Topology-generating interfacial pattern formation during liquid metal dealloying

Geslin, Pierre-Antoine; McCue, Ian; Gaskey, Bernard; Erlebacher, Jonah; Karma, Alain

doi:10.1038/ncomms9887

Cited by 149 publications

(134 citation statements)

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“…To synthesize the 3DNP HEA, we utilized liquid metal dealloying (LMD), a unique technique to fabricate non‐noble porous materials used in structural, functional, and medical products by preventing oxidation in a metallic melt . The high‐entropy design of LMD based on the enthalpy of mixing is depicted in Figure a,b.…”

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confidence: 99%

Beating Thermal Coarsening in Nanoporous Materials via High‐Entropy Design

et al. 2019

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produced by dealloying have outstanding physical properties due to their unique structure with open porous networks, [3][4][5] the undesirable coarsening phenomenon leads to degradation of physical properties over time, even at room temperature. [6][7][8] The originally proposed idea behind high-entropy alloy (HEA) with multiprinciple elements is maximizing the configuration entropy to stabilize a solid-solution alloy without undesired ordered intermetallics. [9][10][11] Many studies have suggested that HEAs uniquely possesses combined desirable properties such as a high strength and ductility paired with high fracture toughness, [12][13][14] fatigue resistance, [15] and creep resistance. [16] HEAs also show promising properties in harsh environments resisting corrosion, [17][18][19] and irradiation [20] attacks. Atomic size differences between constituting elements in HEA increase the activation energy for grain growth, and sluggish diffusion kinetics has considered as the main reason for the exceptional high strength and structural stability of HEAs at high temperatures. [21,22] The rationale behind it, the multiprinciple elements cause larger fluctuations in lattice potential energy (LPE), providing many low-LPE sites that hinder atomic diffusion. [23] Grain growth and ligament coarsening rely on the same physical background of surface diffusion. In that context, the high-entropy design in nanoporous materials has a potential for achieving an exceptional stability against the coarsening.Controlling the feature sizes of 3D bicontinuous nanoporous (3DNP) materials is essential for their advanced applications in catalysis, sensing, energy systems, etc., requiring high specific surface area. However, the intrinsic coarsening of nanoporous materials naturally reduces their surface energy leading to the deterioration of physical properties over time, even at ambient temperatures. A novel 3DNP material beating the universal relationship of thermal coarsening is reported via high-entropy alloy (HEA) design. In newly developed TiVNbMoTa 3DNP HEAs, the nanoporous structure is constructed by very fine nanoscale ligaments of a solid-solution phase due to enhanced phase stability by maximizing the configuration entropy and suppressed surface diffusion. The smallest size of 3DNP HEA synthesized at 873 K is about 10 nm, which is one order of magnitude smaller than that of conventional porous materials. More importantly, the yield strength of ligament in 3DNP HEA approaches its theoretical strength of G/2π of the corresponding HEA alloy even after thermal exposure. This finding signifies the key benefit of high-entropy design in nanoporous materials-exceptional stability of size-related physical properties. This high-entropy strategy should thus open new opportunities for developing ultrastable nanomaterials against its environment.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.

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Beating Thermal Coarsening in Nanoporous Materials via High‐Entropy Design

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“…Traditionally, PS templates have been sensitized utilizing SnCl 2 as a seeding agent for the activation step, i.e., the templates were soaked in an aqueous solution of SnCl 2 . However, this depends on the ability of Sn 21 ions to adhere to the surface of the nanochannels in the template. 41 An alternative sensitization process employs a surface modification technique that enhances the ability of metallizing ions to adhere to the pore surfaces.…”

Section: Electroless Deposition Processmentioning

confidence: 99%

“…(iii) Upon introducing activated templates to an ionic nickel plating bath, nickel ions are reduced at palladium sites where Pd acts as catalyst of the reduction of Ni 21 to Ni. In general, electroless plating processes are autocatalyzed as redox reactions.…”

Section: Electroless Deposition Processmentioning

confidence: 99%

“…20 In recent years, dealloying using a liquid metal instead of an aqueous solution has been developed to produce nanocomposites as well as nanoporous metals. 21 For example, an Nb-Ni alloy was immersed in molten Mg where Ni atoms were dealloyed (i.e., dissolved in Mg), and removal of the Mg-Ni phase by immersing the composite in nitric acid leads to a porous Nb structure. 22 Porous Ti, 23 Fe, and Fe-Cr 24 have also been produced by a similar method.…”

Section: Introductionmentioning

confidence: 99%

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Template-based fabrication of nanoporous metals

