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Article(id=1295068442940428796, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295068190569164906, articleNumber=null, orderNo=null, doi=10.19666/j.rlfd.202510025, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1760457600000, receivedDateStr=2025-10-15, revisedDate=1764691200000, revisedDateStr=2025-12-03, acceptedDate=1765468800000, acceptedDateStr=2025-12-12, onlineDate=1786697978004, onlineDateStr=2026-08-14, pubDate=1782316800000, pubDateStr=2026-06-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1786697978004, onlineIssueDateStr=2026-08-14, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1786697978004, creator=13701087609, updateTime=1786697978004, updator=13701087609, issue=Issue{id=1295068190569164906, tenantId=1146029695717560320, journalId=1210938733613449225, year='2026', volume='55', issue='6', pageStart='1', pageEnd='192', issueExtLink='null', onlineDate='null', pubDate='1782316800000', pubDateStr='2026-06-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=1, specialIssue=null, createTime=1786697917835, creator='13701087609', updateTime=1786698816898, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1295071961596584952, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295068190569164906, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1295071961596584953, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1295068190569164906, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=175, endPage=183, ext={EN=ArticleExt(id=1295068443154338301, articleId=1295068442940428796, tenantId=1146029695717560320, journalId=1210938733613449225, language=EN, title=Experimental study on low-temperature oxidation and adsorption of pollutants in coal-fired flue gas, columnId=1211002405299294959, journalTitle=Thermal Power Generation, columnName=Thermal energy science research, runingTitle=null, highlight=null, articleAbstract=
[Objective]

The low-temperature (–20~ –40 ℃) oxidation adsorption of multiple pollutants from coal-fired flue gas onto activated carbons enables their integrated removal, which has promising application prospect and environmental benefits.

[Methods]

This article studied the adsorption processes of NO and SO2 by four activated carbons (graded-pore activated carbon, coal-based activated carbon, and two coconut shell-based activated carbons) in inert atmosphere and simulated flue gas under low temperature conditions of –20 ℃.

[Results]

The experimental results showed that in an inert atmosphere, the adsorption performance of the four activated carbons for NO was weak, with a saturated nitrogen capacity of less than 0.07 mg/g, and the saturated sulfur capacity for adsorbing SO2 was 31.70~57.07 mg/g. In simulated flue gas conditions, the presence of O2 increased the saturated nitrogen capacity of activated carbons by three orders of magnitude and the saturated sulfur capacity by 2~5 times. The optimal coconut shell activated carbon-2 had a saturated nitrogen capacity of 175.70 mg/g and a saturated sulfur capacity of 320.65 mg/g. Density functional theory (DFT) calculations show that the adsorption binding energies of NO, SO2, and their oxides on the zigzag edge carbon model follow the order of NO2> SO3> SO2> NO. After NO and SO2 are oxidized by O2 into NO2 and SO3, their adsorption on activated carbon surfaces is significantly enhanced.

[Conclusion]

The research results can provide an important theoretical basis for the integrated adsorption and removal of NO and SO2 in coal-fired flue gas under low temperature conditions.

, authors=Yisheng MAO, Huafeng YE, authorsList=Yisheng MAO, Huafeng YE, authorCompany=null, correspAuthors=null, 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=1295068446216180239, articleId=1295068442940428796, tenantId=1146029695717560320, journalId=1210938733613449225, language=CN, title=燃煤烟气污染物低温氧化吸附实验研究, columnId=1211002405437706993, journalTitle=热力发电, columnName=热能科学研究, runingTitle=null, highlight=null, articleAbstract=
【目的】

燃煤烟气多污染物在活性炭上的低温（–20~–40 ℃）氧化吸附可实现其一体化脱除，具有良好的应用前景和环境效益。

【方法】

在–20 ℃的低温条件下，分别研究了惰性气氛和模拟烟气中分级孔活性炭、煤基活性炭和2种椰壳活性炭对NO和SO2的吸附过程。

【结果】

实验结果表明，惰性气氛下，4种活性炭对NO的吸附性能较弱，饱和氮容低于0.07 mg/g；吸附SO2的饱和硫容为31.70~57.07 mg/g。在模拟烟气条件下，O2的氧化作用使得活性炭的饱和氮容提高了3个数量级，饱和硫容提高了2~5倍，性能最优的椰壳活性炭–2的饱和氮容可达175.70 mg/g，饱和硫容可达320.65 mg/g。DFT计算表明，锯齿形边缘炭模型上NO、SO2及其氧化物的吸附结合能遵循NO2> SO3> SO2>NO的顺序，表明NO和SO2被氧化为NO2和SO3后，其在活性炭表面的吸附能力得到显著增强。

【结论】

研究结果可为低温条件下燃煤烟气中NO和SO2的一体化吸附脱除提供重要的理论依据。

, authors=毛奕升, 叶华锋, authorsList=毛奕升, 叶华锋, authorCompany=null, correspAuthors=null, authorNote=

毛奕升（1985），男，高级工程师，主要从事火力发电厂生产运行、检修管理工作，。

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毛奕升（1985），男，高级工程师，主要从事火力发电厂生产运行、检修管理工作，。

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毛奕升（1985），男，高级工程师，主要从事火力发电厂生产运行、检修管理工作，。

