Atom Probe Tomography Unveils Formation Mechanisms of Wear-Protective Tribofilms by ZDDP, Ionic Liquid, and Their Combination
Abstract
The development of advanced lubricant additives has been a critical component in paving the way for increasing energy efficiency and durability for numerous industry applications. However, the formation mechanisms of additive-induced protective tribofilms are not yet fully understood because of the complex chemomechanical interactions at the contact interface and the limited spatial resolution of many characterizing techniques currently used. In this paper, the tribofilms on a gray cast iron surface formed by three antiwear additives are systematically studied; a phosphonium-phosphate ionic liquid (IL), a zinc dialkyldithiophosphate (ZDDP), and an IL+ZDDP combination. All three additives provide excellent wear protection, with the IL+ZDDP combination exhibiting a synergetic effect, resulting in further reduced friction and wear. Atom probe tomography (APT) and scanning transmission electron microscopy (STEM) imaging and electron energy loss spectroscopy (EELS) were used to interrogate the subnm chemistry and bonding states for each of the tribofilms of interest. The IL tribofilm appeared amorphous and was Fe, P, and O rich. Wear debris particles having an Fe-rich core and an oxide shell were present in this tribofilm and a transitional oxide (Fe2O3)-containing layer was identified at the interface between the tribofilm and the cast iron substrate. The ZDDP+IL tribofilm shared some ofmore »
- Authors:
-
[1];
[1];
[2];
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1376428
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 27; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atom probe tomography; ionic liquid; lubricant; STEM-EELS; tribofilm; ZDDP
Citation Formats
Guo, Wei, Zhou, Yan, Sang, Xiahan, Leonard, Donovan N., Qu, Jun, and Poplawsky, Jonathan D. Atom Probe Tomography Unveils Formation Mechanisms of Wear-Protective Tribofilms by ZDDP, Ionic Liquid, and Their Combination. United States: N. p., 2017.
Web. doi:10.1021/acsami.7b04719.
Guo, Wei, Zhou, Yan, Sang, Xiahan, Leonard, Donovan N., Qu, Jun, & Poplawsky, Jonathan D. Atom Probe Tomography Unveils Formation Mechanisms of Wear-Protective Tribofilms by ZDDP, Ionic Liquid, and Their Combination. United States. https://doi.org/10.1021/acsami.7b04719
Guo, Wei, Zhou, Yan, Sang, Xiahan, Leonard, Donovan N., Qu, Jun, and Poplawsky, Jonathan D. Tue .
"Atom Probe Tomography Unveils Formation Mechanisms of Wear-Protective Tribofilms by ZDDP, Ionic Liquid, and Their Combination". United States. https://doi.org/10.1021/acsami.7b04719. https://www.osti.gov/servlets/purl/1376428.
@article{osti_1376428,
title = {Atom Probe Tomography Unveils Formation Mechanisms of Wear-Protective Tribofilms by ZDDP, Ionic Liquid, and Their Combination},
author = {Guo, Wei and Zhou, Yan and Sang, Xiahan and Leonard, Donovan N. and Qu, Jun and Poplawsky, Jonathan D.},
abstractNote = {The development of advanced lubricant additives has been a critical component in paving the way for increasing energy efficiency and durability for numerous industry applications. However, the formation mechanisms of additive-induced protective tribofilms are not yet fully understood because of the complex chemomechanical interactions at the contact interface and the limited spatial resolution of many characterizing techniques currently used. In this paper, the tribofilms on a gray cast iron surface formed by three antiwear additives are systematically studied; a phosphonium-phosphate ionic liquid (IL), a zinc dialkyldithiophosphate (ZDDP), and an IL+ZDDP combination. All three additives provide excellent wear protection, with the IL+ZDDP combination exhibiting a synergetic effect, resulting in further reduced friction and wear. Atom probe tomography (APT) and scanning transmission electron microscopy (STEM) imaging and electron energy loss spectroscopy (EELS) were used to interrogate the subnm chemistry and bonding states for each of the tribofilms of interest. The IL tribofilm appeared amorphous and was Fe, P, and O rich. Wear debris particles having an Fe-rich core and an oxide shell were present in this tribofilm and a transitional oxide (Fe2O3)-containing layer was identified at the interface between the tribofilm and the cast iron substrate. The ZDDP+IL tribofilm shared some of the characteristics found in the IL and ZDDP tribofilms. Finally, tribofilm formation mechanisms are proposed on the basis of the observations made at the atomic level.},
doi = {10.1021/acsami.7b04719},
journal = {ACS Applied Materials and Interfaces},
number = 27,
volume = 9,
place = {United States},
year = {Tue Jun 20 00:00:00 EDT 2017},
month = {Tue Jun 20 00:00:00 EDT 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 28 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
The History and Mechanisms of ZDDP
journal, October 2004
- Spikes, H.
