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Article(id=1241408717007155410, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241408710791189399, articleNumber=null, orderNo=null, doi=null, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1739548800000, receivedDateStr=2025-02-15, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1773904502392, onlineDateStr=2026-03-19, pubDate=1745078400000, pubDateStr=2025-04-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1773904502392, onlineIssueDateStr=2026-03-19, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1773904502392, creator=13701087609, updateTime=1773904502392, updator=13701087609, issue=Issue{id=1241408710791189399, tenantId=1146029695717560320, journalId=1234093305789726721, year='2025', volume='45', issue='4', pageStart='1777', pageEnd='2368', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1773904500911, creator=13701087609, updateTime=1773904624658, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1241409229878259747, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241408710791189399, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1241409229878259748, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241408710791189399, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=1889, endPage=1900, ext={EN=ArticleExt(id=1241408717460140255, articleId=1241408717007155410, tenantId=1146029695717560320, journalId=1234093305789726721, language=EN, title=Conversion of waste oils to green diesel by non-precious metal materials, columnId=1234106386360103680, journalTitle=China Environmental Science, columnName=Water Pollution Control, runingTitle=null, highlight=null, articleAbstract=

Varieties of non-noble metal catalysts were prepared and screened by hydrothermal deoxidation of stearic acid for the purpose of efficiently catalyzing the conversion of waste oil into green diesel. The experimental results demonstrated that the nano-Ni-Cu alloy exhibited a significant catalytic effect on stearic acid, with its catalytic performance and product distribution being the most comparable to those of the Pt/C catalyst. Furthermore, the optimization of reaction conditions, stability analysis, catalyst characterization, reaction mechanism exploration and broad-spectrum analysis were carried out for nano Ni-Cu alloy. The characterization results revealed that the structure of nano-Ni-Cu alloy remained stable, and no significant structural changes were observed after continuous cyclic use. Under the optimum reaction conditions of 330℃, 120min, with the addition of 20µL methanol,30mg catalyst and 80µL water in a 1.67ml micro reactor, stearic acid was primarily converted into heptadecane through catalytic hydrodeoxygenation and decarbonylation. Additionally, the broad-spectrum analysis indicated that the yield of C8-C18 alkanes from various fatty acids and fatty acid esters catalyzed by nano-Ni-Cu alloy could exceed 95%, conforming its excellent catalytic performance.

, correspAuthors=Jing ZHANG, Chun YANG, 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=Xiao LIU, Tao XIA, Jing ZHANG, Chun YANG), CN=ArticleExt(id=1241408724871475952, articleId=1241408717007155410, tenantId=1146029695717560320, journalId=1234093305789726721, language=CN, title=非贵金属材料催化废弃油脂制备绿色柴油, columnId=1234106386565624579, journalTitle=中国环境科学, columnName=水污染与控制, runingTitle=null, highlight=null, articleAbstract=

以高效催化废弃油脂水热脱氧制备绿色柴油为目标，制备了多种非贵金属催化剂并通过硬脂酸水热脱氧实验对其进行了筛选.其中纳米铜镍合金针对硬脂酸催化效果较佳且催化性能与产物分布与Pt/C催化剂最为接近，进一步对其进行了反应条件优化、稳定性分析、催化剂表征、反应机理探究以及广谱性分析.表征结果显示纳米铜镍合金结构较为稳定，在多次循环使用后并未发生明显结构改变.反应温度330℃、反应时间120min、在1.67mL微型反应釜中加入20µL甲醇、30mg催化剂、80µL水的最佳反应条件下，纳米铜镍合金主要通过催化加氢脱氧及脱羰过程将硬脂酸转化为十七烷.广谱性分析表明其催化多种脂肪酸及脂肪酸酯的C8-C18烷烃产率均可达95%以上，证明了其优异的催化性能.

, correspAuthors=张静, 阳春, authorNote=null, correspAuthorsNote=
* 责任作者，教授，;
** 教授，
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刘骁(2002-)，男，陕西汉中人，哈尔滨工业大学硕士研究生，主要从事污水处理以及生物质资源化方向研究..

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刘骁(2002-)，男，陕西汉中人，哈尔滨工业大学硕士研究生，主要从事污水处理以及生物质资源化方向研究..

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刘骁(2002-)，男，陕西汉中人，哈尔滨工业大学硕士研究生，主要从事污水处理以及生物质资源化方向研究..

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articleId=1241408717007155410, language=CN, orderNo=4, keyword=非贵金属催化剂)], refs=[Reference(id=1241408736099627933, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, doi=null, pmid=null, pmcid=null, year=2024, volume=43, issue=S1, pageStart=351, pageEnd=364, url=null, language=null, rfNumber=[1], rfOrder=0, authorNames=李新月, 李振京, 韩沂杭, journalName=化工进展, refType=null, unstructuredReference=李新月，李振京，韩沂杭，等.油脂加氢脱氧生产绿色柴油催化剂的研究进展[J]. 化工进展，2024，43(S1):351-364., articleTitle=油脂加氢脱氧生产绿色柴油催化剂的研究进展, refAbstract=null), Reference(id=1241408736225457066, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, doi=null, pmid=null, pmcid=null, year=2024, volume=43, issue=S1, pageStart=351, pageEnd=364, url=null, language=null, rfNumber=[1], rfOrder=1, authorNames=Li X, Li Z J, Han Y H, journalName=Chemical Industry and Engineering Progress, refType=null, unstructuredReference=Li X，Li Z J，Han Y H，et al. 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Applied Catalysis B: Environmental，2020，260:118114., articleTitle=A novel catalyst with variable active sites for the direct hydrogenation of waste oils into jet fuel, refAbstract=null)], funds=[Fund(id=1241408735428539248, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, awardId=22076016, language=CN, fundingSource=国家自然科学基金面上项目(22076016), fundOrder=null, country=null), Fund(id=1241408735688586117, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, awardId=22422602, language=CN, fundingSource=国家自然科学基金优秀青年科学基金项目(22422602), fundOrder=null, country=null), Fund(id=1241408735952827279, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, awardId=Z2024A016, language=CN, fundingSource=全处置与资源化技术国家工程研究中心科研基金项目(Z2024A016), fundOrder=null, country=null)], companyList=[AuthorCompany(id=1241408725248963358, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, xref=1., ext=[AuthorCompanyExt(id=1241408725257351967, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, companyId=1241408725248963358, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1.National Engineering Research Center for Safe Disposal and Resources Recovery of Sludge, School of Environment, Harbin Institute of Technology, Harbin 150000, China), AuthorCompanyExt(id=1241408725265740578, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, companyId=1241408725248963358, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1.哈尔滨工业大学环境学院，污泥安全处置与资源化技术国家工程研究中心，黑龙江 哈尔滨 150000)]), AuthorCompany(id=1241408725387375405, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, xref=2., ext=[AuthorCompanyExt(id=1241408725395764014, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, companyId=1241408725387375405, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2.College of Environment and Ecology, Chongqing University, Chongqing 400044, China), AuthorCompanyExt(id=1241408725404152623, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, companyId=1241408725387375405, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2.重庆大学环境与生态学院，重庆 400044)])], figs=[ArticleFig(id=1241408729422295280, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.1, caption=Screening of non-precious metal materials, figureFileSmall=ctCJ3QY3XT38YXutht3kXw==, figureFileBig=5uor5RAosnK0FMAqKCa6Cw==, tableContent=null), ArticleFig(id=1241408729573290239, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图1, caption=非贵金属材料的筛选

