小，同时初始烟气总流量随CO2的富集逐渐减小，最终导致系统总能耗降低。工况2、工况3中，初始烟气总流量增大使得烟气压缩能耗较大，此时CO2产品的回收率较低，导致系统单位总能耗显著增加。
初始烟气中CO2体积分数对CO2提纯工艺产品CO2纯度、CO2回收率的影响如图4所示。
由图4可知：产品CO2的回收率和纯度均随初始烟气中CO2体积分数的增大而提高，但后者受初始烟气条件的影响并不明显，提高趋势缓慢；CO2回收率受初始烟气中CO2体积分数影响较为显著，当初始烟气中CO2体积分数为32%时，CO2回收率仅约36%，只有当初始烟气中CO2体积分数大于60%时，产品CO2的回收率才会保持80%以上。
2.2　压缩净化工艺影响因素研究
2.2.1　压力影响
在恒定其他操作参数条件下，压力对NOx脱除率的影响如图5所示。由图5可以看出，NOx脱除率随系统压力升高而明显提升：低压条件下NOx几乎未被脱除，而当压力增至2.8 MPa时，NOx脱除率可达94.89%，高于文献值89%。该差异主要源于本研究对压力敏感性的分析是建立在其余工艺参数均为最佳值的基础上。其次，针对燃煤富氧燃烧烟气压缩过程的硫氮（S/N）协同脱除研究[14]表明，气相中引入SO2会对NOx脱除产生抑制作用。在含1 000×10–6 SO2、2.0 MPa条件下，NOx脱除效率较无SO2条件降低了8.1%。此外，SO2与NO在液相中的反应产物之间存在相互作用亦可能导致N2O的生成[27]，进一步降低NOx脱除率。本研究基于天然气富氧燃烧产生的烟气开展压缩净化研究，在污染物脱除过程中无需考虑SO2的不利影响，因此最终模拟值中的NOx脱除率更高。
2.2.2　液气比影响
保持烟气流量不变，通过改变液气比（0.1~2.7 L/m3）研究给水量对NOx脱除率的影响，结果如图6所示。由图6可以看出，压力2.8 MPa工况下，在液气比为0.6~2.7 L/m3范围内，NOx脱除率达到最大值95.14%并保持稳定。此变化趋势与Laribi等人[22]关于液气比敏感性的研究结果基本吻合，均出现脱除率平台现象。然而，本研究观测到的最大NOx脱除率95.14%高于文献值88%，这主要源于实验装置（吸收塔尺寸）及操作条件（烟气流量）的不同，因此最大传质效率存在差异。此外，本文深入研究了较低液气比区间（特别是液气比小于1 L/m3）内的性能变化，结果发现，在该区间内适当增加给水量可有效提升NOx脱除率。其机理在于：在保持其他条件不变的前提下，增加水量显著稀释了液相中反应产物的浓度，而对气相初始反应物浓度影响甚微。该浓度变化等效于降低了生成物浓度，根据化学平衡移动原理，促使反应平衡向正方向移动，从而提高了NOx脱除率。针对较低液气比范围的研究对降低工业应用中的运行水耗及提升工艺流程整体经济性具有更重要的指导意义。
2.2.3　初始O2体积分数影响
通过改变烟气组分中的初始O2体积分数（1%~10%），研究O2体积分数变化对NOx脱除率的影响，结果如图7所示。由图7可知，总体上，O2体积分数升高会促进NOx的脱除，但该作用大多集中在O2体积分数从1%上升至5%的过程中，当O2体积分数继续增大时，其对污染物脱除的影响逐渐减弱。不同于其他影响因素，烟气中SO2的存在对初始O2体积分数影响NO氧化的效应较弱，这与文献[13]中含SO₂条件下的脱除趋势一致。其机理在于：O2体积分数变化主要调控NO的氧化环节，而SO2的脱除以吸收过程（物理/化学溶解）为主，受氧化过程影响较小，故O2体积分数波动对SO2脱除效率的影响有限。模拟结果表明，在烟气经降温脱水后，维持富CO2环境中约5%的O₂体积分数可有效促进NO氧化反应，从而实现较高的脱硝效率。
2.2.4　停留时间影响
停留时间通过蒸汽持留体积与气体体积流量的比值计算得出。通过调节烟气流量探究停留时间对NOx脱除率的影响规律，结果如图8所示。
由图8可见，NOx脱除率对停留时间呈现高度敏感性，其值随停留时间增加显著提升。分析表明，延长停留时间为气相中NO与O2的反应以及液相中NO2、O2和H2O之间的复杂反应提供了更充分的时间，增加了活性组分的有效接触时长[25]，从而显著提升了化学吸收效率。值得注意的是，实际工业应用中调节停留时间常通过改变气体流量实现，这与单纯改变反应器尺寸的实验室方法存在差异。过高的烟气流量导致停留时间过短，吸收效果不佳；而过度延长停留时间虽提升NOx脱除率，却会降低设备单位时间的污染物处理能力。因此，在工程设计与运行中，需在经济性与脱除效果之间寻求最优平衡点，以实现系统的最佳运行状态。
