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Article(id=1236321544515932231, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236321537146540956, articleNumber=null, orderNo=null, doi=10.19666/j.rlfd.202501018, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1736438400000, receivedDateStr=2025-01-10, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1772691625955, onlineDateStr=2026-03-05, pubDate=1761321600000, pubDateStr=2025-10-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1772691625955, onlineIssueDateStr=2026-03-05, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1772691625955, creator=13701087609, updateTime=1772691625955, updator=13701087609, issue=Issue{id=1236321537146540956, tenantId=1146029695717560320, journalId=1210938733613449225, year='2025', volume='54', issue='10', pageStart='1', pageEnd='174', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1772691624199, creator=13701087609, updateTime=1772691865526, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1236322549404070348, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236321537146540956, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1236322549408264653, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236321537146540956, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=157, endPage=167, ext={EN=ArticleExt(id=1236321546243985500, articleId=1236321544515932231, tenantId=1146029695717560320, journalId=1210938733613449225, language=EN, title=Removal of SO3 from coal-fired flue gas by efficient and low-cost blended alkaline absorbent: performance study and experimental analysis, columnId=1211002409397129992, journalTitle=Thermal Power Generation, columnName=Power generation technology forum, runingTitle=null, highlight=null, articleAbstract=

The formation and emission of SO3 in coal-fired flue gas not only pose significant threats to atmospheric environments and human health but also negatively affect power plant operations. Injecting alkaline sorbents into flue gas has proven to be an effective method for SO3 removal. The removal efficiency of SO3 by injecting Na2CO3 and Ca(OH)2 absorbents was investigated under different flue gas conditions, and the removal performance was compared with that of the blended absorbents. Moreover, the physicochemical properties of the alkaline absorbents before and after the reaction were characterized using SEM, XRD, FT-IR, and XPS techniques. Based on experimental data and characterization results, the gas-solid reaction model were proposed to elucidate the mechanisms of SO3 removal by Na2CO3 and Ca(OH)2. Furthermore, the adsorption process of Na2CO3 on SO3 was simulated, and the adsorption energy was calculated and compared with that of Ca(OH)2. The results showed that, Na2CO3 demonstrated superior SO3 removal efficiency compared with Ca(OH)2, and the removal efficiency was enhanced by increasing the reaction temperature, SO3 mass concentration, absorbent stoichiometric ratio and residence time. The blended absorbent with a molar ratio of Ca:2Na:S=5.00:1.25:1.00 achieved an SO3 removal efficiency of 86.07% under practical operating conditions at a low cost. The findings indicated that the gas-solid reaction between Na2CO3 and SO3 followed the shrinking core model, while the reaction between Ca(OH)2 and SO3 adhered to the grain model. The adsorption energy of SO3 on Na2CO3 was higher than that on Ca(OH)2. This study can provide theoretical insights and technical support for efficient and cost-effective removal of SO3 from coal-fired flue gas.

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燃煤烟气中SO3的生成与排放不仅严重影响大气环境及人体健康，而且对电厂的运行具有负面影响。向烟气中喷射碱性吸收剂是脱除SO3的有效手段。通过在不同条件下向烟气注入Na2CO3和Ca(OH)2吸收剂，并与复配吸收剂进行性能对比，研究了碱性吸收剂对SO3的脱除效率；利用SEM、XRD、FT-IR、XPS等表征手段探究了反应前、后碱性吸收剂的理化性质特征，根据实验及表征结果推测了其气固反应模型，以阐明Na2CO3和Ca(OH)2脱除SO3的机理，通过模拟Na2CO3对SO3的吸附过程，计算了吸附过程的吸附能，并与Ca(OH)2进行对比。结果表明：Na2CO3的SO3脱除效率优于Ca(OH)2，且反应温度、SO3质量浓度、吸收剂当量比和停留时间的增加均有利于SO3的脱除；复配吸收剂Ca:2Na:S=5.00:1.25:1.00（当量比）在实际工况下可达到86.07%的SO3脱除效率，且成本较低；Na2CO3与SO3的气固反应遵循缩核模型，而Ca(OH)2与SO3的反应遵循晶粒反应模型，SO3在Na2CO3上的吸附能高于Ca(OH)2。该结论可为燃煤烟气中SO3的高效低成本脱除提供理论依据和技术支持。

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杨林军（1957），男，博士，教授，主要研究方向为大气污染控制技术，。
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单传家（2000），男，硕士研究生，主要研究方向为燃煤烟气处理技术，。

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单传家（2000），男，硕士研究生，主要研究方向为燃煤烟气处理技术，。

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单传家（2000），男，硕士研究生，主要研究方向为燃煤烟气处理技术，。

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Initial mass concentrations of SO3 in flue gas