T=330℃，t=120min，50mg硬脂酸，20µL甲醇，480µL水，30mg催化剂1-18 & 催化剂20-23，15mg催化剂24

, figureFileSmall=ctCJ3QY3XT38YXutht3kXw==, figureFileBig=5uor5RAosnK0FMAqKCa6Cw==, tableContent=null), ArticleFig(id=1241408729938194733, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.2, caption=Distribution of alkane products of stearic acid catalyzed by Devarda’s alloy, nano-Ni-Cu alloy and Pt/C catalyst, figureFileSmall=riZHU892tMIQbnSEi3D9Jg==, figureFileBig=OZhpWfEAgZBhcNmrSJwpOg==, tableContent=null), ArticleFig(id=1241408730068218171, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图2, caption=第威德合金、纳米铜镍合金和Pt/C催化剂催化硬脂酸的烷烃产物分布

T=330℃，t=120min，50mg硬脂酸，20µL甲醇，480µL水，30mg第威德合金或纳米铜镍合金，15mg Pt/C催化剂

, figureFileSmall=riZHU892tMIQbnSEi3D9Jg==, figureFileBig=OZhpWfEAgZBhcNmrSJwpOg==, tableContent=null), ArticleFig(id=1241408730189853007, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.3, caption=(a) Conversion and product yield, (b) product selectivity and distribution of stearic acid under different reaction temperature, figureFileSmall=CPK+BH7qOfbMJpFivEVAaQ==, figureFileBig=v5bkhdDCGH0fuT5QXc0WIw==, tableContent=null), ArticleFig(id=1241408730303099228, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图3, caption=不同反应温度下(a)硬脂酸转化率与产物产率以及(b)产物选择性与分布

T=260~360℃，t=120min，50mg硬脂酸，20µL甲醇，480µL水，30mg纳米铜镍合金

, figureFileSmall=CPK+BH7qOfbMJpFivEVAaQ==, figureFileBig=v5bkhdDCGH0fuT5QXc0WIw==, tableContent=null), ArticleFig(id=1241408730462482798, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.4, caption=(a) Conversion and product yield, (b) product selectivity and distribution of stearic acid under different reaction time, figureFileSmall=QLteJyHUATXQMKw+1UVl6g==, figureFileBig=A0YIXiMDmHq0wUhRP4yU6Q==, tableContent=null), ArticleFig(id=1241408730672198018, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图4, caption=不同反应时间下(a)硬脂酸转化率与产物产率以及(b)产物选择性与分布

T=330℃，t=30~150min，50mg硬脂酸，20µL甲醇，480µL水，30mg纳米铜镍合金

, figureFileSmall=QLteJyHUATXQMKw+1UVl6g==, figureFileBig=A0YIXiMDmHq0wUhRP4yU6Q==, tableContent=null), ArticleFig(id=1241408730793832844, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.5, caption=(a) Stearic acid conversion and product yield, (b) product selectivity and distribution with different dosage of catalyst, figureFileSmall=h2gf0v9d0rD1iRQ+XnywHA==, figureFileBig=0d5/CflQEaYtFUBayOXeWg==, tableContent=null), ArticleFig(id=1241408730915467678, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图5, caption=不同催化剂投加量下(a)硬脂酸转化率与产物产率以及(b)产物选择性与分布

T=330℃，t=120min，50mg硬脂酸，20µL甲醇，480µL水，7~50mg纳米铜镍合金

, figureFileSmall=h2gf0v9d0rD1iRQ+XnywHA==, figureFileBig=0d5/CflQEaYtFUBayOXeWg==, tableContent=null), ArticleFig(id=1241408731007742379, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Fig.6, caption=(a) Conversion and product yield, (b) product selectivity and distribution of stearic acid with different dosage of water, figureFileSmall=lHpbJSyn9lZmU+A/urM92w==, figureFileBig=v7IevD47Jo+46oHw5jy5bA==, tableContent=null), ArticleFig(id=1241408731129377212, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=图6, caption=不同水投加量下(a)硬脂酸转化率与产物产率以及(b)产物选择性与分布

T=330℃，t=120min，50mg硬脂酸，20µL甲醇，0~780µL水，30mg纳米铜镍合金

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T=330℃，t=120min，50mg硬脂酸，0~40µL甲醇，80µL水，30mg纳米铜镍合金

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T=330℃，t=120min，50mg硬脂酸，20µL甲醇，80µL水，30mg纳米铜镍合金

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Product distribution of stearic acid under optimum reaction conditions

