Tribochemistry of alcohols and their tribological properties: a review

doi:10.1007/s11706-023-0633-0

Front. Mater. Sci.

2023, Vol. 17

Issue (1) : 230633 https://doi.org/10.1007/s11706-023-0633-0

REVIEW ARTICLE

Tribochemistry of alcohols and their tribological properties: a review

Liping Xiong^1,²(

), Xiaoya Sun¹, Qi Chen¹, Mengyue Zhu¹, Zhongyi He^1,^2,³(

), Lili Li¹

¹. School of Materials Science and Engineering, East China Jiaotong University, Nanchang 330013, China
². Jiangxi Railway Transit Key Materials Engineering Technology Research Center, Nanchang 330013, China
³. State Key Laboratory of Rail Transit Infrastructure Performance Monitoring and Guarantee, East China Jiaotong University, Nanchang 330013, China

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Abstract

Recently, alcohols have attracted more attention due to their excellent tribological performance, especially superlubricity under low loads. Alcohol solution, as a liquid lubricant, can easily reach the superlubricity state under low loads because of the formed low shear hydroxylation interfaces induced by the tribochemical reactions. A general picture and its influencing factors have been elucidated, not only at the macroscopic scale but also at the nanoscale, which is sufficient to provide effective guidance for lubrication design and tribology research in engineering. Herein, we provide a review on the recent applications of alcohols in lubrication. In addition, the material transformation caused by alcohols in friction is a key factor affecting the tribological properties. As an important two-dimensional material, the growth mechanisms of graphene are variable, and the most famous is the formation of carbon radicals under the action of metal catalysts. Thus, based on the formation mechanism of carbon friction film (such as amorphous carbon and graphene), the main content of this review also includes the transformation of graphene in alcohol solution friction process.

Keywords alcohol tribochemistry graphene carbon-based material

Corresponding Author(s): Liping Xiong,Zhongyi He

About author:

Changjian Wang and Zhiying Yang contributed equally to this work.

Issue Date: 06 March 2023

Cite this article:

Liping Xiong,Xiaoya Sun,Qi Chen, et al. Tribochemistry of alcohols and their tribological properties: a review[J]. Front. Mater. Sci., 2023, 17(1): 230633.

URL:

https://academic.hep.com.cn/foms/EN/10.1007/s11706-023-0633-0
https://academic.hep.com.cn/foms/EN/Y2023/V17/I1/230633

Fig.2 (a) The lubrication mechanism of 2D materials. Reproduced with permission from Ref. [19] (Copyright 2017 Elsevier). (b) The lubrication mechanism of nanoparticles. Reproduced with permission from Ref. [20] (Copyright 2015 Hindawi Limited).

