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<p>Transition-metal nanocrystal (TMN) catalysts are essential for energy conversion and storage, but their facile and controllable synthesis remains challenging. Here we report a general precursor-valence-gating strategy to prepare various monocrystalline and polycrystalline TMNs (MC/PC-TMNs, M = Co, Ni or Cu). Unlike complex regulation of traditional experimental parameters, we discover that the solid-state precursor’s oxidation state—an intrinsic parameter—governs the nucleation rate and ultimately dictates atomic crystallization periodicity. Consequently, the controllable preparation of MC/PC-TMNs was readily achieved through designing the valence diversity of the corresponding precursors. Furthermore, taking MC/PC-Co catalysts as examples, we investigate the correlation between atomic arrangements and catalytic dynamics and reveal that the PC-Co catalyst with the lower-coordination environment, compared with MC-Co, substantially promotes the conversion of reaction intermediates in the hydrazine oxidation reaction. As a result, PC-Co exhibits an ultralow Tafel slope of 14 mV dec<sup>−1</sup>, and an assembled hydrazine oxidation reaction-based battery demonstrates excellent stability for 1,200 h at 10 mA cm<sup>−2</sup>. This work paves the way for controllable synthesis of MC/PC-TMNs and fundamentally advances the understanding of precursor-guided crystal growth kinetics.</p><p></p>

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A precursor-valence-gating strategy for controllable synthesis of metal nanocrystal catalysts with varied periodicities

  • 期刊论文

  • 发表日期：

    2026年3月10日

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  • Zhiyang Zheng,
  • Feng-Yi Zheng,
  • Yifei Zhu,
  • Bosi Huang,
  • Tongtong Li,
  • Boran Wang,
  • Xiongwei Zhong,
  • Zhexuan Liu,
  • Guanjun Ji,
  • Qingjin Fu,
  • Guangmin Zhou

摘要

Transition-metal nanocrystal (TMN) catalysts are essential for energy conversion and storage, but their facile and controllable synthesis remains challenging. Here we report a general precursor-valence-gating strategy to prepare various monocrystalline and polycrystalline TMNs (MC/PC-TMNs, M = Co, Ni or Cu). Unlike complex regulation of traditional experimental parameters, we discover that the solid-state precursor’s oxidation state—an intrinsic parameter—governs the nucleation rate and ultimately dictates atomic crystallization periodicity. Consequently, the controllable preparation of MC/PC-TMNs was readily achieved through designing the valence diversity of the corresponding precursors. Furthermore, taking MC/PC-Co catalysts as examples, we investigate the correlation between atomic arrangements and catalytic dynamics and reveal that the PC-Co catalyst with the lower-coordination environment, compared with MC-Co, substantially promotes the conversion of reaction intermediates in the hydrazine oxidation reaction. As a result, PC-Co exhibits an ultralow Tafel slope of 14 mV dec−1, and an assembled hydrazine oxidation reaction-based battery demonstrates excellent stability for 1,200 h at 10 mA cm−2. This work paves the way for controllable synthesis of MC/PC-TMNs and fundamentally advances the understanding of precursor-guided crystal growth kinetics.