Overcoming immiscibility toward bimetallic catalyst library
Overcoming immiscibility toward bimetallic catalyst library
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DOI：
10.1126/sciadv.aaz6844
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发表时间：
2020-04-01
期刊：
影响因子：
13.6
通讯作者：
Hu, Liangbing
中科院分区：
文献类型：
--
作者：
Yang, Chunpeng;Ko, Byung Hee;Hu, Liangbing
双金属材料是新兴的重要材料，通常表现出与单金属材料不同的化学性质。然而，由于组成元素的热力学不混溶性，获得均合金双金属的途径有限。克服双金属体系固有的不互溶性将创造出具有独特性质的双金属文库。在这里，我们提出了一种非平衡合成策略来解决双金属化合物的不混溶性挑战。作为概念的证明，我们合成了广泛的均匀合金铜基双金属纳米颗粒，而不考虑热力学不混溶性。进一步研究了非平衡双金属纳米颗粒在商业相关电流密度（>100 mA cm(-2)）下作为一氧化碳还原电催化剂的作用，其中Cu0.9Ni0.1在电流密度约为93 mA cm（-2）时表现出最高的多碳产物法拉第效率，接近76%。在多金属合成中克服热力学不混相的能力为设计和合成具有所需化学成分和催化性能的新型功能纳米材料提供了自由。
Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm(-2)), in which Cu0.9Ni0.1 shows the highest multicarbon product Faradaic efficiency of similar to 76% with a current density of similar to 93 mA cm(-2). The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties.