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铜纳米颗粒过热的原位高分辨率透射电子显微镜研究

In-Situ High-Resolution Transmission Electron Microscopy Investigation of Overheating of Cu Nanoparticles.

作者信息

Chen Chunlin, Hu Ziyu, Li Yanfen, Liu Limin, Mori Hirotaro, Wang Zhangchang

机构信息

Advanced Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan.

Beijing Computational Science Research Center, No. 3 He-Qing Road, Hai-Dian District, Beijing 100084, China.

出版信息

Sci Rep. 2016 Jan 20;6:19545. doi: 10.1038/srep19545.

Abstract

Synthesizing and functionalizing metal nanoparticles supported on substrates is currently the subject of intensive study owing to their outstanding catalytic performances for heterogeneous catalysis. Revealing the fundamental effect of the substrates on metal nanoparticles represents a key step in clarifying mechanisms of stability and catalytic properties of these heterogeneous systems. However, direct identification of these effects still poses a significant challenge due to the complicacy of interactions between substrates and nanoparticles and also for the technical difficulty, restraining our understanding of these heterogeneous systems. Here, we combine in situ high-resolution transmission electron microscopy with molecular dynamics simulations to investigate Cu nanoparticles supported on graphite and Cu2O substrates, and demonstrate that melting behavior and thermal stability of Cu nanoparticles can be markedly influenced by substrates. The graphite-supported Cu nanoparticles do not melt during annealing at 1073 K until they vanish completely, i.e. only the sublimation occurs, while the Cu2O-supported Cu nanoparticles suffer melting during annealing at 973 K. Such selective superheating of the Cu nanoparticles can be attributed to the adsorption of a thin carbon layer on the surface of the Cu nanoparticles, which helps guide further stability enhancement of functional nanoparticles for realistic applications.

摘要

由于负载在基底上的金属纳米颗粒在多相催化中具有出色的催化性能,目前其合成与功能化是深入研究的课题。揭示基底对金属纳米颗粒的基本影响是阐明这些多相体系稳定性和催化性能机制的关键一步。然而,由于基底与纳米颗粒之间相互作用的复杂性以及技术难度,直接识别这些影响仍然面临重大挑战,这限制了我们对这些多相体系的理解。在此,我们将原位高分辨率透射电子显微镜与分子动力学模拟相结合,研究负载在石墨和Cu2O基底上的Cu纳米颗粒,并证明Cu纳米颗粒的熔化行为和热稳定性会受到基底的显著影响。负载在石墨上的Cu纳米颗粒在1073 K退火期间不会熔化,直到它们完全消失,即仅发生升华,而负载在Cu2O上的Cu纳米颗粒在973 K退火期间会熔化。Cu纳米颗粒的这种选择性过热可归因于Cu纳米颗粒表面吸附的一层薄碳层,这有助于指导功能纳米颗粒在实际应用中进一步提高稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f858/4726356/42e62e4af009/srep19545-f1.jpg

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