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Article(id=1276616366408995675, tenantId=1146029695717560320, journalId=1235980609244409860, issueId=1276616263778562546, articleNumber=null, orderNo=null, doi=10.3969/j.issn.1000-2561.2025.11.018, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1748188800000, receivedDateStr=2025-05-26, revisedDate=null, revisedDateStr=null, acceptedDate=1752422400000, acceptedDateStr=2025-07-14, onlineDate=1782298660137, onlineDateStr=2026-06-24, pubDate=1764000000000, pubDateStr=2025-11-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1782298660137, onlineIssueDateStr=2026-06-24, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1782298660137, creator=13701087609, updateTime=1782298660137, updator=13701087609, issue=Issue{id=1276616263778562546, tenantId=1146029695717560320, journalId=1235980609244409860, year='2025', volume='46', issue='11', pageStart='2549', pageEnd='2815', issueExtLink='null', onlineDate='null', pubDate='1764000000000', pubDateStr='2025-11-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1782298635668, creator='13701087609', updateTime=1782299117657, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1276618285483426694, tenantId=1146029695717560320, journalId=1235980609244409860, issueId=1276616263778562546, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1276618285487620999, tenantId=1146029695717560320, journalId=1235980609244409860, issueId=1276616263778562546, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=2733, endPage=2741, ext={EN=ArticleExt(id=1276616366706791261, articleId=1276616366408995675, tenantId=1146029695717560320, journalId=1235980609244409860, language=EN, title=Optimization and Analysis of Natural Rubber Latex Film Formulation Based on Spherical Symmetric Design, columnId=1237814980427444960, journalTitle=Chinese Journal of Tropical Crops, columnName=Post-harvest Treatment & Agricultural Ecology, runingTitle=null, highlight=null, articleAbstract=

Natural rubber latex serves as the primary raw material for various products, including medical gloves, condoms and tires. Enhancing its formulation can effectively reduce production costs, improve product performance, and enhance the competitiveness of manufacturing industry. In this study, a spherical symmetric design method was employed to optimize the rubber compound formulation. Sulfur, zinc oxide, accelerator UH-301 and antioxidant WSL were selected as key components for the formulation. The investigation focused on three comprehensive indicators: elongation at break, tear strength and tensile strength. The indicators were analyzed through hypothesis modeling, regression analysis and programming solutions to determine the optimal formulation. The vulcanization characteristics and mechanical properties of both the optimized formula and the basic formula for latex vulcanization were tested. The results indicated that the optimized formula (sulfur: 1.50 phr, zinc oxide: 0.25 phr, accelerator UH-301: 0.40 phr, antioxidant WSL: 1.36 phr) was obtained via regression analysis, with an estimated comprehensive strength of 1.2891. Verification tests confirmed the feasibility of the mathematical model constructed using the spherical symmetrical design method. Comparing the optimized formula with the basic latex vulcanization formula revealed that the former significantly outperformed the latter in vulcanization rate and physical-mechanical properties. Specifically, the tensile strength of the vulcanized rubber film with the optimized formula reached 32.2 MPa, an increase of 212.4%, while the tear strength reached 60 kN/m, an increase of 180.1%. The findings further demonstrate the practical application value of the optimized rubber compound formulation and would provide a solid foundation for enhancing the performance of natural latex rubber films.

, authors=null, authorsList=Yulan LI, Shangqi MA, Yingping HE, authorCompany=null, correspAuthors=Yingping HE, 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=1276616367914750825, articleId=1276616366408995675, tenantId=1146029695717560320, journalId=1235980609244409860, language=CN, title=基于球面对称设计天然胶乳胶膜配方优化与分析, columnId=1236286112877048492, journalTitle=热带作物学报, columnName=采后处理与质量安全, runingTitle=null, highlight=null, articleAbstract=

天然胶乳是医用手套、避孕套、轮胎等产品的核心原料，对其进行配方优化可降低生产成本、提升产品性能，直接助力制造业竞争力提升。本研究采用球面对称设计方法，选用硫磺、氧化锌、促进剂UH-301和防老剂WSL进行胶料配方设计，并以断裂伸长率、撕裂强度和拉伸强度为综合考察指标进行假设模型、回归分析、规划求解，从而得到最优配方，检测优化配方与胶乳硫化基础配方的硫化特性和力学性能。结果表明：通过回归分析得到优化配方，即硫磺为1.50 phr（每百克胶乳添加克数），氧化锌为0.25 phr，促进剂UH-301为0.40 phr，防老剂WSL为1.36 phr，综合强度估计值为1.2891，验证试验表明通过球面对称设计构建的数学模型可信。将优化配方与胶乳硫化的基础配方进行比较，前者的硫化速率和力学性能远远优于后者，优化配方硫化胶膜的拉伸强度可达32.2 MPa，增幅达212.4%；撕裂强度可达60 kN/m，增幅达180.1%，进一步表明所得胶料优化配方具有应用价值，为天然胶乳胶膜高性能化奠定基础。

, authors=

李玉兰（2000—），女，硕士研究生，研究方向：天然胶乳加工、改性及应用。

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* 何映平（HE Yingping），E-mail：。
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李玉兰（2000—），女，硕士研究生，研究方向：天然胶乳加工、改性及应用。