, figureFileSmall=null, figureFileBig=null, tableContent=
工况SO2流量/(mL·min–1)O2流量/(mL·min–1)SO3理论初始质量浓度/(mg·m–3)SO3实际初始质量浓度/(mg·m–3)
工况1100508.97.1
工况220010017.915.2
工况330015026.823.0
工况440020035.731.4
工况5（实际工况）50025044.639.2
), ArticleFig(id=1236321564543734552, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=CN, label=表1, caption=

烟气中SO3的初始质量浓度

, figureFileSmall=null, figureFileBig=null, tableContent=
工况SO2流量/(mL·min–1)O2流量/(mL·min–1)SO3理论初始质量浓度/(mg·m–3)SO3实际初始质量浓度/(mg·m–3)
工况1100508.97.1
工况220010017.915.2
工况330015026.823.0
工况440020035.731.4
工况5（实际工况）50025044.639.2
), ArticleFig(id=1236321564644397852, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=EN, label=Tab.2, caption=

Parameters of alkaline absorbents Ca(OH)2 and Na2CO3

, figureFileSmall=null, figureFileBig=null, tableContent=
项目Ca(OH)2Na2CO3
粒径/μm5、10、25、50、755、10、25、50、75
纯度/%9595
密度/(g·cm–3)2.242.53
分子量74106
分解温度/℃580~650500~851
价格/(元·t–1)420~7001 800~4 000
), ArticleFig(id=1236321564749255455, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=CN, label=表2, caption=

碱性吸收剂Ca(OH)2和Na2CO3的参数

, figureFileSmall=null, figureFileBig=null, tableContent=
项目Ca(OH)2Na2CO3
粒径/μm5、10、25、50、755、10、25、50、75
纯度/%9595
密度/(g·cm–3)2.242.53
分子量74106
分解温度/℃580~650500~851
价格/(元·t–1)420~7001 800~4 000
), ArticleFig(id=1236321564879278883, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=EN, label=Tab.3, caption=

Physical properties of the alkaline absorbents before and after absorption

, figureFileSmall=null, figureFileBig=null, tableContent=
吸收剂比表面积/(m2·g–1)孔容/(cm3·g–1)平均孔径/nm
反应前Na2CO30.9050.0119.168
反应后Na2CO31.8090.0216.653
反应前Ca(OH)215.8210.09517.506
反应后Ca(OH)29.8750.08115.571
), ArticleFig(id=1236321564979942182, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=CN, label=表3, caption=

碱性吸收剂反应前、后物理特性

, figureFileSmall=null, figureFileBig=null, tableContent=
吸收剂比表面积/(m2·g–1)孔容/(cm3·g–1)平均孔径/nm
反应前Na2CO30.9050.0119.168
反应后Na2CO31.8090.0216.653
反应前Ca(OH)215.8210.09517.506
反应后Ca(OH)29.8750.08115.571
), ArticleFig(id=1236321565063828265, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=EN, label=Tab.4, caption=

The simulated adsorption energy of SO3 on surfaces of Na2CO3 (0 0 1) crystal and Ca(OH)2 (1 0 0) crystal

, figureFileSmall=null, figureFileBig=null, tableContent=
碱性吸收剂位置总吸附能吸收剂间吸附能SO3分子间吸附能吸附能
Na2CO3顶位点–226 717.45–209 745.82–16 968.12–3.54
桥位点–226 719.34–5.40
空位点–226 719.69–5.75
Ca(OH)2顶位点–1.60
桥位点–1.32
空位点–1.34
), ArticleFig(id=1236321565151908651, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236321544515932231, language=CN, label=表4, caption=

Na2CO3晶体（0 0 1）和Ca(OH)2晶体（1 0 0）表面SO3的模拟吸附能

, figureFileSmall=null, figureFileBig=null, tableContent=
碱性吸收剂位置总吸附能吸收剂间吸附能SO3分子间吸附能吸附能
Na2CO3顶位点–226 717.45–209 745.82–16 968.12–3.54
桥位点–226 719.34–5.40
空位点–226 719.69–5.75
Ca(OH)2顶位点–1.60
桥位点–1.32
空位点–1.34
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高效低成本复配吸收剂在燃煤烟气SO3脱除中的性能实验研究
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单传家 1 , 于航 1 , 陈恒 2 , 李津津 3 , 孙佳兴 4 , 杭文林 4 , 杨林军 1
热力发电 | 发电技术论坛 2025,54(10): 157-167
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热力发电 | 发电技术论坛 2025, 54(10): 157-167
高效低成本复配吸收剂在燃煤烟气SO3脱除中的性能实验研究
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单传家1 , 于航1, 陈恒2, 李津津3, 孙佳兴4, 杭文林4, 杨林军1
作者信息
  • 1.东南大学能源与环境学院，江苏　南京　210096
  • 2.浙大宁波理工学院机电与能源工程学院，浙江　宁波　315100
  • 3.南京林业大学材料科学与工程学院，江苏　南京　210037
  • 4.江苏国信扬州发电有限责任公司，江苏　扬州　225131

