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Article(id=1149738727481716794, tenantId=1146029695717560320, journalId=1146031787341344770, issueId=1149738718707237637, articleNumber=1003-3033(2024)08-0186-09, orderNo=null, doi=10.16265/j.cnki.issn1003-3033.2024.08.1592, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1708963200000, receivedDateStr=2024-02-27, revisedDate=1716652800000, revisedDateStr=2024-05-26, acceptedDate=null, acceptedDateStr=null, onlineDate=1752048673744, onlineDateStr=2025-07-09, pubDate=1724774400000, pubDateStr=2024-08-28, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1752048673744, onlineIssueDateStr=2025-07-09, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1752048673744, creator=13701087609, updateTime=1752048673744, updator=13701087609, issue=Issue{id=1149738718707237637, tenantId=1146029695717560320, journalId=1146031787341344770, year='2024', volume='34', issue='8', pageStart='1', pageEnd='252', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=0, createTime=1752048671651, creator=13701087609, updateTime=1756376992009, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1167893010143519453, tenantId=1146029695717560320, journalId=1146031787341344770, issueId=1149738718707237637, language=EN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1167893010143519454, tenantId=1146029695717560320, journalId=1146031787341344770, issueId=1149738718707237637, language=CN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=186, endPage=194, ext={EN=ArticleExt(id=1149738727896952897, articleId=1149738727481716794, tenantId=1146029695717560320, journalId=1146031787341344770, language=EN, title=Preparation and properties of CuCl-CeO2 composite CO scavenger, columnId=1149733269173878863, journalTitle=China Safety Science Journal, columnName=Safety engineering technology, runingTitle=null, highlight=null, articleAbstract=

In order to avoid the accident of CO poisoning in coal mines，according to the principle of adsorption catalysis，CuCl-CeO2，a composite CO scavenger with both adsorption and catalytic properties，was prepared by thermal dispersion method using rare earth oxide CeO2 as catalyst carrier and CuCl as adsorbent. The CO elimination performance of CuCl，CeO2 and CuCl-CeO2 was studied by cone calorimeter. At the same time，the peak pressure of gas explosion and the CO elimination effect of CuCl-CeO2 were studied by a 20 L explosion ball-gas chromatography system. The results show that the CuCl-CeO2 composite scavenger can effectively reduce the release rate of CO during the whole heating process，and its elimination performance is better than that of CuCl or CeO2 alone. When the mass fraction of CuCl is 50 %，the CO elimination rate of CuCl-CeO2 is the highest，reaching 88.0 %. With the increase of CuCl-CeO2 mass concentration，the peak pressure of gas explosion gradually decreases，the time to reach the peak pressure of explosion is significantly delayed，and the amount of CO released is also decreasing. When the mass concentration of CuCl-CeO2 is 1.00 g/L，the effect of explosion suppression and CO elimination is the best. The peak pressure of gas explosion is reduced from 0.508 MPa to 0.387 MPa，the time to reach the peak pressure of explosion is delayed from 237.6 ms to 483.2 ms，and the volume fraction of CO is reduced from 0.879 7% to 0.108 9%，which effectively reduces the peak pressure of gas explosion and CO release.

, correspAuthors=Leilin ZHANG, 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, authorCompany=null, fund=null, authors=null, authorsList=Yong YU, Leilin ZHANG), CN=ArticleExt(id=1149738744170853277, articleId=1149738727481716794, tenantId=1146029695717560320, journalId=1146031787341344770, language=CN, title=CuCl-CeO2复合型CO消除剂的制备及其性能, columnId=1149733269727526997, journalTitle=中国安全科学学报, columnName=安全工程技术, runingTitle=null, highlight=null, articleAbstract=