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李玉兰（2000—），女，硕士研究生，研究方向：天然胶乳加工、改性及应用。

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A：硫化曲线；B：硫化时间；C：转矩。

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A、C：基础配方；B、D：优化配方。

, figureFileSmall=11edlwGpAnstHSgiwiirpA==, figureFileBig=6xtmdQT6WAu1c5fLTzF9Mw==, tableContent=null), ArticleFig(id=1276616376710206350, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 1, caption=

Experimental scope and level of independent variables

, figureFileSmall=null, figureFileBig=null, tableContent=
样本Sample因素Factor编码形式的因子水平Factor level of encoding form/phr
–2–1012
A硫磺0.5000.7501.0001.2501.500
B氧化锌0.2500.3750.5000.6250.750
C促进剂UH-3010.4000.5000.6000.7000.800
D防老剂WSL0.8000.9751.1501.3251.500
), ArticleFig(id=1276616376932504463, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表1, caption=

自变量的试验范围和水平

, figureFileSmall=null, figureFileBig=null, tableContent=
样本Sample因素Factor编码形式的因子水平Factor level of encoding form/phr
–2–1012
A硫磺0.5000.7501.0001.2501.500
B氧化锌0.2500.3750.5000.6250.750
C促进剂UH-3010.4000.5000.6000.7000.800
D防老剂WSL0.8000.9751.1501.3251.500
), ArticleFig(id=1276616377024779152, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 2, caption=

Experimental scheme

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.硫磺（A）Sulfu/phr氧化锌（B）ZnO/phr促进剂UH-301（C）Accelerator UH-301/phr防老剂WSL（D）Antioxidant WSL/phr
10.75（–1）0.375（–1）0.50（–1）0.975（–1）
20.75（–1）0.375（–1）0.50（–1）1.325（1）
30.75（–1）0.375（–1）0.70（1）0.975（–1）
40.75（–1）0.375（–1）0.70（1）1.325（1）
50.75（–1）0.625（1）0.50（–1）0.975（–1）
60.75（–1）0.625（1）0.50（–1）1.325（1）
70.75（–1）0.625（1）0.70（1）0.975（–1）
80.75（–1）0.625（1）0.50（–1）1.325（1）
90.75（–1）0.375（–1）0.50（–1）0.975（–1）
101.25（1）0.375（–1）0.70（1）1.325（1）
111.25（1）0.375（–1）0.70（1）0.975（–1）
121.25（1）0.375（–1）0.50（–1）1.325（1）
131.25（1）0.625（1）0.50（–1）0.975（–1）
141.25（1）0.625（1）0.50（–1）1.325（1）
151.25（1）0.625（1）0.70（1）0.975（–1）
161.25（1）0.625（1）0.70（1）1.325（1）
170.50（–2）0.500（0）0.60（0）1.150（0）
181.50（2）0.500（0）0.60（0）1.150（0）
191.00（0）0.250（–2）0.60（0）1.150（0）
201.00（0）0.750（2）0.60（0）1.150（0）
211.00（0）0.500（0）0.40（–2）1.150（0）
221.00（0）0.500（0）0.80（2）1.150（0）
231.00（0）0.500（0）0.60（0）0.800（–2）
241.00（0）0.500（0）0.60（0）1.500（2）
251.00（0）0.500（0）0.60（0）1.150（0）
), ArticleFig(id=1276616377112859537, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表2, caption=

试验方案

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.硫磺（A）Sulfu/phr氧化锌（B）ZnO/phr促进剂UH-301（C）Accelerator UH-301/phr防老剂WSL（D）Antioxidant WSL/phr
10.75（–1）0.375（–1）0.50（–1）0.975（–1）
20.75（–1）0.375（–1）0.50（–1）1.325（1）
30.75（–1）0.375（–1）0.70（1）0.975（–1）
40.75（–1）0.375（–1）0.70（1）1.325（1）
50.75（–1）0.625（1）0.50（–1）0.975（–1）
60.75（–1）0.625（1）0.50（–1）1.325（1）
70.75（–1）0.625（1）0.70（1）0.975（–1）
80.75（–1）0.625（1）0.50（–1）1.325（1）
90.75（–1）0.375（–1）0.50（–1）0.975（–1）
101.25（1）0.375（–1）0.70（1）1.325（1）
111.25（1）0.375（–1）0.70（1）0.975（–1）
121.25（1）0.375（–1）0.50（–1）1.325（1）
131.25（1）0.625（1）0.50（–1）0.975（–1）
141.25（1）0.625（1）0.50（–1）1.325（1）
151.25（1）0.625（1）0.70（1）0.975（–1）
161.25（1）0.625（1）0.70（1）1.325（1）
170.50（–2）0.500（0）0.60（0）1.150（0）
181.50（2）0.500（0）0.60（0）1.150（0）
191.00（0）0.250（–2）0.60（0）1.150（0）
201.00（0）0.750（2）0.60（0）1.150（0）
211.00（0）0.500（0）0.40（–2）1.150（0）
221.00（0）0.500（0）0.80（2）1.150（0）
231.00（0）0.500（0）0.60（0）0.800（–2）
241.00（0）0.500（0）0.60（0）1.500（2）
251.00（0）0.500（0）0.60（0）1.150（0）
), ArticleFig(id=1276616377179968402, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 3, caption=

