Deep Eutectic Solvent Based on Choline Hydroxide for Advanced Aqueous Lubrication
Abstract
1. Introduction
2. Materials and Methods
2.1. Materials Details
2.2. Preparation of Choline Hydroxide DES-Based Lubricants
2.3. Characterization
2.4. Electrochemical Tests
2.5. Tribological Tests
3. Results
3.1. Characterization of the Novel DES: Choline Hydroxide–Glycerol
3.2. Tribological Performance
3.2.1. Wettability
3.2.2. Tribological Analysis
3.2.3. Electrochemical Analysis
3.2.4. Surface Analysis
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
- Mannekote, J.K.; Kailas, S.V.; Venkatesh, K.; Kathyayini, N. Environmentally Friendly Functional Fluids from Renewable and Sustainable Sources—A Review. Renew. Sustain. Energy Rev. 2018, 81, 1787–1801. [Google Scholar] [CrossRef]
- Hörner, D. Recent Trends in Environmentally Friendly Lubricants. J. Synth. Lubr. 2002, 18, 327–347. [Google Scholar] [CrossRef]
- Donato, M.T.; Colaço, R.; Branco, L.C.; Saramago, B. A Review on Alternative Lubricants: Ionic Liquids as Additives and Deep Eutectic Solvents. J. Mol. Liq. 2021, 333, 116004. [Google Scholar] [CrossRef]
- Sernaglia, M.; Bartolomé, M.; Viesca, J.L.; González, R.; Battez, A.H. Application of Deep Eutectic Solvents in Lubrication: A Review. J. Mol. Liq. 2025, 427, 127464. [Google Scholar] [CrossRef]
- Abranches, D.O.; Coutinho, J.A.P. Everything You Wanted to Know about Deep Eutectic Solvents but Were Afraid to Be Told. Annu. Rev. Chem. Biomol. Eng. 2023, 14, 141–163. [Google Scholar] [CrossRef] [PubMed]
- Meredith, L.; Elbourne, A.; Greaves, T.L.; Bryant, G.; Bryant, S.J. Physico-Chemical Characterisation of Glycerol- and Ethylene Glycol-Based Deep Eutectic Solvents. J. Mol. Liq. 2024, 394, 123777. [Google Scholar] [CrossRef]
- Smith, E.L.; Abbott, A.P.; Ryder, K.S. Deep Eutectic Solvents (DESs) and Their Applications. Chem. Rev. 2014, 114, 11060–11082. [Google Scholar] [CrossRef]
- Yeow, A.T.H.; Hayyan, A.; Hayyan, M.; Usman Mohd Junaidi, M.; Saleh, J.; Jefrey Basirun, W.; Roslan Mohd Nor, M.; Al Abdulmonem, W.; Zulhaziman, M.; Mohamed Zuki, F.; et al. A Comprehensive Review on the Physicochemical Properties of Deep Eutectic Solvents. Results Chem. 2024, 7, 101378. [Google Scholar] [CrossRef]
- Omar, K.A.; Sadeghi, R. Physicochemical Properties of Deep Eutectic Solvents: A Review. J. Mol. Liq. 2022, 360, 119524. [Google Scholar] [CrossRef]
- Zhang, Q.; De Oliveira Vigier, K.; Royer, S.; Jérôme, F. Deep Eutectic Solvents: Syntheses, Properties and Applications. Chem. Soc. Rev. 2012, 41, 7108–7146. [Google Scholar] [CrossRef] [PubMed]
- Abbott, A.P.; Capper, G.; Davies, D.L.; Rasheed, R.K.; Tambyrajah, V. Novel Solvent Properties of Choline Chloride/Urea Mixtures. Chem. Commun. 2003, 39, 70–71. [Google Scholar] [CrossRef]