为避免煤矿井下CO中毒事故的发生，根据吸附催化原理，以稀土氧化物二氧化铈(CeO2)为催化剂载体，氯化亚铜(CuCl)为吸附剂，通过热分散法将氯化亚铜负载在二氧化铈表面，制备一种兼具吸附和催化性能的复合型CO消除剂CuCl-CeO2。利用锥形量热仪分析CuCl、CeO2和CuCl-CeO2的CO消除性能，并通过20 L爆炸球-气相色谱联用系统，研究CuCl-CeO2对瓦斯爆炸峰值压力及其产生的CO消除效果。结果表明：CuCl-CeO2复合型消除剂能在整个升温过程中有效降低CO的释放率，其消除性能比单一CuCl或CeO2的消除性能更佳，且当CuCl的质量分数为50% 时，CuCl-CeO2的CO消除率最高，达88.0 %。随着CuCl-CeO2质量浓度的增加，瓦斯爆炸峰值压力逐渐降低，达到爆炸峰值压力的时刻显著延迟，CO释放量也不断减少。当加入CuCl-CeO2的质量浓度为1.00 g/L时，抑爆和CO消除效果最佳；瓦斯爆炸峰值压力由0.508 MPa降至0.387 MPa，达到爆炸峰值压力时间由237.6 ms延迟至483.2 ms，CO体积分数由0.879 7%降至0.108 9%，有效地降低了瓦斯爆炸峰值压力和CO释放量。

, correspAuthors=张雷林, authorNote=null, correspAuthorsNote=
** 张雷林(1985—)，男，江苏盐城人，博士，教授，主要从事矿井灾害防治方面的研究。E-mail：。
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虞勇 (2000—)，男，安徽安庆人，硕士研究生，主要研究方向为矿井灾害防治。E-mail：。

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虞勇 (2000—)，男，安徽安庆人，硕士研究生，主要研究方向为矿井灾害防治。E-mail：。

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虞勇 (2000—)，男，安徽安庆人，硕士研究生，主要研究方向为矿井灾害防治。E-mail：。

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Drugs used in the experiment

, figureFileSmall=null, figureFileBig=null, tableContent=
试验材料 化学式 性状
亚硫酸钠 Na2SO3 白色晶体性粉末
浓盐酸 HCl 无色溶液
(工业级，质量分数为37%)
氯化亚铜 CuCl 黄绿色粉末
(分析纯，纯度≥97.0%)
二氧化铈 CeO2 黄色球形粉末
(分析纯，纯度≥99.9%)
), ArticleFig(id=1167877870849368523, tenantId=1146029695717560320, journalId=1146031787341344770, articleId=1149738727481716794, language=CN, label=表1, caption=

试验使用药品

, figureFileSmall=null, figureFileBig=null, tableContent=
试验材料 化学式 性状
亚硫酸钠 Na2SO3 白色晶体性粉末
浓盐酸 HCl 无色溶液
(工业级，质量分数为37%)
氯化亚铜 CuCl 黄绿色粉末
(分析纯，纯度≥97.0%)
二氧化铈 CeO2 黄色球形粉末
(分析纯，纯度≥99.9%)
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CuCl-CeO2复合型CO消除剂的制备及其性能
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虞勇 1, 2 , 张雷林 1, 2, **
中国安全科学学报 | 安全工程技术 2024,34(8): 186-194
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中国安全科学学报 | 安全工程技术 2024, 34(8): 186-194
CuCl-CeO2复合型CO消除剂的制备及其性能
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虞勇1, 2 , 张雷林1, 2, **
作者信息
  • 1 安徽理工大学 煤炭高效开采省部共建教育部重点实验室，安徽 淮南 232001
  • 2 安徽理工大学安全科学与工程学院，安徽 淮南 232001

    • 虞勇 (2000—)，男，安徽安庆人，硕士研究生，主要研究方向为矿井灾害防治。E-mail：。

通讯作者:

** 张雷林(1985—)，男，江苏盐城人，博士，教授，主要从事矿井灾害防治方面的研究。E-mail：。
Preparation and properties of CuCl-CeO2 composite CO scavenger
Yong YU1, 2 , Leilin ZHANG1, 2, **
Affiliations
  • 1 Key Laboratory of Safe and Effective Coal Mining Anhui University of Science and Technology，Ministry of Education，Huainan Anhui 232001，China
  • 2 School of Safety Science and Engineering，Anhui University of Science and Technology，Huainan Anhui 232001，China
出版时间: 2024-08-28 doi: 10.16265/j.cnki.issn1003-3033.2024.08.1592
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摘要
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为避免煤矿井下CO中毒事故的发生，根据吸附催化原理，以稀土氧化物二氧化铈(CeO2)为催化剂载体，氯化亚铜(CuCl)为吸附剂，通过热分散法将氯化亚铜负载在二氧化铈表面，制备一种兼具吸附和催化性能的复合型CO消除剂CuCl-CeO2。利用锥形量热仪分析CuCl、CeO2和CuCl-CeO2的CO消除性能，并通过20 L爆炸球-气相色谱联用系统，研究CuCl-CeO2对瓦斯爆炸峰值压力及其产生的CO消除效果。结果表明：CuCl-CeO2复合型消除剂能在整个升温过程中有效降低CO的释放率，其消除性能比单一CuCl或CeO2的消除性能更佳，且当CuCl的质量分数为50% 时，CuCl-CeO2的CO消除率最高，达88.0 %。随着CuCl-CeO2质量浓度的增加，瓦斯爆炸峰值压力逐渐降低，达到爆炸峰值压力的时刻显著延迟，CO释放量也不断减少。当加入CuCl-CeO2的质量浓度为1.00 g/L时，抑爆和CO消除效果最佳；瓦斯爆炸峰值压力由0.508 MPa降至0.387 MPa，达到爆炸峰值压力时间由237.6 ms延迟至483.2 ms，CO体积分数由0.879 7%降至0.108 9%，有效地降低了瓦斯爆炸峰值压力和CO释放量。

氯化亚铜(CuCl)-二氧化铈(CeO2)  /  复合型CO消除剂  /  消除性能  /  爆炸峰值压力  /  CO释放量

In order to avoid the accident of CO poisoning in coal mines，according to the principle of adsorption catalysis，CuCl-CeO2，a composite CO scavenger with both adsorption and catalytic properties，was prepared by thermal dispersion method using rare earth oxide CeO2 as catalyst carrier and CuCl as adsorbent. The CO elimination performance of CuCl，CeO2 and CuCl-CeO2 was studied by cone calorimeter. At the same time，the peak pressure of gas explosion and the CO elimination effect of CuCl-CeO2 were studied by a 20 L explosion ball-gas chromatography system. The results show that the CuCl-CeO2 composite scavenger can effectively reduce the release rate of CO during the whole heating process，and its elimination performance is better than that of CuCl or CeO2 alone. When the mass fraction of CuCl is 50 %，the CO elimination rate of CuCl-CeO2 is the highest，reaching 88.0 %. With the increase of CuCl-CeO2 mass concentration，the peak pressure of gas explosion gradually decreases，the time to reach the peak pressure of explosion is significantly delayed，and the amount of CO released is also decreasing. When the mass concentration of CuCl-CeO2 is 1.00 g/L，the effect of explosion suppression and CO elimination is the best. The peak pressure of gas explosion is reduced from 0.508 MPa to 0.387 MPa，the time to reach the peak pressure of explosion is delayed from 237.6 ms to 483.2 ms，and the volume fraction of CO is reduced from 0.879 7% to 0.108 9%，which effectively reduces the peak pressure of gas explosion and CO release.