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Carbon, 2017, 115: 409-421., articleTitle=Carbon sponge-type nanostructures based on coaxial nitrogen-doped multi-walled carbon nanotubes grown by CVD using benzylamine as precursor, refAbstract=null), Reference(id=1295068454982275669, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2022, volume=32, issue=5, pageStart=null, pageEnd=null, url=null, language=null, rfNumber=[15], rfOrder=14, authorNames=MAHATO M, NAM S, TABASSIAN R, journalName=Advanced Functional Materials, refType=null, unstructuredReference=MAHATO M, NAM S, TABASSIAN R, et al. Electronically conjugated multifunctional covalent triazine framework for unprecedented CO2 selectivity and high-power flexible supercapacitor[J]. Advanced Functional Materials, 2022, 32(5): 2107442., articleTitle=Electronically conjugated multifunctional covalent triazine framework for unprecedented CO2 selectivity and high-power flexible supercapacitor, refAbstract=null), Reference(id=1295068455057773142, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2008, volume=83, issue=1/2, pageStart=63, pageEnd=71, url=null, language=null, rfNumber=[16], rfOrder=15, authorNames=ZHANG W J, RABIEI S, BAGREEV A, journalName=Applied Catalysis B: Environmental, refType=null, unstructuredReference=ZHANG W J, RABIEI S, BAGREEV A, et al. Study of NO adsorption on activated carbons[J]. Applied Catalysis B: Environmental, 2008, 83(1/2): 63-71., articleTitle=Study of NO adsorption on activated carbons, refAbstract=null), Reference(id=1295068455124882007, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2015, volume=163, issue=null, pageStart=573, pageEnd=583, url=null, language=null, rfNumber=[17], rfOrder=16, authorNames=ZHANG Z Q, ATKINSON J D, JIANG B Q, journalName=Applied Catalysis B: Environmental, refType=null, unstructuredReference=ZHANG Z Q, ATKINSON J D, JIANG B Q, et al. NO oxidation by microporous zeolites: Isolating the impact of pore structure to predict NO conversion[J]. Applied Catalysis B: Environmental, 2015, 163: 573-583., articleTitle=NO oxidation by microporous zeolites: Isolating the impact of pore structure to predict NO conversion, refAbstract=null), Reference(id=1295068455191990872, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2022, volume=335, issue=null, pageStart=null, pageEnd=null, url=null, language=null, rfNumber=[18], rfOrder=17, authorNames=QU Z B, SUN F, PI X X, journalName=Journal of Cleaner Production, refType=null, unstructuredReference=QU Z B, SUN F, PI X X, et al. One-step synergistic optimization of hierarchical pore topology and nitrogen dopants in activated coke for efficient catalytic oxidation of nitric oxide[J]. Journal of Cleaner Production, 2022, 335: 130360., articleTitle=One-step synergistic optimization of hierarchical pore topology and nitrogen dopants in activated coke for efficient catalytic oxidation of nitric oxide, refAbstract=null), Reference(id=1295068455259099737, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2016, volume=369, issue=null, pageStart=552, pageEnd=557, url=null, language=null, rfNumber=[19], rfOrder=18, authorNames=LIU X, SUN F, QU Z B, journalName=Applied Surface Science, refType=null, unstructuredReference=LIU X, SUN F, QU Z B, et al. The effect of functional groups on the SO2 adsorption on carbon surface I: a new insight into noncovalent interaction between SO2 molecule and acidic oxygen-containing groups[J]. Applied Surface Science, 2016, 369: 552-557., articleTitle=The effect of functional groups on the SO2 adsorption on carbon surface I: a new insight into noncovalent interaction between SO2 molecule and acidic oxygen-containing groups, refAbstract=null), Reference(id=1295068455326208602, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, doi=null, pmid=null, pmcid=null, year=2019, volume=9, issue=16, pageStart=4327, pageEnd=4338, url=null, language=null, rfNumber=[20], rfOrder=19, authorNames=QU Z B, SUN F, GAO J H, journalName=Catalysis Science & Technology, refType=null, unstructuredReference=QU Z B, SUN F, GAO J H, et al. A new insight into SO2 low-temperature catalytic oxidation in porous carbon materials: non-dissociated O2 molecule as oxidant[J]. Catalysis Science & Technology, 2019, 9(16): 4327-4338., articleTitle=A new insight into SO2 low-temperature catalytic oxidation in porous carbon materials: non-dissociated O2 molecule as oxidant, refAbstract=null)], funds=[Fund(id=1295068451828159045, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, awardId=2022YFB4100203, language=EN, fundingSource=National Key Research and Development Program(2022YFB4100203), fundOrder=null, country=null), Fund(id=1295068451933016646, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, awardId=2022YFB4100203, language=CN, fundingSource=国家重点研发计划项目(2022YFB4100203), fundOrder=null, country=null)], companyList=[AuthorCompany(id=1295068446421701136, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, xref=null, ext=[AuthorCompanyExt(id=1295068446430089745, tenantId=1146029695717560320, journalId=1210938733613449225, 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articleId=1295068442940428796, language=CN, label=图1, caption=锯齿形边缘炭模型（Zig）和NO、NO2、SO2、SO3模型, figureFileSmall=+J0+j78O6qZpSNBCJvVUkw==, figureFileBig=nLi0R9nwA21iSmec4LhDEQ==, tableContent=null), ArticleFig(id=1295068448225251881, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.2, caption=XPS spectra and fitting results of C1s and O1s peaks of four activated carbons, figureFileSmall=71YecL+NVQd+U41EeaRA4g==, figureFileBig=L59c/VHodWvnIecjGWmn/g==, tableContent=null), ArticleFig(id=1295068448283972138, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图2, caption=4种活性炭的XPS谱图及C1s峰和O1s峰拟合结果, figureFileSmall=71YecL+NVQd+U41EeaRA4g==, figureFileBig=L59c/VHodWvnIecjGWmn/g==, tableContent=null), ArticleFig(id=1295068448342692395, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.3, caption=N2 adsorption-desorption isotherms and pore size distributions of the four activated carbons, figureFileSmall=uxztRuepdQIIESW26axBMA==, figureFileBig=VBaLFTB4HhyWsxvNfCueHg==, tableContent=null), ArticleFig(id=1295068448409801260, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图3, caption=4种活性炭的N2吸附-解吸等温线和孔径分布, figureFileSmall=uxztRuepdQIIESW26axBMA==, figureFileBig=VBaLFTB4HhyWsxvNfCueHg==, tableContent=null), ArticleFig(id=1295068448481104429, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.4, caption=NO removal rate of coconut shell activated carbon under inert atmosphere, figureFileSmall=cdc3aSQgBxQ3K6FIRZRb4g==, figureFileBig=jNYA5jE5NxJLJoQa6vKfkg==, tableContent=null), ArticleFig(id=1295068448556601902, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图4, caption=惰性气氛下椰壳活性炭的NO脱除率, figureFileSmall=cdc3aSQgBxQ3K6FIRZRb4g==, figureFileBig=jNYA5jE5NxJLJoQa6vKfkg==, tableContent=null), ArticleFig(id=1295068448623710767, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.5, caption=NO removal rates of coconut shell activated carbons under simulated flue gas conditions, figureFileSmall=posSmWsKvMhF3oC4Wn8Z2w==, figureFileBig=UCMNGNrDZ8BYgpuQcLyZEw==, tableContent=null), ArticleFig(id=1295068448690819632, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图5, caption=模拟烟气条件下椰壳活性炭的NO脱除率, figureFileSmall=posSmWsKvMhF3oC4Wn8Z2w==, figureFileBig=UCMNGNrDZ8BYgpuQcLyZEw==, tableContent=null), ArticleFig(id=1295068450330792497, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.6, caption=SO2 removal rates of four types of activated carbons in inert atmosphere, figureFileSmall=iv4pbPKyBucTGFyW4j2Bpw==, figureFileBig=/TuL8tXX7Vil/kiCcd4UBg==, tableContent=null), ArticleFig(id=1295068450406289970, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图6, caption=惰性气氛下4种活性炭的SO2脱除率, figureFileSmall=iv4pbPKyBucTGFyW4j2Bpw==, figureFileBig=/TuL8tXX7Vil/kiCcd4UBg==, tableContent=null), ArticleFig(id=1295068450473398835, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.7, caption=SO2 removal rates of four types of activated carbons under simulated flue gas conditions, figureFileSmall=Z2HbuMXzoqydIrEn98gq0Q==, figureFileBig=XIc8wFuHDnfemlta8sfgkA==, tableContent=null), ArticleFig(id=1295068450544702004, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图7, caption=模拟烟气条件下4种活性炭的SO2脱除率, figureFileSmall=Z2HbuMXzoqydIrEn98gq0Q==, figureFileBig=XIc8wFuHDnfemlta8sfgkA==, tableContent=null), ArticleFig(id=1295068450620199477, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Fig.8, caption=Adsorption energies and configurations of NO, NO2, SO2, and SO3 on the Zig model, figureFileSmall=efdLs4s/9vC/iJsK0El+zw==, figureFileBig=clkW37YLvO+O/4TrvxT9bQ==, tableContent=null), ArticleFig(id=1295068450695696950, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=图8, caption=Zig模型上NO、NO2、SO2和SO3的吸附能和吸附构型, figureFileSmall=efdLs4s/9vC/iJsK0El+zw==, figureFileBig=clkW37YLvO+O/4TrvxT9bQ==, tableContent=null), ArticleFig(id=1295068450767000119, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.1, caption=