Particle sizes of various compounding agent dispersions

, figureFileSmall=null, figureFileBig=null, tableContent=
样品SampleD10/µmD50/µmD90/µm
硫磺0.320.882.05
氧化锌0.360.972.37
促进剂UH-3010.421.032.55
防老剂WSL0.681.533.48
浓缩天然胶乳（CK）0.380.802.02
), ArticleFig(id=1276616377242882963, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表3, caption=

各种配合剂分散体粒径

, figureFileSmall=null, figureFileBig=null, tableContent=
样品SampleD10/µmD50/µmD90/µm
硫磺0.320.882.05
氧化锌0.360.972.37
促进剂UH-3010.421.032.55
防老剂WSL0.681.533.48
浓缩天然胶乳（CK）0.380.802.02
), ArticleFig(id=1276616377377100692, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 4, caption=

Mechanical properties of natural latex vulcanized film

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.300%定伸应力Stress at 300% elongation/MPa500%定伸应力Stress at 500% elongation/MPa断裂伸长率Elongation at break/%撕裂强度Tear strength/（kN∙m–1）拉伸强度Tensile strength/MPa
10.71.010442622.4
20.81.010455319.2
30.81.011294122.6
40.81.010892420.0
50.81.010262819.2
60.70.911784022.0
70.81.010524824.5
80.81.111063127.9
90.81.110992725.0
100.81.19713017.1
110.81.111602522.3
120.81.110825525.1
130.81.010623822.4
140.81.19874919.1
150.81.110752923.8
160.81.110725527.7
170.60.810871915.3
180.91.311015230.4
190.81.110692720.4
200.81.110223225.1
210.81.012092725.0
220.81.011415424.3
230.91.19793020.4
240.81.110292721.0
250.81.010822725.4
), ArticleFig(id=1276616377452598165, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表4, caption=

天然胶乳硫化胶膜力学性能

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.300%定伸应力Stress at 300% elongation/MPa500%定伸应力Stress at 500% elongation/MPa断裂伸长率Elongation at break/%撕裂强度Tear strength/（kN∙m–1）拉伸强度Tensile strength/MPa
10.71.010442622.4
20.81.010455319.2
30.81.011294122.6
40.81.010892420.0
50.81.010262819.2
60.70.911784022.0
70.81.010524824.5
80.81.111063127.9
90.81.110992725.0
100.81.19713017.1
110.81.111602522.3
120.81.110825525.1
130.81.010623822.4
140.81.19874919.1
150.81.110752923.8
160.81.110725527.7
170.60.810871915.3
180.91.311015230.4
190.81.110692720.4
200.81.110223225.1
210.81.012092725.0
220.81.011415424.3
230.91.19793020.4
240.81.110292721.0
250.81.010822725.4
), ArticleFig(id=1276616377528095638, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 5, caption=

Comprehensive strength calculation results

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.隶属度Membership degree综合强度Comprehensive strength
断裂伸长率Elongationat break撕裂强度Tear strength拉伸强度Tensilestrength
10.30620.18500.47090.3401
20.30830.93610.26010.5353
30.66410.59940.48840.5504
40.49740.12600.31700.2586
50.22870.23580.25810.2462
60.87140.58340.44610.5435
70.33800.81220.60920.6633
80.56650.31780.83980.6037
90.53780.23020.64300.4673
100.00000.29190.12280.1781
110.79330.16370.46590.3778
120.46430.99470.65320.7709
130.38270.53760.47050.4886
140.06430.83960.25280.4687
150.43620.26480.56590.4325
160.42211.00000.82200.8532
170.48640.00000.00000.0486
180.54710.90061.00000.9149
190.40950.22720.34150.3026
200.21260.36020.65450.4926
211.00000.21900.64260.5089
220.71510.95820.59660.7531
230.03140.29590.34220.2926
240.24130.21640.37890.3001
250.46770.22700.67170.4735
), ArticleFig(id=1276616377599398807, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表5, caption=

综合强度计算结果

, figureFileSmall=null, figureFileBig=null, tableContent=
编号No.隶属度Membership degree综合强度Comprehensive strength
断裂伸长率Elongationat break撕裂强度Tear strength拉伸强度Tensilestrength
10.30620.18500.47090.3401
20.30830.93610.26010.5353
30.66410.59940.48840.5504
40.49740.12600.31700.2586
50.22870.23580.25810.2462
60.87140.58340.44610.5435
70.33800.81220.60920.6633
80.56650.31780.83980.6037
90.53780.23020.64300.4673
100.00000.29190.12280.1781
110.79330.16370.46590.3778
120.46430.99470.65320.7709
130.38270.53760.47050.4886
140.06430.83960.25280.4687
150.43620.26480.56590.4325
160.42211.00000.82200.8532
170.48640.00000.00000.0486
180.54710.90061.00000.9149
190.40950.22720.34150.3026
200.21260.36020.65450.4926
211.00000.21900.64260.5089
220.71510.95820.59660.7531
230.03140.29590.34220.2926
240.24130.21640.37890.3001
250.46770.22700.67170.4735
), ArticleFig(id=1276616379239371673, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 6, caption=