cuprous chloride(CuCl)-cerium dioxide(CeO2)  /  composite CO scavenger  /  elimination performance  /  explosion peak pressure  /  CO release
虞勇, 张雷林. CuCl-CeO2复合型CO消除剂的制备及其性能. 中国安全科学学报, 2024 , 34 (8) : 186 -194 . DOI: 10.16265/j.cnki.issn1003-3033.2024.08.1592
Yong YU, Leilin ZHANG. Preparation and properties of CuCl-CeO2 composite CO scavenger[J]. China Safety Science Journal, 2024 , 34 (8) : 186 -194 . DOI: 10.16265/j.cnki.issn1003-3033.2024.08.1592
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0 引言
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CO不仅是煤自燃预测预报的标志气体之一，还是典型的有毒化合物，过量吸入会导致窒息死亡，严重威胁煤矿工作人员的生命安全[1]。在煤矿井下，CO的来源主要有3方面，一是原生煤层因发生氧化反应生成的CO气体赋存其中，即煤层原生赋存的CO[2]。二是遗煤长期滞留在采空区内，与氧气发生反应生成的CO[3]。三是井下爆破、机轮车尾气以及瓦斯爆炸等产生的CO[4-5]。据统计，煤矿井下爆炸事故中，70%以上遇难者是由于CO中毒导致 [6]。因此，有效消除CO，对于保护井下工作人员生命安全意义重大。
近年来，为解决CO超限问题，国内外学者对于CO的吸收与催化开展了大量研究，如PENG Linlin等[7]通过新型质子亚铜功能化离子液体与CO的络合反应，实现了在低温时对CO的高效吸收，并证实了Cu(CO)Cl物种的形成；翟小伟等[8]研究了不同氯盐阻化剂对CO的吸附性能，对于CO消除具有一定指导意义；DAVID等[9]将氯化亚铜与1-己基-3-甲基咪唑氯化铵直接混合，制备的离子液体1-己基-3-甲基咪唑氯化亚铜酸盐成功地通过铜(I)络合吸收了CO;ZHANG Rongbin等[10]以CO氧化为模型反应，采用共沉淀法制备了一系列活性较低的Au/NiOx催化剂；ZHANG Chengmin等[11]采用沉积法制备了活性和稳定性较高的Au/二氧化铈(Cerium Dioxide，CeO2)催化剂，用于烧结烟气CO的催化；金奇杰等[12]采用挤出成型法，制备了铜铈负载钛铝氧化物催化剂，表现出对CO良好的催化活性；DONG等[13]制备了高催化活性和耐水性的棒状纳米多孔PdO/CeO2复合材料，用于CO的催化氧化。上述研究对CO的消除起到了一定作用，但在实际应用中存在一定局限性，如大多数吸附剂吸收CO的本质是利用Cu+或Ag+与CO形成金属羰基络合物，但在高温下，这些羰基络合物不稳定，会发生分解再次生成CO;催化氧化法大多使用贵金属单体物质或过渡金属氧化物，但贵金属在自然界中的含量较少且价格昂贵，过渡金属在低温时催化活性不佳且无法快速消除CO。因此，对于采空区遗煤自燃和瓦斯爆炸这些温度变化较大，CO释放速率较快的情形，上述吸附剂或催化剂无法达到理想的消除效果。
鉴于此，笔者拟开展试验，以CeO2为催化剂载体，氯化亚铜(Cuprous Chloride，CuCl)为吸附剂，采用热分散的方法，将氯化亚铜负载于二氧化铈表面，制备一种兼具低温吸附和高温催化的复合型CO消除剂；通过锥形量热仪研究CuCl-CeO2对CO的消除性能；通过20 L爆炸球-气相色谱研究CuCl-CeO2对瓦斯爆炸峰值压力及其产生的CO消除效果，以期为矿井安全生产和环境保护提供一定的指导。