, figureFileSmall=null, figureFileBig=null, tableContent=
序号产物产率(%)
1C1797.25
2C180.99
3十八醇0
4硬脂酸甲酯0
), ArticleFig(id=1241408733926978286, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=表1, caption=

最佳反应条件下硬脂酸的产物分布

, figureFileSmall=null, figureFileBig=null, tableContent=
序号产物产率(%)
1C1797.25
2C180.99
3十八醇0
4硬脂酸甲酯0
), ArticleFig(id=1241408734040224503, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Table 2, caption=

Structural properties of nano-Ni-Cu alloy before and after reaction

, figureFileSmall=null, figureFileBig=null, tableContent=
项目比表面积(m2/g)孔容(cm2/g)平均孔径(nm)
使用前8.8480.026793.841
使用3次后1.8080.0053983.430
), ArticleFig(id=1241408734249939721, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=表2, caption=

纳米铜镍合金反应前后的结构性质

, figureFileSmall=null, figureFileBig=null, tableContent=
项目比表面积(m2/g)孔容(cm2/g)平均孔径(nm)
使用前8.8480.026793.841
使用3次后1.8080.0053983.430
), ArticleFig(id=1241408734426100507, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Table 3, caption=

Reaction results of octadecyl alcohol catalyzed by nano-Ni-Cu alloy

, figureFileSmall=null, figureFileBig=null, tableContent=
序号产物加入20 µL甲醇的产物产率(%)不加甲醇的产物产率(%)
1C80.660.50
2C90.830.52
3C100.900.59
4C111.060.58
5C121.060.56
6C131.060.59
7C141.230.80
8C152.261.77
9C165.084.00
10C1782.3389.73
11C180.670.59
), ArticleFig(id=1241408734564512551, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=表3, caption=

纳米铜镍合金催化十八醇的反应结果

, figureFileSmall=null, figureFileBig=null, tableContent=
序号产物加入20 µL甲醇的产物产率(%)不加甲醇的产物产率(%)
1C80.660.50
2C90.830.52
3C100.900.59
4C111.060.58
5C121.060.56
6C131.060.59
7C141.230.80
8C152.261.77
9C165.084.00
10C1782.3389.73
11C180.670.59
), ArticleFig(id=1241408734640010034, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Table 4, caption=

Reaction results of different fatty acids and fatty acid esters catalyzed by nano-Ni-Cu alloy

, figureFileSmall=null, figureFileBig=null, tableContent=
底物硬脂酸转化率(%)98.99C8-C18烷烃的总产率(%)98.24
棕榈酸99.2196.89
油酸99.1058.13
月桂酸100.0098.35
硬脂酸甲酯100.0093.07
), ArticleFig(id=1241408734744867647, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=表4, caption=

纳米铜镍合金催化不同脂肪酸和脂肪酸酯的反应结果

, figureFileSmall=null, figureFileBig=null, tableContent=
底物硬脂酸转化率(%)98.99C8-C18烷烃的总产率(%)98.24
棕榈酸99.2196.89
油酸99.1058.13
月桂酸100.0098.35
硬脂酸甲酯100.0093.07
), ArticleFig(id=1241408735000720201, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=EN, label=Table 5, caption=

Reaction products of oleic acid catalyzed by nano-Ni-Cu alloy

, figureFileSmall=null, figureFileBig=null, tableContent=
产物产率(%)
硬脂酸26.46
C8-C18烷烃58.13
硬脂酸甲酯1.46
十八醇1.48
杂质13.00
), ArticleFig(id=1241408735143326548, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241408717007155410, language=CN, label=表5, caption=

纳米铜镍合金催化油酸的反应产物

, figureFileSmall=null, figureFileBig=null, tableContent=
产物产率(%)
硬脂酸26.46
C8-C18烷烃58.13
硬脂酸甲酯1.46
十八醇1.48
杂质13.00
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非贵金属材料催化废弃油脂制备绿色柴油
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刘骁 1 , 夏涛 2 , 张静 1, * , 阳春 2, **
中国环境科学 | 水污染与控制 2025,45(4): 1889-1900
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中国环境科学 | 水污染与控制 2025, 45(4): 1889-1900
非贵金属材料催化废弃油脂制备绿色柴油
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刘骁1 , 夏涛2, 张静1, * , 阳春2, **
作者信息
  • 1.哈尔滨工业大学环境学院，污泥安全处置与资源化技术国家工程研究中心，黑龙江 哈尔滨 150000
  • 2.重庆大学环境与生态学院，重庆 400044

    • 刘骁(2002-)，男，陕西汉中人，哈尔滨工业大学硕士研究生，主要从事污水处理以及生物质资源化方向研究..

通讯作者:

* 责任作者，教授，;
** 教授，
Conversion of waste oils to green diesel by non-precious metal materials
Xiao LIU1 , Tao XIA2, Jing ZHANG1, * , Chun YANG2, **
Affiliations
  • 1.National Engineering Research Center for Safe Disposal and Resources Recovery of Sludge, School of Environment, Harbin Institute of Technology, Harbin 150000, China
  • 2.College of Environment and Ecology, Chongqing University, Chongqing 400044, China
出版时间: 2025-04-20
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摘要
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以高效催化废弃油脂水热脱氧制备绿色柴油为目标，制备了多种非贵金属催化剂并通过硬脂酸水热脱氧实验对其进行了筛选.其中纳米铜镍合金针对硬脂酸催化效果较佳且催化性能与产物分布与Pt/C催化剂最为接近，进一步对其进行了反应条件优化、稳定性分析、催化剂表征、反应机理探究以及广谱性分析.表征结果显示纳米铜镍合金结构较为稳定，在多次循环使用后并未发生明显结构改变.反应温度330℃、反应时间120min、在1.67mL微型反应釜中加入20µL甲醇、30mg催化剂、80µL水的最佳反应条件下，纳米铜镍合金主要通过催化加氢脱氧及脱羰过程将硬脂酸转化为十七烷.广谱性分析表明其催化多种脂肪酸及脂肪酸酯的C8-C18烷烃产率均可达95%以上，证明了其优异的催化性能.

