Elsevier

Applied Surface Science

Volume 541, 1 March 2021, 148524
Applied Surface Science

Full Length Article
Understanding heterogeneous metal-mediated interfacial enhancement mechanisms in graphene-embedded copper matrix composites

https://doi.org/10.1016/j.apsusc.2020.148524Get rights and content

Highlights

  • Graphene-Cu interfaces were tuned via alloying heterogeneous elements.

  • The enhanced interfaces are favourable to improving tensile properties.

  • The preferable atomic orientation arrangement states were identified.

  • The underlying interfacial enhancement mechanisms were analysed.

Abstract

Graphene-embedded Cu matrix composites (GE-CMCs), as one of typical versatile functional composite materials, have great potential to be widely utilized in many engineering fields. Unfortunately, one of major issues is the weak interfacial interactions between metallic matrix and carbonaceous graphene, leading to the rapid mechanical failure. In this work, some heterogeneous alloying elements, including Ni, Ti, Mn and Al, are proposed to be incorporated into Cu matrix to re-construct graphene-Cu interface with the attempt to improve tensile properties of GE-CMCs via first-principles calculations. Meanwhile, a systematical investigation is given on the atomic orientation arrangement states to identify the preferable conditions, which reveal that alloying Mn element with Cu matrix with an equal atomic arrangement over the graphene-Cu interface delivers the most robust interfacial bonding ability, thus resulting in obvious strength (364%) and elongation increasement (415%) in comparison with the pristine graphene-Cu interface in GE-CMCs. Furthermore, the electronic structures and the underlying deformation and enhancement mechanisms of Mn-alloyed GE-CMCs are analyzed to verify the presence of enhanced Mn-C bonds over graphene-Cu interfaces as the external strain increases. It is expected that this work opens an avenue to understand the interfacial enhancement mechanisms and offers an effective interfacial optimization strategy via tuning the atomic arrangement orientation states to achieve high-performance tensile performance for GE-CMCs or other graphene-metal composites.

Introduction

Functional composite materials that constituent two and more naturally occurring and/or artificially designed components have been evidenced to deliver various remarkably physical, chemical, and mechanical properties [1], [2], [3], [4], [5], [6], [7], [8], [9]. For example, the deliberate implantation of the emerging graphene into the widely utilized metallic copper matrix can bring about some superior characteristics, such as the significantly improved mechanical strengths, which definitively endows these graphene-embedded Cu matrix composites (GE-CMCs) with great potential to be widely applied in many engineering fields, including aeronautics, transportation and marine sectors [10], [11], [12], [13], [14], [15]. In principle, these reinforcement effects in GE-CMCs by using the emerging two-dimensional (2D) graphene are closely related to its exceptional properties, including an ultrahigh aspect ratio, a high elastic modulus, a superior mechanical strength, a high electrical and thermal conductivity [16], [17], [18], [19]. However, the poor binding compatibility between graphene and Cu matrix in GE-CMCs is still a major challenge to meet the practical requirements on mechanical properties [20], [21], [22]. Therefore, it is of much significance to further promote the reinforcement effects over carbon–metal interfaces, which can be achieved by several effective interfacial manipulation strategies, such as structural modifications on graphene or the Cu matrix [23], [24], [25], [26], [27], [28], [29], [30], [31].

To address this issue, one commonly used and effective strategy is to alloy heteroatoms with Cu matrix, especially within these crucial regions near graphene-Cu interfaces in GE-CMCs, and these new atom configuration may induce new electronic or chemically bonding interfacial states, which are much favorable to consolidating graphene-Cu interfaces and thus results in attractive mechanically tensile properties of GE-CMCs [12], [31], [32], [33], [34], [35], [36], [37], [38], [39]. For example, it has been verified that the interfacial bonding capacity could be considerably boosted in the presence of some new-formed chemically carbide species (e.g. Ti8C5, Cr7C3 and Al4C3), and the strong pdπ hybridization effects graphene-nickel interfaces initiated by the single pz electron in graphene and the d electron in nickel matrix [12], [27], [32], [33], [34], [35], [36], [37], [38], [39]. These introduced alloy elements act as “interfacial rivets” to bridge the graphene and metallic matrix to accommodate the desired mechanical property requirements. Similarly, the deliberate incorporation of heterogeneous atoms into Cu matrix is expected to be a feasible strategy to re-construct graphene-Cu interfaces in GE-CMCs for mechanical enhancement, More importantly, the further exploration on the optimal alloying element type and the preferable atomic orientation arrangement states over graphene-Cu interfaces are the prerequisite conditions for understanding the in-depth interfacial enhancement mechanisms in GE-CMCs, however, these two aspects have been rarely investigated until now. From this viewpoint, the accurate identification on the desired alloying element type with the specific orientation state for graphene-Cu interfaces are critically needed and the underlying interface-induced enhancement mechanisms for GE-CMCs are urgently revealed.