- Álvarez, M.S.; Longo, M.A.; Rodríguez, A.; Deive, F.J. The Role of Deep Eutectic Solvents in Catalysis. A Vision on Their Contribution to Homogeneous, Heterogeneous and Electrocatalytic Processes. J. Ind. Eng. Chem. 2024, 132, 36–49. [Google Scholar] [CrossRef]
- Guzmán, E. Catalysis With Deep Eutectic Solvents: Challenges and Opportunities. ChemCatChem 2025, 17, e202500522. [Google Scholar] [CrossRef]
- Zhong, Y.; Wu, J.; Kang, H.; Liu, R. Choline Hydroxide Based Deep Eutectic Solvent for Dissolving Cellulose. Green Chem. 2022, 24, 2464–2475. [Google Scholar] [CrossRef]
- Abbott, A.P. Deep Eutectic Solvents and Their Application in Electrochemistry. Curr. Opin. Green Sustain. Chem. 2022, 36, 100649. [Google Scholar] [CrossRef]
- Carriazo, D.; Serrano, M.C.; Gutiérrez, M.C.; Ferrer, M.L.; del Monte, F. Deep-Eutectic Solvents Playing Multiple Roles in the Synthesis of Polymers and Related Materials. Chem. Soc. Rev. 2012, 41, 4996–5014. [Google Scholar] [CrossRef]
- Tomé, L.I.N.; Baião, V.; da Silva, W.; Brett, C.M.A. Deep Eutectic Solvents for the Production and Application of New Materials. Appl. Mater. Today 2018, 10, 30–50. [Google Scholar] [CrossRef]
- Lawes, S.D.A.; Hainsworth, S.V.; Blake, P.; Ryder, K.S.; Abbott, A.P. Lubrication of Steel/Steel Contacts by Choline Chloride Ionic Liquids. Tribol. Lett. 2010, 37, 103–110. [Google Scholar] [CrossRef]
- Kumar Patro, B.D.; Shivakumar; Suvin, P.S.; Dalimba, U.; Kreivaitis, R. Effect of Temperature on Tribological Behavior of L–Proline–Based Green Deep Eutectic Solvents for Ti6Al4V Interfaces: A Study of Novel Potential Lubricant. Tribol. Int. 2025, 208, 110667. [Google Scholar] [CrossRef]
- Li, Y.; Li, Y.; Li, H.; Fan, X.; Yan, H.; Cai, M.; Xu, X.; Zhu, M. Insights into the Tribological Behavior of Choline Chloride—Urea and Choline Chloride—Thiourea Deep Eutectic Solvents. Friction 2023, 11, 76–92. [Google Scholar] [CrossRef]
- Shi, Y.; Mu, L.; Feng, X.; Lu, X. Friction and Wear Behavior of CF/PTFE Composites Lubricated by Choline Chloride Ionic Liquids. Tribol. Lett. 2013, 49, 413–420. [Google Scholar] [CrossRef]
- Wu, C.; Han, Y.; Zhao, H.; Zheng, C.; Li, X.; Ni, J. Effect of Choline Chloride/Multiple Diols Deep Eutectic Solvents on the Friction and Vibration Performance of Si3N4/GCr15 Hybrid Ceramic Ball Bearings. Tribol. Int. 2024, 198, 109845. [Google Scholar] [CrossRef]
- Donato, M.T.; Diogo, H.P.; Deuermeier, J.; Colaço, R.; Branco, L.C.; Saramago, B. Hydrophobic Deep Eutectic Solvents with Anti-Wear Properties for MEMS/NEMS. J. Mol. Liq. 2024, 393, 123643. [Google Scholar] [CrossRef]
- Antunes, M.; Campinhas, A.-S.; de Sá Freire, M.; Caetano, F.; Diogo, H.P.; Colaço, R.; Branco, L.C.; Saramago, B. Deep Eutectic Solvents (DES) Based on Sulfur as Alternative Lubricants for Silicon Surfaces. J. Mol. Liq. 2019, 295, 111728. [Google Scholar] [CrossRef]
- Garcia, I.; Guerra, S.; de Damborenea, J.; Conde, A. Reduction of the Coefficient of Friction of Steel-Steel Tribological Contacts by Novel Graphene-Deep Eutectic Solvents (DESs) Lubricants. Lubricants 2019, 7, 37. [Google Scholar] [CrossRef]
