Tribochemistry of Diamond-like Carbon: Interplay between Hydrogen Content in the Film and Oxidative Gas in the Environment

Seokhoon Jang; Muztoba Rabbani; Andrew L. Ogrinc; Maxwell T. Wetherington; Ashlie Martini; Seong H. Kim

doi:10.1021/acsami.3c05316

Tribochemistry of Diamond-like Carbon: Interplay between Hydrogen Content in the Film and Oxidative Gas in the Environment

Seokhoon Jang
, Muztoba Rabbani
, Andrew L. Ogrinc
, Maxwell T. Wetherington
, Ashlie Martini
, Seong H. Kim

Research output: Contribution to journal › Article › peer-review

14 Scopus citations

Abstract

The lubricity of hydrogenated diamond-like carbon (HDLC) films is highly sensitive to the hydrogen (H) content in the film and the oxidizing gas in the environment. The tribochemical knowledge of HDLC films with two different H-contents (mildly hydrogenated vs highly hydrogenated) was deduced from the analysis of the transfer layers formed on the counter-surface during friction tests in O₂ and H₂O using Raman spectroscopic imaging and X-ray photoelectron spectroscopy (XPS). The results showed that, regardless of H-content in the film, shear-induced graphitization and oxidation take place readily. By analyzing the O₂ and H₂O partial pressure dependence of friction of HDLC with a Langmuir-type reaction kinetics model, the oxidation probability of the HDLC surface exposed by friction as well as the removal probability of the oxidized species by friction were determined. The HDLC film with more H-content exhibited a lower oxidation probability than the film with less H-content. The atomistic origin of this H-content dependence was investigated using reactive molecular dynamics simulations, which showed that the fraction of undercoordinated carbon species decreased as the H-content in the film increased, corroborating the lower oxidation probability of the highly-hydrogenated film. The H-content in the HDLC film influenced the probabilities of oxidation and material removal, both of which vary with the environmental condition.

Original language	English
Pages (from-to)	37997-38007
Number of pages	11
Journal	ACS Applied Materials and Interfaces
Volume	15
Issue number	31
DOIs	https://doi.org/10.1021/acsami.3c05316
State	Published - Aug 9 2023
Externally published	Yes

Funding

This work was supported by the National Science Foundation (Grant No. CMMI-1912199, 2038494, and 2038499). The authors acknowledge Dr. Osman Levent Eryilmaz and Prof. Ali Erdemir for providing HDLC samples used in this study. All Raman, XPS, and contact angle measurements were performed in the Materials Characterization Laboratory in the Materials Research Institute at Pennsylvania State University.

Keywords

environmental sensitivity
hydrogenated diamond-like carbon
shear-induced graphitization
superlubricity
surface oxidation

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10.1021/acsami.3c05316

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@article{38697a4ba3a34f86ad77338cd548701f,

title = "Tribochemistry of Diamond-like Carbon: Interplay between Hydrogen Content in the Film and Oxidative Gas in the Environment",

abstract = "The lubricity of hydrogenated diamond-like carbon (HDLC) films is highly sensitive to the hydrogen (H) content in the film and the oxidizing gas in the environment. The tribochemical knowledge of HDLC films with two different H-contents (mildly hydrogenated vs highly hydrogenated) was deduced from the analysis of the transfer layers formed on the counter-surface during friction tests in O2 and H2O using Raman spectroscopic imaging and X-ray photoelectron spectroscopy (XPS). The results showed that, regardless of H-content in the film, shear-induced graphitization and oxidation take place readily. By analyzing the O2 and H2O partial pressure dependence of friction of HDLC with a Langmuir-type reaction kinetics model, the oxidation probability of the HDLC surface exposed by friction as well as the removal probability of the oxidized species by friction were determined. The HDLC film with more H-content exhibited a lower oxidation probability than the film with less H-content. The atomistic origin of this H-content dependence was investigated using reactive molecular dynamics simulations, which showed that the fraction of undercoordinated carbon species decreased as the H-content in the film increased, corroborating the lower oxidation probability of the highly-hydrogenated film. The H-content in the HDLC film influenced the probabilities of oxidation and material removal, both of which vary with the environmental condition.",