- Tribology Letters, Vol. 17, Issue 3
Review of the lubrication of metallic surfaces by zinc dialkyl-dithiophosphates
journal, January 2005
- Nicholls, Mark A.; Do, Than; Norton, Peter R.
- Tribology International, Vol. 38, Issue 1
Phosphonium-Organophosphate Ionic Liquids as Lubricant Additives: Effects of Cation Structure on Physicochemical and Tribological Characteristics
journal, December 2014
- Barnhill, William C.; Qu, Jun; Luo, Huimin
- ACS Applied Materials & Interfaces, Vol. 6, Issue 24
Comparison of an oil-miscible ionic liquid and ZDDP as a lubricant anti-wear additive
journal, March 2014
- Qu, Jun; Luo, Huimin; Chi, Miaofang
- Tribology International, Vol. 71, p. 88-97
Impact of Lubricant Additives on thePhysicochemical Properties and Activity of Three‐Way Catalysts
journal, April 2016
- Xie, Chao; Toops, Todd; Lance, Michael
- Catalysts, Vol. 6, Issue 4
Synergistic Effects Between Phosphonium-Alkylphosphate Ionic Liquids and Zinc Dialkyldithiophosphate (ZDDP) as Lubricant Additives
journal, July 2015
- Qu, Jun; Barnhill, William C.; Luo, Huimin
- Advanced Materials, Vol. 27, Issue 32
Molecular Mechanisms for the Functionality of Lubricant Additives
journal, March 2005
- Mosey, N. J.
- Science, Vol. 307, Issue 5715
Mechanisms of antiwear tribofilm growth revealed in situ by single-asperity sliding contacts
journal, March 2015
- Gosvami, N. N.; Bares, J. A.; Mangolini, F.
- Science, Vol. 348, Issue 6230
Experimental and Molecular Dynamics Simulations of Tribochemical Reactions with ZDDP: Zinc Phosphate–Iron Oxide Reaction
journal, September 2008
- Minfray, Clotilde; Le Mogne, Thierry; Martin, Jean-Michel
- Tribology Transactions, Vol. 51, Issue 5
Interaction of phosphonium ionic liquids with borate esters at tribological interfaces
journal, January 2016
- Sharma, Vibhu; Doerr, Nicole; Erdemir, Ali
- RSC Advances, Vol. 6, Issue 58
Comparison of the tribological behavior of steel–steel and Si3N4–steel contacts in lubricants with ZDDP or ionic liquid
journal, November 2014
- Cai, Zhen-bing; Meyer, Harry M.; Ma, Cheng
- Wear, Vol. 319, Issue 1-2
Ionic Liquids Composed of Phosphonium Cations and Organophosphate, Carboxylate, and Sulfonate Anions as Lubricant Antiwear Additives
journal, October 2014
- Zhou, Yan; Dyck, Jeffrey; Graham, Todd W.
- Langmuir, Vol. 30, Issue 44
A variable temperature mechanical analysis of ZDDP-derived antiwear films formed on 52100 steel
journal, February 2007
- Pereira, Gavin; Munoz-Paniagua, David; Lachenwitzer, Andreas
- Wear, Vol. 262, Issue 3-4
Mechanism of tribofilm formation with P and S containing ionic liquids
journal, December 2015
- Sharma, Vibhu; Gabler, Christoph; Doerr, Nicole
- Tribology International, Vol. 92
A multi-technique approach of tribofilm characterisation
journal, January 2004
- Minfray, C.; Martin, J. M.; Esnouf, C.
- Thin Solid Films, Vol. 447-448
Low-friction tribofilm formed by the reaction of ZDDP on iron oxide
journal, December 2006
- Ito, Kosuke; Martin, Jean-Michel; Minfray, Clotilde
- Tribology International, Vol. 39, Issue 12
Ionic Liquid Adsorption and Nanotribology at the Silica–Oil Interface: Hundred-Fold Dilution in Oil Lubricates as Effectively as the Pure Ionic Liquid
journal, November 2014
- Li, Hua; Cooper, Peter K.; Somers, Anthony E.
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 23
Does the Use of Diamond-Like Carbon Coating and Organophosphate Lubricant Additive Together Cause Excessive Tribochemical Material Removal?
journal, August 2015
- Zhou, Yan; Leonard, Donovan N.; Meyer, Harry M.