Alcohol solution	Lubricant	Friction pair	Condition	Highlight	Ref.
Alcohol + nanoparticles	PG/FG/GO coating + 20% glycerol in water	Si₃N₄/SiO₂	1.5?4 N, 240 r·min^?1; different speeds	The PG coating (the coefficient of friction (COF) is about 0.004) exhibited better lubrication and anti-wear performance than those of the FG and GO coatings.	[29]
	GO + glycerol (with 0.025?0.1 wt.%)	Steel 40Cr, pin-on-disk	98 N, 196 N, 200 r·min^?1	The significant reduction in the COF to 0.005 occurs in a concentration of 0.05% GO.	[30]
	Aqueous glycerol + 0.1 wt.% nanodiamonds	Steel 52100	Ball-on-disk (rotary and reciprocation), 0.7 GPa	The superlubricity behavior of aqueous glycerol was achieved during the rotary test method; for the same lubricant, the rotary test shows a lower COF and wear because of its micro-polishing behavior.	[34]
	Si, SiC, and SWCNT + isopropyl alcohol	C/C composites	Ring-on-ring	The nano additives Si at 0.24%, SiC at 0.02%, and SWCNT at 0.01% concentrations lowered oxidative and abrasive wear; the presence of Si led to chemical changes of the friction layer and the formation of carbides.	[35]
	Ethylene glycol in water	Si₃N₄ balls and discs	Ball-on-disk, 10 N (1.3 GPa)	Due to the viscosity enhancement and pressure-viscosity effect, the ethylene glycol can greatly improve the load-carrying capacity, especially in high-concentration solutions.	[36]
	Glycerol/paraffin	Steel/DLC, AISI 52100	Coating (CVD (Cr⁺) a-C:H); 80 N, 300 N (1.95 GPa)	The glycerol-DLC combination in some cases gives a COF below 0.01.	[37]
	Ta-C + glycerol	AISI 52100 steel/ta-C	Ball-on-fat, 3 N (386 MPa)	An impressive super-low COF as low as 0.004 (nearly equivalent to the rolling coefficient) was obtained; the hydrophobic FeOOH formed by tribochemical reaction causes the formation of a double-hydroxyl-terminated surface.	[38]
	Graphene + water + ethanaol	Si₃N₄ balls/SiC	Ball-on-disk, 1?10 N	The introduction of alcohol is beneficial in the distribution of graphene films in the solution, exhibiting an ultra-low friction coefficient of 0.009	[39]
	Layered double hydroxide (LDH) + ionic liquid alcohol solution (IL(as))	Si₃N₄ balls/Al₂O₃ sapphire disk	8?16 N, 24 mm·s^?1	The contact pressures up to 1.044 GPa, which resulted in a COF of 0.004 and a robust superlubricity state lasting for 2 h.	[40]
Alcohol	Ethylene glycol/1,4-butylene glycol	AISI 52100 steel	Slide to roll, 3 N (290 MPa)	Ethylene glycol and 1,4-butylene glycol significantly reduced friction, ?OH present at of the additive molecules increase corrosion and wear rate of the steel specimens.	[31]
	Methanol	2 H-terminated DLC films	TB-QCMD simulation	OH-termination by the tribochemical reaction of alcohol molecules is the reason why the alcohol environments lead to low friction properties. The process is as follows: O?C bond formation, C?C bond formation, C?O bond dissociation, and O?H bond formation.	[41]
	Various linear normal alcohols, branched alcohol	440C steel/ceramics/glasses/carbons/polymers	Ball-on-flat, 0.1?1 N	The longer chain length of the adsorbed alcohols results in lower friction and that n-pentanol gives the lowest friction and wear; branched and fluorinated alcohol lubricate less effectively than normal alcohols at the same chain length.	[42]
	n-Alcohols	Ti₃SiC₂	Pin-on-disk, 1?10 N (1.9?3.3 GPa)	The friction coefficients decrease with carbon numbers and sliding velocity in the n-alcohols, which is determined by the increase of the viscosity of alcohols.	[43]
	Ethanol, methanol, isopropanol	AISI 440C steel, copper, silica slide glass	Ball-on-flat, 1 N (350?642 MPa)	The substrate evaporated by alcohol solvents exhibits good boundary lubrication and resistance to wear.	[44]
	Allyl alcohol	SiO₂, borosilicate balls	Ball-on-flat, 0.25 GPa	The deformation of molecules to a certain extent is a necessary condition for the occurrence of mechanically induced chemical reactions.	[45]
	Allyl alcohol	SiO₂, borosilicate balls	Ball-on-flat, 0.34 GPa	Compared to the alcohol-only case, the tribo-polymerization yield was found to be significantly enhanced in both water-rich and alcohol-rich regimes.	[46]
	Ethanol	Ti₃SiC₂, Al₂O₃/Si₃N₄ ball	Ball-on-disk, 20 N	Flowing and non-flowing states of ethanol are related to the tribological behavior of Ti₃SiC₂, cumulated debris in the non-flowing ethanol leads to the continuous increase in friction and wear.	[47]
	Glycerol	Si₃N₄	3.1 N (0.75 GPa)	Shear induces a phase transition of the CNx layer to 2D aromatic graphene nitride; the continuous involvement of surface-bound N atoms is essential for promoting aromatization, and thus passivation, of the topmost atomic surface layer.	[48]
	1-Dodecanol	AlSI 52100 steel/glass balls/discs	1?50 N	The anomalous EHL film formation and friction behavior are due to polymorphic transformations, and uncover a novel super lubricity mechanism for 1-dodecanol, based on the formation of a lamellar hexagonal polymorph inside the contact.	[49]
Alcohol in water- based lubricant (water)	Glycerol; glycerol + inositol	Steel/steel	0.5?2.0 N; different temperatures, sliding speed, contact speed	Approaching super-low friction; tribo-degradation of glycerol molecules; higher contact pressures give lower friction coefficients.	[26]