    • 单传家（2000），男，硕士研究生，主要研究方向为燃煤烟气处理技术，。

通讯作者:

杨林军（1957），男，博士，教授，主要研究方向为大气污染控制技术，。
Removal of SO3 from coal-fired flue gas by efficient and low-cost blended alkaline absorbent: performance study and experimental analysis
Chuanjia SHAN1 , Hang YU1, Heng CHEN2, Jinjin LI3, Jiaxing SUN4, Wenlin HANG4, Linjun YANG1
Affiliations
  • 1.School of Energy and Environment, Southeast University, Nanjing 210096, China
  • 2.School of Mechatronics and Energy Engineering, Ningbo Tech University, Ningbo 315100, China
  • 3.College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China
  • 4.Jiangsu Guoxin Yangzhou Power Generation Co., Ltd., Yangzhou 225131, China
出版时间: 2025-10-25 doi: 10.19666/j.rlfd.202501018
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摘要
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燃煤烟气中SO3的生成与排放不仅严重影响大气环境及人体健康，而且对电厂的运行具有负面影响。向烟气中喷射碱性吸收剂是脱除SO3的有效手段。通过在不同条件下向烟气注入Na2CO3和Ca(OH)2吸收剂，并与复配吸收剂进行性能对比，研究了碱性吸收剂对SO3的脱除效率；利用SEM、XRD、FT-IR、XPS等表征手段探究了反应前、后碱性吸收剂的理化性质特征，根据实验及表征结果推测了其气固反应模型，以阐明Na2CO3和Ca(OH)2脱除SO3的机理，通过模拟Na2CO3对SO3的吸附过程，计算了吸附过程的吸附能，并与Ca(OH)2进行对比。结果表明：Na2CO3的SO3脱除效率优于Ca(OH)2，且反应温度、SO3质量浓度、吸收剂当量比和停留时间的增加均有利于SO3的脱除；复配吸收剂Ca:2Na:S=5.00:1.25:1.00（当量比）在实际工况下可达到86.07%的SO3脱除效率，且成本较低；Na2CO3与SO3的气固反应遵循缩核模型，而Ca(OH)2与SO3的反应遵循晶粒反应模型，SO3在Na2CO3上的吸附能高于Ca(OH)2。该结论可为燃煤烟气中SO3的高效低成本脱除提供理论依据和技术支持。

燃煤烟气  /  SO3脱除  /  碱性吸收剂  /  复配碱性吸收剂

The formation and emission of SO3 in coal-fired flue gas not only pose significant threats to atmospheric environments and human health but also negatively affect power plant operations. Injecting alkaline sorbents into flue gas has proven to be an effective method for SO3 removal. The removal efficiency of SO3 by injecting Na2CO3 and Ca(OH)2 absorbents was investigated under different flue gas conditions, and the removal performance was compared with that of the blended absorbents. Moreover, the physicochemical properties of the alkaline absorbents before and after the reaction were characterized using SEM, XRD, FT-IR, and XPS techniques. Based on experimental data and characterization results, the gas-solid reaction model were proposed to elucidate the mechanisms of SO3 removal by Na2CO3 and Ca(OH)2. Furthermore, the adsorption process of Na2CO3 on SO3 was simulated, and the adsorption energy was calculated and compared with that of Ca(OH)2. The results showed that, Na2CO3 demonstrated superior SO3 removal efficiency compared with Ca(OH)2, and the removal efficiency was enhanced by increasing the reaction temperature, SO3 mass concentration, absorbent stoichiometric ratio and residence time. The blended absorbent with a molar ratio of Ca:2Na:S=5.00:1.25:1.00 achieved an SO3 removal efficiency of 86.07% under practical operating conditions at a low cost. The findings indicated that the gas-solid reaction between Na2CO3 and SO3 followed the shrinking core model, while the reaction between Ca(OH)2 and SO3 adhered to the grain model. The adsorption energy of SO3 on Na2CO3 was higher than that on Ca(OH)2. This study can provide theoretical insights and technical support for efficient and cost-effective removal of SO3 from coal-fired flue gas.

