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Direct in Situ Observation and Analysis of the Formation of Palladium Nanocrystals with High-Index Facets
Nano Letters ( IF 9.6 ) Pub Date : 2018-10-05 00:00:00 , DOI: 10.1021/acs.nanolett.8b02953 Wenpei Gao , Yusheng Hou , Zachary D. Hood 1 , Xue Wang 2 , Karren More 3 , Ruqian Wu , Younan Xia 1, 2, 4 , Xiaoqing Pan , Miaofang Chi 3
Nano Letters ( IF 9.6 ) Pub Date : 2018-10-05 00:00:00 , DOI: 10.1021/acs.nanolett.8b02953 Wenpei Gao , Yusheng Hou , Zachary D. Hood 1 , Xue Wang 2 , Karren More 3 , Ruqian Wu , Younan Xia 1, 2, 4 , Xiaoqing Pan , Miaofang Chi 3
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Synthesizing concave-structured nanoparticles (NP) with high-index surfaces offers a viable method to significantly enhance the catalytic activity of NPs. Current approaches for fabricating concave NPs, however, are limited. Exploring novel synthesis methods requires a thorough understanding of the competing mechanisms that contribute to the evolution of surface structures during NP growth. Here, by tracking the evolution of Pd nanocubes into concave NPs at atomic scale using in situ liquid cell transmission electron microscopy, our study reveals that concave-structured Pd NPs can be formed by the cointroduction of surface capping agents and halogen ions. These two chemicals jointly create a new surface energy landscape of Pd NPs, leading to the morphological transformation. In particular, Pd atoms dissociate from the {100} surfaces with the aid of Cl– ions and preferentially redeposit to the corners and edges of the nanocubes when the capping agent polyvinylpyrrolidone is introduced, resulting in the formation of concave Pd nanocubes with distinctive high-index facets. Our work not only demonstrates a potential route for synthesizing NPs with well-defined high-index facets but also reveals the detailed atomic-scale kinetics during their formation, providing insight for future predictive synthesis.
中文翻译：
高指数面钯纳米晶体形成的直接原位观察和分析
合成具有高折射率表面的凹面结构纳米颗粒（NP）提供了一种显着增强NPs催化活性的可行方法。然而，制造凹形NP的当前方法受到限制。探索新的合成方法需要透彻理解在NP生长过程中有助于表面结构演变的竞争机制。在这里，通过使用原位液体细胞透射电子显微镜跟踪Pd纳米立方在原子尺度上向凹形NPs的演化，我们的研究表明，凹形结构的Pd NPs可以通过表面加盖剂和卤素离子的共引入而形成。这两种化学物质共同创造了Pd NPs的新表面能态势，从而导致了形态转变。尤其是，–当引入封端剂聚乙烯吡咯烷酮时，离子会优先沉积在纳米立方体的角部和边缘，从而形成具有独特的高折射率刻面的凹面Pd纳米立方体。我们的工作不仅展示了合成具有明确定义的高折射率刻面的NP的潜在途径，而且还揭示了其形成过程中详细的原子级动力学，从而为未来的预测合成提供了见识。
更新日期：2018-10-05
中文翻译：
高指数面钯纳米晶体形成的直接原位观察和分析
合成具有高折射率表面的凹面结构纳米颗粒（NP）提供了一种显着增强NPs催化活性的可行方法。然而，制造凹形NP的当前方法受到限制。探索新的合成方法需要透彻理解在NP生长过程中有助于表面结构演变的竞争机制。在这里，通过使用原位液体细胞透射电子显微镜跟踪Pd纳米立方在原子尺度上向凹形NPs的演化，我们的研究表明，凹形结构的Pd NPs可以通过表面加盖剂和卤素离子的共引入而形成。这两种化学物质共同创造了Pd NPs的新表面能态势，从而导致了形态转变。尤其是，–当引入封端剂聚乙烯吡咯烷酮时，离子会优先沉积在纳米立方体的角部和边缘，从而形成具有独特的高折射率刻面的凹面Pd纳米立方体。我们的工作不仅展示了合成具有明确定义的高折射率刻面的NP的潜在途径，而且还揭示了其形成过程中详细的原子级动力学，从而为未来的预测合成提供了见识。
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