{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T09:06:45Z","timestamp":1788944805474,"version":"build-2803163510"},"reference-count":45,"publisher":"MDPI AG","issue":"18","license":[{"start":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T00:00:00Z","timestamp":1788912000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["12302165"],"award-info":[{"award-number":["12302165"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"award":["12302165"],"award-info":[{"award-number":["12302165"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Polymers"],"abstract":"<jats:p>Adaptive vibration control under variable dynamic loading requires damping materials that combine structural stability, efficient energy dissipation, and field-tunable mechanical response. Here, natural-rubber-based magnetorheological elastomers containing coumarone resin (MRE-C), naphthenic oil (MRE-N), or paraffin (MRE-P) were systematically compared through microstructural characterization, dynamic viscoelastic testing, vulcanization kinetics, and equilibrium swelling. MRE-C exhibited pronounced strain-induced softening, whereas MRE-P showed a high relative dynamic sensitivity but limited absolute stiffness. MRE-N achieved the most favorable overall balance, with more continuous anisotropic particle-chain structures and the lowest Payne-effect amplitude (37.90%). At 5 A, its storage modulus increased by 25.8%, close to the 30.9% increase in MRE-P, while maintaining substantially higher absolute G\u2032 and G\u2033 and a nearly unchanged tan \u03b4. MRE-N\u2019s macroscopic advantage was associated with more favorable network formation, with 17.9% and 7.4% lower apparent activation energies and 7.2% and 18.1% higher apparent crosslink densities than MRE-C and MRE-P, respectively. Molecular simulations of representative sulfur bridges further indicated that monosulfidic bridges favored geometric constraint and structural recovery, whereas disulfidic bridges exhibited greater conformational adaptability. These results link plasticizer-dependent vulcanization and crosslinking state with macroscopic magneto-viscoelastic performance and identify naphthenic oil as the most effective of the investigated plasticizers for balancing stiffness, energy dissipation, and magnetic responsiveness.<\/jats:p>","DOI":"10.3390\/polym18182195","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T08:05:43Z","timestamp":1788941143000},"page":"2195","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Plasticizer-Dependent Vulcanization, Crosslinking, and Magneto-Viscoelasticity of Natural Rubber-Based Magnetorheological Elastomers"],"prefix":"10.3390","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3318-784X","authenticated-orcid":false,"given":"Lili","family":"Fan","sequence":"first","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"conceptualization","vocabulary":"credit"},{"role":"funding-acquisition","vocabulary":"credit"},{"role":"writing-original-draft","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"},{"role":"methodology","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7080-5048","authenticated-orcid":false,"given":"Haimin","family":"Zhu","sequence":"additional","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"methodology","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"}]},{"given":"Jianhua","family":"Du","sequence":"additional","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"validation","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-4359-0899","authenticated-orcid":false,"given":"Zhichao","family":"Li","sequence":"additional","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"validation","vocabulary":"credit"}]},{"given":"Haisong","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"writing-review-editing","vocabulary":"credit"}]},{"given":"Yicheng","family":"Su","sequence":"additional","affiliation":[{"name":"School of Automobile and Traffic Engineering, Liaoning University of Technology, Jinzhou 121001, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"data-curation","vocabulary":"credit"}]},{"given":"Wangwei","family":"Li","sequence":"additional","affiliation":[{"name":"School of Automobile and Traffic Engineering, Liaoning University of Technology, Jinzhou 121001, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"validation","vocabulary":"credit"}]},{"given":"Junhui","family":"Yao","sequence":"additional","affiliation":[{"name":"School of Automotive Engineering, Suzhou University of Technology, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"data-curation","vocabulary":"credit"}]}],"member":"1968","published-online":{"date-parts":[[2026,9,9]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"117450","DOI":"10.1016\/j.engstruct.2024.117450","article-title":"Vibration Control of Offshore Wind Turbines with a Novel Energy-Adaptive Self-Powered Active Mass Damper","volume":"302","author":"Li","year":"2024","journal-title":"Eng. Struct."