coal-fired flue gas  /  SO3 removal  /  alkaline absorbent  /  blended alkaline absorbent
单传家, 于航, 陈恒, 李津津, 孙佳兴, 杭文林, 杨林军. 高效低成本复配吸收剂在燃煤烟气SO3脱除中的性能实验研究. 热力发电, 2025 , 54 (10) : 157 -167 . DOI: 10.19666/j.rlfd.202501018
Chuanjia SHAN, Hang YU, Heng CHEN, Jinjin LI, Jiaxing SUN, Wenlin HANG, Linjun YANG. Removal of SO3 from coal-fired flue gas by efficient and low-cost blended alkaline absorbent: performance study and experimental analysis[J]. Thermal Power Generation, 2025 , 54 (10) : 157 -167 . DOI: 10.19666/j.rlfd.202501018
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近年来，我国火力发电站普遍采用中高硫煤作为燃料，并广泛使用选择性催化还原（selective catalytic reduction，SCR）技术进行脱硝处理，导致大量SO3排放[1-2]。在燃煤锅炉运行过程中，0.5%~1.0%的SO2会被氧化成SO3[3]，而在经过SCR脱硝反应装置时，又有0.5%~1.5%的SO2会被钒钛催化剂等氧化为SO3[4]。SO3不仅是一种环境污染物，还会在SCR脱硝系统中与逃逸的NH3反应生成黏性的NH4HSO4（ABS），附着在SCR脱硝催化剂的活性位点上，降低脱硝效率，并堵塞和腐蚀空气预热器等设备[5-6]。
目前，喷射碱性吸收剂是脱除SO3的主流方法之一。碱性吸收剂与SO3反应生成硫酸盐，形成颗粒物后被除尘装置去除。一般在炉内喷射碱性吸收剂时，可以有效降低SCR反应器入口处的SO3质量浓度，解决SO3带来的催化剂中毒失活问题；在炉后喷射碱性吸收剂时（一般选择空预器之前），可以降低烟道气的SO3质量浓度，有效解决空气预热器（以下简称预热器）堵塞及腐蚀的问题。常见的碱性吸收剂包括钾基、镁基、钙基及钠基吸收剂等[7]。钾基吸收剂如K2CO3对SO3的脱除效率较高，但吸收剂成本较高。镁基吸收剂在反应过程中对温度较为敏感，如MgCO3和Mg(OH)2吸收剂在较高温度下易于分解，影响反应效率[8]。钙基吸收剂具有成本低、材料来源广泛等特点，然而要实现较高的SO3脱除率需要使钙基吸收剂中的钙硫当量比（物质的量比，下同，记作Ca:S）达到8:1~17:1，这极大增加了后续除尘的难度[9-11]。钠基吸收剂由于碱性较强，因此具备较高的SO3脱除效率，例如Na2CO3、Na2SO3、NaHCO3等。Xie等人[12]的研究表明，在2Na:S为2:1左右时，喷射Na2CO3和NaHCO3复配吸收剂可达到约85%的SO3脱除率。钠基吸收剂脱除SO3产生的NaHSO4和亚NaHSO3具有黏性和腐蚀性。由于干粉喷射操作简单，维护和运行成本较低，本研究基于碱性吸收剂干粉喷射脱除SO3方法，选定Ca(OH)2和Na2CO3 2种吸收剂，探究二者在不同影响因素下的SO3脱除效率及脱除机理。单独使用Ca(OH)2和Na2CO3无法兼顾良好的SO3去除性能和低成本，且两者在理化性质、SO3去除性能和成本等方面具有一定的互补性，因此本研究将两者进行复配喷射，以期在提高SO3脱除效率的同时降低成本。
1　实验系统及方法
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1.1　实验SO3脱除系统
本实验碱性吸收剂喷射脱除SO3实验平台如图1所示。实验平台由电加热器、配气系统、SO3发生器、给料器、管道、保温棉、布袋除尘器、引风机等部件组成。设有TP1—TP5多个采样位点，TP1设置在给料器之前，而TP2—TP5均匀分布在给料器至布袋除尘器入口的沿程。实验过程中引风机的总气体流量设置为100 m3/h（标准工况，下同），管道内的气体流速约为12.8 m/s。实验利用钒钛催化剂（V2O5/TiO2）催化氧化SO2产生SO3，并通过改变SO3发生器中通入的SO2和O2质量浓度，调节烟气中的SO3质量浓度。SO3的初始质量浓度在TP1采样位点测试确定，SO3的初始质量浓度如表1所示，SO3发生器的催化转化率为80%~90%。
