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Superfast tellurizing synthesis of unconventional phase-controlled small Pd-Te nanoparticles

一种超快的碲化法用于非常规相控碲化钯小纳米颗粒的合成

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Abstract

Large-scale production of unconventional phase-controlled telluride catalysts in a simple and fast manner still poses a great challenge. Herein, we develop a superfast tellurizing synthesis method that can quickly prepare unconventional phase-controlled palladium telluride nanoparticles (Pd-Te NPs) on carbon nanotubes (CNTs) (i.e., PdTe/CNT, Pd20Te7/CNT) in 60 s. By merely tuning the mass of the tellurium precursors under the same conditions, fine (about 5.5 nm) and high-yield (about 90%) hexagonal structured PdTe/CNT and rhombohedral structured Pd20Te7/CNT can be precisely synthesized. The hexagonal structured PdTe/CNT exhibits excellent performance for glycerol oxidation reaction (GOR) and ethylene glycol oxidation reaction (EGOR). Specifically, the highest current density for GOR is 2.72 A mgPd−1, which is 1.9-fold higher than that of rhombohedral structured Pd20Te7/CNT, and 2.8-fold higher than that of Pd/CNT. It also outperforms most catalysts reported in GOR. Meanwhile, the specific activity for EGOR is 3.65 A mgPd−1, which is 2.1 and 3.9 times higher than those of rhombohedral structured Pd20Te7/CNT and Pd/CNT. We hope that this work can provide guidance for the preparation of crystalline phase-controlled telluride catalysts via new tellurization and inspire the application of crystalline phase-controlled materials.

摘要

本研究发展了一种超快的碲化方法, 可以在碳纳米管上快速制备非常规相控碲化钯小纳米颗粒. 这种碲化方法只需要一台家用微波炉, 整个过程非常快(60秒), 简单, 不含表面活性剂, 可规模化生产. 通过在相同条件下仅调整前驱体Te粉的使用量, 可以精确调控合成小尺寸(约5.5 nm)、 高产率(约90%)的六方结构PdTe/CNT和菱方结构Pd20Te7/CNT. 其中, 六方结构的PdTe/CNT在甘油氧化反应(GOR)和乙二醇氧化反应(EGOR)中表现出卓越的性能. 具体来说, 六方结构的PdTe/CNT在甘油氧化反应中, 最高电流密度可达2.72 A mgPd−1, 比菱方结构Pd20Te7/CNT的最高电流密度高1.9倍, 比Pd/CNT最高电流密度高2.8倍, 超过了目前文献中报道过的大多数催化剂. 同时, 六方结构的PdTe/CNT在乙二醇氧化反应中比活性达到3.65 A mgPd−1, 比菱方结构的Pd20Te7/CNT和Pd/CNT分别高2.1倍和3.9倍. 我们希望这项工作可以为小尺寸非常规相控碲化物催化剂的制备提供新的碲化方法指导, 并为相控材料的应用提供启发.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51772162, 22001143, and 52072197), the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China (2019KJC004), the Outstanding Youth Foundation of Shandong Province, China (ZR2019JQ14), Taishan Scholar Young Talent Program (tsqn201909114 and tsqn201909123), the Natural Science Foundation of Shandong Province (ZR2020YQ34), the Major Scientific and Technological Innovation Project (2019JZZY020405), and the Major Basic Research Program of Natural Science Foundation of Shandong Province (ZR2020ZD09).

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Authors and Affiliations

  1. Key Laboratory of Eco-Chemical Engineering, Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Yi Han  (**艺), Yanyun Zhang  (张燕云), **nyi Zhang  (张新义), Yuyao Sun  (孙玉垚), Wenwen Cai  (蔡雯雯), Jian** Lai  (赖建**) & Lei Wang  (王磊)

  2. Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Lei Wang  (王磊)

  3. College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Zhenjiang Li  (**镇江)

Authors
  1. Yi Han  (**艺)
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  2. Yanyun Zhang  (张燕云)
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  3. **nyi Zhang  (张新义)
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  5. Wenwen Cai  (蔡雯雯)
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  6. Zhenjiang Li  (**镇江)
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  7. Jian** Lai  (赖建**)
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  8. Lei Wang  (王磊)
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Contributions

Author contributions Han Y performed the experiments, analyzed the data and wrote the manuscript. Zhang Y and Zhang X performed partial experiments and offered helpful suggestions. Sun Y and Cai W analyzed the data and offered helpful suggestions. Li Z contributed to the software and sources. Lai J contributed to the analysis, supervision and editing. Wang L contributed to the supervision and editing. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Jian** Lai  (赖建**) or Lei Wang  (王磊).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Yi Han is a PhD student at Qingdao University of Science and Technology. Her research mainly focuses on the design and synthesis of nanomaterials and their electrocatalytic applications.

Jian** Lai received his PhD degree from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences in 2017, and then he worked as a postdoctoral scholar at Peking University (2017–2019). In 2019, he joined Qingdao University of Science and Technology as a professor. His current research interests focus on clean energy electrocatalytic materials.

Lei Wang obtained his PhD degree in inorganic chemistry from Jilin University in 2006. He is now a professor in inorganic chemistry at the College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology. The current research of his group focuses on the synthesis of nanosized functional materials for applications in photocatalysis, electrocatalysis, and batteries.

Supplementary information Supporting data are available in the online version of the paper.

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Han, Y., Zhang, Y., Zhang, X. et al. Superfast tellurizing synthesis of unconventional phase-controlled small Pd-Te nanoparticles. Sci. China Mater. 65, 1853–1860 (2022). https://doi.org/10.1007/s40843-021-1952-4

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  • DOI: https://doi.org/10.1007/s40843-021-1952-4

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