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Synthesis of PdH0.43 nanocrystals with different surface structures and their catalytic activities towards formic acid electro-oxidation

不同表面结构PdH0.43纳米晶的制备及其甲酸电氧化性能

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Abstract

The synthesis of nanocrystals (NCs) with defined morphology and surface structure provides an effective way to investigate the structure-activity relationship of nanocatalytsts, and it will facilitate the design of nanocatalysts with excellent catalytic performance. In this paper, we developed a facile method to synthesize PdH0.43 NCs with the shape of cube, octahedron and rhombic dodecahedron (RD), whose surface facets are {100}, {111} and {110}, respectively. The asprepared PdH0.43 NCs are highly stable and exhibit enhanced catalytic activity and extremely low overpotential towards electro-oxidation of formic acid compared with the commercial Pd black and three types of Pd NCs. The specific activity of the cubic PdH0.43 NCs is more than five times that of the commercial Pd black and two times that of the cubic Pd NCs. Among the three types of PdH0.43 NCs with different surface structure, the activity order is followed by PdH0.43 {100} > PdH0.43{111} > PdH0.43{110}.

摘要

制备具有确定形貌和表面结构的纳米晶为研究其构效关系提供了有效途径, 且有利于设计开发具有优异催化性能的纳米催化剂. 本研究发展了一种制备不同形貌PdH0.43纳米晶的简易方法其形貌分别为立方体、 八面体和菱形十二面体, 对应的裸露晶面分别为{100}, {111}和{110}晶面. 不同形貌PdH0.43纳米晶都非常稳定. 其与商业Pd黑和三种纯Pd纳米晶相比, 在甲酸电催化氧化反应中显示出更高的催化活性和极低的氧化过电位. 立方体PdH0.43纳米晶的催化活性分别高于商业Pd黑的5倍和立方体Pd纳米晶的2倍. 不同表面结构PdH0.43纳米晶的催化活性依次为PdH0.43 {100} PdH0.43 {111} > PdH0.43 {110}.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21771153, 21721001, and 21773190), and the Natural Science Foundation of Fujian Province (2018J01015).

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Authors and Affiliations

  1. State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Chenyang Zhan  (詹晨阳), Huiqi Li  (李慧齐), Xuemin Li  (李学敏), Yaqi Jiang  (蒋亚琪) & Zhaoxiong Xie  (谢兆雄)

  2. Pen-Tung Sah Institute of Micro-Nano Science and Technology, Xiamen University, Xiamen, 361005, China

    Zhaoxiong Xie  (谢兆雄)

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  1. Chenyang Zhan  (詹晨阳)
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  2. Huiqi Li  (李慧齐)
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  3. Xuemin Li  (李学敏)
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  4. Yaqi Jiang  (蒋亚琪)
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Contributions

Author contributions Xie Z and Jiang Y conceived the study and guided the whole project. Zhan C designed and performed the experiments. Li H and Li X participated in the materials preparation and data analysis; Jiang Y and Zhan C wrote the manuscript. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Yaqi Jiang  (蒋亚琪) or Zhaoxiong Xie  (谢兆雄).

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Conflict of interest The authors declare no conflict of interest.

Additional information

Chenyang Zhan received his BSc degree in applied chemistry from Hunan University in 2016. He is currently a master’s graduate under the supervision of Assoc. Prof. Yaqi Jiang and Prof. Zhaoxiong Xie. His research focuses on the development of Pd-based nanocrystals with controllable morphology and their electrochemical catalytic properties.

Yaqi Jiang received her BSc degree (1986), MSc degree (1989) and PhD degree (2011) from the Department of Chemistry at Shanghai Jiao Tong University, Fuzhou University and Xiamen University, respectively. She has been an associate professor of physical chemistry at Xiamen University since 2004. Her current research interest mainly focuses on the structure-activity relationship of inorganic nanomaterials.

Zhaoxiong Xie received his BSc degree (1987), MSc degree (1990), and PhD degree (1995) in physical chemistry from Xiamen University, China. He worked as a postdoctoral fellow at the Centre d’Etudes de Saclay in France from 1997 to 1998. Since 2002, he has been a professor of physical chemistry at Xiamen University. His current research is focused on the surface/interface chemistry of inorganic nanomaterials.

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Zhan, C., Li, H., Li, X. et al. Synthesis of PdH0.43 nanocrystals with different surface structures and their catalytic activities towards formic acid electro-oxidation. Sci. China Mater. 63, 375–382 (2020). https://doi.org/10.1007/s40843-019-1187-6

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