诸如镓(Ga)的室温液态金属(LM)具有与特定材料反应的潜力,这将培育新的应用类别。这里,报告了由于Ga基LM团簇在金(Au)膜上的非平衡反应扩散和扩散限制而导致的各种自组织环模式,其中扩散是控制步骤,自限制氧化物层起到动力学屏障的作用。这种现象,传统上被称为Liesegang戒指,主要发生在电解质介质中。与现有系统不同,当前的周期性结晶机制在环境条件下可以在较小的尺度上实现高度对称的时空周期性Liesegang环。通常,构造了Ga-Au和共晶镓铟合金(EGaIn)-Au反应-扩散-扩散系统,获得回复型和混合型同心列塞冈模式,分别。通过改变初始Ga/In质量比,进一步分析了混合Liesegang图案中中间相产物AuGa2和AuIn2的竞争图案行为,第一原理计算,和分子动力学模拟。当GaIn合金中In的质量比超过15%时,它将优先与Au反应。LMLiesegang现象的发现预计将成为自组织反应扩散系统的爆发点,并为材料合成和珠宝设计行业等不同领域提供有希望的规则。
Room temperature liquid metals (LM) such as gallium (Ga) own the potential to react with specific materials which would incubate new application categories. Here, diverse self-organized ring patterns due to nonequilibrium reaction-diffusion and spreading-limitation of Ga-based LM clusters on gold (Au) film are reported, among which diffusion is the controlling step and the self-limiting oxide layer plays the role of kinetic barrier. Such phenomena, classically known as the Liesegang rings, mainly occur in electrolyte media. Unlike existing systems, the present periodic crystallization mechanism enables highly symmetric spatiotemporal periodic Liesegang rings on a smaller scale under ambient conditions. Typically, the Ga-Au and eutectic gallium-indium alloy (EGaIn)-Au reaction-diffusion-spreading systems are constructed, obtaining the revert type and hybrid type concentric Liesegang patterns, respectively. The competitive patterning behavior of the intermediate phase products AuGa2 and AuIn2 in hybrid Liesegang patterns is further analyzed by altering the initial Ga/In mass ratio, first-principles calculations, and molecular dynamic simulations. When the mass ratio of In in GaIn alloy exceeds 15%, it will preferentially react with Au. The discovery of LM Liesegang phenomenon is expected to be a flashpoint for self-organized reaction-diffusion systems and offers promising rules for diverse areas such as materials synthesis and the jewelry design industry.