Experimental instruments and equipment

, figureFileSmall=null, figureFileBig=null, tableContent=
仪器名称生产厂家型号
水平管式炉合肥科晶有限公司OTF-1200X
低温反应釜上海力辰邦西仪器科技有限公司LC-DFY-30/40
电子天平梅特勒托利多集团公司XS105
电热鼓风干燥箱力辰科技有限公司GZX-9070 MBE
比表面积及微孔分析仪贝士德仪器科技有限公司BSD-660M
X射线衍射仪日本岛津有限公司Thermo Scientific K-Alpha
在线质谱分析仪英国TILON公司LC-D200M
), ArticleFig(id=1295068450825720376, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表1, caption=

实验仪器与设备

, figureFileSmall=null, figureFileBig=null, tableContent=
仪器名称生产厂家型号
水平管式炉合肥科晶有限公司OTF-1200X
低温反应釜上海力辰邦西仪器科技有限公司LC-DFY-30/40
电子天平梅特勒托利多集团公司XS105
电热鼓风干燥箱力辰科技有限公司GZX-9070 MBE
比表面积及微孔分析仪贝士德仪器科技有限公司BSD-660M
X射线衍射仪日本岛津有限公司Thermo Scientific K-Alpha
在线质谱分析仪英国TILON公司LC-D200M
), ArticleFig(id=1295068450892829241, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.2, caption=

Surface composition of the samples based on XPS test results

, figureFileSmall=null, figureFileBig=null, tableContent=
样品元素含量含氧官能团含量
CONO/CC−OC=O−COOH
分级孔活性炭84.2114.051.7416.687.073.623.36
煤基活性炭85.5112.591.9014.720.794.807.00
椰壳活性炭-176.5422.201.2629.003.917.4910.80
椰壳活性炭-287.7210.681.6012.183.325.122.24
), ArticleFig(id=1295068450955743802, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表2, caption=