1 CuCl-CeO2的制备及性能测试
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1.1 CuCl-CeO2的制备原料
选取CuCl为吸附剂，CeO2为催化剂，基于二者的物理特性制备CuCl-CeO2，具体参数见表1。
1.2 煤样和CuCl-CeO2的制备
1)煤样制备。所选煤样为安徽省朱集西煤矿11-3煤，采样后迅速放入密封袋储存。试验前，先剥去其表面的氧化层，然后将煤样破碎、过筛，选取粒径为40~80目的煤粉备用。
2)CuCl-CeO2制备。由于CuCl 在空气中易被氧化成黄绿色，试验前将一定量CuCl粉末置于蒸馏水中，以(Na2SO3)作为还原剂，边搅拌边缓慢加入Na2SO3的HCl溶液，直至出现白色沉淀后，过滤、干燥，即得纯净的CuCl。将提纯得到的CuCl和CeO2按所需比例充分搅拌后，迅速放入真空干燥箱中干燥10 h，取出干燥后的样品，立即在马弗炉中以400 ℃的温度焙烧3 h，使CuCl均匀分布在CeO2表面，制得CuCl-CeO2负载型CO消除剂。
1.3 CuCl-CeO2的CO消除性能测试方法
1) 锥形量热仪试验。分别称取60 g煤样与CuCl、CeO2和CuCl-CeO2粉末按质量比4:1充分混合，随后在真空干燥箱中干燥12h取出，放入锥形加热器中进行试验。利用锥形量热仪研究不同样品加热过程中气体释放情况，为消除锥形量热仪管道内留存气体的影响，试验从60 s后开始采集数据。锥形量热仪设置热通量为25 kW/m2，加热温度为650 ℃。试验装置如图1所示。
2) 20 L爆炸球-气相色谱试验。试验前对爆炸球抽取真空，向粉仓内放入所需CO消除剂粉末后，通入甲烷和空气。启动试验，电磁阀喷粉，点火器在设定的点火延迟时间60 ms后点火，点火能量为10 J，爆炸在常压下进行，数据采集系统同步采集甲烷爆炸压力信号。将爆炸后的气体通入气相色谱仪中，点击碳氧按钮开始检测气体浓度，记录数据，试验装置如图2所示。为突出表现CO消除性能，试验所选甲烷体积分数为9.5%。
2 CuCl-CeO2的吸附催化原理
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在吸附方面，按照吸附作用力的不同，吸附可分为化学吸附、物理吸附和络合吸附。CO与亚铜离子发生反应形成金属羰基络合物Cu(CO)nCl，这属于Π络合吸附[14]。Π络合吸附CO的理论基础是CO的碳原子和氧原子二者原子轨道能量相近，可以互相重叠形成CO分子的分子轨道，既可给出电子，也能接受电子[15];而过渡金属原子Cu具有不同的价态和配位数，其价电子层有(n-1)d轨道，在能量上与ns，np轨道相近，可作为价层的一部分使用，具有接受电子的能力。同时，其占据的d轨道又可以提供电子。因此，在金属羰基络合物的形成中，CO一方面可提供孤电子对给Cu+，另一方面又有空轨道与Cu+的d轨道重叠形成Π键，两者相互促进，协同作用，如图3所示。
在催化方面，铈是一种重要的稀土元素，由于其未充满的不同能级轨道有利于接纳孤电子(或孤电子对)，使之在催化领域具有较大潜力，其稀土氧化物CeO2作为一种催化剂和多相催化剂载体时，具有比表面积大、富含氧空位和价格低廉等特点，被广泛应用在催化和载体领域。CeO2通常以立方萤石结构存在，在这一结构中，每个铈离子与8个氧离子配位，且O2-都处在以Ce4+为中心的立方体顶点上，由于铈的特殊电子结构，其更容易在Ce4+和Ce3+级之间进行可逆电荷转移，在转移的过程中，氧物种会从CeO2中逃逸，形成氧空位，如图4所示[16]。由于氧空位的缺陷和铈离子价态的变化可以改善氧气的吸附和活化，当氧扩散在非化学计量的CeO2晶格中时，能很大程度地促进其氧化还原过程和催化反应，提高CeO2的催化性能。