- Gao, Q.; Liu, S.; Hou, K.; Miao, X.; Li, Z.; Wang, J. Tribological Properties of MoSx/RGO Nanohybrids as Additives in Deep Eutectic Solvent. Tribol. Int. 2023, 186, 108652. [Google Scholar] [CrossRef]
- Liñeira del Río, J.M.; Aourdou, A.; García-Marquínez, G.; Amado, J.M.; Tobar, M.J. Deep Eutectic Solvents as Green and Novel Lubricant Additives for Castor Oil with High Tribological Performance. Lubricants 2025, 13, 456. [Google Scholar] [CrossRef]
- Prado, D.M.; Gonzaga, A.N.; Carter, B.; Burda, C. Thermodynamic Water Activity Explains the Unusual Electrochemical Stability of Aqueous Deep Eutectic Solvents. Chem. Eur. J. 2025, 31, e202500717. [Google Scholar] [CrossRef] [PubMed]
- El Achkar, T.; Fourmentin, S.; Greige-Gerges, H. Deep Eutectic Solvents: An Overview on Their Interactions with Water and Biochemical Compounds. J. Mol. Liq. 2019, 288, 111028. [Google Scholar] [CrossRef]
- Ma, C.; Laaksonen, A.; Liu, C.; Lu, X.; Ji, X. The Peculiar Effect of Water on Ionic Liquids and Deep Eutectic Solvents. Chem. Soc. Rev. 2018, 47, 8685–8720. [Google Scholar] [CrossRef]
- Abbott, A.P.; Ahmed, E.I.; Harris, R.C.; Ryder, K.S. Evaluating Water Miscible Deep Eutectic Solvents (DESs) and Ionic Liquids as Potential Lubricants. Green Chem. 2014, 16, 4156–4161. [Google Scholar] [CrossRef]
- Florindo, C.; Oliveira, F.S.; Rebelo, L.P.N.; Fernandes, A.M.; Marrucho, I.M. Insights into the Synthesis and Properties of Deep Eutectic Solvents Based on Cholinium Chloride and Carboxylic Acids. ACS Sustain. Chem. Eng. 2014, 2, 2416–2425. [Google Scholar] [CrossRef]
- Du, C.; Zhao, B.; Chen, X.B.; Birbilis, N.; Yang, H. Effect of Water Presence on Choline Chloride-2urea Ionic Liquid and Coating Platings from the Hydrated Ionic Liquid. Sci. Rep. 2016, 6, 29225. [Google Scholar] [CrossRef] [PubMed]
- Ma, J.; Xu, J.; Pang, S.; Zhou, W.; Xia, B.; An, Y. Novel Environmentally Friendly Lubricants for Drilling Fluids Applied in Shale Formation. Energy Fuels 2021, 35, 8153–8162. [Google Scholar] [CrossRef]
- Zhou, X.; Pang, S.; Zhao, L.; An, Y. Performance Evaluation of a Novel Environmentally Friendly Lubricants for Water-Based Drilling Fluids. J. Dispers. Sci. Technol. 2025, 1–10. [Google Scholar] [CrossRef]
- Buzolic, J.J.; Tiecco, M.; Atkin, R.; Li, H. Tuning the Nanostructure and Tribological Properties of a Non-Ionic Deep Eutectic Solvent with Water Addition. J. Colloid Interface Sci. 2025, 683, 722–730. [Google Scholar] [CrossRef]
- Hallett, J.E.; Hayler, H.J.; Perkin, S. Nanolubrication in Deep Eutectic Solvents. Phys. Chem. Chem. Phys. 2020, 22, 20253–20264. [Google Scholar] [CrossRef]
- Gao, Q.; Liu, S.; Hou, K.; Li, Z.; Wang, J.; Yang, S. Peculiar Effect of Water on Tribological Properties of Natural Deep Eutectic Solvent. Langmuir 2024, 40, 26936–26946. [Google Scholar] [CrossRef]