基于XPS 测试结果获得的样品表面成分

, figureFileSmall=null, figureFileBig=null, tableContent=
样品元素含量含氧官能团含量
CONO/CC−OC=O−COOH
分级孔活性炭84.2114.051.7416.687.073.623.36
煤基活性炭85.5112.591.9014.720.794.807.00
椰壳活性炭-176.5422.201.2629.003.917.4910.80
椰壳活性炭-287.7210.681.6012.183.325.122.24
), ArticleFig(id=1295068451035435579, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.3, caption=

Porosity and surface parameters of the samples

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2·g–1）微孔比表面积/（m2·g–1）介孔比表面积/（m2·g–1）孔容/（cm3·g–1）微孔孔容/（cm3·g–1）平均孔径/nm
分级孔活性炭362.67302.5860.080.190.122.12
煤基活性炭467.86328.85131.550.350.143.30
椰壳活性炭-1856.61787.2669.340.390.321.84
椰壳活性炭-21 002.54978.623.930.410.391.63
), ArticleFig(id=1295068451094155836, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表3, caption=

样品的孔隙和表面参数

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2·g–1）微孔比表面积/（m2·g–1）介孔比表面积/（m2·g–1）孔容/（cm3·g–1）微孔孔容/（cm3·g–1）平均孔径/nm
分级孔活性炭362.67302.5860.080.190.122.12
煤基活性炭467.86328.85131.550.350.143.30
椰壳活性炭-1856.61787.2669.340.390.321.84
椰壳活性炭-21 002.54978.623.930.410.391.63
), ArticleFig(id=1295068451165459005, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.4, caption=

Low-temperature adsorption nitrogen capacity of four activated carbons in an inert atmosphere

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2∙g–1）微孔比表面积/（m2∙g−1）饱和时间/min饱和氮容/（mg∙g−1）
分级孔活性炭362.67302.58≈0
煤基活性炭467.86328.85≈0
椰壳活性炭-1856.61787.261.450.02
椰壳活性炭-21 002.54978.605.350.07
), ArticleFig(id=1295068451232567870, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表4, caption=

惰性气氛下4种活性炭的低温吸附氮容

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2∙g–1）微孔比表面积/（m2∙g−1）饱和时间/min饱和氮容/（mg∙g−1）
分级孔活性炭362.67302.58≈0
煤基活性炭467.86328.85≈0
椰壳活性炭-1856.61787.261.450.02
椰壳活性炭-21 002.54978.605.350.07
), ArticleFig(id=1295068451303871039, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.5, caption=

Low-temperature adsorption nitrogen capacities of four activated carbons under simulated flue gas conditions

, figureFileSmall=null, figureFileBig=null, tableContent=
样品穿透时间/min穿透氮容/（mg∙g–1）饱和时间/min饱和氮容/（mg∙g–1）
分级孔活性炭3815.585023.27
煤基活性炭5623.077333.91
椰壳活性炭-17831.7411850.05
椰壳活性炭-2284154.12358175.70
), ArticleFig(id=1295068451379368512, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表5, caption=

模拟烟气条件下4种活性炭的低温吸附氮容

, figureFileSmall=null, figureFileBig=null, tableContent=
样品穿透时间/min穿透氮容/（mg∙g–1）饱和时间/min饱和氮容/（mg∙g–1）
分级孔活性炭3815.585023.27
煤基活性炭5623.077333.91
椰壳活性炭-17831.7411850.05
椰壳活性炭-2284154.12358175.70
), ArticleFig(id=1295068451521974849, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.6, caption=

Low-temperature sulfur adsorption capacities of four types of activated carbons in inert atmosphere

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2∙g–1）微孔比表面积/（m2∙g–1）穿透时间/min穿透硫容/（mg∙g–1）饱和时间/min饱和硫容/（mg∙g–1）
分级孔活性炭362.67302.58931.70
煤基活性炭467.86328.8529.741133.57
椰壳活性炭-1856.61787.26313.061234.12
椰壳活性炭-21 002.54978.60318.431557.07
), ArticleFig(id=1295068451580695106, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=CN, label=表6, caption=

惰性气氛下4种活性炭的低温吸附硫容

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2∙g–1）微孔比表面积/（m2∙g–1）穿透时间/min穿透硫容/（mg∙g–1）饱和时间/min饱和硫容/（mg∙g–1）
分级孔活性炭362.67302.58931.70
煤基活性炭467.86328.8529.741133.57
椰壳活性炭-1856.61787.26313.061234.12
椰壳活性炭-21 002.54978.60318.431557.07
), ArticleFig(id=1295068451656192579, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1295068442940428796, language=EN, label=Tab.7, caption=

Low-temperature sulfur adsorption capacities of four types of activated carbons under simulated flue gas conditions

, figureFileSmall=null, figureFileBig=null, tableContent=
样品比表面积/（m2∙g–1）穿透时间/min穿透硫容/（mg∙g–1）饱和时间/min饱和硫容/（mg∙g–1）
分级孔活性炭362.67836.352271.62
煤基活性炭467.861465.562589.05
椰壳活性炭-1856.611360.322897.71
椰壳活性炭-21 002.5443204.3083320.65
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模拟烟气条件下4种活性炭的低温吸附硫容

