Transient and general synthesis of high-density and ultrasmall nanoparticles on two-dimensional porous carbon via coordinated carbothermal shock

作者：Wenhui Shi, Zezhou Li, Zhihao Gong, Zihui Liang, Hanwen Liu, Ye‐Chuang Han, Huiting Niu, Bo Song, Xiaodong Chi, Jihan Zhou, Hua Wang, Bao Yu Xia, Yonggang Yao, Zhong‐Qun Tian · 发表于：Nature Communications · 年份：2023 · DOI：10.1038/s41467-023-38023-5 · 被引用次数：122 · 研究领域：Electrocatalysts for Energy Conversion、Graphene research and applications、Advancements in Battery Materials

Abstract Carbon-supported nanoparticles are indispensable to enabling new energy technologies such as metal-air batteries and catalytic water splitting. However, achieving ultrasmall and high-density nanoparticles (optimal catalysts) faces fundamental challenges of their strong tendency toward coarsening and agglomeration. Herein, we report a general and efficient synthesis of high-density and ultrasmall nanoparticles uniformly dispersed on two-dimensional porous carbon. This is achieved through direct carbothermal shock pyrolysis of metal-ligand precursors in just ~100 ms, the fastest among reported syntheses. Our results show that the in situ metal-ligand coordination (e.g., N → Co 2+ ) and local ordering during millisecond-scale pyrolysis play a crucial role in kinetically dominated fabrication and stabilization of high-density nanoparticles on two-dimensional porous carbon films. The as-obtained samples exhibit excellent activity and stability as bifunctional catalysts in oxygen redox reactions. Considering the huge flexibility in coordinated precursors design, diversified single and multielement nanoparticles (M = Fe, Co, Ni, Cu, Cr, Mn, Ag, etc) were generally fabricated, even in systems well beyond traditional crystalline coordination chemistry. Our method allows for the transient and general synthesis of well-dispersed nanoparticles with great simplicity and versatility for various application schemes.