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Kinetics-induced orientational morphological evolution of Pd-Sb rhombohedra from regular nanocrystals to distorted ones

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Abstract

Although distorted crystals are ubiquitous in nature, the artificial creation of distorted nanoscale crystals with tailored morphology and structure are greatly challenging, since the formation of ideal nanocrystals requires extremely rigorous condition. We herein demonstrate a kinetics-induced orientational morphological evolution of distorted Pd20Sb7 rhombohedral nanocrystals (RNCs) by altering the temperature for growth. Detailed characterizations and experiments show that the retarded kinetics leads to the morphological evolution from regular rhombohedron to distorted rhombohedron, while the crystalline structure is kept identical by exposing six {211} facets. Moreover, the morphological evolution of distorted Pd20Sb7 RNCs is further validated by the similar normalized activity towards formic oxidation reaction based on the surface Pd atoms. This work advances the precisely controlled synthesis of Pd-based nanocrystals with tailored morphologies, which may attract great interests in various fields including chemistry, materials science, catalysis and beyond.

摘要

尽管扭曲的晶体在自然界中无处不在, 但由于理想纳米晶体的形成需要极其严格的条件, 因此人工制造具有定制形态和扭曲结构的纳米晶体具有极大的挑战性. 本研究通过改变生长温度实现了动力学诱导的扭曲Pd20Sb7菱面体纳米晶体的定向形貌演变. 详细的表征和实验表明, 缓慢的动力学导致Pd20Sb7从正菱面体到扭曲菱面体的形态演变, 而在此演变过程中纳米晶体的结构保持相同, 均暴露6个{211}晶面. 此外, 不同形貌的Pd20Sb7纳米晶体表现出相似的甲酸氧化反应活性(基于表面钯原子的归一化活性), 进一步验证了该动力学诱导形貌演变过程不改变Pd20Sb7纳米晶体的结构. 本研究拓展了具有特定形貌的钯基纳米晶体的精确控制合成, 并有望推动其在化学、材料科学、催化等相关领域的实际应用.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2020YFB1505802), the Ministry of Science and Technology (2017YFA0208200), the National Natural Science Foundation of China (22025108, U21A20327, and 22121001), Guangdong Provincial Natural Science Fund for Distinguished Young Scholars (2021B1515020081), and the start-up support from Xiamen University and Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices (20195010002).

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Mengjun Wang  (王梦君), Linzhe Lü  (吕林喆), Qiaorong Jiang  (蒋巧荣), Guang Li  (李广), Mingmin Wang  (王明敏) & Xiaoqing Huang  (黄小青)

  2. Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, Guangzhou, 510006, China

    Yong Xu  (徐勇)

  3. Testing and Analysis Center, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Qiming Hong  (洪麒明)

Authors
  1. Mengjun Wang  (王梦君)
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  2. Linzhe Lü  (吕林喆)
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  3. Qiaorong Jiang  (蒋巧荣)
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  4. Guang Li  (李广)
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  5. Qiming Hong  (洪麒明)
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  6. Mingmin Wang  (王明敏)
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  7. Yong Xu  (徐勇)
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  8. Xiaoqing Huang  (黄小青)
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Contributions

Huang X and Xu Y conceived and directed the study; Wang M conducted the synthesis/characterizations of materials, and prepared the manuscript; Xu Y revised the manuscript; Lü L and Jiang Q analyzed the SAED and HRTEM data; Li G performed the FTIR measurements. Hong Q conducted the HRTEM and SAED measurements.

Corresponding authors

Correspondence to Yong Xu  (徐勇) or Xiaoqing Huang  (黄小青).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Experimental details and supporting data are available in the online version of the paper.

Mengjun Wang is currently a doctoral candidate at Xiamen University. Her research interest focuses on the design and catalytic applications of Pd-metalloid alloys.

Yong Xu is current a professor at the College of Materials and Energy, Guangdong University of Technology. He obtained his PhD degree from the College of Chemistry and Materials Science, University of Science and Technology of China in 2013 under the supervision of Prof. Quanxin Li. In 2014–2017, he worked in Prof. Qiao Zhang’s group at Soochow University and Prof. Jinghua Guo’s group at the Advanced Light Source, Lawrence Berkeley National Laboratory as a postdoctoral research fellow. He became an associate professor in 2017 at Soochow University. His research interest currently focuses on the design of functional catalysts for the selective activation of light molecules.

Xiaoqing Huang is currently a professor at the College of Chemistry and Chemical Engineering, Xiamen University. He obtained his PhD degree in organic chemistry from Xiamen University (2011) under the supervision of Profs Nanfeng Zheng and Lansun Zheng. Then he worked in Profs Yu Huang and Xiangfeng Duan’s group as a postdoctoral research associate from September 2011 to June 2014 at the University of California, Los Angeles. His current research interests are the design of nanoscale materials for electrocatalysis and heterogenous catalysis.

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40843_2022_2334_MOESM1_ESM.pdf

Kinetics-induced orientational morphological evolution of Pd-Sb rhombohedra from regular nanocrystals to distorted ones at

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Wang, M., Lü, L., Jiang, Q. et al. Kinetics-induced orientational morphological evolution of Pd-Sb rhombohedra from regular nanocrystals to distorted ones. Sci. China Mater. 66, 1847–1853 (2023). https://doi.org/10.1007/s40843-022-2334-4

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  • DOI: https://doi.org/10.1007/s40843-022-2334-4

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