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样品比表面积/（m2∙g–1）穿透时间/min穿透硫容/（mg∙g–1）饱和时间/min饱和硫容/（mg∙g–1）
分级孔活性炭362.67836.352271.62
煤基活性炭467.861465.562589.05
椰壳活性炭-1856.611360.322897.71
椰壳活性炭-21 002.5443204.3083320.65
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燃煤烟气污染物低温氧化吸附实验研究
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毛奕升 , 叶华锋
热力发电 | 热能科学研究 2026,55(6): 175-183
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热力发电 |热能科学研究 2026 , 55 (6) : 175 -183
燃煤烟气污染物低温氧化吸附实验研究
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毛奕升（1985），男，高级工程师，主要从事火力发电厂生产运行、检修管理工作，。

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毛奕升 , 叶华锋
作者信息
  • 广东电力发展股份有限公司，广东 广州 510000
作者简介:

毛奕升（1985），男，高级工程师，主要从事火力发电厂生产运行、检修管理工作，。

Experimental study on low-temperature oxidation and adsorption of pollutants in coal-fired flue gas
Yisheng MAO , Huafeng YE
Affiliations
  • Guangdong Electric Power Development Co., Ltd., Guangzhou 510000, China
出版时间: 2026-06-25 doi: 10.19666/j.rlfd.202510025
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摘要
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【目的】

燃煤烟气多污染物在活性炭上的低温（–20~–40 ℃）氧化吸附可实现其一体化脱除，具有良好的应用前景和环境效益。

【方法】

在–20 ℃的低温条件下，分别研究了惰性气氛和模拟烟气中分级孔活性炭、煤基活性炭和2种椰壳活性炭对NO和SO2的吸附过程。

【结果】

实验结果表明，惰性气氛下，4种活性炭对NO的吸附性能较弱，饱和氮容低于0.07 mg/g；吸附SO2的饱和硫容为31.70~57.07 mg/g。在模拟烟气条件下，O2的氧化作用使得活性炭的饱和氮容提高了3个数量级，饱和硫容提高了2~5倍，性能最优的椰壳活性炭–2的饱和氮容可达175.70 mg/g，饱和硫容可达320.65 mg/g。DFT计算表明，锯齿形边缘炭模型上NO、SO2及其氧化物的吸附结合能遵循NO2> SO3> SO2>NO的顺序，表明NO和SO2被氧化为NO2和SO3后，其在活性炭表面的吸附能力得到显著增强。

【结论】

研究结果可为低温条件下燃煤烟气中NO和SO2的一体化吸附脱除提供重要的理论依据。

活性炭  /  低温吸附  /  饱和氮容  /  饱和硫容  /  密度泛函理论
[Objective]

The low-temperature (–20~ –40 ℃) oxidation adsorption of multiple pollutants from coal-fired flue gas onto activated carbons enables their integrated removal, which has promising application prospect and environmental benefits.

[Methods]

This article studied the adsorption processes of NO and SO2 by four activated carbons (graded-pore activated carbon, coal-based activated carbon, and two coconut shell-based activated carbons) in inert atmosphere and simulated flue gas under low temperature conditions of –20 ℃.

[Results]

The experimental results showed that in an inert atmosphere, the adsorption performance of the four activated carbons for NO was weak, with a saturated nitrogen capacity of less than 0.07 mg/g, and the saturated sulfur capacity for adsorbing SO2 was 31.70~57.07 mg/g. In simulated flue gas conditions, the presence of O2 increased the saturated nitrogen capacity of activated carbons by three orders of magnitude and the saturated sulfur capacity by 2~5 times. The optimal coconut shell activated carbon-2 had a saturated nitrogen capacity of 175.70 mg/g and a saturated sulfur capacity of 320.65 mg/g. Density functional theory (DFT) calculations show that the adsorption binding energies of NO, SO2, and their oxides on the zigzag edge carbon model follow the order of NO2> SO3> SO2> NO. After NO and SO2 are oxidized by O2 into NO2 and SO3, their adsorption on activated carbon surfaces is significantly enhanced.

[Conclusion]

The research results can provide an important theoretical basis for the integrated adsorption and removal of NO and SO2 in coal-fired flue gas under low temperature conditions.