本研究采用控制冷凝/异丙醇吸收法对烟气中的SO3初始质量浓度进行采样测定，SO3采样设备示意如图2所示。将采样枪从采样位点插入烟道内，采样枪末端连接0.5 m蛇形冷凝管（冷凝温度为65 ℃）和2只装有150 mL 80%异丙醇溶液的吸收瓶，吸收瓶连接全自动烟尘采样器。用蒸馏水将冷凝管内壁附着的酸雾液滴收集，定容至200 mL，采用离子色谱（IC）测定溶液中SO42–质量浓度，确定不同位点处SO3质量浓度[13]。
碱性吸收剂对SO3的脱除效率ηSO3为[14]：
ηSO3=Cin(SO3)−Cout(SO3)Cin(SO3)×100
式中：Cin(SO3)、Cout(SO3)分别为SO3初始质量浓度和脱除后质量浓度。
实验用碱性吸收剂Ca(OH)2和Na2CO3采用球磨机研磨，并通过激光粒度分析仪测量，获得不同粒径水平的吸收剂，相关参数见表2。复配吸收剂由一定比例的Ca(OH)2和Na2CO3经由球磨机混合研磨复配而成。
1.2　材料表征方法
使用扫描电镜（SEM）观察反应前、后吸收剂的形态及其表面结构（FEI，美国）。利用激光粒度分析仪（BT-9300ST，中国）测试吸收剂的粒度，所用分散剂为无水乙醇。使用TriStar II 3030吸附-解吸装置测定了样品的N2吸附-解吸等温线（77 K），得到样品的物理特性及孔径分布图。碱性吸收剂结晶相的表征使用X射线衍射仪（XRD，Empyrean，英国）进行，靶源为铜靶，2θ范围为10°~90°。使用光谱仪（FT-IR，IRTracer-100，日本）记录吸收剂在4 000~400 cm–1内的傅里叶变换红外光谱。通过X射线光电子能谱（XPS，Escalab 250Xi，美国）分析材料的表面元素组成和价态。通过离子色谱法（IC，ICS2100，美国）测定采样溶液中硫酸根离子的质量浓度。
1.3　模拟和计算
在本研究中，所有计算均采用Materials Studio软件包DMol3代码中实现的自旋无限制DFT方法[15]。电子交换和关联效应由基于Perdew-Burke-Ernzerhof（PBE）的广义梯度近似（GGA）来描述，并采用了双数值加极化（DNP）基集[16]。所有计算都采用了0.005 Ha的轨道占用涂抹值。能量变化、最大力和最大位移的收敛容限分别为2.0×10–5 Ha、0.004 Ha/Å和0.005 Å。采用3×3×1 Monkhorst-Pack网格执行布里渊区积分[17]。
SO3分子在Na2CO3上的吸附能Eads定义为：
Eads=E*(SO3)−E*−E(SO3)
式中：E*(SO3)、E*和E(SO3)分别代表Na2CO3与SO3分子、孤立的Na2CO3和SO3分子吸附的能量。
2　结果与讨论
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2.1　碱性吸收剂喷射脱除SO3测试
碱性吸收剂喷射脱除SO3的脱除效率受喷射的吸收剂种类、吸收剂粒径、烟气温度、烟气停留时间等条件的影响[18]。因此，为了探究不同实验条件对吸收剂喷射脱除SO3的影响，利用控制变量法改变以上条件，进行Na2CO3、Ca(OH)2及复配吸收剂喷射实验。参考实际工况即表1中工况5条件，令吸收剂粒径为10 μm，停留时间为2 s，烟气温度为380 ℃。
2.1.1　吸收剂用量对SO3脱除影响
图3为当量比对Na2CO3和Ca(OH)2脱除SO3性能的影响。由图3可见，碱性吸收剂对SO3的脱除效率随当量比的减少而降低，且Na2CO3的SO3脱除效率明显优于Ca(OH)2。在较高的吸收剂用量下，吸收剂颗粒与SO3接触的机会大大增加，导致SO3脱除效率提高[19]。但Ca(OH)2在Ca:S>8:1时，SO3脱除率增幅减小，吸收剂利用率降低[20]。Na2CO3在较低的用量下即可达到较高的SO3脱除率，当2Na:S为2:1时，Na2CO3吸收剂的SO3去除率可达74.31%。
为了在满足SO3脱除效率达到85%的前提下进一步降低成本，采用不同比例Ca(OH)2和Na2CO3混合的吸收剂去除烟气中的SO3。当量比对复配吸收剂SO3脱除性能的影响如图4所示。在复配比保持不变的情况下，随着吸收剂用量的减小，复配吸收剂的脱除SO3性能也逐渐降低。与单一吸收剂相比，复配吸收剂以更少的吸收剂用量即可达到较高的SO3脱除效率，如Ca:2Na:S=5:1.25:1、4.5:1.5:1和4:2:1时，即可达到85%左右的SO3脱除效率。对比不同的复配比可发现，随着Na2CO3比例的提高，SO3脱除效率逐渐提高，这是由于Na2CO3具有更快的反应动力学；复配吸收剂性能也有较高的提升，是由于较高用量的Ca(OH)2在与Na2CO3混合喷射时增大了Na2CO3与SO3接触的几率。