- Advanced Materials Interfaces, Vol. 2, Issue 15
Correlative Energy-Dispersive X-Ray Spectroscopic Tomography and Atom Probe Tomography of the Phase Separation in an Alnico 8 Alloy
journal, December 2016
- Guo, Wei; Sneed, Brian T.; Zhou, Lin
- Microscopy and Microanalysis, Vol. 22, Issue 6
Atom-probe tomography characterization of the oxidation of stainless steel
journal, June 2010
- Lozano-Perez, Sergio; Saxey, David W.; Yamada, Takuyo
- Scripta Materialia, Vol. 62, Issue 11
Probing corrosion initiation at interfacial nanostructures of AA2024-T3
journal, February 2017
- Parvizi, Reza; Hughes, Anthony E.; Tan, Mike Y.
- Corrosion Science, Vol. 116
Nanoscale characterisation of grain boundary oxidation in cold-worked stainless steels
journal, October 2012
- Kruska, Karen; Lozano-Perez, Sergio; Saxey, David W.
- Corrosion Science, Vol. 63
An atom probe tomography study of internal oxidation processes in Alloy 600
journal, May 2016
- Langelier, B.; Persaud, S. Y.; Newman, R. C.
- Acta Materialia, Vol. 109
Atom-probe tomography of tribological boundary films resulting from boron-based oil additives
journal, January 2016
- Kim, Yoon-Jun; Baik, Sung-Il; Bertolucci-Coelho, Leonardo
- Scripta Materialia, Vol. 111
In situ site-specific specimen preparation for atom probe tomography
journal, February 2007
- Thompson, K.; Lawrence, D.; Larson, D. J.
- Ultramicroscopy, Vol. 107, Issue 2-3
An atom probe perspective on phase separation and precipitation in duplex stainless steels
journal, May 2016
- Guo, Wei; Garfinkel, David A.; Tucker, Julie D.
- Nanotechnology, Vol. 27, Issue 25
Atomic-resolution imaging of oxidation states in manganites
journal, February 2009
- Varela, M.; Oxley, M. P.; Luo, W.
- Physical Review B, Vol. 79, Issue 8
Oxidation states of Mn and Fe in various compound oxide systems
journal, July 2006
- Schmid, H. K.; Mader, W.
- Micron, Vol. 37, Issue 5
Oxidation state and chemical shift investigation in transition metal oxides by EELS
journal, May 2012
- Tan, Haiyan; Verbeeck, Jo; Abakumov, Artem
- Ultramicroscopy, Vol. 116
Atom probe tomography study of alloying element distributions in Zr alloys and their oxides
journal, November 2013
- Dong, Yan; Motta, Arthur T.; Marquis, Emmanuelle A.
- Journal of Nuclear Materials, Vol. 442, Issue 1-3
The Relative Oxidation Inhibition Performance of Some Neutral and Basic Zinc Dithiophosphate Salts
journal, January 1999
- Yamaguchi, E. S.; Onopchenko, A.; Francisco, M. M.
- Tribology Transactions, Vol. 42, Issue 4
The origin of anti-wear chemistry of ZDDP
journal, January 2012
- Martin, Jean Michel; Onodera, Tasuku; Minfray, Clotilde
- Faraday Discussions, Vol. 156
Works referencing / citing this record:
Engine Oils in the Field: A Comprehensive Chemical Assessment of Engine Oil Degradation in a Passenger Car
journal, May 2019
- Dörr, Nicole; Agocs, Adam; Besser, Charlotte
- Tribology Letters, Vol. 67, Issue 3
Five-Stage Selection Procedure of Ionic Liquids for Lubrication of Steel–Steel Contacts in Space Mechanisms
journal, May 2019
- Dörr, Nicole; Merstallinger, Andreas; Holzbauer, Roland
- Tribology Letters, Vol. 67, Issue 3
Material‐Dependent Antagonistic Effects between Soot and ZDDP
journal, February 2020
- Kumara, Chanaka; Meyer, Harry M.; Qu, Jun
- Advanced Materials Interfaces, Vol. 7, Issue 6
High lubricity and electrical responsiveness of solvent-free ionic SiO 2 nanofluids
journal, January 2018
- Guo, Yuexia; Zhang, Ligang; Zhang, Ga
- Journal of Materials Chemistry A, Vol. 6, Issue 6
Correlation Between Engine Oil Degradation, Tribochemistry, and Tribological Behavior with Focus on ZDDP Deterioration
journal, May 2019
- Dörr, Nicole; Brenner, Josef; Ristić, Andjelka
- Tribology Letters, Vol. 67, Issue 2