废弃油脂  /  催化脱氧  /  绿色柴油  /  非贵金属催化剂

Varieties of non-noble metal catalysts were prepared and screened by hydrothermal deoxidation of stearic acid for the purpose of efficiently catalyzing the conversion of waste oil into green diesel. The experimental results demonstrated that the nano-Ni-Cu alloy exhibited a significant catalytic effect on stearic acid, with its catalytic performance and product distribution being the most comparable to those of the Pt/C catalyst. Furthermore, the optimization of reaction conditions, stability analysis, catalyst characterization, reaction mechanism exploration and broad-spectrum analysis were carried out for nano Ni-Cu alloy. The characterization results revealed that the structure of nano-Ni-Cu alloy remained stable, and no significant structural changes were observed after continuous cyclic use. Under the optimum reaction conditions of 330℃, 120min, with the addition of 20µL methanol,30mg catalyst and 80µL water in a 1.67ml micro reactor, stearic acid was primarily converted into heptadecane through catalytic hydrodeoxygenation and decarbonylation. Additionally, the broad-spectrum analysis indicated that the yield of C8-C18 alkanes from various fatty acids and fatty acid esters catalyzed by nano-Ni-Cu alloy could exceed 95%, conforming its excellent catalytic performance.

waste oils  /  catalytic deoxygenation  /  green diesel  /  non-noble metal catalysts
刘骁, 夏涛, 张静, 阳春. 非贵金属材料催化废弃油脂制备绿色柴油. 中国环境科学, 2025 , 45 (4) : 1889 -1900 .
Xiao LIU, Tao XIA, Jing ZHANG, Chun YANG. Conversion of waste oils to green diesel by non-precious metal materials[J]. China Environmental Science, 2025 , 45 (4) : 1889 -1900 .
正文
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废弃油脂包括废弃食用油、地沟油、煎炸老油等，主要化学组分为脂肪酸甘油酯、游离脂肪酸及多种杂质.废弃油脂不仅产量高、存在广泛且危害较大.目前，通过催化废弃油脂水热脱氧制备绿色柴油被认为是对其进行资源化处理的有效方法[1].绿色柴油热值高、性能优异且排放低，是一种潜力巨大的新型燃料[2].将废弃油脂转化为绿色柴油能够有效促进能源结构优化，实现碳减排目标.
废弃油脂制备绿色柴油的关键是通过加氢脱氧、脱羧[3]、脱羰[4]等方式选择性脱除油脂中的多种含氧基团.这些反应均需在催化剂和高温条件下才能高效进行.金属类非均相催化剂由于活性较高、便于回收而应用广泛，尤其是Pt[5]、Pd[6]、Ru[7]等多种贵金属催化剂由于催化活性极佳而备受关注，但其使用成本较高.
研究指出，采用Cu、Ni、Co、Mo、W等活性非贵金属制备催化剂，可在确保催化活性的同时降低成本.常见的制备处理手段包括改性处理、掺杂及制备合金等.目前已有多项研究证实了非贵金属催化剂应用于油脂催化脱氧的可行性.如NiMo基催化剂对废弃大豆油[8]、麻风树油[9]、棕榈油[10]和废食用油[11]均具有较好催化效果，负载NiFe[12]、NiCo[13]、Fe/Cu[14]的催化剂也表现出良好催化性能.
本研究通过针对硬脂酸的催化脱氧实验对多种非贵金属材料催化剂进行了筛选.最终选取了其中催化性能及产物分布最优的纳米铜镍合金催化剂进行了表征、反应条件优化、广谱性分析、稳定性探究及反应机理探究.旨在为废弃油脂催化脱氧制备绿色柴油提供一种新思路.
1　材料与方法
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1.1　实验试剂与催化剂材料
实验所用试剂与催化剂材料均从商家购买.