In this work, four types of alloying elements, including Ni, Ti, Mn, and Al, are proposed to be embedded into Cu matrix to optimize the graphene-Cu interface with the attempt to improve tensile properties of GE-CMCs via first-principles calculations. Meanwhile, a systematical investigation on the atomic orientation arrangement states for each alloying element is given to identify the preferable conditions. These results reveal that alloying Mn element with Cu matrix with an equal atomic arrangement over the graphene-Cu interface (denoted as A1A2A'1A'2-Mn) delivers the most robust interfacial bonding ability, which results in obvious strength (364%) and elongation increasement (415%) in comparison with the pristine graphene-Cu interface in GE-CMCs. Furthermore, the electronic structures of the heterogeneous metal-alloyed GE-CMCs with the preferable atomic arrangement orientation interface (A1A2A'1A'2) are analyzed to confirm the closely interaction between alloying atoms with graphene. Finally, the underlying deformation and enhancement mechanisms of Mn-alloyed GE-CMCs are detailed analyzed via the stress–strain relations and crystal orbital Hamilton population (COHP), which verifies that the increased mechanical properties of Mn-alloyed GE-CMCs are largely associated with the enhanced Mn-C bonds over graphene-Cu interfaces as the external strain increases. It is expected that this work opens an avenue to understand the interfacial enhancement mechanisms, and offers an effective interfacial optimization strategy via manipulating the heterogeneous alloying element types and atomic arrangement orientation states to achieve high-performance tensile performance for GE-CMCs or other graphene-metal composites.

Section snippets

Computational methods

All the geometry optimization and energy analysis processes were performed using Cambridge Sequential Total Energy Package (CASTEP) code with density functional theory (DFT). The generalized gradient approximation (GGA) with the Perdew-Burke-Ernzerholf (PBE) method was used as the exchange–correlation interaction [40], [41]. The DFT-D method was proposed to account the long-range van der Waals interactions between graphene and matrix Cu [42]. A kinetic energy cutoff of 340 eV was used with a

Atomic arrangement orientation

In this part, the graphene-Cu interfaces in GE-CMCs are reinforced by optimizing atomic arrangement orientation types, including A1A'1, A1A2A'1A'2 and A1B1A'1B'1 systems, for different heterogeneous alloyed elements.

A1A'1 Type. By comparison on the optimized geometries of A1A'1 systems (Fig. S1), when different metal atoms are embedded into the graphene-Cu interfaces to form A1A'1-M (M = Ti, Mn, Al and Ni) systems, Ti and Mn atoms tends to approach the middle graphene while Al atoms buck the

Conclusions

The incorporation of heterogeneous alloying atoms (e.g. Ni, Ti and Mn) into Cu matrix is verified as an effective strategy for enhancing graphene-Cu interfaces in GE-CMCs. Furthermore, the optimization of alloying element type and the preferable atomic orientation arrangement states for mechanically tensile property enhancement are systematically investigated by the ab initio calculation, which revels that the Mn-alloyed Cu matrix with a full-concentration atomic arrangement state near the

CRediT authorship contribution statement

Qian Zhang: Conceptualization, Methodology, Software, Investigation, Writing - original draft. Zonglin Yi: Methodology, Investigation. Ying Liu: Formal analysis, Methodology. Peide Han: Resources, Writing - review & editing, Supervision. Jun Mei: Formal analysis, Writing - review & editing.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No.51871159, U1820204). We acknowledge the grants of high-performance computer time from the computing facility at the Queensland University of Technology.

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