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Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media

镨铱氧化物高效催化酸性介质析氧反应

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Abstract

Amorphous iridium oxides (IrOx) are highly active for oxygen evolution reaction (OER) in acid media; however, it is generally unstable compared with commercial IrO2. Recently, many non-noble metal-iridium mixed oxides are prepared for catalyzing OER efficiently. Herein, we report a cubic fluorite-type praseodymium iridium oxide with the surface of IrOx (IrOx/Pr3IrO7) that shows the improved activity and stability in 0.1 mol L−1 HClO4 solution, characterized by an overpotential of 305 mV at the benchmark of 10 mA cm−2 and a small Tafel slope of 37 mV dec−1, indicating a fast reaction kinetics and a competitive activity compared with the benchmark IrO2 and most reported electrocatalysts. The initial potential increases by less than 0.07 V after continuous OER testing over 60,000 s. In contrast, IrO2 becomes nearly inactive for the OER within 20,000 s. Density functional theory calculations uncover that the optimal energy level path follows lattice oxygen mechanism (LOM). This work enlarges the family of the IrOx-type OER electrocatalyst in acid media.

摘要

非晶态铱氧化物(IrOx)在酸性介质中具有高的电催化析氧反 应(OER)活性, 但其稳定性不如商业IrO2. 近年来, 多种非贵金属-铱 混合氧化物展现出高效催化析氧反应的性能. 本文报道了一种含 IrOx高活性表面层的立方萤石结构镨铱氧化物(Pr3IrO7)催化剂. 该 催化剂在0.1 mol L−1 HClO4溶液中, 表现出高的析氧反应催化活性 和良好的稳定性, 优于商业IrO2和目前报道的大多数催化剂. 在电 流密度为10 mA cm−2时, 该催化剂的过电位为305 mV, 并具有低的 Tafel斜率, 约为37 mV dec−1, 表明该催化剂具有更快的反应动力 学. 在持续60000 s的稳定性测试后, 该催化剂的初始电位仅增加了 0.07 V, 而IrO2只经过20000 s测试就几乎丧失活性. 密度泛函理论 计算表明, IrOx/Pr3IrO7催化析氧反应遵循晶格氧机理(LOM). 这项 工作拓展了IrOx型酸性OER电催化剂的种类.

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Acknowledgements

This work was supported by Taishan Scholar Program of Shandong Province, China (ts201712045), Shandong Provincial Key Research and Development Program (SPKR&DP, 2019GGX102069), the Natural Science Foundation of Shandong Province of China (ZR2018BB008), and the Doctoral Found of Qingdao University of Science and Technology (0100229001, 010029081, 010029075).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. College of Chemical Engineering, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Yimeng Wang  (王一盟), Shangguo Liu  (刘尚果), Qing Qin  (秦清), Huihui Liu  (刘慧慧), Lijie Zhang  (张立杰), Tao Wei  (魏涛), Haisen Li  (李海森) & Xien Liu  (刘希恩)

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  1. Yimeng Wang  (王一盟)
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  2. Shangguo Liu  (刘尚果)
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Contributions

Liu X proposed the research ideas and designed the experiments. Qin Q and Liu X wrote the manuscript and performed the analysis. Wang Y, Liu H, Zhang L, Wei T, and Li H carried out the synthetic, electrochemical experiments and physical characterizations. Liu S carried out the DFT calculations. All the authors participated in this research project.

Corresponding authors

Correspondence to Qing Qin  (秦清) or Xien Liu  (刘希恩).

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Conflict of interest

The authors declare that they have no conflict of interest.

Yimeng Wang is currently studying for his Master degree under the supervision of Prof. Xien Liu at Qingdao University of Science and Technology. At present, his research focuses on the synthesis of metal-doped iridium-based oxide and electrocatalytic oxygen evolution performance in acidic media.

Shangguo Liu received his PhD degree from Beijing University of Chemical Technology in 2019. And then, He joined the College of Chemical Engineering, Qingdao University of Science and Technology. His research interests focus on exploring chemical and physical properties of materials by theoretical and computational tools.

Qing Qin received her PhD degree from Nankai University in 2017. Now she is a professor of Qingdao University of Science and Technology. Her current research interests focus on the design and synthesis of noble metal- and non-noble metal-based electrocatalysts for overall water splitting and Zn-air batteries.

Xien Liu received his PhD degree from Dalian University of Technology. He is currently a professor of Qingdao University of Science and Technology. His research interests focus on the design of electrocatalysts for electrochemical energy conversion and storage devices.

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Wang, Y., Liu, S., Qin, Q. et al. Praseodymium iridium oxide as a competitive electrocatalyst for oxygen evolution reaction in acid media. Sci. China Mater. 64, 2193–2201 (2021). https://doi.org/10.1007/s40843-020-1598-5

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