负载型CO消除剂是吸附催化反应领域的一项重要操作技术[17]。以CeO2作为多相催化剂载体时，其良好的储释氧能力可以对环境气氛起到缓冲作用，在贫氧气氛下，CeO2可以提供CO氧化所需的氧，有效避免煤矿井下氧气浓度波动带来的影响，并且CeO2独特的立方萤石结构会使其表面积和表面结合能迅速增大，为其负载物提供更多的活性位点。将CuCl作为负载物时，由于其熔点(426 ℃左右)不高，在高温焙烧的条件下可在CeO2载体表面自发单层分散[18]，从而使CuCl在载体内外表面达到原子水平的分散，实现低温吸附CO的效果。负载型CO消除剂中的CuCl和CeO2的相互作用主要通过几何结构来实现，一方面，CeO2载体中的氧空位可以锚定CuCl中的单原子以达到吸附的作用，另一方面，CuCl的掺杂造成CeO2晶胞的扭曲和压缩，促进氧空位的形成，提高其催化性能。因此，通过热分散的方法把能与CO形成Π络合物的Cu+高度分散于CeO2上，形成复合型CO消除剂 [19]，兼具低温吸附和高温催化的效果，其吸附催化机制如图5所示。
3 CuCl-CeO2的CO消除性能分析
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3.1 CuCl-CeO2消除CO的性能分析
将经过等质量CuCl、CeO2和CuCl-CeO2复合型CO消除剂处理后的煤样分别放入锥形量热仪中加热，随着温度上升，不同煤样的CO释放率如图6所示。
由图6可知：经CeO2处理过的煤样，在300 s前CO释放率与原煤接近，后期发生大幅降低。这是因为锥形量热仪在加热过程中，经历了由低温到高温的过程。在300 s前，样品温度较低，氧物种不活跃，CeO2的催化活性不明显，随着样品温度升高，提供了足以跨越催化反应能垒的能量，晶胞内的氧化物转变成具有强氧化能力的过氧化物，CeO2的催化活性被提高，CO逐渐被催化氧化为CO2。相反，经CuCl混合处理后的煤样，在350s前，其CO释放率最低，后期却逐渐升高。这是由于添加纯CuCl时，Cu+含量较高，吸附性更强，在低温时，CO会被Cu+吸附形成金属羰基络合物Cu(CO)Cl，但该化学键不稳定，会随着温度的升高而断裂，因此后期Cu(CO)Cl会发生分解再次生成CO。经CuCl-CeO2处理后的煤样在整个升温过程中均能有效降低CO的释放率，这是因为经过热分散的方法将CuCl负载在CeO2上实现了吸附和催化的有效结合，起到了低温吸附和高温催化的双重效果。
CO在经过吸附催化后会转变为CO2，经不同消除剂处理后的煤样，其CO2释放率各不相同，通过CO2释放率可进一步验证CuCl-CeO2复合型消除剂对CO的氧化性能。图7为不同煤样的CO2释放率。
由图7可知：经CeO2处理过的煤样，前期CO2释放率与原煤接近，后期明显高于原煤；而经CuCl和CuCl-CeO2处理过的煤样，前期CO2释放率低于原煤，后期高于原煤。这主要因为CeO2在前期的催化活性不明显，经其处理的煤样在前期的CO2释放率与原煤接近，随着温度升高，CeO2的催化活性被激活，煤样释放的CO被催化氧化，导致后期的CO2释放率明显高于原煤。相反，经CuCl和CuCl-CeO2处理过的煤样，由于Cu+的低温吸附作用，致使煤样释放的CO在前期被吸附，并未参与催化氧化，因此其CO2释放率在前期低于原煤。而经过CuCl-CeO2处理过的煤样在后期的CO2释放率明显高于其他3种煤样，这是因为前期被吸附的CO经过高温分解后又被催化氧化为CO2，并且由于焙烧作用使存在氧空位的CeO2能够为负载物CuCl提供更多的活性位点，帮助形成具有超高反应活性的复合型CO消除剂，提高了CuCl-CeO2的催化效果，使其催化性能强于单一催化剂。因此，经CuCl-CeO2处理后的煤样，其CO和 CO2的释放率与预期结果一致，起到了低温吸附和高温催化的效果。
