通过d带中心调控将钌单原子选择性耦合到铂镍凹面用于高性能甲醇氧化
Selectively Coupling Ru Single Atoms to PtNi Concavities for High-Performance Methanol Oxidation via d-Band Center Regulation.
作者信息
Kong Fanpeng, Liu Xiaozhi, Song Yajie, Qian Zhengyi, Li Junjie, Zhang Lei, Yin Geping, Wang Jiajun, Su Dong, Sun Xueliang
机构信息
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, Harbin Institute of Technology, Harbin, China.
Department of Mechanical and Materials Engineering, University of Western Ontario, London, Canada.
出版信息
Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202207524. doi: 10.1002/anie.202207524. Epub 2022 Sep 14.
Single atom tailored metal nanoparticles represent a new type of catalysts. Herein, we demonstrate a single atom-cavity coupling strategy to regulate performance of single atom tailored nano-catalysts. Selective atomic layer deposition (ALD) was conducted to deposit Ru single atoms on the surface concavities of PtNi nanoparticles (Ru-ca-PtNi). Ru-ca-PtNi exhibits a record-high activity for methanol oxidation reaction (MOR) with 2.01 A mg . Also, Ru-ca-PtNi showcases a significant durability with only 16 % activity loss. Operando electrochemical Fourier transform infrared spectroscopy (FTIR) and theoretical calculations demonstrate Ru single atoms coupled to cavities accelerate the CO removal by regulating d-band center position. Further, the high diffusion barrier of Ru single atoms in concavities accounts for excellent stability. The developed Ru-ca-PtNi via single atom-cavity coupling opens an encouraging pathway to design highly efficient single atom-based (electro)catalysts.
单原子定制金属纳米颗粒是一种新型催化剂。在此，我们展示了一种单原子-腔耦合策略来调节单原子定制纳米催化剂的性能。通过选择性原子层沉积（ALD）将Ru单原子沉积在PtNi纳米颗粒的表面凹处（Ru-ca-PtNi）。Ru-ca-PtNi对甲醇氧化反应（MOR）表现出创纪录的高活性，电流密度为2.01 A mg 。此外，Ru-ca-PtNi还表现出显著的耐久性，活性损失仅为16%。原位电化学傅里叶变换红外光谱（FTIR）和理论计算表明，与凹处耦合的Ru单原子通过调节d带中心位置加速了CO的去除。此外，Ru单原子在凹处的高扩散势垒解释了其优异的稳定性。通过单原子-腔耦合开发的Ru-ca-PtNi为设计高效的单原子基（电）催化剂开辟了一条令人鼓舞的途径。
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