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"119442","DOI":"10.1016\/j.oceaneng.2024.119442","article-title":"Fatigue Reliability Assessment of Floating Offshore Wind Turbines under Correlated Wind\u2013Wave\u2013Current Loads","volume":"313","author":"Yu","year":"2024","journal-title":"Ocean Eng."},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"107601","DOI":"10.1016\/j.ijthermalsci.2022.107601","article-title":"Effect of Thermal Cycling with Various Heating Rates on the Performance of Thermoelectric Modules","volume":"178","author":"Riyadi","year":"2022","journal-title":"Int. J. Therm. Sci."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"113166","DOI":"10.1016\/j.solmat.2024.113166","article-title":"Sequential Thermomechanical Stress and Cracking Analysis of Photovoltaic Modules with Full and Half-Cut Cells","volume":"278","author":"Papargyri","year":"2024","journal-title":"Sol. Energy Mater. Sol. Cells"},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"234274","DOI":"10.1016\/j.jpowsour.2024.234274","article-title":"Impacts of Vibration and Cycling on Electrochemical Characteristics of Batteries","volume":"601","author":"Wang","year":"2024","journal-title":"J. Power Sources"},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"2300182","DOI":"10.1002\/adem.202300182","article-title":"The Modeling of Magnetorheological Elastomers: A State-of-the-Art Review","volume":"25","author":"Saber","year":"2023","journal-title":"Adv. Eng. Mater."},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"7240","DOI":"10.1021\/acsapm.2c01096","article-title":"Magnetorheological Elastomer Films with Controlled Anisotropic Alignment of Polystyrene-Modified Fe3O4 Nanoplates","volume":"4","author":"Shen","year":"2022","journal-title":"ACS Appl. Polym. Mater."},{"key":"ref_8","doi-asserted-by":"crossref","unstructured":"Perales-Mart\u00ednez, I.A., Palacios-Pineda, L.M., El\u00edas-Z\u00fa\u00f1iga, A., Olvera-Trejo, D., Del \u00c1ngel-S\u00e1nchez, K., Cruz-Cruz, I., Ram\u00edrez-Herrera, C.A., and Mart\u00ednez-Romero, O. (2023). Magnetic and Viscoelastic Response of Magnetorheological Elastomers Based on a Combination of Iron Nano- and Microparticles. Polymers, 15.","DOI":"10.3390\/polym15183703"},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"116467","DOI":"10.1016\/j.oceaneng.2023.116467","article-title":"Experimental Study on Semi-Active Magnetorheological Elastomer-Based Isolation System for Offshore Platform Using Wave Tank","volume":"292","author":"Leng","year":"2024","journal-title":"Ocean Eng."},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"3319","DOI":"10.1007\/s11071-023-09194-z","article-title":"A New Method to Characterize the Nonlinear Magneto-Viscoelasticity Behavior of Magneto-Active Elastomers under Large Amplitude Oscillatory Axial (LAOA) Loading","volume":"112","author":"Vatandoost","year":"2024","journal-title":"Nonlinear Dyn."},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"6090","DOI":"10.1021\/acs.macromol.1c00354","article-title":"Correlation between Macroscopic Elasticity and Chain Dynamics of Natural Rubber during Vulcanization as Determined by a Unique Rheo-NMR Combination","volume":"54","author":"Nie","year":"2021","journal-title":"Macromolecules"},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"12623","DOI":"10.1021\/acsapm.4c02147","article-title":"How Do Active Chain Density and Cross-Link Length Influence the Mullins Softening in Filled and Unfilled Natural Rubbers?","volume":"6","author":"Delahaye","year":"2024","journal-title":"ACS Appl. Polym. Mater."},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"110513","DOI":"10.1016\/j.polymdegradstab.2023.110513","article-title":"Evolution of Crosslinking Structure in Vulcanized Natural Rubber during Thermal Aging in the Presence of a Constant Compressive Stress","volume":"217","author":"Kong","year":"2023","journal-title":"Polym. Degrad. Stab."},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"110871","DOI":"10.1016\/j.polymdegradstab.2024.110871","article-title":"The Effect of Apparent Density of Sulfidic Crosslink and Their Chemical Nature on Self-Heat Build-Up in Carbon Black Filled Natural Rubber under Cyclic Mechanical Loading","volume":"227","author":"Kratina","year":"2024","journal-title":"Polym. Degrad. Stab."