Rebbecchi

Chen

2017

J. Mater. Res.

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Nanoporous metallic foams with high surface area and novel functional behavior are positioned to stimulate new multifunctional and metamaterial applications. However, there are fundamental challenges in achieving uniform nanopores and tailorable morphology. Emerging templating methods offer a wide range of applicable metallic species while enhancing control of pore morphology, uniformity, and interconnectivity. Here, a critical review of nanoporous metal fabrication is presented, with focus on templating methods utilizing nanoporous polymeric templates. Metals are introduced into percolative nanochannels of sacrificial templates by deposition, and subsequent removal of templates yields ordered nanoporous metals. We introduce approaches for preparing nanoporous templates, including utilizing block copolymer self-assembly that yields periodic gyroid networks. While metallization of templates by electrodeposition has been demonstrated, electroless deposition permits uniform deposition by many metallic species and infiltration of narrow pores. Examples of nanoporous metals with uniform pore sizes below 50 nm fabricated by templating methods are examined.

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“…14 Conversely, if interaction strengths vary too greatly then either macroscopic phase segregation (like interactions favoured, e.g. eutectics 15 ) or component ordering (unlike interactions favoured, e.g. double perovskites 16,17 ) occurs.…”

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Compositional nanodomain formation in hybrid formate perovskites

et al. 2017

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We report the synthesis and structural characterisation of three mixed-metal formate perovskite families [C(NH 2 ) 3 ]M 1−x Cu x (HCOO) 3 (M = Mn, Zn, Mg). Using a combination of infrared spectroscopy, non-negative matrix factorization, and reverse Monte Carlo refinement, we show that the Mn-and Zn-containing compounds support compositional nanodomains resembling the polar nanoregions of conventional relaxor ferroelectrics. The M = Mg family exhibits a miscibility gap that we suggest reflects the limiting behaviour of nanodomain formation.Compositional heterogeneity is an essential ingredient in a number of important classes of functional materials. 1 Arguably the clearest example is that of the relaxor ferroelectrics, such as (1 − x)Pb(Mg 1/3 Nb 2/3 )O 3 -xPbTiO 3 (PMN-PT): 2 here an inhomogeneous distribution of B-site cations allows the formation of polar nanoregions (PNRs), 3-5 the collective motion of which is responsible for the giant electromechanical response observed and exploited experimentally. 6,7 Recently, the same ideas have been extended to relaxor ferromagnets, 8 which are in turn conceptually related to cluster spin glasses, 9 known for their exotic magnetic memory effects. 10 Likewise, in some porous metal-organic frameworks (MOFs), inhomogeneous vacancy distributions 11 affect gas uptake 12 via a mechanism that is analogous to ion conduction pathways in compositionally-heterogeneous solid-oxide fuel-cell materials. 13 From a materials design perspective, the existence of nanoscale compositional inhomogeneities relies on a delicate balance of interaction strengths at the atomic scale. If the interaction between [18][19][20] It was in this context that we sought to explore cation distributions in the mixed-metal formate perovskites [Gua]Cu x M 1−x (HCOO) 3 (Gua + = C(NH 2 ) + 3 ; M = Mn, Zn, Mg). It has been known for some time that many formate perovskites show relaxor-like dielectric behaviour, [21][22][23] which is usually associated with glassy dynamics of the organic (A-site) cation. 24,25 Indeed a recent 13 C NMR study of [(CH 3 ) 2 NH 2 ]Zn(HCOO) 3 even demonstrated the spontaneous formation of fluxional PNRs during the onset of ferroelectric order. 26 By contrast, the exploration of mixed-metal formate perovskites is rather less well developed. 27-31 Our focus here on the [Gua]M(HCOO) 3 family is motivated by the link in this particular system between polarization and cooperative Jahn-Teller (JT) order for M = Cu [ Fig. 1]. 28,32,33 In particular, we anticipated that substitution on the Cu site by JT-inactive cations (i.e., Mn, Zn, Mg; note Cd gives a different structure type 28,34 ) might be expected to reduce the length-scale of polar order, and-if clustering were found to occur-then favour the formation of PNRs in Cu dilute compositions.Moreover, a computational study of [Gua]Mn 0.5 Cu 0.5 (HCOO) 3 has recently suggested strong enhancement in both polarization and magnetization relative to the Mn-and Cu-containing end-members. 35 Our focus here is on the synthesis and structural char...

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Topology-generating interfacial pattern formation during liquid metal dealloying

Cited by 149 publications

References 48 publications

Beating Thermal Coarsening in Nanoporous Materials via High‐Entropy Design

Beating Thermal Coarsening in Nanoporous Materials via High‐Entropy Design

Template-based fabrication of nanoporous metals

Compositional nanodomain formation in hybrid formate perovskites

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