Analysis of variance result

, figureFileSmall=null, figureFileBig=null, tableContent=
项目ItemdfSSMSFP
回归分析80.73000.09124.40460.0057
残差160.33140.0207
总计241.0614
), ArticleFig(id=1276616379340034970, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表6, caption=

方差分析

, figureFileSmall=null, figureFileBig=null, tableContent=
项目ItemdfSSMSFP
回归分析80.73000.09124.40460.0057
残差160.33140.0207
总计241.0614
), ArticleFig(id=1276616379528778651, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=EN, label=Tab. 7, caption=

Parameters related to variable terms

, figureFileSmall=null, figureFileBig=null, tableContent=
项目Item系数Coefficient标准误差Standard errortP95%置信区间95% confidence interval
Interce-pt–4.15231.3974–2.97140.0090–7.1146~–1.1899
x113.07513.95233.30820.00444.6966~21.4536
x2–4.17981.4933–2.79900.0127–7.3456~–1.0141
x12–13.22654.0285–3.28330.0047–21.7665~–4.6866
x423.61481.16193.11120.00671.1518~6.0779
x134.38291.33333.28730.00461.5564~7.2093
x43–1.54290.5957–2.58990.0197–2.8058~–0.2800
x2x37.69922.47423.11170.00672.4541~12.9444
x3x4–3.18661.0854–2.93600.0097–5.4875~–0.8858
), ArticleFig(id=1276616379600081820, tenantId=1146029695717560320, journalId=1235980609244409860, articleId=1276616366408995675, language=CN, label=表7, caption=

变量项相关参数

, figureFileSmall=null, figureFileBig=null, tableContent=
项目Item系数Coefficient标准误差Standard errortP95%置信区间95% confidence interval
Interce-pt–4.15231.3974–2.97140.0090–7.1146~–1.1899
x113.07513.95233.30820.00444.6966~21.4536
x2–4.17981.4933–2.79900.0127–7.3456~–1.0141
x12–13.22654.0285–3.28330.0047–21.7665~–4.6866
x423.61481.16193.11120.00671.1518~6.0779
x134.38291.33333.28730.00461.5564~7.2093
x43–1.54290.5957–2.58990.0197–2.8058~–0.2800
x2x37.69922.47423.11170.00672.4541~12.9444
x3x4–3.18661.0854–2.93600.0097–5.4875~–0.8858
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基于球面对称设计天然胶乳胶膜配方优化与分析
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李玉兰 , 马尚圻 , 何映平 *
热带作物学报 | 采后处理与质量安全 2025,46(11): 2733-2741
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热带作物学报 |采后处理与质量安全 2025 , 46 (11) : 2733 -2741
基于球面对称设计天然胶乳胶膜配方优化与分析
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李玉兰, 马尚圻, 何映平*
作者信息
  • 海南大学材料科学与工程学院，海南海口　570228
通讯作者:
* 何映平（HE Yingping），E-mail：。
Optimization and Analysis of Natural Rubber Latex Film Formulation Based on Spherical Symmetric Design
Yulan LI, Shangqi MA, Yingping HE*
Affiliations
  • College of Materials Science and Engineering, Hainan University, Haikou, Hainan 570228, China
出版时间: 2025-11-25 doi: 10.3969/j.issn.1000-2561.2025.11.018
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摘要
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天然胶乳是医用手套、避孕套、轮胎等产品的核心原料，对其进行配方优化可降低生产成本、提升产品性能，直接助力制造业竞争力提升。本研究采用球面对称设计方法，选用硫磺、氧化锌、促进剂UH-301和防老剂WSL进行胶料配方设计，并以断裂伸长率、撕裂强度和拉伸强度为综合考察指标进行假设模型、回归分析、规划求解，从而得到最优配方，检测优化配方与胶乳硫化基础配方的硫化特性和力学性能。结果表明：通过回归分析得到优化配方，即硫磺为1.50 phr（每百克胶乳添加克数），氧化锌为0.25 phr，促进剂UH-301为0.40 phr，防老剂WSL为1.36 phr，综合强度估计值为1.2891，验证试验表明通过球面对称设计构建的数学模型可信。将优化配方与胶乳硫化的基础配方进行比较，前者的硫化速率和力学性能远远优于后者，优化配方硫化胶膜的拉伸强度可达32.2 MPa，增幅达212.4%；撕裂强度可达60 kN/m，增幅达180.1%，进一步表明所得胶料优化配方具有应用价值，为天然胶乳胶膜高性能化奠定基础。

