Abstract
During the last decade, two-dimensional (2D) materials have emerged as versatile building blocks for the next generation of engineered materials. However, the intrinsically brittle behavior of 2D materials has thus far delayed their adoption in applications such as sensors and structural materials. Herein, we demonstrate a strategy for toughening graphene oxide (GO) through synergistic interfacial interactions between GO monolayers and ultrathin layers of strongly interacting poly(vinyl alcohol) (PVA). By creating GO-PVA and PVA-GO-PVA nanolaminates, we demonstrate a 2-fold increase in GO toughness, which translates into dramatic increases in energy dissipation and piercing resistance. Atomistic simulations show that this remarkable behavior arises from a polymer chain crack-bridging mechanism, resulting from a synergistic combination of interdomain reinforcements across the GO monolayer and extensive GO-polymer interfacial hydrogen-bonding interactions. The reported findings highlight the potential for achieving engineered 2D materials with superior mechanical properties by incorporating deformation and failure-resistant mechanics arising from tailored chemical interactions between constituents.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 369-388 |
| Number of pages | 20 |
| Journal | Matter |
| Volume | 1 |
| Issue number | 2 |
| DOIs | |
| State | Published - Aug 7 2019 |
Funding
The authors acknowledge the support of NSF through DMREF award no. CMMI-1235480, Multi-University Research Initiative (MURI) awards through the Air Force of Scientific Research ( AFOSR-FA9550-15-1-0009 ), and the Army Research Office ( W911NF-08-1-0541 ). Material characterization used the Keck-II facility (NUANCE Center-Northwestern University). Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences , under contract no. DE-AC02-06CH11357 . The authors thank Dr. Fan Zhou for assistance in the preparation of the Si substrate. R.A.S.-C. acknowledges support from NSF through the Graduate Research Fellowships Program (GRFP), partial support from the Northwestern University Ryan Fellowship, and partial support from Northwestern University through a Royal Cabell Terminal Year Fellowship. H.T.N. acknowledges support from the Vietnam Education Foundation. The authors thank R. Ramachandramoorthy, M. Chon, R. Yang, M. Daly, and D. Restrepo for helpful discussions. The authors acknowledge the support of NSF through DMREF award no. CMMI-1235480, Multi-University Research Initiative (MURI) awards through the Air Force of Scientific Research (AFOSR-FA9550-15-1-0009), and the Army Research Office (W911NF-08-1-0541). Material characterization used the Keck-II facility (NUANCE Center-Northwestern University). Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. The authors thank Dr. Fan Zhou for assistance in the preparation of the Si substrate. R.A.S.-C. acknowledges support from NSF through the Graduate Research Fellowships Program (GRFP), partial support from the Northwestern University Ryan Fellowship, and partial support from Northwestern University through a Royal Cabell Terminal Year Fellowship. H.T.N. acknowledges support from the Vietnam Education Foundation. The authors thank R. Ramachandramoorthy, M. Chon, R. Yang, M. Daly, and D. Restrepo for helpful discussions. H.D.E. S.T.N. and J.H. designed and supervised the research. H.D.E. guided the experimental and computational mechanics aspects of the project. J.H. and S.T.N. guided material synthesis and polymer modification. R.A.S.-C. and X.W. conducted the mechanical experiments and analyzed the data. L.M. conducted the sample-synthesis and -characterization experiments. J.W. conducted the HRTEM, STEM, and EELS characterization of the samples and analyzed the results. R.A.S.-C. and X.Z. conducted the all-atom MD simulations, and H.T.N. performed the finite-element modeling calculations and crack-bridging analysis in GO-PVA. All authors contributed in writing, reading, and commenting on the manuscript. The authors declare no competing interests.
Keywords
- 2D materials
- AFM indentation
- GO
- GO-PVA
- MAP 3: Understanding
- crack bridging
- energy dissipation
- fracture
- graphene oxide nanolaminates
- hydrogen bonding
- nanoconfinement
ASJC Scopus subject areas
- General Materials Science