3.2 不同质量分数CuCl对CO的消除效果
为研究不同CuCl质量分数对CuCl-CeO2的CO消除效果，固定煤样与CuCl-CeO2的质量比为4:1不变，分别制备CuCl质量分数为20%、30%、40%、50%和60%的5种CuCl-CeO2样品，测试不同质量配比CuCl-CeO2处理后的煤样CO释放率，结果如图8a所示，消除率如图8b所示。
由图8a可知：在400 s前，经不同质量配比CuCl-CeO2处理后的煤样，其CO释放率基本相同，呈现缓慢上升趋势，但400 s后，CO释放率随着CuCl质量分数的变化而改变。这是因为后期温度升高，CuCl的吸附效果减弱，CO的消除主要依靠CuCl-CeO2的催化作用。根据CO总释放量求得的CO消除率如图8b所示，可以看出，随着CuCl质量分数的增加，CO消除率先升高后降低，当CuCl的质量分数为50%时，CO消除率最高，为88.0%，继续增加CuCl的质量分数时，CO消除率开始降低，说明CuCl已经达到最佳分散量。这是因为CuCl的熔点为426 ℃，CeO2的熔点为2 397 ℃，在经过400 ℃焙烧后，CuCl可在载体表面自发单层分散，从而附着在CeO2催化剂上，但CuCl的分散量存在一个阈值，当超过该阈值时，多余的CuCl会堆叠，进而不能有效地使所有一价铜离子活性中心与CO络合。同时，CuCl的堆叠容易限制氧物种的活跃，掩盖CeO2的催化性能，从而达不到最佳的消除效果。
3.3 不同类型CO消除剂的抑制效果
瓦斯爆炸会产生高温、高压和冲击波，且在爆炸后易产生大量CO等有毒气体[20]。为研究消除剂对瓦斯爆炸过程中压力、CO体积分数等影响，在20 L爆炸球-气相色谱试验系统中，以体积分数9.5%的甲烷爆炸为对照组(记为纯甲烷)，然后分别加入等质量的CuCl、CeO2和CuCl-CeO2消除剂粉末，研究其对爆炸峰值压力与CO体积分数的抑制效果，结果如图9所示。
由图9a—图9c可知：不同类型CO消除剂均能起到抑制瓦斯爆炸的效果，其爆炸峰值压力和到达爆炸峰值压力时间均发生明显的降低和延迟，且CuCl-CeO2复合型消除剂相较于单一CuCl或CeO2的抑爆效果更佳。同时，由图9d可知：不同类型CO消除剂均起到降低CO体积分数作用，但CuCl-CeO2的消除效果最显著。这是因为瓦斯爆炸是甲烷与氧气发生的剧烈氧化还原反应，而消除剂粉末主要通过消耗反应的自由基进而起到抑制作用[21]。氧化还原反应的关键步骤为：
C H 4 + O 2 → C H 3 · + O H ·
C H 3 · + O 2 → H C O · + H 2 O
C H O · + O H · → C O + H 2 O
其中，CuCl的吸附能力较强，导致CH4在低温时被吸附未参与爆炸[22]，延缓了步骤(1)的进行，使其达到爆炸峰值压力时刻显著延迟，但由于吸附的可逆性，致使其爆炸峰值压力和CO体积分数降低幅度较小。相反，由于CeO2的低温催化效果并不理想，所以其达到爆炸峰值压力的时间并未得到较大延迟，随着爆炸产生的高温高压使CeO2的催化活性被激发，CO被催化氧化为CO2，催化过程消耗了大量氧气，阻碍反应步骤(1)、步骤(2)的进行，使其爆炸峰值压力和CO体积分数显著降低。而加入兼具低温吸附和高温催化性能的CuCl-CeO2较好地弥补了两者的劣势，使其爆炸峰值压力和CO体积分数均低于单一CuCl和CeO2，并延缓了其达到爆炸峰值压力的时刻。
3.4 不同质量浓度CuCl-CeO2的抑制效果
为研究不同质量浓度的CuCl-CeO2消除剂粉末对瓦斯爆炸的抑制效果，固定CuCl的质量分数为50%，分别在20 L爆炸球中加入质量浓度为0.5、0.75、1.00、1.25、1.50 g/L的CuCl-CeO2粉末，测试其对瓦斯爆炸的影响，结果如图10所示。