球面对称设计  /  天然胶乳  /  力学性能  /  回归分析  /  配方优化

Natural rubber latex serves as the primary raw material for various products, including medical gloves, condoms and tires. Enhancing its formulation can effectively reduce production costs, improve product performance, and enhance the competitiveness of manufacturing industry. In this study, a spherical symmetric design method was employed to optimize the rubber compound formulation. Sulfur, zinc oxide, accelerator UH-301 and antioxidant WSL were selected as key components for the formulation. The investigation focused on three comprehensive indicators: elongation at break, tear strength and tensile strength. The indicators were analyzed through hypothesis modeling, regression analysis and programming solutions to determine the optimal formulation. The vulcanization characteristics and mechanical properties of both the optimized formula and the basic formula for latex vulcanization were tested. The results indicated that the optimized formula (sulfur: 1.50 phr, zinc oxide: 0.25 phr, accelerator UH-301: 0.40 phr, antioxidant WSL: 1.36 phr) was obtained via regression analysis, with an estimated comprehensive strength of 1.2891. Verification tests confirmed the feasibility of the mathematical model constructed using the spherical symmetrical design method. Comparing the optimized formula with the basic latex vulcanization formula revealed that the former significantly outperformed the latter in vulcanization rate and physical-mechanical properties. Specifically, the tensile strength of the vulcanized rubber film with the optimized formula reached 32.2 MPa, an increase of 212.4%, while the tear strength reached 60 kN/m, an increase of 180.1%. The findings further demonstrate the practical application value of the optimized rubber compound formulation and would provide a solid foundation for enhancing the performance of natural latex rubber films.