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"e25592","DOI":"10.1016\/j.heliyon.2024.e25592","article-title":"Vulcanization Kinetics and Reinforcement Behaviour of Natural Rubber-Carbon Black Composites: Addition of Shea-Butter versus Aromatic Oil as Plasticizers","volume":"10","author":"Mensah","year":"2024","journal-title":"Heliyon"},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"298","DOI":"10.1021\/acspolymersau.5c00009","article-title":"Competing Effects of Plasticization and Miscibility on the Structure and Dynamics of Natural Rubber: A Comparative Study on Bio and Commercial Plasticizers","volume":"5","author":"Lenzi","year":"2025","journal-title":"ACS Polym. Au"},{"key":"ref_17","first-page":"169","article-title":"A Study on the Use of Castor Oil as Plasticizer in Natural Rubber Compounds","volume":"23","author":"Raju","year":"2007","journal-title":"Prog. Rubber Plast. Recycl. Technol."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"4835","DOI":"10.1002\/app.24811","article-title":"A Comparative Study of Cardanol and Aromatic Oil as Plasticizers for Carbon-Black-Filled Natural Rubber","volume":"102","author":"Alexander","year":"2006","journal-title":"J. Appl. Polym. Sci."},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"116270","DOI":"10.1016\/j.indcrop.2023.116270","article-title":"Utilization of Palm Oil as an Alternative Processing Oil in Carbon Black-Filled Natural Rubber Compounds","volume":"194","author":"Hayichelaeh","year":"2023","journal-title":"Ind. Crops Prod."},{"key":"ref_20","doi-asserted-by":"crossref","unstructured":"Muhammad Zaki, N., Yunus, N.A., Yusoff, M.S., Mazlan, S.A., Abdul Aziz, S.A., Izni, N.A., and Bahiuddin, I. (2021). Effects of Petroleum-Based Oils as Dispersing Aids on Physicochemical Characteristics of Magnetorheological Elastomers. Materials, 14.","DOI":"10.3390\/ma14227026"},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"115940","DOI":"10.1088\/1402-4896\/ae1cf8","article-title":"Rheological Behavior of Natural Rubber-Based Magnetorheological Elastomer Incorporating Petroleum-Based Oil","volume":"100","author":"Yusoff","year":"2025","journal-title":"Phys. Scr."},{"key":"ref_22","doi-asserted-by":"crossref","unstructured":"Ahmad Khairi, M.H., Abd Fatah, A.Y., Mazlan, S.A., Nordin, N.A., Nik Ismail, N.I., Choi, S.-B., and Abdul Aziz, S.A. (2019). Enhancement of Particle Alignment Using Silicone Oil Plasticizer and Its Effects on the Field-Dependent Properties of Magnetorheological Elastomers. Int. J. Mol. Sci., 20.","DOI":"10.3390\/ijms20174085"},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"162","DOI":"10.1016\/0095-8522(51)90036-0","article-title":"The Viscosity of a Concentrated Suspension of Spherical Particles","volume":"6","author":"Mooney","year":"1951","journal-title":"J. Colloid Sci."},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"106888","DOI":"10.1016\/j.polymertesting.2020.106888","article-title":"Effect of Pre-Strain on Compression Mode Properties of Magnetorheological Elastomers","volume":"93","author":"Vatandoost","year":"2021","journal-title":"Polym. Test."},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"3322","DOI":"10.1021\/ie201976e","article-title":"Magnetic-Field-Induced Normal Force of Magnetorheological Elastomer under Compression Status","volume":"51","author":"Liao","year":"2012","journal-title":"Ind. Eng. Chem. Res."},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"8765","DOI":"10.1039\/C4SM01738B","article-title":"Experimental Study of the Magnetic Field Enhanced Payne Effect in Magnetorheological Elastomers","volume":"10","author":"Sorokin","year":"2014","journal-title":"Soft Matter"},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"1800696","DOI":"10.1002\/adem.201800696","article-title":"Role of Additives in Enhancing the Rheological Properties of Magnetorheological Solids: A Review","volume":"21","author":"Mazlan","year":"2019","journal-title":"Adv. Eng. Mater."},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"7434536","DOI":"10.1155\/2018\/7434536","article-title":"Fabrication and Characterization of Natural Rubber-Based Magnetorheological Elastomers at Large Strain for Base Isolators","volume":"2018","author":"Lee","year":"2018","journal-title":"Shock Vib."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"1189","DOI":"10.1177\/1045389X19835940","article-title":"Study of Crosslink Structure and Dynamic Mechanical Properties of Magnetorheological Elastomer: Effect of Vulcanization System","volume":"30","author":"Shi","year":"2019","journal-title":"J. Intell. Mater. Syst. Struct."},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"771","DOI":"10.1021\/ie302536e","article-title":"Effect of Cross-Link Density of the Matrix on the Damping Properties of Magnetorheological Elastomers","volume":"52","author":"Fan","year":"2013","journal-title":"Ind. Eng. Chem. Res."