activated carbon  /  low-temperature adsorption  /  saturated nitrogen capacity  /  saturated sulfur capacity  /  density functional theory
毛奕升, 叶华锋. 燃煤烟气污染物低温氧化吸附实验研究. 热力发电, 2026 , 55 (6) : 175 -183 . DOI: 10.19666/j.rlfd.202510025
Yisheng MAO, Huafeng YE. Experimental study on low-temperature oxidation and adsorption of pollutants in coal-fired flue gas[J]. Thermal Power Generation, 2026 , 55 (6) : 175 -183 . DOI: 10.19666/j.rlfd.202510025
正文
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SO2和NO是常见的大气污染物，会引发呼吸道、心肺等相关疾病，也会对环境造成极大的危害[1]。为减少NO和SO2的排放，我国已经开展了多种技术路径探索。相较于常规技术，燃煤污染物低温（–20~–40 ℃）深度一体化脱除技术（COAP技术）可协同氧化吸附脱除多污染物，其核心工艺流程为：烟气除尘后经冷却塔冷却至目标低温，进入净化塔协同氧化吸附去除SO2、NOx、SO3、卤化物、Hg及其他重金属、二噁英、VOCs等污染物，以近零排放标准排放；脱除物经回收净化后可资源化利用。该技术无需石灰石、尿素及脱硝催化剂，无脱硫废水、氨逃逸等二次污染，还能回收硫与烟气水分，兼具应用前景与经济环保效益[2]，而高效低温吸附剂的研发是实现该技术的关键。
目前，碳基吸附剂[3]、金属基吸附剂[4]等的应用已获得广泛关注和研究[5]。金属基吸附剂成本较高、工作温度范围窄以及可回收性差等问题，限制了其在实际生产中的应用[4]。碳基吸附剂不仅成本低、可回收性良好，还具有物化特性稳定、表面官能团丰富、孔隙结构发达等特点，使得气体污染物更容易在碳表面被吸附[6]。其中活性炭制备工艺简单、成本低廉，是一种非常有潜力的吸附材料[7-8]，但关于其在不高于−20 ℃的低温下对NO和SO2的吸附特性及关键影响机制研究较少。
本研究以典型的煤基活性炭和椰壳活性炭为研究对象，通过−20 ℃下的低温吸附实验分别探索了惰性气氛和模拟烟气中4种活性炭对NO和SO2的吸附性能，进一步结合密度泛函理论（DFT）计算，阐释了O2对NO和SO2低温吸附特性的影响机制。
1　实验方法
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1.1　仪器与设备
实验采用的主要仪器和设备如表1所示。
1.2　活性炭制备
1）分级孔活性炭　将一定量低阶原煤颗粒放置到水平管式炉中，在N2保护下以10 ℃/min的升温速率升至750 ℃后，将气体切换至水蒸气，通入流速为100 mL/min，恒温2 h后在N2气氛中冷却至室温。
2）煤基活性炭　将一定量烟煤大颗粒放置到水平管式炉中，在N2保护下以10 ℃/min的速率升温至500 ℃后恒温1 h进行碳化；进一步以10 ℃/min的速率升温至750 ℃，并将部分惰性气体切换至100 mL/min的水蒸气，恒温2 h后在N2气氛中冷却至室温。
3）椰壳活性炭　将一定量椰壳颗粒放置到水平管式炉中，在400 mL/min的N2气氛下以1.5 ℃/min的升温速率升至650 ℃碳化1 h。再以1.5 ℃/min的升温速率升至750 ℃后，将气体切换至水蒸气，通入流速为100 mL/min，恒温2 h后在N2气氛中冷却至室温。根据所用椰壳原料的差异，将获得了椰壳活性炭-1和椰壳活性炭-2 2种材料。
1.3　活性炭表征
1）氮气等温吸附/脱附曲线　使用BSD-660M高性能比表面积及微孔分析仪分析样品的孔结构特征。首先将样品经300 ℃加热真空脱气，去除表面吸附的水、油等杂质；随后在液氮环境中测量不同分压下N2的吸附和脱附量，获得氮气等温吸附/脱附数据；最后采用Brunauer-Emmett-Teller（BET）方程、t-plot方法、Horvath-Kawazoe方法和非局部密度函数理论，计算碳材料的比表面积、微孔面积、微孔体积、介孔面积、介孔体积和孔径分布。
2）X射线光电子能谱（XPS）　采用XPS（Thermo Scientific K-Alpha型光谱仪）分析样品的元素组成、半定量分析样品中C、O、N、P等元素的含量以及元素的存在形式。
1.4　活性炭低温吸附NO和SO2的性能测试
活性炭对NO和SO2的低温（−20 ℃）吸附脱除实验是在低温反应釜内进行。将一定量的活性炭放置在U型管（内径为20 mm）中的穿孔砂芯（≤10 μm）上，待环境温度降至−20 ℃后，将惰性Ar气流切换为携带NO和SO2的Ar气流（500 mL/min），从上至下流过2 mm高的炭层，并采用在线质谱分析仪（LC-D200M）实时监测出口的污染物气体浓度。在NO吸附实验中，NO体积分数为250 μL/L；在SO2吸附实验中，SO2体积分数为1 000 μL/L。
为探索实际烟气条件下活性炭对NO和SO2的吸附性能，进一步将6%CO2（体积分数，下同）和8%O2加入反应气，测试了活性炭分别对250 μL/L NO和1 000 μL/L SO2的低温吸附性能。记录出口的NO和SO2体积分数随时间的变化，通过式（1）和式（2）计算NO和SO2的脱除率η和低温吸附容量S。当出口SO2体积分数达到50 μL/L时，认为此时的吸附时间与吸附硫容分别为穿透时间与穿透硫容；而当出口SO2体积分数达到1 000 μL/L时，则分别为饱和时间与饱和硫容。当出口NO体积分数达到50 μL/L时，认为此时的吸附时间与吸附氮容分别为穿透时间与穿透氮容；而当出口NO体积分数达到250 μL/L时，则分别为饱和时间与饱和氮容。
η=c0−cc0×100%