其中纯度98%的硬脂酸（C18H36O2）、棕榈酸（C16H32O2）、月桂酸（C12H24O2）、氢氧化钠（NaOH）及99.5%的甲醇（CH4O）、乙醇（C2H6O）购自麦克林试剂有限公司；纯度99.75%的硬脂酸甲酯（C19H38O2）及99.08%的十八醇（C18H38O）购自上海毕得医药科技有限公司；30%的过氧化氢（H2O2）、分析纯的C8-C20烷烃标准溶液购自默克生命科学有限公司；纯度98%的油酸（C18H34O2）及分析纯的二氯甲烷（CH2Cl2）购自成都科隆化学品有限公司；实验用水均为超纯水.
纯度99.5%的纳米四氧化三钴（Co3O4）、纳米氧化铜（CuO）、纳米氧化镍（NiO）、纳米二硫化钼（MoS2）、氧化钨铜（CuO4W）及第威德合金（AlCuZn）购自麦克林试剂有限公司.实验所用纳米四氧化三钴具有尖晶石型晶体特性，最大粒径约为250nm；纳米氧化铜具有单斜晶系结构，最大粒径约为150nm；纳米二硫化钼具有独特的钼、硫原子层间夹层结构，Mo含量约60%，平均粒径约为100nm；氧化钨铜中WO6正八面体通过共用顶角氧原子形成四方晶系，粒径为纳米级；第威德合金中Cu:Al:Zn质量比约为10:9:1，粒径为40~80μm.碳化钨钴（CHCoW）、纯度99.5%的纳米铁镍钴合金（FeNiCo）、纯度98%的纳米镍铜合金（NiCu）及镍铝合金（AlNi）购自上海阿拉丁生化科技股份有限公司.碳化钨钴中碳化钨（WC）颗粒与钴（Co）的质量比为94:6，粒径为纳米级；纳米铁镍钴合金中Fe:Ni:Co质量比约为54.3:28.7:17，最大粒径约为500nm；镍铜合金具有单相面心立方结构，Ni:Cu质量比约为70:30，最大粒径约为150μm；镍铝合金中Ni:Al质量比约为50:50，最大粒径约为150μm.5wt%的Pt/C催化剂购自默克生命科学有限公司，催化剂中Pt纳米颗粒均匀分散于高比表面积的活性炭表面，活性位点丰富.镍包铝（NiAl）购自华北金属合金材料，该材料是由镍包覆在铝芯核表面形成的复合粉，Ni:Al质量比约为80:20.高熵合金（FeCoNiCuAl）购自北京中科言诺新材料科技有限公司，材料中Fe:Al:Co:Ni:Cu质量比约为10:35:10:35:10，最大粒径约为105μm.白铜粉（CuNi）购自北京市金属粉末研究院，具有面心立方晶格，材料中Al:Cu质量比约为25:75，最大粒径约为50μm.镍钴锰酸锂（LiNixCoyMn1-x-yO2）购自深圳市锂优新能源科技有限公司，该材料具有独特的层状结构，材料中Li:Ni:Co:Mn:O质量比约为7.6:20.6:21:16.6:34.2，最大粒径约为16μm.
1.2　试验方法
1.2.1　催化剂改性
本研究对镍包铝、高熵合金、白铜粉三种催化剂分别进行氧化改性和碱腐蚀改性，步骤如下.
氧化改性:将适量催化剂置于过氧化氢溶液（30%）中搅拌反应5h后离心分离.分离后的固体在超声中用超纯水和乙醇清洗3次，在80℃下干燥5h后研磨过筛（100目），得到所需催化剂粉末，记作白铜粉-O、镍包铝-O、高熵合金-O.
碱腐蚀改性:将适量催化剂在80℃的5mol/L的NaOH水溶液中反应12h后离心回收固体.分离后的固体在超声中用去离子水和乙醇清洗3次后在80℃下干燥5h后研磨过筛（100目）得到所需催化剂粉末，记作白铜粉-OH、镍包铝-OH、高熵合金-OH.
1.2.2　硬脂酸水热催化脱氧反应
在微型反应釜中加入50mg（0.176mmol）硬脂酸、30mg催化剂、480μL水和20μL甲醇后密闭并摇晃均匀，置于预热至反应温度的管式炉中加热.加热过程中每隔5min旋转一次以确保釜内温度均匀，达到预设时间后立即冷却反应釜以终止反应.完全冷却后打开反应釜，将其放入50mL的离心管中加入35mL乙酸乙酯密封，摇晃30min后静置24h.随后将浸泡液倒入50mL容量瓶中定容，溶液经过0.22μm聚四氟乙烯滤膜过滤后，用GC-FID定量分析.所有实验结果均以至少3次重复的平均±标准偏差为准.
每次实验结束后将浸泡液在4000r/min下离心5min后回收固体催化剂.分离后的催化剂经二氯甲烷洗涤、真空抽滤、滤膜过滤、干燥后收集以进行表征或用于重复试验.
1.3　产物检测与分析
实验中采用气相色谱仪（GC-FID）对液态产物进行定量分析.仪器型号为Aglient 8890-2，色谱柱为Aglient HP-5（30m×0.32mm×0.25µm），进样温度280℃，FID检测器温度为300℃.程序升温从60℃开始，保持1min后，以每8℃/min的速率升至290℃.本次实验采用外标法对测样结果进行定量分析.自行配置标准样并以峰面积为纵坐标，脂浓度为横坐标绘制标准曲线，并拟合回归方程、确定线性范围及相关性.反应中相关参数的计算方法如下:
式中:α为反应物的转化率，%；N为投加反应物的总量，mol；n1为反应后剩余反应物的量，mol.
式中:γ为目标产物的产率，%；nx为反应后对应产物的量，mol.
式中:Se为目标产物的选择性，%.
实验中多次重复实验的数据值为3次实验平均值，其实验误差范围用标准偏差表示.
式中:S为标准偏差值；n为实验次数；xi为每次实验的测量值；为实验测量值的平均值.
1.4　催化剂表征
运用ZEISS SIGMA 500型扫描电子显微镜（SEM）对催化剂进行了形貌表征，表征前催化剂样品被分散在碳导电极上.全自动比表面积孔隙度分析仪（QuadraSorb Station 3）用于测定样品的氮气吸附-脱附等温线，运用Brunauer-Emmett-Telle（BET）法与Barrett-Joyner-Halenda（BJH）法分别计算催化剂的比表面积与孔径分布、孔容.通过X'Pert PRO衍射仪分析样品的晶体结构及物相组成.运用ESCALAB 250Xi型XPS仪在测试电压15kV、测试电流10mA时分析催化剂表面的元素组成、元素含量、化学状态.测试中所用靶源为Al Kα （1486.6eV），测试所得信号通过Cls（284.8eV）进行校正.使用电感耦合等离子体发射光谱仪（ICP-OES）测定催化剂内部元素种类及含量，测试中选用酸试剂为空白样品以消除背景元素干扰.