由图10a—图10c可知：加入不同质量浓度的CuCl-CeO2的爆炸压力曲线均低于未加入CO消除剂的曲线，说明CuCl-CeO2的抑爆效果稳定，且随着CuCl-CeO2质量浓度的增加，其爆炸峰值压力呈先减少后增加的趋势，达到爆炸峰值压力时刻呈先上升后降低的现象，当质量浓度为1.00 g/L时，抑爆效果最佳。这是因为消除剂粉末均匀分散在爆炸腔体内，形成多个微型屏障，减少了可燃气体与氧气的接触，进而达到抑爆效果，但消除剂粉末的质量浓度越高，团聚现象越严重，热分解效率降低[23]。由图10d可知：随着CuCl-CeO2质量浓度的增加，CO释放量先降低后趋于平稳，这是因为在有限空间内，由于氧气不足以及温度的骤变，导致CuCl-CeO2对CO的吸附和催化逐渐达到饱和，继续增加CuCl-CeO2无法支撑吸附催化反应的进行。综上，当CuCl-CeO2质量浓度为1.00 g/L时，其抑爆和CO消除性能最佳，可将爆炸峰值压力由0.508 MPa降至0.387 MPa、达到爆炸峰值压力时刻由237.6 ms延缓至483.2 ms，CO体积分数由0.879 7%降至0.108 9%。
4 结论
收起
1) 利用热分散法制备兼具吸附和催化性能的CuCl-CeO2复合型CO消除剂，通过研究得出，随着温度的升高，CO先被吸附后被催化，表现出比单一CuCl和CeO2更好的CO消除效果。
2) 通过研究不同CuCl负载量对CuCl-CeO2复合型CO消除剂的影响，得出当CuCl的质量分数为50%时，其CO的消除率最高，为88.0%。
3) 通过20L爆炸球-气相色谱试验得出，当在瓦斯-空气混合气体中加入不同质量浓度的CuCl-CeO2时，瓦斯爆炸压力与CO释放量均大幅降低，且达到爆炸峰值压力时刻也发生明显延迟，当CuCl-CeO2的质量浓度为1.00 g/L时，可将爆炸峰值压力由0.508 MPa降至0.387 MPa，达到爆炸峰值压力时刻由237.6 ms延迟至483.2 ms，CO体积分数由0.879 7%降至0.108 9%。
基金
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  • 国家自然科学基金(51874008)
文献
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2024年第34卷第8期
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doi: 10.16265/j.cnki.issn1003-3033.2024.08.1592
  • 接收时间：2024-02-27
  • 首发时间：2025-07-09
  • 出版时间：2024-08-28
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  • 收稿日期：2024-02-27
  • 修回日期：2024-05-26
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国家自然科学基金(51874008)
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    1 安徽理工大学 煤炭高效开采省部共建教育部重点实验室，安徽 淮南 232001
    2 安徽理工大学安全科学与工程学院，安徽 淮南 232001

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** 张雷林(1985—)，男，江苏盐城人，博士，教授，主要从事矿井灾害防治方面的研究。E-mail：。
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