- Yu, M.; Zhang, J.; Joedicke, A.; Booth, J.; Reddyhoff, T. Using Electrical Impedance Spectroscopy to Identify Equivalent Circuit Models of Lubricated Contacts with Complex Geometry: In-Situ Application to Mini Traction Machine. Tribol. Int. 2024, 192, 109286. [Google Scholar] [CrossRef]
- Lvovich, V.F.; Smiechowski, M.F. Impedance Characterization of Industrial Lubricants. Electrochim. Acta 2006, 51, 1487–1496. [Google Scholar] [CrossRef]
- Duque, A.; Sanjuan, A.; Bou-Ali, M.M.; Alonso, R.M.; Campanero, M.A. Physicochemical Characterization of Hydrophobic Type III and Type V Deep Eutectic Solvents Based on Carboxylic Acids. J. Mol. Liq. 2023, 392, 123431. [Google Scholar] [CrossRef]
- Mudalige, A.; Pemberton, J.E. Raman Spectroscopy of Glycerol/D2O Solutions. Vib. Spectrosc. 2007, 45, 27–35. [Google Scholar] [CrossRef]
- Hadjiivanov, K.I.; Panayotov, D.A.; Mihaylov, M.Y.; Ivanova, E.Z.; Chakarova, K.K.; Andonova, S.M.; Drenchev, N.L. Power of Infrared and Raman Spectroscopies to Characterize Metal-Organic Frameworks and Investigate Their Interaction with Guest Molecules. Chem. Rev. 2021, 121, 1286–1424. [Google Scholar] [CrossRef]
- de Souza, Í.F.T.; Ribeiro, M.C.C. A Raman Spectroscopy and Rheology Study of the Phase Transitions of the Ionic Liquid Choline Acetate. J. Mol. Liq. 2021, 322, 114530. [Google Scholar] [CrossRef]
- Yuniarto, K.; Purwanto, Y.A.; Purwanto, S.; Welt, B.A.; Purwadaria, H.K.; Sunarti, T.C. Infrared and Raman Studies on Polylactide Acid and Polyethylene Glycol-400 Blend. AIP Conf. Proc. 2016, 1725, 020101. [Google Scholar] [CrossRef]
- Mostaza, P.; Avilés, M.D.; Martínez-Rubio, P.M.; Bermúdez, M.D.; Carrión-Vilches, F.J. Novel Water-Based Biolubricants Using Choline Ionic Liquids. Lubricants 2025, 13, 122. [Google Scholar] [CrossRef]
- Westerholt, A.; Weschta, M.; Bösmann, A.; Tremmel, S.; Korth, Y.; Wolf, M.; Schlücker, E.; Wehrum, N.; Lennert, A.; Uerdingen, M.; et al. Halide-Free Synthesis and Tribological Performance of Oil-Miscible Ammonium and Phosphonium-Based Ionic Liquids. ACS Sustain. Chem. Eng. 2015, 3, 797–808. [Google Scholar] [CrossRef]
- Rahimi, E.; Offoiach, R.; Baert, K.; Terryn, H.; Lekka, M.; Fedrizzi, L. Role of Phosphate, Calcium Species and Hydrogen Peroxide on Albumin Protein Adsorption on Surface Oxide of Ti6Al4V Alloy. Materialia 2021, 15, 100988. [Google Scholar] [CrossRef]
- Giray, D.; Şeref Sönmez, M.; Yamanoglu, R.; Ismail Yavuz, H.; Muratal, O. Characterization of Corrosion Products Formed in High-Strength Dual-Phase Steels under an Accelerated Corrosion Test. Eng. Sci. Technol. Int. J. 2024, 57, 101796. [Google Scholar] [CrossRef]
- Cui, Y.; Liu, S.; Smith, K.; Yu, K.; Hu, H.; Jiang, W.; Li, Y. Characterization of Corrosion Scale Formed on Stainless Steel Delivery Pipe for Reclaimed Water Treatment. Water Res. 2016, 88, 816–825. [Google Scholar] [CrossRef] [PubMed]