2　结果与讨论
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2.1　非贵金属吸附剂的筛选
购买了14种常见非贵金属材料，对其中部分材料进行改性处理，共获得了22种不同的催化剂.通过以硬脂酸为底物的水热催化脱氧反应，比较了不同催化剂的性能.
如图1所示，在330℃、反应时间120min，加入50mg底物、20μL甲醇、480μL水的反应条件下，第威德合金和纳米铜镍合金的催化性能最好.反应过程中两者对应的硬脂酸转化率分别为100.00%、98.16%，C8-C18烷烃产率分别为99.16%、96.43%，总体性能与Pt/C催化剂相近.
进一步对第威德合金、纳米铜镍合金和Pt/C催化剂的催化产物进行表征，结果如图2所示.在Pt/C催化产物中十七烷与十八烷产率分别为94.34%、5.55%，此时硬脂酸主要通过脱羧/脱羰转化为十七烷，同时通过加氢脱氧生成少量十八烷[15].纳米铜镍合金的催化产物分布与Pt/C催化剂最为相似，十七烷与十八烷产率分别为95.89%、0.57%，其催化硬脂酸加氢脱氧的活性略低于Pt/C.而第威德合金的催化产物中十七烷产率较低，包含多种C8-C16裂解烷烃.此时硬脂酸除脱氧反应外还发生了裂解反应，促进了短链烷烃产生.相比之下，纳米铜镍合金催化裂解反应的能力更弱，可能是因为铜镍合金抑制了C-C键的断裂，提高了十七烷的选择性[16].基于以上实验结果，选择纳米铜镍合金开展后续研究.
2.2　纳米铜镍合金催化脱氧反应条件优化
2.2.1　反应温度优化
在不同反应温度（260~360℃）下，向反应釜内加入50mg硬脂酸、30mg催化剂、20μL甲醇、480μL水，反应120min.
由图3（a）可知，随着反应温度从260℃上升至330℃，硬脂酸转化率快速上升.进一步升高温度至360℃，硬脂酸转化率增加缓慢，几乎达到完全转化.
图3（b）中的产物选择性分布表明260℃时硬脂酸主要转化产物为硬脂酸甲酯，同时产生少量十七烷和十八醇.在260~300℃的升温过程中，硬脂酸甲酯选择性下降，十八醇和十七烷的选择性上升.至300℃时，十八醇选择性最高、十七烷次之.升温至330℃，十七烷成为主要产物，其余产物选择性极低.继续升温至360℃，十七烷选择性几乎达到100%.产物选择性变化表明，硬脂酸催化脱氧过程中前期与中期的主要中间产物分别是硬酯酸甲酯与十八醇.反应温度高于330℃时，中间产物基本完全转化，釜内主要反应为硬脂酸脱氧生成烷烃.基于经济性原则，选择330℃为最佳反应温度进行后续研究.
2.2.2　反应时间优化
在反应温度330℃时，向反应釜内加入50mg硬脂酸、30mg催化剂、20μL甲醇、480μL水，探究反应时间对催化脱氧反应的影响.
如图4（a）所示，当反应时间从30min延长到120min时硬脂酸转化率迅速增加.继续增加反应时间至150min，硬脂酸的转化率略有上升，几乎完全转化.
图4（b）中产物选择性分布显示硬脂酸的转化产物主要是十八醇及十七烷，并未观察到硬脂酸甲酯的产生.反应时间30~120min时，随着反应时间增加，反应主要产物从十八醇逐渐转变为十七烷，印证了十八醇是反应中的主要中间产物.继续延长反应时间，十七烷选择性保持稳定.除此之外，在整个反应过程中均未观察到裂解烷烃，只观察到了微量十八烷.基于经济性原则，选择120min作为最佳反应时间.
2.2.3　纳米铜镍合金投加量优化
在反应温度为330℃时，向反应釜内加入50mg硬脂酸、20μL甲醇、480μL水，在反应时间120min时探究催化剂投加量对催化脱氧反应的影响.
由图5（a）可知，当催化剂的投加量从7mg增加到30mg时，硬脂酸转化率和十七烷产率逐渐增加，硬酯酸甲酯与十八醇产率逐渐下降.进一步增加催化剂用量至50mg，硬脂酸转化率几乎不变，十八醇与硬酯酸甲酯几乎完全转化生成十七烷.
图5（b）中的产物选择性分布显示在催化剂投加量为7mg时主要产物为十八醇，次要产物为十七烷，同时还出现了硬脂酸甲酯和微量十八烷.随着催化剂投加量的增加，十七烷选择性逐渐增加，而其余产物的选择性逐渐降至几乎为0.这说明催化剂投加量的增加促进了硬酯酸甲酯的转化以及十八醇脱羰产生十七烷.综合考虑，选择催化剂投加量30mg作为最佳的反应条件.
2.2.4　水投加量优化
在反应温度为330℃时，向反应釜内加入50mg硬脂酸、20μL甲醇、30mg催化剂，在反应时间120min时探究水投加量对催化脱氧反应的影响.
如图6（a）所示，水的投加量变化对硬脂酸转化几乎没有影响.在无水条件下硬脂酸的转化率仍超过98%，但此时产物中十七烷、十八烷、十八醇和硬脂酸甲酯的产率之和远小于硬脂酸的转化率，表明还有其他副产物存在.结合GC-FID结果和往期研究进行分析，推测这些物质可能是:1.硬脂酸通过聚合反应产生的酸酐或酮[17]；2.十八醇与硬脂酸通过酯化生成的硬脂酸酯[18]；3.硬脂酸脱羧产生的十七烷自由基通过二聚作用产生的C34等长链烷烃[19].
图6（b）显示无水条件下产物以十七烷为主，此时出现了少量硬脂酸甲酯和痕量的十八烷.增加水的投加量至80μL，十七烷的选择性略有上升，而硬脂酸甲酯几乎完全消失.进一步将水的投加量增加至780μL，此过程中硬脂酸的转化率和产物选择性几乎不变，且无裂解烷烃产生.秉承经济性原则，确定80μL为水的最佳投加量.
2.2.5　甲醇投加量优化
在反应温度为330℃时，向反应釜内加入50mg硬脂酸、80μL水、30mg催化剂，在反应120min时探究甲醇投加量对催化脱氧反应的影响.
如图7（a）所示，在无甲醇条件下硬脂酸转化率较低.此时硬脂酸可能通过脱羧产生少量十七烷，也可通过水热原位产生微量氢气参与反应.随着甲醇投加量增加，硬脂酸转化率和十七烷产率同步增加，并在投加量20μL时达到最大.继续增加甲醇投加量，硬脂酸转化率几乎不变，而十七烷选择性下降、十八烷选择性略有上升.这是因为甲醇投加量的增加导致氢气产量和压力增大，促进了硬脂酸通过加氢脱氧产生十八烷.
