Jun Yang

Versatile organic ligands can notably enhance the stability and tunability of metal nanoclusters (NCs), and, consequently, all-organic ligand–protected metal nanoclusters have recently attracted widespread attention. Platinum (Pt) remains an indispensable metal in various fields, particularly in catalysis and cancer therapeutics. However, all-organic ligand–protected Pt nanoclusters are rarely reported due to substantial synthesis challenges, which have hindered progress in Pt nanocluster research and their practical applications. Herein, we report the successful synthesis of the largest all-organic ligand–protected Pt nanocluster to date, [Pt19(NapNC)27][PF6]2 (abbreviated as Pt19; NapNC: isocyanonaphthalene), achieved through the development of a ligand-exchange method. Single-crystal X-ray diffraction (SC-XRD) revealed a face-centered cubic (FCC), nonequivalent structure that has not been previously documented for all-organic ligand–protected Pt nanoclusters. Compared with its partially organic parent nanoclusters, this novel nanocluster exhibits considerably enhanced stability in both the ground and excited states. Furthermore, the Pt19 nanocluster demonstrates superior activity in the electrocatalytic methanol oxidation reaction (MOR) relative to its parent nanoclusters and commercial Pt/C. Based on its well-defined structure, we gained deep insights into the exceptional MOR activity of Pt19 and revealed, for the first time, the steric and electronic preferences of the active sites for electrocatalytic MOR.

Surface atomic steps serve as highly active sites for electrocatalysis, yet their controllable construction remains challenging. Herein, we report a facile strategy combining galvanic replacement and Au‐catalyzed reduction to fabricate AuCu@Pd core‐shell nanoparticles with dense surface Pd atomic steps on carbon substrate. Binary AuCu nanoalloy seeds were prepared via a Joule‐heating‐driven solid‐state diffusion method. Subsequently, Pd atoms substitute Cu atoms on the surface of AuCu alloy seeds, maintaining a flat surface morphology; next, Pd atoms selectively deposit on Au sites, forming atomic steps together with the Pd atoms that substituted Cu atoms in the last step. The optimized Au ₁₀ Cu ₅ @Pd ₄ /C catalyst exhibits exceptional oxygen reduction reaction (ORR) performance in alkaline media, with a half‐wave potential of 0.92 V versus RHE, a specific activity of 1.29 mA cm ⁻² and a mass activity of 2.86 A mg _Pd ⁻¹ , significantly outperforming commercial Pd/C. Control experiments verify that surface Pd atomic steps dominate the enhanced ORR activity. This strategy is further extended to synthesize AuCu@Pt nanoparticles with surface Pt steps, which show superior methanol oxidation activity. This work provides a universal approach to engineering surface atomic steps for high‐performance electrocatalysts.

Conventional wet-chemistry synthesis of Au-based nanoalloys often suffers from core–shell/segregated structures or incomplete alloying due to mismatched metal redox kinetics, limiting their structural uniformity and electrocatalytic performance. To address this challenge, we herein develop a robust, versatile strategy for fabricating carbon-supported Au-based nanoalloys by coupling rapid Joule-heating with the basic solid-state diffusion theory. This method offers distinct advantages: Joule-heating enables ultrafast, controllable high-temperature generation, which efficiently drives rapid solid-state diffusion of metal atoms; meanwhile, pre-synthesized ∼1.5 nm Au clusters (as seeds) ensure homogeneous elemental mixing by shortening diffusion distances and promoting substitutional diffusion. It successfully produces well-dispersed, crystalline AuPd nanoalloys with uniform Au/Pd distribution. Moreover, the strategy is universal, extending to binary AuM/C (M = Fe, Ni, Cu, Rh, Pt) and multi-component nanoalloys (e.g., ternary AuCuPd/C, quaternary AuCuPtPd/C). Electrocatalytic tests show that Au1Pd1/C outperforms commercial Pd/C in the alkaline oxygen reduction reaction and ethanol oxidation reaction, confirming the strategy's value for developing high-performance electrocatalysts.

High-value regeneration of waste graphite (WG) anodes is critical for sustainable lithium-ion battery recycling, yet precise defect repair and mechanistic understanding remain challenging.

A facile solid-phase synthesis strategy that couples ball milling with rapid Joule-heating to fabricate Pd/C catalysts for high-performance electrocatalysis.