Progress in Interfacial Thermodynamics and Grain Boundary Complexion Diagram

doi:10.11900/0412.1961.2021.00036

Acta Metall Sin

2021, Vol. 57

Issue (9): 1199-1214 DOI: 10.11900/0412.1961.2021.00036

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Progress in Interfacial Thermodynamics and Grain Boundary Complexion Diagram

HU Biao¹, ZHANG Huaqing², ZHANG Jin¹, YANG Mingjun², DU Yong²(

), ZHAO Dongdong³

^1.School of Materials Science and Engineering, Anhui University of Science and Technology, Huainan 232001, China
^2.State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China
^3.School of Materials Science and Engineering, Tianjin University, Tianjin 300350, China

Cite this article:

HU Biao, ZHANG Huaqing, ZHANG Jin, YANG Mingjun, DU Yong, ZHAO Dongdong. Progress in Interfacial Thermodynamics and Grain Boundary Complexion Diagram. Acta Metall Sin, 2021, 57(9): 1199-1214.

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Abstract

Grain boundaries (GBs), a crucial component of microstructures, have a significant influence on the properties of materials. The GB complexion (GBC) transitions are essential information to accurately explain numerous material phenomena. However, owing to the complexity of GB structures and the difficulty in observation of GBC transitions, there is still no direct evidence and mechanism explanation for these material phenomena. With the advancement of characterization equipment, especially spherical aberration-correction transmission electron microscopy, coupled with powerful computer simulation, the establishment of interfacial thermodynamic models to construct different types of GBC diagrams, which provide a broad prospect for the study of GB structures and GBC transitions, is essential. In this paper, the progress of interface thermodynamics and GBC diagrams from the aspects of the classification and characterization of GBs and GBC transitions, interface thermodynamic models, and the construction of GBC diagrams were reviewed. The paper also looks forward to the future development of interface thermodynamics and GBC diagrams.

Key words: grain boundary grain boundary complexion transition interface thermodynamic model grain boundary complexion diagram

Received: 21 January 2021

ZTFLH:

TB113.14

Fund: National Natural Science Foundation of China(52071002);Natural Science Foundation of Anhui Province(2008085QE200)

About author: DU Yong, professor, Tel: (0731)88877300, E-mail: yong-du@csu.edu.cn

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https://www.ams.org.cn/EN/10.11900/0412.1961.2021.00036 OR https://www.ams.org.cn/EN/Y2021/V57/I9/1199

Fig.1 Six types of Dillon-Harmer complexions as originally discovered in undoped and doped Al₂O₃^[26] (a-f), analogous examples of Dillon-Harmer complexions in metallic materials^{[12,27,37-39]} (g-l), and schematics of six types of Dillon-Harmer complexions^[37] (m-r)

Fig.2 Schematics of wetting transition^[37]

Fig.3 Coexistence and phase transformation of Σ5 (310)[001] grain boundary and two grain boundary phases in bcc structure W^[53]

Fig.4 The grain boundary mobility (γM_b) versus temperature for undoped and doped alumina^[26] along with schematic depiction of the six Dillon-Harmer complexions (AGG—abnormal grain growth, NGG—normal grain growth)

Type	Definition mode	Terminology	Meaning
Complexion	Defined by	Congruent	Grain boundary characters (R and n) remain invariant, atomic structure
transitions	geometry	transition	and composition of the grain boundary core change
category		Non-congruent	Grain boundary characters (R and/or n) change
		transition
		Structural	Bulk thermodynamic parameters (T, P, μ, etc.) change, interfacial
		transition	thermodynamic parameters (R, n, etc.) remain invariant
		Faceting	A single complexion decomposes into two complexions, the grain
		transition	boundary plane normal n decomposes into n₁ and n₂
		Dissociation	A single complexion decomposes into two complexions, a single grain
		transition	boundary dissociates into two new interfaces with the misorientation
			relationship of R→ R₁+ R₂
	Defined by	Premelting	A disordered, liquid-like film at a grain boundary forms below the
	structure and/or	transition	melting temperature (or solidus) of the bulk phase
	composition	Prewetting	A nanolayer complexion with fixed equilibrium thickness forms at the
		transition	interface near the temperature or composition of the wetting transition
		Adsorption	A dramatic change in the composition of an interface in which the
		transition	relative amount of solute increases or decreases significantly
Complexion	Defined by	Intrinsic	The complexion exists in pure systems, its composition is identical to
category	composition	complexion	the bulk composition
		Extrinsic	The complexion exists in a non-pure system, its composition is in
		complexion	general not equal to the bulk composition
	Dillon-Harmer	Clean	A complexion is structurally abrupt, solute segregation is not
	complexion	complexion	necessarily entirely absent, but is minimal or is not observed at all,
			which does not lead to an increase in thickness of the grain boundary
			core
		Monolayer	The majority of the adsorbed solute is confined to a thickness of a
		complexion	single atomic layer
		Bilayer	The most of the adsorbed solute occupies a thickness of two atomic
		complexion	layers
		Trilayer	The most of the adsorbed solute occupies a thickness of three atomic
		complexion	layers
		Nanolayer	The adsorbed solute occupies a thickness larger than three atomic
		complexion	layers, but which is still finite, fixed and governed by equilibrium
			thermodynamics, equivalent to intergranular film (IGF)
		Wetting	The bulk wetting film (solid or liquid) at a grain boundary, it has two
		complexion	complexions on each side of the wetting film
	Defined by	Dry	A complexion with no adsorbed solute or very little adsorption,
	thickness and	complexion	corresponds to the monolayer Dillon-Harmer complexion
	composition	Moist	A complexion with multilayer solute adsorption, corresponds to the
		complexion	bilayer, trilayer and nanolayer Dillon-Harmer complexions
		Wet	Refers to the bulk wetting film at a boundary, corresponds to the
		complexion	wetting Dillon-Harmer complexion

Table 1 Terminology related to complexion transitions and complexions^[37]

Fig.5 APT analyses of Al-Zn-Mg-Cu alloy after aging at 120^oC for 0.5 h^[42]

Fig.6 Schematics of subsolidus quasi-liquid intergranular films^[92] (γ_cl and γ_GB are the excess free energies for crystal-liquid and grain boundary, respectively. The superscript “(0)” is used to denote a hypothetic “dry” and “perfectly crystalline” interface. Δγ is the change of interface energy. h is the thickness of the quasi-liquid intergranular film, σ_interfacial(h) is the interfacial potential that represents the interactions of two interfaces when the film is thin)

Fig.7 Schematic of a symmetrical flat grain boundary^[94] (ρ is the atomic density at the grain boundary relative to the bulk, ρ^GB is the average relative atomic density within the grain boundary plane)

Fig.8 Schematics of procedures to construct an isothermal section of a ternary grain boundary λ diagram for W-Ni-Fe at 1673 K (W—the primary element with underline, λ—the thermodynamic parameter, T—absolute temperature)^[35] and HRTEM image^[10]

Fig.9 Density-based Gibbs free energy of the Pt-Au system at 300 K^[94] ( $G S S G B$ is the density-based Gibbs free energy of a regular solid solution for grain boundary, X_Au is the composition of Au in mole fraction)

Fig.10 The bulk phase diagram (ρ = 1) and grain boundary phase diagram (ρ^GB = 0.75) of the Pt-Au system^[94]

Fig.11 The segregation isotherm of the Pt-Au system at 700 K^[94] ( $X A u G B$ is the Au composition of the grain boundary, $X A u B u l k$ is the Au composition of the bulk far from the grain boundary)

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