Bottom-up precise synthesis of stable platinum dimers on graphene.

Bottom-up precise synthesis of stable platinum dimers on graphene.
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石墨烯上自下而上精确合成稳定的铂二聚体

DOI:
10.1038/s41467-017-01259-z
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发表时间:
2017-10-20
影响因子:
16.6
通讯作者:
Lu J
Lu J
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Yan H;Lin Y;Wu H;Zhang W;Sun Z;Cheng H;Liu W;Wang C;Li J;Huang X;Yao T;Yang J;Wei S;Lu J

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含少量原子的负载金属簇合物引起了人们极大的兴趣。金属单原子催化剂的合成已取得进展。然而,在高表面积载体上精确合成金属二聚体仍然是一个巨大的挑战。在这里,我们表明,Pt 2二聚体可以制造与自下而上的方法在石墨烯上使用原子层沉积,通过适当的成核位点的创建,Pt 1单原子沉积和附加的第二铂原子选择性的初步之一。扫描透射电子显微镜,X-射线吸收光谱,和理论计算表明,Pt 2dimers可能是在氧化形式的Pt 2 Ox。在氨硼烷的水解脱氢中,Pt 2二聚体在室温下表现出2800 molH 2 molPt − 1 min − 1的高比速率,分别比石墨烯负载的Pt单原子和纳米颗粒高约17倍和45倍。这些发现为自下而上制备支撑原子级精确的超细金属团簇的实际应用开辟了一条途径。
Supported metal clusters containing only a few atoms are of great interest. Progress has been made in synthesis of metal single-atom catalysts. However, precise synthesis of metal dimers on high-surface area support remains a grand challenge. Here, we show that Pt2dimers can be fabricated with a bottom–up approach on graphene using atomic layer deposition, through proper nucleation sites creation, Pt1single-atom deposition and attaching a secondary Pt atom selectively on the preliminary one. Scanning transmission electron microscopy, x-ray absorption spectroscopy, and theoretical calculations suggest that the Pt2dimers are likely in the oxidized form of Pt2Ox. In hydrolytic dehydrogenation of ammonia borane, Pt2dimers exhibit a high specific rate of 2800 molH2molPt−1min−1at room temperature, ~17- and 45-fold higher than graphene supported Pt single atoms and nanoparticles, respectively. These findings open an avenue to bottom–up fabrication of supported atomically precise ultrafine metal clusters for practical applications.
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