spherical symmetric design  /  natural rubber latex  /  mechanical properties  /  regression analysis  /  formulation optimization
李玉兰, 马尚圻, 何映平. 基于球面对称设计天然胶乳胶膜配方优化与分析. 热带作物学报, 2025 , 46 (11) : 2733 -2741 . DOI: 10.3969/j.issn.1000-2561.2025.11.018
Yulan LI, Shangqi MA, Yingping HE. Optimization and Analysis of Natural Rubber Latex Film Formulation Based on Spherical Symmetric Design[J]. Chinese Journal of Tropical Crops, 2025 , 46 (11) : 2733 -2741 . DOI: 10.3969/j.issn.1000-2561.2025.11.018
正文
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天然胶乳（NRL）具有优异的成膜性和易硫化性等综合性能，在日常生活及工业生产中发挥着至关重要的作用[1-2]。已广泛应用于浸渍产品的制造，例如气球、手套、避孕套和导尿管[3-5]。NRL手套和避孕套是其最常见的2种产品。在2019年新冠病毒大流行期间，橡胶手套的需求显著增加，至2021年全球每月销量达650万双[6]。毫无疑问，这种激增极大地促进了NRL产品的生产。然而，随着人们对高性能材料的需求不断增加，NRL产品因其抗拉强度低、抗撕裂性差、易老化等问题，其应用范围受到一定程度的限制[7]。
NRL产品是一种多组分复合材料，包含多种固体和液体添加剂，如交联剂、促进剂、活化剂、填料、抗降解剂、稳定剂以及表面活性剂[8-9]。为了提高NRL产品的力学性能，必须形成交联结构，而交联结构的形成受到硫化配方的影响[10-11]。另外，在天然胶乳产品中产生的喷霜现象与配合剂的用量以及加工工艺有很大关系，并且这一现象也受天然乳胶中各种添加剂比例变化的影响。当前，NRL研究主要集中在先进改性技术[12-13]和生产工艺优化[14-15]方面。尽管这些措施能够显著提高天然胶乳的性能，但同时也可能导致成本增加和环境污染。在此之前，通过合理设计配方以优化材料性能，可以减少后续改性与优化所需的人力物力。因此，合理安排胶乳中配合剂的配比，以实现效果最大化并达到最优配方设计，对于提升胶膜性能具有极其重要的意义。
球面对称设计[16]是在球面设计的基础上，试验次数与正交相当，但试验精度高，并且由此得到的关系式可以确定任何范围内的试验点的预测值，对于需要控制指标和多指标的试验，效果尤为显著[17]，因此该方法已广泛用于药物制剂配方优化[18]、发酵条件优化[19]、药物提取工艺优化[20]等领域。例如，倪孟祥等[21]采用球面对称设计优化两相体系生物转化合成5-氟尿苷，确定其最佳条件，使5-氟尿苷的转化率达75.7%，产量较单水相时提高近5倍。这些特点使球面对称设计适用于配方设计。然而，在天然胶乳配方设计中，各种配合剂的用量需要控制，以此发挥各自最大的作用，却鲜有球面对称设计与其相关配方设计的研究。本研究主要采用球面对称设计方法，根据其原理设计试验水平，进行25个配方试验，随后以断裂伸长率、撕裂强度和拉伸强度为综合考察指标进行假设模型、回归分析、规划求解，从而得到最优配方，并研究最优配方的天然胶乳膜的机械性能和硫化特性，与胶乳硫化的基础配方进行比较。
1　材料与方法
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1.1　材料
浓缩天然胶乳的质量分数为61.5%，由海南象元实业有限公司提供；氢氧化钾为分析纯，广州化学试剂厂；亚甲基二萘磺酸钠（分散剂NF），上海玻尔化学试剂有限公司；硫磺为工业级，上海朗丽化学有限公司；氧化锌为工业级，上海笛柏生物科技有限公司；促进剂UH-301为分析纯，河南鹤壁元昊新材料集团股份有限公司；防老剂WSL为工业级，上海玻尔化学试剂有限公司；纯水，实验室自制。
1.2　方法
1.2.1　试验设计
在本研究中着重考察硫磺、氧化锌、促进剂UH-301和防老剂WSL用量4个因子，每个因子取5个水平，采用球面对称设计法（SSD）对天然胶乳配方进行优化，其因素与水平如表1所示。具体试验方案见表2。
为便于对照，设置基础配方（干基）：NRL为100 phr；KOH为0.1 phr；平平加O为0.1 phr；S为1.0 phr；ZnO为0.4 phr；促进剂UH-301为0.5 phr。
1.2.2　配合剂分散体的制备
称取200 g硫磺置于分散机容器内，然后加入6 g扩散剂NF和300 g水进行搅拌，待搅拌均匀后缓慢加入氧化锆，随后调整转速至2500 r/min，研磨6 h，初步得到预分散悬浊液。最后将悬浊液置于超声波细胞粉碎机中进行超声处理，超声功率调到100%，超声3 s停2 s，超声30 min停止，即可得到细化的硫磺分散体。后续氧化锌、促进剂UH-301和防老剂WSL的研磨步骤与硫磺的研磨步骤一致。
1.2.3　天然胶乳硫化胶膜的制备
根据球面对称设计原理，按表2将硫磺、氧化锌、促进剂UH-301和防老剂WSL分别加入天然胶乳（100 phr）中，在搅拌时加入0.1 phr KOH溶液和适量纯水，得到25个配方的配合胶乳。混合均匀后将配合胶乳转移至水浴锅中，从室温开始加热，当温度为60 ℃并保持不变时，开始计时至1 h结束，及时取出并在室温条件下静置12 h，备用。将预硫化胶乳均匀倒置在水平玻璃板上进行自然干燥，随后置于80 ℃的烘箱中硫化2 h，便可得到硫化胶膜。基础配方硫化胶膜制备流程与上述25个配方的胶膜制备相同。
1.2.4　测试及分析方法
（1）配合剂分散体粒径的测定。采用北京海鑫瑞科技有限公司HL2020-C激光粒度分析仪，在遮光度（光学浓度）为15%左右，湿法测试标准下，测定胶乳和各分散体的粒径大小与分布，粒径基准选择面积，控制其浓度在测试范围内。
（2）天然胶乳硫化胶膜力学性能的测定。参照GB/T 528—2009和GB/T 529—2009的方法测定天然胶乳硫化胶膜的拉伸强度、断裂伸长率和撕裂强度。将硫化胶膜用特定的裁刀裁成哑铃状和直角形，使用高铁科技股份有限公司AI-7000-SU2型拉力机以500 mm/min的速度进行力学性能测试。