- Reinert, L.; Lasserre, F.; Gachot, C.; Grützmacher, P.; Maclucas, T.; Souza, N.; Mücklich, F.; Suarez, S. Long-Lasting Solid Lubrication by CNT-Coated Patterned Surfaces. Sci. Rep. 2017, 7, 42873. [Google Scholar] [CrossRef]
- Nins, B.; Penagos, J.J.; Moreira, L.; Münch, D.; Falqueto, P.; Viáfara, C.C.; da Costa, A.R. Abrasiveness of Iron Ores: Analysis of Service-Worn Conveyor Belts and Laboratory Dry Sand/Rubber Wheel Tests. Wear 2022, 506–507, 204439. [Google Scholar] [CrossRef]
- Gialanella, S.; Girardi, F.; Ischia, G.; Lonardelli, I.; Mattarelli, M.; Montagna, M. On the Goethite to Hematite Phase Transformation. J. Therm. Anal. Calorim. 2010, 102, 867–873. [Google Scholar] [CrossRef]
- Yu, X.; Jiang, Z.; Wei, D.; Zhou, C.; Huang, Q.; Yang, D. Tribological Properties of Magnetite Precipitate from Oxide Scale in Hot-Rolled Microalloyed Steel. Wear 2013, 302, 1286–1294. [Google Scholar] [CrossRef]
- Sun, C.; Ding, F.; Li, W.; Yang, Z.; Ma, Z.; Song, C. Effects of Relative Humidity on Iron-Oxide Composition and Wear Mechanism on Steel Friction Interface. Wear 2025, 582–583, 206360. [Google Scholar] [CrossRef]
- Vedaei-Sabegh, A.; Morin, J.B.; Champliaud, H.; Jahazi, M. Influence of Thermally Grown Oxides on Interfacial Friction during Hot Deformation of Large-Size Forging Ingots. J. Mater. Res. Technol. 2022, 21, 3412–3424. [Google Scholar] [CrossRef]
- Urtis, L.A.; Arcifa, A.; Zhang, P.; Du, J.; Fantauzzi, M.; Rauber, D.; Hempelmann, R.; Kraus, T.; Rossi, A.; Spencer, N.D. Influence of Water on Tribolayer Growth When Lubricating Steel with a Fluorinated Phosphonium Dicyanamide Ionic Liquid. Lubricants 2019, 7, 27. [Google Scholar] [CrossRef]
- Jagst, E. Surface Functional Group Characterization Using Chemical Derivatization X-Ray Photoelectron Spectroscopy (CD-XPS). Doctoral Dissertation, Freien Universität Berlin, Berlin, Germany, 2010. [Google Scholar]
- Hryniewicz, T.; Rokosz, K. Analysis of XPS Results of AISI 316L SS Electropolished and Magnetoelectropolished at Varying Conditions. Surf. Coat. Technol. 2010, 204, 2583–2592. [Google Scholar] [CrossRef]
- Wijanarko, W.; Khanmohammadi, H.; Espallargas, N. Ionic Liquids as Boundary Additives in Water-Based and PAO Lubricants. Friction 2022, 10, 1405–1423. [Google Scholar] [CrossRef]
- Erdogan, Y.K.; Ercan, B. Anodized Nanostructured 316L Stainless Steel Enhances Osteoblast Functions and Exhibits Anti-Fouling Properties. ACS Biomater. Sci. Eng. 2023, 9, 693–704. [Google Scholar] [CrossRef]















| Lubricants | pH |
|---|---|
| 1% [ChOH][G] | 12.6 (±0.1) |
| 10% [ChOH][G] | 12.9 (±0.1) |
| [ChOH][G] | 13.4 (±0.1) |
| Test Parameter | Value | Schematic of the Tribosystem |
|---|---|---|
| Sliding distance (m) | 500 | ![]() |
| Applied load (N) | 1.0 | |
| Sliding speed (m/s) | 0.1 | |
| Mean contact pressure (GPa) | 1.30 | |
