Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742.
Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, IL 60607.
Proc Natl Acad Sci U S A. 2020 Mar 24;117(12):6316-6322. doi: 10.1073/pnas.1903721117. Epub 2020 Mar 10.
Multimetallic nanoclusters (MMNCs) offer unique and tailorable surface chemistries that hold great potential for numerous catalytic applications. The efficient exploration of this vast chemical space necessitates an accelerated discovery pipeline that supersedes traditional "trial-and-error" experimentation while guaranteeing uniform microstructures despite compositional complexity. Herein, we report the high-throughput synthesis of an extensive series of ultrafine and homogeneous alloy MMNCs, achieved by 1) a flexible compositional design by formulation in the precursor solution phase and 2) the ultrafast synthesis of alloy MMNCs using thermal shock heating (i.e., ∼1,650 K, ∼500 ms). This approach is remarkably facile and easily accessible compared to conventional vapor-phase deposition, and the particle size and structural uniformity enable comparative studies across compositionally different MMNCs. Rapid electrochemical screening is demonstrated by using a scanning droplet cell, enabling us to discover two promising electrocatalysts, which we subsequently validated using a rotating disk setup. This demonstrated high-throughput material discovery pipeline presents a paradigm for facile and accelerated exploration of MMNCs for a broad range of applications.
多金属纳米团簇 (MMNCs) 提供了独特且可定制的表面化学性质，在许多催化应用中具有巨大的潜力。为了有效地探索这一广阔的化学空间，需要一种加速的发现管道，该管道取代了传统的“反复试验”实验，同时保证了即使在组成复杂的情况下也具有均匀的微观结构。在本文中，我们报告了通过 1）在前驱体溶液相中通过配方进行灵活的组成设计和 2）使用热冲击加热（即 ∼1650 K，∼500 ms）快速合成合金 MMNCs，实现了大量超细且均匀的合金 MMNCs 的高通量合成。与传统的气相沉积相比，这种方法更加简便易行，而且颗粒尺寸和结构均匀性使得能够对组成不同的 MMNCs 进行比较研究。通过使用扫描液滴池进行快速电化学筛选，证明了这种方法的有效性，使我们能够发现两种有前途的电催化剂，然后使用旋转圆盘装置对其进行验证。这种经过验证的高通量材料发现管道为 MMNC 广泛应用的简便和加速探索提供了范例。
