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Ultrafast, Controllable Synthesis of Sub-Nano Metallic Clusters through Defect Engineering

机译:缺陷工程超快,可控合成子纳米金属簇

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摘要

Supported metallic nanoclusters (NCs, < 2 nm) are of great interests in various catalytic reactions with enhanced activities and selectivities, yet it is still challenging to efficiently and controllably synthesize ultrasmall NCs with a high-dispersal density. Here we report the in situ synthesis of surfactant-free, ultrasmall, and uniform NCs via a rapid thermal shock on defective substrates. This is achieved by using high-temperature synthesis with extremely fast kinetics while limiting the synthesis time down to milliseconds (e.g., similar to 1800 K for 55 ms) to avoid aggregation. Through defect engineering and optimized loading, the particle size can be robustly tuned from >50 nm nanoparticles to <1 nm uniform NCs with a high-dispersal density. We demonstrate that the ultrasmall NCs exhibit drastically improved activities for catalytic CO oxidation as compared to their nanoparticulated counterparts. In addition, the reported method shows generality in synthesizing most metallic NCs (e.g., Pt, Ru, Ir, Ni) in an extremely facile and efficient manner. The ultrafast and controllable synthesis of uniform, high-density, and size-controllable NCs paves the way for the utilization and nanomanufacturing of NCs for a range of catalytic reactions.
机译:支持的金属纳米团簇(NCS,<2nm)对具有增强的活性和选择性的各种催化反应具有很大的兴趣,但它仍然有效可控制地合成具有高分散密度的超低释放超声NC。在这里,我们通过对缺陷基板的快速热冲击来报告原位合成表面活性剂,超声和均匀的NC。这是通过使用极快的动力学使用高温合成来实现的,同时将合成时间限制为毫秒(例如,类似于1800 k的55毫秒)以避免聚集。通过缺陷工程和优化的负载,粒度可以从> 50nm纳米颗粒中鲁棒地调谐到<1nm均匀的NCs,具有高分散密度。与其纳米颗粒对应物相比,我们证明超大NCS表现出催化CO氧化的急剧改善的活性。此外,报告的方法显示了以极其容易和有效的方式合成大多数金属NCS(例如,Pt,Ru,IR,Ni)的一般性。超快和可控合成均匀,高密度和尺寸可控的NCS为一系列催化反应提供了利用和NCS的利用和纳米制造方式。

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