（3）天然胶乳预硫化胶乳胶膜硫化特性的测定。参照GB/T 16584—1996的方法，采用MDR-2000E型无转子硫化仪测定配合胶乳胶膜的硫化特性，将试验温度设定在100 ℃，试验时间为30 min。
（4）天然胶乳硫化胶膜交联密度的测定。根据经典的Flory-Rehner方程，采用平衡溶胀法确定硫化胶膜的交联密度。
（5）天然胶乳硫化胶膜拉伸断面形貌的测定。采用场发射扫描电镜（SEM）测定硫化胶膜拉伸断面的形貌。将拉伸断截面涂覆上20 nm的金层，工作电压为20 kV。
（6）综合强度的计算。采用指标隶属度加权评分法，计算胶膜力学性能的综合强度。隶属度按照公式（1）计算，综合强度按照拟定权重（拉伸强度为0.5、撕裂强度为0.4和断裂伸长率为0.1）进行计算（公式2）。
式中，M是指标隶属度，X是指标值，Xmin是指标最小值，Xmax是指标最大值，Y是综合强度，M1、M2、M3分别是断裂伸长率、撕裂强度和拉伸强度的隶属度。
1.3　数据处理
采用Excel 2010软件进行试验数据的整理、统计和分析，采用Origin Pro 2024软件制图。
2　结果与分析
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2.1　配合剂分散体粒径测试结果
根据前期对细化工艺的探索，确定了硫磺、氧化锌等助剂合适的研磨工艺。按照相同步骤对试验所需助剂进行研磨和超声处理，最终得到分散体。利用粒度分析仪进行分散体粒径的检测，结果如表3。从表3可以看出，当累积体积达到90%时，硫磺、氧化锌等配合剂分散体的粒径与天然胶乳粒子粒径接近，证明各配合剂可以与天然胶乳互相融合，并进行反应。配合剂通过细化之后达到更小的粒径，为后续在天然胶乳中的相互反应奠定基础。
2.2　球面对称设计试验分析
为了使天然胶乳胶膜性能达到最佳，需调节硫磺、氧化锌、促进剂UH-301和防老剂WSL四种重要助剂的用量，通过球面对称设计试验配方，并进行假设模型、回归分析和规划求解得到最优配比。
2.2.1　25个配方力学性能测定结果
根据球面对称设计四因素五水平，测定25个配方硫化胶膜的力学性能，其断裂伸长率、撕裂强度和拉伸强度见表4。从表4可以看出，配方21胶膜的断裂伸长率最大，配方12和16胶膜的撕裂强度最大，而配方18胶膜的拉伸强度最大，结果表明，不同用量配合剂之间的作用有差异，使胶膜性能也存在差异。
为综合考虑，将断裂伸长率、撕裂强度和拉伸强度引入隶属度（M）的概念，消除指标的单位，综合强度（Y）按公式（1）和公式（2）进行计算，结果如表5所示。从表5可以看出，配方18胶膜的综合强度最大，这表明配方18中各配合剂充分作用，使得胶膜性能最佳。
2.2.2　回归分析
为进一步考察综合强度与各指标之间的关系，利用Excel软件自带的数据分析工具进行回归分析。
首先，假设回归模型为四元三次一阶方程：y=a+b1x1+b2x2+b3x3+b4x4+b11x12+b22x22+b33x32+b44x42+b111x13+b222x23+b333x33+b444x43+b12x1x2+b13x1x3+b14x1x4+b23x2x3+b24x2x4+b34x3x4+b123x1x2x3+b124x1x2x4+b134x1x3x4+b234x2x3x4。
其次，利用Excel工具库进行“逐步回归择优分析”，结果如表6~表7所示。通过回归分析可以得出R2为0.6877，调整后的R2为0.5316，2个值均在0.5~1.0之间，证明回归模型拟合程度较高。在表6可以得到P值为0.0057，显著小于0.05水平，说明各指标对综合强度具有统计意义的显著影响。同样，在表7中可以看出所有P值均小于0.05，证明此回归模型可用。
将求得的系数代入四元三次一阶方程中，得到回归方程为：y=–4.1523+13.0751x1–4.1798x2– 13.2265x12+3.6148x42+4.3829x13–1.5429x43+7.6992x2x3–3.1866x3x4。其中，F=4.4046，R2=0.6877，P<0.05。可以看出硫磺、氧化锌、促进剂UH-301和防老剂WSL添加量对天然胶乳胶膜性能均有重要影响。
最后，利用Excel工具库进行“规划求解”，以综合强度（Y）作为衡量指标，对上述回归方程在–2<Xi<2范围内进行偏回归求解最大值，得到最优点：A=1.5 phr，B=0.25 phr，C=0.4 phr，D=1.36 phr；理论综合强度（Y）为1.2891。
2.2.3　验证优化配方
以最优解进行验证试验，进行3次试验，得到胶膜的断裂伸长率为1210%，撕裂强度为60 kN/m，拉伸强度为32.2 MPa，转换成Y值为1.1139。与理论预测值相近。综上所述，通过球面对称设计构建的数学模型可信，且得到的最优配方也具有可行性。
2.3　优化配方与基础配方的对比分析
2.3.1　硫化特性对比
不同胶乳配方胶膜的硫化特性对比情况见图1。由图1A可知，优化配方的转矩明显高于基础配方的转矩。焦烧时间（t10）与橡胶烧焦时间之间存在一定相关性；焦烧时间越长，橡胶的加工安全性相对更高。t90为正硫化时间，即在硫化过程中，橡胶达到最佳性能所需的时间。由图1B可知，基础配方与优化配方的t10几乎相同，这表明二者的加工性基本一致。而基础配方的t90明显大于优化配方，这表明优化配方的硫化速率高于基础配方，其原因可能与优化配方中硫磺的用量有关，并且跟其他配合剂的相互作用促进了硫化。最小扭矩（ML）、最大扭矩（MH）和转矩差（MH-ML）的变化情况见图1C。可以看出，优化配方与基础配方相比，二者的ML相差不大，但是前者的MH明显大于后者，因此前者的转矩差大于后者。转矩差与硫化橡胶的交联密度存在一定相关性，其值越大，表明交联密度越高。可以得出，优化配方的交联密度大于基础配方，表明优化配方中的配合剂作用更加明显，提高了硫化胶膜的交联网络。
2.3.2　物理机械性能对比
浓缩天然胶乳硫化胶膜物理机械性能是衡量胶乳制品尤其是浸渍制品产品性能的重要指标[22]。通过测定优化配方和基础配方硫化胶膜的物理机械性能可知，优化配方硫化胶膜的拉伸强度为32.2 MPa，基础配方的拉伸强度为10.3 MPa（图2A）。优化配方的断裂伸长率为1210%，基础配方的断裂伸长率为929%（图2B）。优化配方和基础配方的撕裂强度分别为60、21 kN/m（图2C）。硫化胶膜的物理机械性能与硫磺用量有关，还与其他配合剂用量有关。配合剂加入浓缩胶乳后，在橡胶烃粒子内起硫化交联反应，从而改变橡胶物理机械性能和使用特性。适量的配合剂能与橡胶烃粒子更好地发生硫化交联反应。如图2D所示，基础配方硫化胶膜的交联密度低于优化配方硫化胶膜。与上述分析结果一致。
