High-throughput, combinatorial synthesis of multimetallic nanoclusters

Abstract

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.

On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles

“…12 In addition to HEA, other alternative denominations have also been discussed elsewhere, such as complex solid solutions, [12][13][14] multiprincipal element alloys, 15 polyelemental particles, 16,17 multi-elemental alloy, 18 and multimetallic clusters/particles. 19 These kinds of alloys may present a class of promising ideal catalysts having desired activity, stability and selectivity and thus make a paradigm shi in catalysis research. 20 These alloy catalysts with appealing performances have been reported recently, [10][11][12][17][18][19][21][22][23][24] yet, the interpretation on their properties is still challenging.…”

“…19 These kinds of alloys may present a class of promising ideal catalysts having desired activity, stability and selectivity and thus make a paradigm shi in catalysis research. 20 These alloy catalysts with appealing performances have been reported recently, [10][11][12][17][18][19][21][22][23][24] yet, the interpretation on their properties is still challenging. Quite recently, Rossmeisl and co-authors have made a great step in theoretically predicting ORR 25 and CO 2 and CO reduction 26 properties on HEAs by combing density functional theory calculations and supervised machine learning.…”

“…To date, the reports on HEA NPs are still scarce compared to HEA bulk, and almost all the syntheses require special techniques such as carbothermal shock, 10,18,19,21 spark ablation, 27 sputtering, 12 and mechanical ball milling. 28 Here, we show the chemical synthesis of single-phase HEA NPs consisting of Ru, Rh, Pd, Ir, and Pt in a nearly equal molar ratio by a simple onepot polyol method.…”

Nano High‐Entropy Materials: Synthesis Strategies and Catalytic Applications

“…It exhibited lower overpotentials, much higher limiting current densities and long-term durability compared to those of unary Pt control sample in alkaline media, indicating the superiority of HEA-NPs electrocatalysts. [78] Noble metal-free CrMnFeCoNi HEA-NPs synthesized by magnetic sputtering method were used in ORR and showed a remarkable intrinsic activity comparable with Pt metal. [32] ORR activities of quaternary and binary control samples were evaluated to study the relevance of each element in the quinary alloy.…”

“…[ 77 ] In the endeavor of efficiently exploring this extensive chemical space, the authors developed a high‐throughput synthesis strategy based on CTS method. [ 78 ] Parallel preparation of ternary (PtPdRh) to octonary (PtPdRhRuIrFeCoNi) alloy NPs was achieved by programmable printing metal salt solutions onto carbon support and a following rapid CTS treatment. This high‐throughput alloy discovery pipeline holds great promise for facile and accelerated exploration of multimetallic alloy nanoparticles.…”