2.3　CO2提纯工艺影响因素研究
对CO2提纯工艺进行了模拟，发现进气压力、二级闪蒸温度是影响CO2产品纯度及回收率的主要因素，二级闪蒸温度决定了提纯工艺CO2的回收率。
2.3.1　进气压力影响
考虑不同进气压力对产品CO2的回收率及纯度的影响，结果如图9所示。随着进气压力的增大，回收率提高，但产品的纯度下降，这是由于进气压力增加使得杂质气体冷凝。当压力增加到2.8 MPa时，CO2的回收率为96.5%，纯度可达97.0%，自产冷量闪蒸工艺脱碳性能良好。高浓度CO2提纯所需的冷量由高压节流获得，提纯工艺采用两级闪蒸实现分离，工艺能耗较低，但是受闪蒸分离限制，产品纯度无法再进一步提高[10]。
2.3.2　闪蒸温度影响
在烟气进气压力2.8 MPa的条件下，分析一级闪蒸温度、二级闪蒸温度对产品CO2纯度、回收率的影响，结果如图10及图11所示。由图10可以看出：随闪蒸温度降低，产品CO2回收率提高，但纯度降低；自产冷量闪蒸分离工艺CO2回收率主要受二级闪蒸温度的影响，而CO2纯度受限于分离工艺，一级闪蒸温度和二级闪蒸温度对其影响并不显著。CO2的三相点温度为–56.6 ℃，二级闪蒸罐的液相产物需要在节流降温后作为冷却介质为换热器提供冷量，在避免管道CO2发生凝固堵塞的前提下，应尽可能降低二级闪蒸温度以提高产物回收率，此处二级闪蒸温度设置为–54 ℃。
3　结论
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1）CO2回收率对烟气中初始CO2体积分数具有显著依赖性。在满足CO2体积分数边界条件（≥60%）的前提下，CO2提纯工艺可实现≥80%的产品回收率，且每提纯1吨CO2的能耗维持在较低水平（120.1~ 152.3 kW·h）。值得注意的是，富氧燃烧后天然气高CO2含量的特性能够有效满足该体积分数边界要求。
2）系统压力是关联NOx脱除效率与CO2提纯性能的核心工艺参数。在压力为2.8 MPa的条件下，可在实现NOx脱除率>94%的同时满足最终产品CO2纯度≥95%、CO2回收率≥80%的要求。
3）该工艺的创新性在于：利用烟气压缩净化环节产生的高压烟气直接进入后续CO2提纯单元，显著降低了CO2提纯过程的压缩能耗。这种一体化设计不仅实现了NOx的高效脱除，更避免了传统分步工艺中重复压缩的能量损失，从而大幅降低了整体运行成本，在发电行业极具应用潜力。
基金
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  • 国家自然科学基金项目(51806076)
文献
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doi: 10.19666/j.rlfd.202505085
  • 接收时间：2025-05-14
  • 首发时间：2026-08-14
  • 出版时间：2026-03-25
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出版历史
  • 收稿日期：2025-05-14
  • 修回日期：2025-06-18
  • 录用日期：2025-06-23
基金
National Natural Science Foundation of China(51806076)
国家自然科学基金项目(51806076)
作者信息
    华中科技大学煤燃烧与低碳利用全国重点实验室，湖北 武汉 430074

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李小姗（1990），女，博士，副教授，主要研究方向碳捕集与污染物控制技术，。
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2种不同金属材料的力学参数
科
Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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