	Glycols + water	AISI 52100 steel	Ball-on-disk, 10 N (430 MPa)	The increase of the length of carbon chain in ethanolamine and glycol molecules to some extent can improve tribological performances.	[31]
	Glycerol in water 5–50 wt.%	Ball/disk AISI 52100 bearing steel	1.35 GPa	Investigating the effect of water on the lubricating properties of glycerol, the boundary and elastohydrodynamic lubricating behavior; water in the glycerol promoted the wear of steel.	[32]
	Glycerol in water	Si₃N₄	30 N, different temperatures, ball-on-disk	The addition of glycerol in water could decrease wear rate. Increase of temperature could intensify wear behavior and obscure running-in process.	[33]
	Ethylene glycol in water	Si₃N₄	Ball-on-disk, 10N (1.3 GPa)	Ethylene glycol can effectively reduce wear when the concentration was greater than 10%, and can greatly improve the load-carrying capacity, especially in high concentration solutions.	[36]
	Water-in-glycerol	Steel/steel	55N (1 GPa), ball and plane	Glycerol produces water, aldehydes and other substances through tribochemical reactions.	[50]
	1-Dodecanol	AISI 52100 steel ball and disk	1?50 N (0.1?1.1 GPa)	Liquid 1-dodecanol undergoes pressure-induced solidification when entrained into EHL contacts; superlubricity is facilitated by the formation of lamellar, hydrogen-bonded structures of hexagonally close-packed molecules, which promote interlayer sliding.	[49]
	Glycerol aqueous solution	AISI 52100 steel	3?6 N	Glycerol aqueous solution with water/glycerol weight ratio of 0.2 can achieve superlubricity: tribochemical polishing + microscopic elastohydrodynamic films.	[51]
Alcohol in water- based lubricant (acid)	Glycerol + acids	Si₃N₄/glass	3 N; different pH and concentration of glycerol	The ultralow friction is dependent on the pH value of the acid and the concentration of glycerol; forming the hydrogen-bonded network of glycerol and water on the Stern layer with a fluid-hydrated water layer.	[27]
	Glycerol, boric acid solution	Si₃N₄/glass	300 MPa	Superlubricity, the strongly adsorbed glycerin borate layer, hydration effect.	[28]
	Polyhydroxy alcohols + acids	Si₃N₄/glass	3 N (700 MPa)	The superlubricity mechanism is attributed to forming the hydrogen-bond network between polyhydroxy alcohol and water molecules on the stern layer, and ?OH is one of the essential factors.	[52]
Alcohol in water- based lubricant (ionic)	Imidazolium sulfate ionic liquid + glycerol (0.25?8.0 wt.%)	100Cr6 steel	Ball-on-flat, 10 N (700 MPa)	With the increase of ionic liquid concentration in the lubricant mixture, wear increases for all selected lubricant mixtures; the COF and wear volume tend to decrease when ionic liquid anion alkyl chain increases, with EtMeImOcSO₄ exhibiting the best friction-reduction and anti-wear properties when blended with glycerol.	[53]
Alcohol in water- based lubricant (ionic)	50 wt.% glycerol + protic ionic liquids	Steel/steel	f125N, 50 Hz	The synergistic lubrication mechanism between both PILs is ascribed to the formation of the mixed adsorption layers and the complex triboflms containing sp² bonded carbon, FeS and orthophosphate.	[63]
Alcohol in coating	Glycerol	ta-C DLC, AISI52100 steel	Cylinder-on-flat, 315 N (0.8 GPa)	By using H₂O₂ as a run-in before glycerol lubrication, the hydroxylation was induced and ultra-low friction (0.05) was obtained.	[54]
	50% P/Psat n-pentanol vapor	DLC + Si/Silica balls	Pin-on-disk, 0.1?1 N (0.19?0.4 GPa)	The alkoxide termination of the SiO₂ surfaces raises the energy barrier required to cleave the adjacent Si?O?Si bonds upon the reaction; the activation energy required to break the Si?O?Si bonds is related to the chain length of the terminal alcohol molecules.	[55]
	Ethanol	TiN/CrN coating, SUS 304 steel	Ball-on-disk, 3.92 N, 10 mm·s^?1	The COF of CrN was approximately 60% lower than that of TiN, but TiN had lower wear; transferred iron has prevented the formation of titanium ethoxide on the TiN surface.	[56]
	40% n-pentanol vapor	DLC + Si/440C steel ball	Pin-on-disk, 1 N (0.86 GPa)	The vapor phase lubrication alcohol can protect the oxidized DLC surface from wear even in humid air conditions although the friction coefficient is not ultralow.	[57]
	Hexadecanol + hexadecanoic in PAO6	DLC (a-C:H:Si:O) + AISI 52100/DIN 100Cr6 steel	Ball-on-flat, 10 N (1 GPa)	The adsorption of alcohol onto the DLC surface reduced the wear of coatings; fatty acid adsorbs better on the steel than on the DLC, while the opposite holds for the alcohol molecules; H passivated the surface dangling bonds, hindering the adsorption process.	[58–60]
	Hexadecanol and hexadecanoic acid in PAO6	a-C:H DLC	Ball-on-flat, 10 N (1 GPa)	Polar molecules of hexadecanol and hexadecanoic acid can adsorb relatively strongly onto the a-C:H coatings by bonding to the native surface oxides and hydroxides.	[61]
	Castor oil, glycerol	DLC/Si₃N₄	Low sliding speed (3 mm·s^?1)	A novel superlubricious technology using a vegetable oil and ceramic materials is proposed; complementary numerical simulation results indicate that degradation products from castor oil preferentially occupy sp²-carbon sites compared to sp³ ones.	[62]