进一步提高Na2CO3的比例，以期用更少的吸收剂达到较高的SO3脱除率，结果如图5所示。
由图5可见，提高Na2CO3的比例进一步提高了SO3脱除效率，与图3a)比较可知，随着Na2CO3的用量不断提高，复配吸收剂的SO3脱除效果与单一Na2CO3吸收剂相近。由于复配吸收剂Ca:2Na:S= 5:1.25:1，4.5:1.5:1和4:2:1及更高比例时均可以达到85%以上的脱除SO3的能力，但考虑到Na2CO3成本是Ca(OH)2的3~6倍，因此在满足SO3脱除效率的情况下，Na2CO3的比例越低，则成本越低。因此，认为Ca:2Na:S=5:1.25:1是较优的选择，其成本低于需要达到相同SO3脱除效率的单一吸收剂。本文后续实验均采用Ca:2Na:S=5:1.25:1复配吸收剂进行。
2.1.2　吸收剂粒径对SO3脱除影响
为了探究吸收剂粒径对SO3脱除效率的影响，对比单一吸收剂Na2CO3（2Na:S为2:1）和Ca(OH)2（Ca:S为5:1）与复配吸收剂Ca:2Na:S=5:1.25:1，结果如图6所示。由图6可见，随着粒径增大，吸收剂的SO3脱除效率总体均呈现下降的趋势。在各粒径下，复配吸收剂均优于单一吸收剂的脱除SO3性能。随着粒径减小，吸收剂的比表面积会增大，吸收剂表面暴露的活性位点增多，吸收性能也逐渐提高[10]。而粒径较大的吸收剂更容易被反应生成的产物等堵塞表面，影响到SO3的扩散，导致吸收率的降低[11]。研究过程中，粒径较大吸收剂研磨不够均匀，而吸收剂的吸湿性令较小粒径吸收剂不易保存，且需要较长的研磨时间，故选择粒径10 μm左右的吸收剂进行相关实验。
2.1.3　烟气停留时间对SO3脱除影响
为了探讨吸收剂在烟气停留时间不同时的性能差异，采样点TP1—TP5的SO3脱除效率结果如图7所示。随着停留时间的延长，各吸收剂的SO3脱除率均提高。单一吸收剂Ca:S=10:1的Ca(OH)2SO3脱除率在2 s可以达到80%以上的SO3脱除率；单一吸收剂2Na:S=3:1的Na2CO3在停留时间2 s时SO3脱除率可达到85%[21]。在停留时间较短（小于1 s）时，Na2CO3的SO3脱除率（尤其是2Na:S=3:1的Na2CO3）明显优于Ca(OH)2和复配吸收剂。在停留时间大于1 s时，对比单一吸收剂，Ca:2Na:S= 5:1.25:1复配吸收剂的SO3脱除性能较好，且其增长趋势稳定。在燃煤电厂中，吸收剂从SCR反应器出口到空预器的停留时间通常为2~5 s，确保了吸收剂与SO3的充分接触。
2.1.4　SO3质量浓度对SO3脱除影响
SO3质量浓度对复配吸收剂脱除SO3性能的影响如图8所示。
由图8可见，碱性吸收剂对SO3的脱除率随SO3质量浓度的升高而不断提高，在SO3初始质量浓度达到39.2 mg/m3时，Ca:S=10:1的Ca(OH)2吸收剂和2Na:S=2:1的Na2CO3吸收剂可以达到近80%的SO3脱除率，而Ca:2Na:S=5:1.25:1的复配吸收剂可以达到85%的SO3脱除率。当Ca:S为10:1，SO3质量浓度为15.7 mg/m3时，Ca(OH)2的SO3脱除效率约为Na2CO3的3倍以上。相同的SO3质量浓度下，Ca(OH)2的用量远大于Na2CO3吸收剂，与气流中的SO3分子的碰撞概率更高，同时在比表面积和孔隙率较高的Ca(OH)2表面上，SO3向颗粒内部的扩散速度更快[11]。由于Na2CO3与SO3的反应速率更快，因此在较高的SO3质量浓度条件下，Na2CO3具有更高的脱除效率[21]。而复配吸收剂在各质量浓度下均表现出较高的脱除性能，尤其是在SO3质量浓度较高时。
2.1.5　烟气温度对SO3脱除影响
烟气温度对吸收剂脱除SO3性能的影响如图9所示。由图9可见，各碱性吸收剂的SO3脱除性能均随着烟气温度的升高而提高，且复配吸收剂展现出较好的性能。反应温度的提高促进了SO3向吸收剂颗粒表面的扩散，提高了吸收剂颗粒与SO3之间的动力学反应速率[22]。在烟气温度250 ℃时，碱性吸收剂的SO3脱除性能大大降低，这主要是因为温度较低时烟气中的SO3易形成气溶胶，其粒径较小不易被吸收剂捕捉[23]；当温度升高至300 ℃时，各吸收剂的脱除效率普遍提升；当烟气温度进一步升高至450 ℃时，3种吸收剂的SO3脱除效率均接近或超过80%，其中Ca:2Na:S=5:1.25:1复配吸收剂在450 ℃时脱除效率最高，达到90.21%，而2Na:S=2:1吸收剂脱除效率也达到84.41%。SCR脱硝系统的运行温度通常高于300 ℃，复配吸收剂可以展现出更优越的SO3脱除性能。