由图7（b）可知，在甲醇投加量的变化过程中，十七烷作为反应主要产物其选择性始终保持较高水平，而其余产物选择性极低.综合考虑，选择20μL为甲醇最佳投加量.
综上所述，将330℃、反应时间120min，投加20μL甲醇、80μL水、30mg纳米铜镍合金催化剂确定为最佳反应条件.此时硬脂酸转化产物分布如表1所示.
2.3　纳米铜镍合金催化剂稳定性分析
在最佳实验条件下，对纳米铜镍合金进行了3次重复利用实验以考察其稳定性.循环实验结果如图8所示，随着循环实验次数的增加，纳米铜镍合金的催化活性逐步下降.催化剂活性的降低可能是由于多种原因造成的，具体原因将在2.4节中结合催化剂表征结果详细分析.
2.4　反应前后纳米铜镍合金催化剂的表征
2.4.1　催化剂的形貌分析
纳米铜镍合金催化剂反应前后的电子扫描显微镜表征如图9所示，可以看出反应前纳米铜镍合金催化剂呈现疏松多孔的结构与较为均匀的球形.而反应三次后的催化剂整体上虽然未发生较大结构改变，但可在其表面发现明显的结块，这可能是由于反应中间体或产物在催化剂表面的吸附造成的.由图10可知，催化剂中Cu和Ni高度重合，形成了稳定的合金结构，有助于减少由于金属流失或结构变化导致的性能下降[20].并且图中氧元素的出现表明催化剂中还可能含有金属氧化物.
2.4.2　催化剂的比表面积和孔隙度分析
纳米铜镍合金催化剂反应前后的N2吸附-脱附等温线和孔径分布如图11所示.催化剂反应前后均存在介孔结构，这可能是纳米铜镍合金具有高活性的因素之一[21].表2是反应前后纳米铜镍合金催化剂N2吸附-脱附表征的结果，BET与BJH计算分析表明反应三次后催化剂比表面积及平均孔径均有较大程度下降，推测其结构性质的变化可能是由于催化剂结块和孔径堵塞造成的.
2.4.3　催化剂的物相和组成分析
图12中的XRD分析显示纳米铜镍合金催化剂反应前后都只在43.99°、51.25°和75.42°处出现了CuNi的衍射峰，并且衍射峰的强度和宽度无明显改变.这表明合金的晶体结构保持稳定，其失活并非是相变导致的.XRD表征中没有观察到金属氧化物，但是形貌分析显示催化剂中含有氧元素.推测催化剂表面的氧元素可能是由于表面微量金属元素氧化或吸附氧造成的.
2.4.4　催化剂的表面化学分析
反应前纳米铜镍合金催化剂的XPS谱图如图13（a-c）所示.可以从图中观察到Ni0对应的Ni 2p1/2、Ni 2p3/2特征峰以及NiO对应的Ni 2p1/2、Ni 2p3/2特征峰与卫星峰，这代表催化剂表面中存在Ni0与NiO.同时，从图中观察到了Cu0对应的Cu 2p3/2、Cu 2p1/2特征峰以及CuO的Cu 2p3/2、Cu 2p1/2特征峰和卫星峰，表明催化剂表面存在Cu0和CuⅡ.晶格氧与吸附氧的特征峰的存在表明催化剂表面存在金属氧化物，印证了XRD分析中的结果.
图13（d-f）为反应后催化剂的XPS谱图，此时观察到了Ni0、NiO、Cu0与表面吸附氧的特征峰，而并未出现CuO的特征峰.分析可知，此时Ni0和NiⅡ的原子比从2.9:97.2变为33.2:66.7，而CuⅡ则几乎全部被还原，同时几乎没有观察到晶格氧的特征峰.这代表催化剂在硬脂酸的脱氧反应中被氢气高度还原.
研究表明，投加氢气或使用供氢剂不仅可以促进油脂的水热脱氧反应，还可同时实现针对活性金属催化剂的再生还原.除此之外，氢气或供氢剂还可实现Cu、Cu2O和CuO之间的循环转化，从而提高含Cu催化剂的催化脱氧活性[16].在本章的研究中，活性金属的连续价态转换导致催化剂中氧空位增加，进而促进了脱氧反应的进行，提高了硬脂酸的转化效率.
2.4.5　催化剂的元素分析
反应前后的纳米铜镍合金催化剂中的元素组成变化通过ICP-OES分析进行测定.使用前纳米铜镍合金催化剂中Cu的含量为52.79wt%，Ni的含量为47.20wt%.在使用3次后，纳米铜镍合金催化剂中的活性金属含量轻微下降，Cu的含量变为50.96wt%，Ni的含量变为45.04wt%.结合XRD分析结果，可以认为纳米铜镍合金具有较高的结构稳定性.催化剂中Cu与Ni的含量轻微降低可能是因为反应中间体或产物在催化剂表面的吸附造成催化剂质量增大，导致活性金属的相对含量降低.
以上表征结果证明了纳米铜镍合金催化剂重复使用后其组成与结构保持稳定.有研究表明，合金催化剂中Cu的存在可以阻止催化剂因结构破坏而失活[22]，因此推测纳米铜镍合金的失活可能是由于催化剂中毒导致的.反应过程中，硬脂酸转化中间产物、副产物与杂质等通过化学吸附结合到催化剂的活性位点上，并通过聚合、沉积将其覆盖[17].多次重复使用后，催化剂的活性位点暴露数下降，其催化活性也显著下降.这种因有机物的吸附或沉积导致的催化剂中毒失活通常是可逆的，可通过洗涤或煅烧实现再生.
为进一步研究纳米铜镍合金失活的可逆性，将反应3次后的催化剂在60℃的二氯甲烷溶剂多次进行2h洗涤，以充分去除其表面吸附与沉积的有机物.再生后的催化剂在最佳条件下重复用于硬脂酸的水热脱氧反应，此时硬脂酸的转化率和烷烃产率恢复到较高水平.充分证明了纳米铜镍合金失活的可逆性.
除了通过再生处理恢复催化剂活性外，还可考虑通过催化剂的结构设计或改性以提高其稳定性.可以向铜镍合金中引入其他金属元素，通过调节金属催化剂的晶体平面结构来减缓其表面的有机物吸附与沉积.此外，还可通过对催化剂表面进行改性，或通过电沉积涂层、合金涂层、有机材料涂层等手段增强其疏水性与稳定性，对催化剂表面形成保护.
2.5　纳米铜镍合金催化硬脂酸脱氧反应机理研究
在反应温度330℃、反应时间120min的条件下，向1.67mL微型反应釜中加入50mg十八醇、80μL水、30mg催化剂，考察了甲醇的投加对十八醇催化转化的影响.