Tab.1 Some reports about alcohol solution as liquid lubrication [26–63]

Fig.3 The mixed application scheme of the alcohol solution combined with the lubrication mechanism in recent years.

Fig.4 Schematic illustration of the possible structure between two friction surfaces (the red circles represent oxygen, and the white circles represent hydrogen) (left). Variation of friction coefficient with time as lubricated by the mixture of sulfuric acid solution (pH 1) and glycerol solution (20% v/v) with a volume ratio of 1:10 (right). Reproduced with permission from Ref. [27] (Copyright 2013 American Chemical Society).

Fig.5 Schematic diagram of the synergistic lubrication mechanism between hydrophobic nanosheets and glycerin aqueous solution. Reproduced with permission from Ref. [29] (Copyright 2020 American Chemical Society).

Fig.6 (a)(b) Variations of friction coefficient with test duration for lubrications of steel/steel, ta-C/ta-C, and steel/ta-C tribo-pairs by glycerol at 50 °C. (c) Schematic of the mechanism of superlubricity of a steel/ta-C tribo-pair in glycerol. Reproduced with permission from Ref. [38] (Copyright 2019 Springer Nature).

Fig.8 DFTB-MD shearing simulations of pure and N-doped bulk ta-C using Lees?Edwards boundary conditions and v = 100 m·s^?1 (left). Schematic diagrams for achieving superlubricity of Si₃N₄ boundary lubricated with glycerol by in situ synthesis of graphene nitride nanolayers (right). Reproduced with permission from Ref. [48] (Copyright 2021 American Chemical Society).

Fig.9 (a) Raman spectra obtained from ball surfaces after testing with PAO4 + CPCa, along with spectra from untested DLC and ball surfaces. (b) Mechanism of carbon formation from CPCa. Reproduced with permission from Ref. [109] (Copyright 2017 Springer Nature).

Fig.10 The line chart showing the research conducted from 2007 to 2021. Source: Web of Science database, 2007 to 2021. Keywords used in the search: TS = (graphene AND (tribological OR friction)).

Fig.11 (a) TEM image of the nanotribofilm sliding in methanol sliced using the FIB technique. (b) Enlarged TEM image of the red circle marked area in panel (a). (c) HRTEM image of the black ellipse marked area in panel (b). (d) Enlarged TEM image of the white circle marked area in panel (a). (e) Enlarged TEM image of black materials in nanotribofilm. (f) HRTEM image of the black circle marked area in panel (e). Reproduced with permission from Ref. [123] (Copyright 2020 American Chemical Society).

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