2.3.3　结构对比
通过扫描电子显微镜（SEM）观察不同配方硫化胶膜的拉伸断口形貌（图3）。基础配方硫化胶膜的拉伸断面形貌相对平坦，仅有少量凸起。相反，优化配方硫化胶膜的断裂形貌则显得更加粗糙，这表明在破坏过程中消耗了更多的应变能。
3　讨论
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本研究以天然胶乳为研究对象，采用球面对称设计方法，根据其试验原理设定5个水平，以硫磺、氧化锌、促进剂UH-301和防老剂WSL为4个因素，设计25个试验配方，测定其物理机械性能，通过对其进行数学模型构建、回归分析、规划求解得到最优配方，并验证优化配方的可行性。此外，将优化配方与胶乳硫化的基础配方进行比较，测定其硫化特性、物理机械性能和形貌结构。结果发现，在配方设计之后通过数学统计分析可以得到天然胶乳优化配方：硫磺为1.50 phr，氧化锌为0.25 phr，促进剂UH-301为0.40 phr，防老剂WSL为1.36 phr，综合强度估计值为1.2891，验证试验表明，通过球面对称设计构建的数学模型可信。在25个配方中，配方18硫化胶膜的综合强度最大，这可能是因为硫磺用量增加，促进交联网络的形成。优化配方中的硫磺用量与配方18相同，其综合强度却高于配方18，可能是经过配方优化之后得到硫磺与促进剂、活性剂和防老剂的最佳配比，使协同效应发挥最大作用，从而加速硫化并优化交联结构，力学性能得到提升。与对照配方（基础配方）相比，优化配方硫化胶膜的硫化速率较快，t90明显小于基础配方，而MH明显大于基础配方，因此转矩差明显大于基础配方。优化配方硫化胶膜的拉伸强度、断裂伸长率和撕裂强度分别为32.2 MPa、1210%和60 kN/m，力学性能和交联密度明显优于基础配方。通过SEM观察得出，优化配方硫化胶膜的拉伸断面较粗糙，而基础配方的断面相对光滑，这与橡胶分子链的交联作用相关，说明分子链在拉伸过程中的运动受到限制，使得在拉伸优化配方硫化胶膜时消耗了更多的应变能。
此前，方豪斌等[23]利用正交设计开展了白炭黑补强天然胶乳胶膜性能的提升研究，揭示不同考察指标（拉伸强度和撕裂强度）对胶乳配方优化的影响，结果表明，相应优化配方硫化胶膜比不含白炭黑配方硫化胶膜性能分别提升35.04%和54.76%。田安伟等[24]采用正交设计法研究硫磺用量、促进剂DPTT用量和填料体系对减振橡胶材料性能的影响，得到兼具低压缩永久变形、优异的物理性能和耐老化性能的减振橡胶材料配方的优化方案：硫磺用量为1.2份，促进剂DPTT用量为0.3份，填料体系采用体系2（炭黑N326、炭黑N774和白炭黑用量分别为20、31、10份）。由此可见，对天然橡胶进行正交设计，选择各种配合剂的最佳组合和配比，可使制品在性能、工艺和成本可行性3个方面取得最佳效果。而本研究采用的球面对称设计方法不仅可以获得最佳配方组合，还可以通过回归分析预测因素间的交互作用，进而以更少试验次数获得最优解，这对复杂配方研究具有显著的效率优势。
球面对称设计方法作为一种常用于药剂学领域的方法，在天然胶乳配方设计的研究中尚无报道。而现阶段国内外缺乏对球面对称设计方法在配方设计方面的研究，同时也缺乏此方法在各领域的应用研究。因此，本研究结果为探究球面对称设计在天然胶乳配方的优化分析提供可靠的理论指导，也为该方法在各领域的应用研究奠定理论基础。
4　结论
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（1）通过采用球面对称设计方法，进行数据模型构建、回归分析和规划求解得到天然胶乳胶膜优化配方：硫磺为1.50 phr，氧化锌为0.25 phr，促进剂UH-301为0.40 phr，防老剂WSL为1.36 phr，综合强度估计值为1.2891，验证试验表明此模型可信。
（2）与胶膜硫化的基础配方相比，优化配方硫化胶膜具有更快的硫化速率和更高的交联密度，拉伸强度和撕裂强度分别提升212.4%和180.1%，说明具有合理配合剂配比的优化配方可以提高其硫化胶的物理机械性能。
基金
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  • 海南省自然科学基金高层次人才项目(521RC1037)
  • 国家自然科学基金项目(52363007)
  • 大学生创新训练计划项目(202410589014)
文献
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2025年第46卷第11期
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doi: 10.3969/j.issn.1000-2561.2025.11.018
  • 接收时间：2025-05-26
  • 首发时间：2026-06-24
  • 出版时间：2025-11-25
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  • 收稿日期：2025-05-26
  • 录用日期：2025-07-14
基金
海南省自然科学基金高层次人才项目(521RC1037)
国家自然科学基金项目(52363007)
大学生创新训练计划项目(202410589014)
作者信息
    海南大学材料科学与工程学院，海南海口　570228

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* 何映平（HE Yingping），E-mail：。
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2种不同金属材料的力学参数
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Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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