| Maximum contact pressure (GPa) | 1.95 | |
| Sliding radius (mm) | 9.0 | |
| Lubricant volume (ml) | 0.2 | |
| Temperature (°C) | 22.2 ± 0.5 | |
| Relative Humidity (%) | 57 ± 4 |
| Lubricant | Initial | After 5 min |
|---|---|---|
| Water | ![]() 48.2° (±2.1) | ![]() 42.4° (±1.8) |
| 1% [ChOH][G] | ![]() 66.4° (±3.6) | ![]() 52.6° (±1.0) |
| 10% [ChOH][G] | ![]() 55.5° (±5.3) | ![]() 29.2° (±2.2) |
| [ChOH][G] | ![]() 79.1° (±1.8) | ![]() 46.7° (±3.5) |
| Lubricant | COF | K × 10−6 (mm3/N·m) |
|---|---|---|
| Water | 0.426 (±0.018) | 19.10 (±1.75) |
| 1% [ChOH][G] | 0.401 (±0.027) | 8.96 (±0.46) |
| 10% [ChOH][G] | 0.234 (±0.013) | 3.80 (±0.40) |
| [ChOH][G] | 0.093 (±0.009) | 7.23 (±0.53) |
| Lubricant | Ecorr (mV) | Icorr (µA) | Vcorr (µm/Year) | Circuit Model | Rs (Ω·cm2) | Cdl × 10−5 (F/cm) | Rct × 106 (Ω·cm2) |
|---|---|---|---|---|---|---|---|
| Water | 0.005 | 0.032 | 0.299 | (QR)(QR) | 1.28 × 104 | 3.75 | 2.40 |
| 1% [ChOH][G] | 6.295 | 0.076 | 0.712 | R(QR) | 82.44 | 3.41 | 8.63 |
| 10% [ChOH][G] | −101.07 | 0.105 | 0.984 | R(QR) | 7.07 | 2.35 | 0.42 |
| [ChOH][G] | 1.073 | 0.171 | 1.602 | R(QR) | 29.18 | 2.28 | 1.42 |
| Lubricant | Wear Track | Fe (%) | C (%) | O (%) | Cr (%) |
|---|---|---|---|---|---|
| Water | in. | 58.58 | 2.46 | 4.92 | 14.63 |
| out. | 64.86 | 2.97 | 0.23 | 15.83 | |
| 1% [ChOH][G] | in. | 61.73 | 2.63 | 8.41 | 14.14 |
| out. | 68.51 | 2.24 | 1.36 | 16.21 | |
| 10% [ChOH][G] | in. | 64.18 | 4.12 | 2.5 | 15.21 |
| out. | 67.08 | 1.68 | 0.2 | 16.17 | |
| [ChOH][G] | in. | 64.76 | 3.49 | 2.89 | 15.11 |
| out. | 67.02 | 1.98 | 0.25 | 16.12 |
| Lubricant | Hematite | Goethite | Magnetite |
|---|---|---|---|
| Water | 16.7% | 43.7% | 39.6% |
| 1% [ChOH][G] | 18.8% | 40.5% | 40.7% |
| 10% [ChOH][G] | 18.5% | 53.8% | 27.7% |
| Neat [ChOH][G] | 18.7% | 49.5% | 31.7% |
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Carrión-Vilches, F.J.; Jiménez, A.E.; Mostaza, P.; Bermúdez, M.-D.; Avilés, M.-D. Deep Eutectic Solvent Based on Choline Hydroxide for Advanced Aqueous Lubrication. Lubricants 2026, 14, 106. https://doi.org/10.3390/lubricants14030106
Carrión-Vilches FJ, Jiménez AE, Mostaza P, Bermúdez M-D, Avilés M-D. Deep Eutectic Solvent Based on Choline Hydroxide for Advanced Aqueous Lubrication. Lubricants. 2026; 14(3):106. https://doi.org/10.3390/lubricants14030106
Chicago/Turabian StyleCarrión-Vilches, Francisco J., Ana Eva Jiménez, Paloma Mostaza, María-Dolores Bermúdez, and María-Dolores Avilés. 2026. "Deep Eutectic Solvent Based on Choline Hydroxide for Advanced Aqueous Lubrication" Lubricants 14, no. 3: 106. https://doi.org/10.3390/lubricants14030106
APA StyleCarrión-Vilches, F. J., Jiménez, A. E., Mostaza, P., Bermúdez, M.-D., & Avilés, M.-D. (2026). Deep Eutectic Solvent Based on Choline Hydroxide for Advanced Aqueous Lubrication. Lubricants, 14(3), 106. https://doi.org/10.3390/lubricants14030106