S=qM∫(c0−c)dtVmm
式中：η为污染物（NO或SO2）的瞬时脱除率，%；c0、c为污染物（NO或SO2）的初始体积分数和出口体积分数，μL/L；S为活性炭对污染物（NO或SO2）的低温吸附容量，mg/g；M为污染物（NO或SO2）的摩尔质量，g/mol；q为总的气体流量，取500 mL/min；t为低温吸附时间，min；Vm为标准摩尔体积，取22.4 L/mol；m为料层中活性炭的质量，g。
1.5　活性炭吸附NO和SO2的密度泛函理论计算
密度泛函理论（DFT）计算是一种有前景的分子结构计算方法，可以有效地确定电子性质、几何形状和反应能。长期以来，锯齿形结构被认为是炭的主要内在边缘，其合理性得到广泛认可[9]。炭键合性能的计算数据和实验结果的对比表明，具有锯齿形边缘的C25H9模型可用于描述石墨/炭的微观结构[10]。本研究采用含锯齿形边缘的、由7个芳香环组成的C25H9模型（简称Zig）来模拟活性炭边缘的活性位点（图1）。
合理的泛函和基组可以在节省计算成本的同时获得更准确的结果。本研究使用Gaussian 16W在M062X/6-311G（d，p）水平上计算了该体系中各平衡几何形状的优化、振动分析和单点能[11]。此外，还考虑了色散校正，这在计算气体分子和碳表面之间的相互作用时至关重要[12]。
2　样品表征
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2.1　XPS分析
4种活性炭的XPS光谱如图2a）所示，可以观察到2个明显的C1s和O1s峰。对XPS光谱上的C1s和O1s峰进行拟合（图2b）—图2i）），其中284.6、286.1、287.6、289.1 eV处的子峰分别对应于C1s峰上的C−C、C−O、C=O和O−C=O结构；而O1s峰可以拟合出C=O（531.28~531.86 eV）、C−O（532.8~533.16 eV）和−COOH（534.41~537.69 eV）3个特征亚峰[13]，C−O主要由弱骨架氧和化学吸附氧组成，包括醚类（C−O−C、C−O−H等）、醇类和羟基[14]。拟合结果如表2所示。由表2可知，椰壳活性炭-2的碳含量最高（87.72%），椰壳活性炭-1的碳含量最低（76.54%）。
在所有测试样品中，椰壳活性炭-1的氧碳比（O/C）最高，含氧官能团含量最高，其中−COOH和C=O含量相较于其他样品明显增多，其原因可能为原料的差异。分级孔活性炭和煤基活性炭的含氧量相近，但通过一步活化法制得的分级孔活性炭拥有更多的C−O，而煤基活性炭拥有更多的−COOH。
2.2　孔隙结构分析
图3给出了4种活性炭的N2吸附-解吸等温线，样品的孔隙和表面参数见表3。根据国际理论化学和应用化学联合会（IUPAC）的分类[15]，分级孔活性炭和煤基活性炭表现为I型和IV型混合的吸附等温线，还存在一个较小的H4回滞环。这表明2种活性炭均含有大量微孔和部分中孔，尤其是煤基活性炭，具有典型的分级孔结构；椰壳活性炭-1和椰壳活性炭-2表现为典型的I型吸附等温线，表明其具有较为发达的微孔结构。
由表3可知，在4种活性炭中，椰壳活性炭-2的总比表面积、微孔比表面积、孔容和微孔孔容最大，微孔占比高达97.61%。微孔不仅可提供较大的比表面积，而且还有助于NO的吸附脱除[16]：受来自孔壁相对面重叠力场的影响，NO可进行自发的微孔填充过程。相较于一步活化法制得的分级孔活性炭，先炭化后活化制得的煤基活性炭比表面积更大，后者比表面积的增加是由于介孔含量升高所致，而两者微孔含量相差不大。从微孔率来看，分级孔活性炭拥有更好的分级孔结构。但从孔容来看，分级孔活性炭是4种活性炭中总孔容和微孔孔容最小的活性炭，这也是限制其氮容和硫容的主要原因。
3　活性炭的低温吸附性能
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3.1　惰性气氛下NO的吸附
图4和表4给出了惰性气氛低温下椰壳活性炭对NO的吸附脱除情况。分级孔活性炭和煤基活性炭的NO脱除率几乎为零，表明这2种活性炭对NO的吸附能力极弱。结合材料的孔隙结构分析可以推测，这与其微孔结构不够发达有关。微孔的不足限制了NO分子与活性炭表面的有效接触，无法提供足够的活性位点或表面积来吸附NO[17]。因此，这2种活性炭在低温下表现出较差的NO吸附性能。
对于具有较为发达微孔结构的椰壳活性炭-1和椰壳活性炭-2，其饱和氮容分别为0.02 mg/g和0.07 mg/g，呈现出比分级孔活性炭和煤基活性炭稍好的NO吸附性能，但吸附能力仍有限。这表明，即使是微孔结构较为发达的材料，通过纯物理吸附的方式也只能吸附少量的NO，饱和氮容依然较低。因此，微孔结构在NO的吸附过程中起着关键作用，但单纯的物理吸附机制对NO的吸附能力仍存在明显的限制。结合上述结果分析，NO的吸附能力不仅依赖于活性炭的微孔结构，还受到其吸附机制的影响。在低温条件下，NO分子难以通过纯物理吸附的方式与活性炭表面发生有效结合。
3.2　模拟烟气条件下NO的吸附
图5和表5给出了模拟烟气条件下低温下椰壳活性炭对NO的吸附脱除情况。从图5和表5可以看出，相较于惰性气氛，模拟烟气条件下4种样品均呈现出更高的穿透氮容量和饱和氮容量，椰壳活性炭的饱和氮容提升了3个数量级。这主要是因为NO可被烟气中的O2氧化，NO被转化为高价态的NO2等，显著促进了NO在活性炭表面的附着和捕获[18]，其吸附机制将在后续的密度泛函理论研究中进一步探索。
对比4种活性炭的氮容量可知，椰壳活性炭-2的吸附性能最佳，这可能是由于其具有最高的微孔比表面积和孔容，从而为NO和NO2分子的扩散和结合提供了更多活性位点，为吸附态含氮物质的储存提供了容积空间；0.4 nm的窄孔径分布也有利于NO和NO2的吸附。
结合含氧官能团的分析可知，4种活性炭中椰壳活性炭-2的含氧官能团最少，但其在惰性气氛和模拟烟气条件下对NO的低温吸附性能均最好，表明含氧官能团在NO的吸附中作用较小，孔隙结构主导了NO的低温吸附过程。
3.3　惰性气氛下SO2的吸附