反应结果如表3所示，未投加甲醇时较高的十七烷产率表明硬脂酸加氢产物十八醇可能通过脱羰过程直接转化为十七烷.加入甲醇后十七烷的产率下降，而裂解产物C8-C16和加氢产物C18的产率上升，这可能是因为甲醇提供了加氢裂解和加氢脱氧所需要的氢气以及反应压力.
基于本章和其他研究[23-25]，提出以纳米铜镍合金催化硬脂酸水热脱氧的3种途径如图14所示:主要途径为硬脂酸通过加氢脱氧转化为十八醇，十八醇进一步通过脱羰生成主要产物十七烷.次要途径共有两种，一种是硬脂酸直接通过脱羧生成十七烷；另一种则是硬脂酸加氢脱氧产生十八醇，而十八醇进一步加氢脱氧产生十八烷.在所有的反应途径中十七烷和十八烷均可通过加氢裂解产生少量短链烷烃.此外，在脱氧前可能会发生副反应:硬脂酸与甲醇酯化生成硬脂酸甲酯，硬脂酸甲酯水解又会重新生成硬脂酸和甲醇.反应中加氢脱氧和加氢裂解所需的氢气则主要来源于甲醇的水相重整和裂解.如上所述，十八醇与硬脂酸甲酯是反应主要中间产物，在最佳反应条件下几乎完全转化.当反应条件选取不当致使中间产物过量时，可能会造成副反应加剧或者影响催化剂活性，最终导致十七烷产率下降.结合以上反应途径，可以进一步优化反应条件，减少副反应的发生，在提高目标产物产率的前提下确保经济性原则.例如，十八醇的加氢脱氧反应相比脱羰消耗更多氢气，可以通过调整反应条件抑制加氢脱氧、促进脱羰过程，从而减少对甲醇的消耗.
2.6　纳米铜镍合金催化剂广谱性分析
实际废弃油脂组成复杂，其主要成分通常包含各类饱和脂肪酸、不饱和脂肪酸和脂肪酸酯等.为此研究了纳米铜镍合金在其最优反应条件下催化硬脂酸、棕榈酸、月桂酸和硬脂酸甲酯的催化活性，反应结果如表4、表5所示.
表4中反应结果表明，纳米铜镍合金对四种脂肪酸及硬脂酸甲酯均具有较好的催化效果.其中硬脂酸、棕榈酸、月桂酸和硬脂酸甲酯的主要催化产物为C8-C18烷烃，产率均超过85.00%.
油酸的转化率与对应C8-C18烷烃产率相差较大，对油酸催化产物进行进一步分析如表5所示.油酸主要催化产物为硬脂酸，此外还存在硬脂酸甲酯、C8-C18烷烃、十八醇和杂质等其他产物，这可能是由于油酸中C=C双键的异构化、芳构化造成的[26].作为一种不饱和脂肪酸，油酸在催化反应过程中先通过双键加氢饱和转化为脂肪酸，脂肪酸进一步脱氧产生烷烃.因此，不饱和脂肪酸在催化脱氧过程中对于催化剂活性与氢气量的消耗显著高于饱和脂肪酸，导致其脱氧难度更大、副产物产量更高.真实油脂中的不饱和脂肪酸可能会影响纳米铜镍合金的催化效果，针对这一问题可给出多种策略.首先，可适当优化反应条件，如增大甲醇投加量、延长反应时间等；其次，可考虑先对不饱和油脂进行加氢饱和处理，再进行催化脱氧；最后，可考虑对催化剂进行进一步的改性与掺杂以提高其催化效能，以确保不饱和脂肪酸的高效催化转化.
3　结论
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3.1　本研究选择并制备了多种非贵金属材料催化剂并通过硬脂酸脱氧实验进行了筛选，其中纳米铜镍合金的催化性能与产物分布最接近Pt/C催化剂.
3.2　纳米铜镍合金催化硬脂酸脱氧的最佳反应条件为:反应温度330℃，反应时间120min，在1.67mL微型反应釜中加入50mg（0.176mmol）硬脂酸、20μL甲醇、30mg催化剂、80μL水.
3.3　在催化脱氧过程中甲醇通过热解和水相重整产生的氢气可将被氧化的活性金属还原再生，从而提升了纳米铜镍合金催化剂的催化效率.而催化剂在重复使用后的活性下降是由于可逆的催化剂中毒导致的，催化剂的内部结构与金属价态则保持稳定.
3.4　纳米铜镍合金催化硬脂酸转化的主要途径是硬脂酸加氢脱氧产生十八醇中间体，进而脱羰生成主要产物十七烷.
3.5　广谱性研究证明纳米铜镍合金催化剂对多种脂肪酸及硬脂酸酯均具有较好催化效果.其对不饱和脂肪酸的催化脱氧效果较差可能是因为加氢饱和过程额外消耗了催化剂活性和氢气.
基金
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  • 国家自然科学基金面上项目(22076016)
  • 国家自然科学基金优秀青年科学基金项目(22422602)
  • 全处置与资源化技术国家工程研究中心科研基金项目(Z2024A016)
文献
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参考文献 引证文献
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2025年第45卷第4期
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  • 接收时间：2025-02-15
  • 首发时间：2026-03-19
  • 出版时间：2025-04-20
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  • 收稿日期：2025-02-15
基金
国家自然科学基金面上项目(22076016)
国家自然科学基金优秀青年科学基金项目(22422602)
全处置与资源化技术国家工程研究中心科研基金项目(Z2024A016)
作者信息
    1.哈尔滨工业大学环境学院，污泥安全处置与资源化技术国家工程研究中心，黑龙江 哈尔滨 150000
    2.重庆大学环境与生态学院，重庆 400044

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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
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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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