2.1.6　SO3脱除率随反应时间变化规律
图10给出了在工况5下，吸收剂粒径为10 μm，停留时间为2 s，烟气温度为380 ℃，不同吸收剂SO3脱除效率随时间的变化。反应前期，固定床中的吸收剂量处于过量状态，化学当量比远大于理论值，反应时SO3能够完全与吸收剂接触并反应，故此时3种吸收剂对SO3的脱除率接近且均高于85%。而随着反应时间增加，各吸收剂对SO3的脱除率逐渐降低，随着反应进行，吸收剂表面形成硫酸盐覆盖在吸收剂表面，影响了SO3与吸收剂的接触。其中，Na2CO3的SO3脱除率降低最为平缓，而对Ca(OH)2吸收剂，随着反应时间的增加，SO3脱除率显著降低，反应进行到60 min时，仅有10%的脱除率。而复配吸收剂则呈现出优于Ca(OH)2但次于Na2CO3吸收剂的稳定性能。
2.2　喷射前、后碱性吸收剂物化性质
为了探讨2Na:S= 2:1的Na2CO3和Ca:S= 5:1的Ca(OH)2 2种吸收剂在反应前、后的性能差异，采用粒径为10 μm的吸收剂进行实验。反应温度为380 ℃，吸收剂的停留时间约为2 s。将不同样品注入烟道，使用配备玻璃纤维筒的取样枪在TP5处回收反应后的吸收剂。利用SEM扫描电镜观察了吸收反应前、后的Na2CO3和Ca(OH)2的形貌特征，结果如图11。反应前的Na2CO3颗粒较大，表面光滑致密；反应后，由于Na2CO3不断放出CO2，颗粒尺寸减小，表面出现空隙结构，比表面积和SO3吸收效率提高。反应前Ca(OH)2的形貌松散，比表面积较大，孔隙率较高；反应生成比表面积和孔容均较小的CaSO4均匀地堆积在Ca(OH)2表面，令其形貌更加致密。
图12为反应前、后Na2CO3和Ca(OH)2的XRD图像。Na2CO3和Ca(OH)2在反应后都呈现较强的Na2SO4和CaSO4衍射峰，反应前、后的衍射峰强度改变，其晶型可能发生变化。
通过傅里叶变换红外图谱（FT-IR）分析了反应前、后Na2CO3和Ca(OH)2的组成及其表面官能团的变化（图13）。样品在3 648 cm–1处的峰为未反应的Ca(OH)2，而在1 445 cm–1和870 cm–1处的峰为Na2CO3。1 130 cm–1和630 cm–1处的峰归因于硫酸根离子的伸缩振动[24]。这表明在样品表面生成了CaSO4和Na2SO4。
反应后Na2CO3和Ca(OH)2相对于氧、硫的XPS光谱如图14所示。为了进一步研究样品表面的产物层成分，将其S峰和O峰分解为特定的官能团。脱硫样品的S2p仅归因于SO42–[25]，表明SO3在碱性吸附剂表面形成了硫酸钙和硫酸钠。样品的O1s位点也证明了SO42–的存在。此外，还出现了较弱的Na2CO3和Ca(OH)2峰，这可能是由于某些吸收剂未完全反应所致。
表3为碱性吸收剂反应前、后物理特性。图15为反应前、后吸收剂的孔径分布。分析表3、图15可以发现，Na2CO3和Ca(OH)2在与SO3 反应后，其物理特性均发生了显著变化：Na2CO3吸收剂的比表面积和孔容在反应后均有所增加，表明反应后其孔结构变得更加发达，这是由于反应过程中Na2CO3不断放出CO2，颗粒尺寸减小，表面出现空隙结构；而Ca(OH)2吸收剂反应后，其孔结构有所减小，这是由于比表面积和孔容更小的硫酸钙沉积覆盖了部分孔道。图15展示了反应前、后2种吸收剂孔径分布的变化，其中Na2CO3的反应后孔径在10 nm以下的孔容占比增加，而Ca(OH)2的反应后孔径分布则显示孔径在20~40 nm的孔容占比有所下降，这与表3数据一致。
2.3　反应机理
Na2CO3和Ca(OH)2与SO3的反应被认为遵循不同的气固反应模型，示意如图16所示。Na2CO3与SO3的反应遵循缩核模型[26]。反应气体首先扩散到颗粒表面，与颗粒反应生成产物，产物层逐渐覆盖颗粒表面。然后SO3通过产物层扩散到未反应核表面与之反应，随着反应的进行，未反应核逐渐减小，而产物层逐渐增厚。同时，SO3与Na2CO3反应不断释放出CO2，以保持颗粒的多孔结构，从而促进了SO3向未反应核心表面的扩散。这一过程与图11和表3中Na2CO3吸收剂的表征结果一致。Ca(OH)2与SO3的反应遵循晶粒反应模型[27]。多孔Ca(OH)2颗粒被视为由许多固体球形颗粒组成，颗粒之间的空隙即为多孔颗粒的内部孔隙。SO3不是直接在大颗粒表面反应，而是通过孔隙扩散到许多细颗粒表面与之反应，细颗粒的反应类似于缩核模型[28]。Ca(OH)2与SO3反应后，孔体积和比表面积变小，形态由松散变致密。