SO2的低温吸附过程如图6所示。由图6可知，分级孔活性炭在实验过程中未能检测到穿透硫容，这可能是由于其微孔比表面积和孔容较小，限制了SO2分子的有效扩散和吸附。相比之下，其他3种活性炭在吸附初期均表现出较强的SO2吸附能力，出口气体中几乎检测不到SO2；随着吸附实验的进行，SO2的出口体积分数逐渐上升，最终达到饱和状态。3种活性炭中，椰壳活性炭-2的SO2吸附性能最佳，穿透硫容与饱和硫容分别达到了18.43 mg/g和57.07 mg/g（表6）。这可能是由于其发达的孔隙结构、较高的孔容以及适合SO2分子吸附的微孔孔径（0.4 nm）。
煤基活性炭与分级孔活性炭的微孔比表面积相近，但其穿透硫容明显更高。这种差异可能源于煤基活性炭表面存在较多的羧基官能团，这些官能团与SO2分子之间的化学作用提高了吸附初期SO2的捕获能力[19]。综合分析表明，活性炭的孔隙结构、表面化学特性及比表面积对SO2的吸附性能均具有显著影响。
3.4　模拟烟气条件下SO2的吸附
图7给出了模拟烟气条件下SO2的吸附脱除情况，与图6相比，氧气的引入显著促进了SO2在4种活性炭上的吸附，饱和硫容（表7）提高了2~5倍。部分研究认为，O2的存在能够促进SO2的催化氧化反应，从而使得SO2分子的吸附能力增强[20]。其吸附机制将在后续的密度泛函理论研究中进一步探索。
4种活性炭中，椰壳活性炭-2表现出最显著的吸附性能提升效果，尤其是饱和硫容的提升。这可归因于椰壳活性炭-2具有最高的比表面积和孔容。丰富的孔隙结构和较高的比表面积为SO2分子的扩散和吸附提供了扩散通道和吸附位点，合适的孔径（0.4 nm）则能够增强材料与SO2分子之间的相互作用，高的孔容有助于吸附态SO2的储存，从而共同提升了椰壳活性炭-2的吸附性能。
4　活性炭吸附的DFT计算
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氧气存在条件下，NO和SO2可被氧化为NO2和SO3，因此，本节在Zig模型上探讨了NO、NO2、SO2、SO3的吸附情况，具体如图8所示。吸附能是分子从自由态转化为固体表面吸附态过程中释放的热量，反映了气体分子与吸附材料表面间形成化学键的难易程度与强度，吸附能数值越大则模型对气体分子吸附的稳定性和选择性越高，模型对该分子的吸附效果也更显著。
4种气体分子在活性炭吸附位点上的结合能大小遵从以下顺序：NO2>SO3>SO2>NO。这表明，NO和SO2在含氧气氛中被分别氧化为NO2和SO3后，在活性炭表面的吸附能力显著增强，尤其是NO。计算结果表明，相比于活性炭上SO2的吸附，SO3吸附后生成的C−S键强度增加（键长由1.79 Å降至1.77 Å），C−O键变化不大；相比于NO，NO2吸附后生成的C−O键强度大幅增强（键长由1.36 Å降至1.34 Å），而C−N键强度小幅降低（键长由1.32 Å增至1.33 Å），整体呈现增加的趋势；其本质在于NO或SO2氧化后电子密度分布的改变。该结果解释了氧气提升活性炭吸附NO和SO2能力的内在原因，即NO和SO2与氧气共存时可被氧化，活性炭与其氧化产物（NO2或SO3）之间的结合能力更强，从而显著提升了活性炭的吸附性能。
5　结论
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1）在惰性气氛下，4种活性炭对NO的低温吸附性能均较弱，即使是性能最优的椰壳活性炭-2，饱和氮容也只有0.07 mg/g；在模拟烟气条件下，O2的存在使得活性炭的氮容提高了3个数量级，其中椰壳活性炭-2的饱和氮容最大，达到了175.70 mg/g，这与其丰富的微孔结构有关。
2）在惰性气氛下，椰壳活性炭-2对SO2的低温吸附性能最佳，饱和硫容可达57.07 mg/g；而在模拟烟气条件下，4种活性炭的饱和硫容提高了2~5倍，性能最优的椰壳活性炭-2，饱和硫容可达320.65 mg/g。
3）DFT计算结果表明，锯齿形边缘炭模型对NO、NO2、SO2、SO3的吸附结合能遵循以下顺序：NO2>SO3>SO2>NO。这表明，在含氧气氛中，NO和SO2分别被氧化为NO2和SO3后，能够显著增强其在活性炭表面的吸附能力，尤其是NO的低温吸附。
基金
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  • 国家重点研发计划项目(2022YFB4100203)
文献
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2026年第55卷第6期
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doi: 10.19666/j.rlfd.202510025
  • 接收时间：2025-10-15
  • 首发时间：2026-08-14
  • 出版时间：2026-06-25
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  • 收稿日期：2025-10-15
  • 修回日期：2025-12-03
  • 录用日期：2025-12-12
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National Key Research and Development Program(2022YFB4100203)
国家重点研发计划项目(2022YFB4100203)
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    广东电力发展股份有限公司，广东 广州 510000
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2种不同金属材料的力学参数
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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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