},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"117002","DOI":"10.1088\/1361-665X\/aae1e1","article-title":"A Comparative Assessment of Different Dispersing Aids in Enhancing Magnetorheological Elastomer Properties","volume":"27","author":"Aziz","year":"2018","journal-title":"Smart Mater. Struct."},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"695","DOI":"10.3144\/expresspolymlett.2008.83","article-title":"Effects of Carbon Blacks with Various Structures on Vulcanization and Reinforcement of Filled Ethylene-Propylene-Diene Rubber","volume":"2","author":"Li","year":"2008","journal-title":"eXPRESS Polym. Lett."},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"1183","DOI":"10.1002\/app.36851","article-title":"Effect of Non-Rubber Substances on Vulcanization Kinetics of Natural Rubber","volume":"126","author":"Wang","year":"2012","journal-title":"J. Appl. Polym. Sci."},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"7131","DOI":"10.1039\/D2SM00021K","article-title":"Modeling Dynamic Swelling of Polymer-Based Artificial Muscles","volume":"18","author":"Bowen","year":"2022","journal-title":"Soft Matter"},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"521","DOI":"10.1063\/1.1723792","article-title":"Statistical Mechanics of Cross-Linked Polymer Networks II. Swelling","volume":"11","author":"Flory","year":"1943","journal-title":"J. Chem. Phys."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"1433","DOI":"10.1002\/macp.200900191","article-title":"Branched Versus Linear Polyisoprene: Flory-Huggins Interaction Parameters for Their Solutions in Cyclohexane","volume":"210","author":"Eckelt","year":"2009","journal-title":"Macromol. Chem. Phys."},{"key":"ref_37","doi-asserted-by":"crossref","first-page":"679","DOI":"10.5254\/1.3540360","article-title":"Vulcanization. Part V. The Formation of Crosslinks in the System: Natural Rubber-Sulfur-MBT-Zinc Ion","volume":"37","author":"Coran","year":"1964","journal-title":"Rubber Chem. Technol."},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"24","DOI":"10.1002\/app.11659","article-title":"Chemistry of the Vulcanization and Protection of Elastomers: A Review of the Achievements","volume":"87","author":"Coran","year":"2003","journal-title":"J. Appl. Polym. Sci."},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"1052","DOI":"10.1016\/j.polymertesting.2013.06.002","article-title":"Mechanistic Modeling of Reversion Phenomenon in Sulphur Cured Natural Rubber Vulcanization Kinetics","volume":"32","author":"Milani","year":"2013","journal-title":"Polym. Test."},{"key":"ref_40","doi-asserted-by":"crossref","first-page":"689","DOI":"10.5254\/1.3540362","article-title":"Vulcanization. Part VI. A Model and Treatment for Scorch Delay Kinetics","volume":"37","author":"Coran","year":"1964","journal-title":"Rubber Chem. Technol."},{"key":"ref_41","doi-asserted-by":"crossref","first-page":"1","DOI":"10.5254\/1.3535628","article-title":"Vulcanization. Part VII. Kinetics of Sulfur Vulcanization of Natural Rubber in Presence of Delayed-Action Accelerators","volume":"38","author":"Coran","year":"1965","journal-title":"Rubber Chem. Technol."},{"key":"ref_42","doi-asserted-by":"crossref","first-page":"455","DOI":"10.1002\/(SICI)1097-4628(19960718)61:3<455::AID-APP8>3.0.CO;2-H","article-title":"A Kinetic Model for Sulfur Accelerated Vulcanization of a Natural Rubber Compound","volume":"61","author":"Ding","year":"1996","journal-title":"J. Appl. Polym. Sci."},{"key":"ref_43","doi-asserted-by":"crossref","first-page":"575","DOI":"10.1016\/j.polymertesting.2013.01.003","article-title":"A Continuous Kinetic Model of Rubber Vulcanization Predicting Induction and Reversion","volume":"32","author":"Leroy","year":"2013","journal-title":"Polym. Test."},{"key":"ref_44","doi-asserted-by":"crossref","first-page":"63","DOI":"10.5254\/1.3536002","article-title":"Temperature Effects on the Stability of Intermediates and Crosslinks in Sulfur Vulcanization","volume":"57","author":"Morrison","year":"1984","journal-title":"Rubber Chem. Technol."},{"key":"ref_45","doi-asserted-by":"crossref","unstructured":"Cataldo, F. (2023). Thermochemistry of Sulfur-Based Vulcanization and of Devulcanized and Recycled Natural Rubber Compounds. Int. J. Mol. Sci., 24.","DOI":"10.3390\/ijms24032623"}],"container-title":["Polymers"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/18\/2195\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T08:16:32Z","timestamp":1788941792000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/18\/2195"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,9,9]]},"references-count":45,"journal-issue":{"issue":"18","published-online":{"date-parts":[[2026,9]]}},"alternative-id":["polym18182195"],"URL":"https:\/\/doi.org\/10.3390\/polym18182195","relation":{},"ISSN":["2073-4360"],"issn-type":[{"value":"2073-4360","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,9,9]]}}}