为了研究碱性吸收剂与SO3反应驱动力，通过模拟Na2CO3在SO3上的吸附过程计算得到吸附能，并与Ca(OH)2比较。图17为SO3分子在Na2CO3晶面上不同位置的吸附构型。考虑到（0 0 1）是最为常见的晶面，选择Na2CO3的（0 0 1）晶面进行计算，并将SO3分子置于吸收剂表面进行结构优化，以此评价其吸收过程。对比Yu等人[29]的研究中Ca(OH)2与SO3的反应情况模型，SO3可与Na2CO3和Ca(OH)2在不同位置发生反应，其O原子与晶体表面的Na和Ca离子相连。
表4为Na2CO3晶体（0 0 1）和Ca(OH)2晶体（1 0 0）表面SO3的模拟吸附能[29]。在Na2CO3晶体上，SO3在空位点的吸附能比其他2种构型的吸附能大，SO3在空位点的构型更稳定；而在Ca(OH)2晶体中，SO3则在顶位点更加稳定。SO3在Na2CO3晶体上的模拟吸附能高于其在Ca(OH)2晶体上的吸附能，因此Na2CO3对SO3的吸附驱动力更强，其吸附过程更加稳定，且SO3会优先与Na2CO3结合。
3　结论
收起
本研究通过在不同条件下向烟气注入Na2CO3和Ca(OH)2吸收剂，进行了SO3脱除实验，并与复配吸收剂进行了性能对比。通过表征分析了反应前、后吸收剂物理和化学性质的变化。此外，还探讨了2种碱性吸收剂脱除SO3的机理，包括两种吸收剂的气固反应模型、与SO3的吸附反应驱动力。通过模拟吸附过程并计算吸附能，进一步分析了吸收剂与SO3的吸附反应。得出的主要结论如下。
1）Na2CO3吸收剂的SO3脱除效率优于Ca(OH)2吸收剂，而复配吸收剂的SO3脱除性能略优于单一Na2CO3和Ca(OH)2吸收剂。Ca(OH)2必须达到Ca:S=10:1的比例，Na2CO3必须达到2Na:S=3:1的比例，才能达到约85%的SO3去除效率。然而，Ca:2Na:S=5:1.25:1、4.5:1.5:1和4:2:1的复配吸收剂均可以达到约85%的SO3去除效率。且复配吸收剂在满足SO3脱除性能的同时，用量及成本更小。
2）反应温度、SO3浓度、吸收剂当量比和停留时间的增加均有利于碱性吸收剂对SO3的脱除，吸收剂粒径越小，SO3脱除效果越好。且在满足实际烟气的条件下，复配吸收剂在各影响条件下均展现出更优的SO3脱除性能。
3）Na2CO3和Ca(OH)2与SO3反应生成硫酸钠和硫酸钙。吸收剂与SO3反应前的比表面积、孔容和平均孔径为Na2CO3<Ca(OH)2。反应后，Na2CO3的比表面积和孔容增大，主要是由于反应不断释放CO2形成孔结构；而Ca(OH)2的比表面积和孔容减小，因为比表面积和孔容更小的硫酸盐在其表面的沉积。
4）SO3与Na2CO3的气固反应遵循缩核模型，而与Ca(OH)2的反应遵循晶粒反应模型。SO3在Na2CO3上的吸附能高于Ca(OH)2的吸附能，因此SO3优先与Na2CO3结合，其吸附反应驱动力更强。而且SO3与Na2CO3晶体反应时，在Hollow位点上的构型更稳定，而在Ca(OH)2晶体上的Top位点上的构型更稳定。
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2025年第54卷第10期
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doi: 10.19666/j.rlfd.202501018
  • 接收时间：2025-01-10
  • 首发时间：2026-03-05
  • 出版时间：2025-10-25
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  • 收稿日期：2025-01-10
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    1.东南大学能源与环境学院，江苏　南京　210096
    2.浙大宁波理工学院机电与能源工程学院，浙江　宁波　315100
    3.南京林业大学材料科学与工程学院，江苏　南京　210037
    4.江苏国信扬州发电有限责任公司，江苏　扬州　225131

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杨林军（1957），男，博士，教授，主要研究方向为大气污染控制技术，。
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