keywords = "environmental sensitivity, hydrogenated diamond-like carbon, shear-induced graphitization, superlubricity, surface oxidation",

author = "Seokhoon Jang and Muztoba Rabbani and Ogrinc, \{Andrew L.\} and Wetherington, \{Maxwell T.\} and Ashlie Martini and Kim, \{Seong H.\}",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

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doi = "10.1021/acsami.3c05316",

language = "English",

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T2 - Interplay between Hydrogen Content in the Film and Oxidative Gas in the Environment

AU - Jang, Seokhoon

AU - Rabbani, Muztoba

AU - Ogrinc, Andrew L.

AU - Wetherington, Maxwell T.

AU - Martini, Ashlie

AU - Kim, Seong H.

PY - 2023/8/9

Y1 - 2023/8/9

N2 - The lubricity of hydrogenated diamond-like carbon (HDLC) films is highly sensitive to the hydrogen (H) content in the film and the oxidizing gas in the environment. The tribochemical knowledge of HDLC films with two different H-contents (mildly hydrogenated vs highly hydrogenated) was deduced from the analysis of the transfer layers formed on the counter-surface during friction tests in O2 and H2O using Raman spectroscopic imaging and X-ray photoelectron spectroscopy (XPS). The results showed that, regardless of H-content in the film, shear-induced graphitization and oxidation take place readily. By analyzing the O2 and H2O partial pressure dependence of friction of HDLC with a Langmuir-type reaction kinetics model, the oxidation probability of the HDLC surface exposed by friction as well as the removal probability of the oxidized species by friction were determined. The HDLC film with more H-content exhibited a lower oxidation probability than the film with less H-content. The atomistic origin of this H-content dependence was investigated using reactive molecular dynamics simulations, which showed that the fraction of undercoordinated carbon species decreased as the H-content in the film increased, corroborating the lower oxidation probability of the highly-hydrogenated film. The H-content in the HDLC film influenced the probabilities of oxidation and material removal, both of which vary with the environmental condition.

AB - The lubricity of hydrogenated diamond-like carbon (HDLC) films is highly sensitive to the hydrogen (H) content in the film and the oxidizing gas in the environment. The tribochemical knowledge of HDLC films with two different H-contents (mildly hydrogenated vs highly hydrogenated) was deduced from the analysis of the transfer layers formed on the counter-surface during friction tests in O2 and H2O using Raman spectroscopic imaging and X-ray photoelectron spectroscopy (XPS). The results showed that, regardless of H-content in the film, shear-induced graphitization and oxidation take place readily. By analyzing the O2 and H2O partial pressure dependence of friction of HDLC with a Langmuir-type reaction kinetics model, the oxidation probability of the HDLC surface exposed by friction as well as the removal probability of the oxidized species by friction were determined. The HDLC film with more H-content exhibited a lower oxidation probability than the film with less H-content. The atomistic origin of this H-content dependence was investigated using reactive molecular dynamics simulations, which showed that the fraction of undercoordinated carbon species decreased as the H-content in the film increased, corroborating the lower oxidation probability of the highly-hydrogenated film. The H-content in the HDLC film influenced the probabilities of oxidation and material removal, both of which vary with the environmental condition.

KW - environmental sensitivity

KW - hydrogenated diamond-like carbon

KW - shear-induced graphitization

KW - superlubricity

KW - surface oxidation

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DO - 10.1021/acsami.3c05316

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JF - ACS Applied Materials and Interfaces

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ER -

Tribochemistry of Diamond-like Carbon: Interplay between Hydrogen Content in the Film and Oxidative Gas in the Environment

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