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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. 

A highly porous 2D nanomaterial, holey graphene oxide (hGO), is synthesized directly from holey graphene powder and employed to create an aqueous 3D printable ink without the use of additives or binders. Stable dispersions of hydrophilic hGO sheets in water (≈100 mg mL⁻¹) can be readily achieved. The shear‐thinning behavior of the aqueous hGO ink enables extrusion‐based printing of fine filaments into complex 3D architectures, such as stacked mesh structures, on arbitrary substrates. The freestanding 3D printed hGO meshes exhibit trimodal porosity: nanoscale (4–25 nm through‐holes on hGO sheets), microscale (tens of micrometer‐sized pores introduced by lyophilization), and macroscale (<500 µm square pores of the mesh design), which are advantageous for high‐performance energy storage devices that rely on interfacial reactions to promote full active‐site utilization. To elucidate the benefit of (nano)porosity and structurally conscious designs, the additive‐free architectures are demonstrated as the first 3D printed lithium–oxygen (Li–O₂) cathodes and characterized alongside 3D printed GO‐based materials without nanoporosity as well as nanoporous 2D vacuum filtrated films. The results indicate the synergistic effect between 2D nanomaterials, hierarchical porosity, and overall structural design, as well as the promise of a freeform generation of high‐energy‐density battery systems.

 

Composite materials with ordered microstructures often lead to enhanced functionalities that a single material can hardly achieve. Many biomaterials with unusual microstructures can be found in nature; among them, many possess anisotropic and even directional physical and chemical properties. With inspiration from nature, artificial composite materials can be rationally designed to achieve this anisotropic behavior with desired properties. Here, a metallic wood with metal continuously filling the wood vessels is developed, which demonstrates excellent anisotropic electrical, thermal, and mechanical properties. The well‐aligned metal rods are confined and separated by the wood vessels, which deliver directional electron transport parallel to the alignment direction. Thus, the novel metallic wood composite boasts an extraordinary anisotropic electrical conductivity (σ_||/σ_⊥) in the order of 10¹¹, and anisotropic thermal conductivity (κ_||/κ_⊥) of 18. These values exceed the highest reported values in existing anisotropic composite materials. The anisotropic functionality of the metallic wood enables it to be used for thermal management applications, such as thermal insulation and thermal dissipation. The highly anisotropic metallic wood serves as an example for further anisotropic materials design; other composite materials with different biotemplates/hosts and fillers can achieve even higher anisotropic ratios, allowing them to be implemented in a variety of applications.