龙冉 博士生导师  硕士生导师

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联系方式:longran@ustc.edu.cn

学位:博士

学科: 核科学与技术 、 化学

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Surface Facet of Palladium Nanocrystals: A Key Parameter to the Activation of Molecular Oxygen for Organic Catalysis and Cancer Treatment

发布时间:2023-01-15
点击次数:
DOI码:
10.1021/ja311739v
发表刊物:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
刊物所在地:
WASHINGTON
摘要:
In many organic reactions, the O-2 activation process involves a key step where inert ground triplet O-2 is excited to produce highly reactive singlet O-2. It remains elusive what factor induces the change in the electron spin state of O-2 molecules, although it has been discovered that the presence of noble metal nanoparticles can promote the generation of singlet O-2. In this work, we first demonstrate that surface facet is a key parameter to modulate the O-2 activation process on metal nanocrystals, by employing single-facet Pd nanocrystals as a model system. The experimental measurements clearly show that singlet O-2 is preferentially formed on {100} facets. The simulations further elucidate that the chemisorption of O-2 to the {100} facets can induce a spin-flip process in the O-2 molecules, which is achieved via electron transfer from Pd surface to O-2. With the capability of tuning O-2 activation, we have been able to further implement the {100}-faceted nanocubes in glucose oxidation. It is anticipated that this study will open a door to designing noble metal nanocatalysts for O-2 activation and organic oxidation. Another perspective of this work would be the controllability in tailoring the cancer treatment materials for high O-1(2) production efficiency, based on the facet control of metal nanocrystals. In the cases of both organic oxidation and cancer treatment, it has been exclusively proven that the efficiency of producing singlet O-2 holds the key to the performance of Pd nanocrystals in the applications.
合写作者:
Long, Ran, Mao, Keke, Ye, Xiaodong, Yan, Wensheng, Huang, Yaobing, Jianyong, Fu, Yao, Wang, Xisheng, Wu, Xiaojun, Xie, Yi, Xiong, Yujie
第一作者:
Long, Ran
通讯作者:
Xiong, YJ
论文编号:
WOS:000315618900054
文献类型:
Article
卷号:
135
期号:
8
页面范围:
3200-3207
ISSN号:
0002-7863
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