IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-49281-2.html
   My bibliography  Save this article

Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis

Author

Listed:
  • Lu Li

    (Peking University)

  • Gengwei Zhang

    (Kunming University of Science and Technology)

  • Chenhui Zhou

    (Peking University)

  • Fan Lv

    (Peking University)

  • Yingjun Tan

    (Peking University)

  • Ying Han

    (Peking University)

  • Heng Luo

    (Peking University)

  • Dawei Wang

    (Peking University)

  • Youxing Liu

    (Peking University)

  • Changshuai Shang

    (Peking University)

  • Lingyou Zeng

    (Peking University)

  • Qizheng Huang

    (Peking University)

  • Ruijin Zeng

    (Peking University)

  • Na Ye

    (Peking University)

  • Mingchuan Luo

    (Peking University)

  • Shaojun Guo

    (Peking University)

Abstract

Precisely modulating the Ru-O covalency in RuOx for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d-valence electrons, which were doped into or alloyed with RuOx, are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5s/5p orbitals. Theoretical calculations confirm that the durability of Ln-RuOx following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuOx, Er-RuOx is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO2. Particularly, the Er-RuOx-based device requires only 1.837 V to reach 3 A cm−2 and shows a long-term stability at 500 mA cm−2 for 100 h with a degradation rate of mere 37 μV h−1.

Suggested Citation

  • Lu Li & Gengwei Zhang & Chenhui Zhou & Fan Lv & Yingjun Tan & Ying Han & Heng Luo & Dawei Wang & Youxing Liu & Changshuai Shang & Lingyou Zeng & Qizheng Huang & Ruijin Zeng & Na Ye & Mingchuan Luo & S, 2024. "Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49281-2
    DOI: 10.1038/s41467-024-49281-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-49281-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-49281-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Li, Zheng & Wang, Yameng & Mu, Yongbiao & Wu, Buke & Jiang, Yuting & Zeng, Lin & Zhao, Tianshou, 2023. "Recent advances in the anode catalyst layer for proton exchange membrane fuel cells," Renewable and Sustainable Energy Reviews, Elsevier, vol. 176(C).
    2. Jiaxin Guo & Yao Zheng & Zhenpeng Hu & Caiyan Zheng & Jing Mao & Kun Du & Mietek Jaroniec & Shi-Zhang Qiao & Tao Ling, 2023. "Direct seawater electrolysis by adjusting the local reaction environment of a catalyst," Nature Energy, Nature, vol. 8(3), pages 264-272, March.
    3. Linlin Cao & Qiquan Luo & Jiajia Chen & Lan Wang & Yue Lin & Huijuan Wang & Xiaokang Liu & Xinyi Shen & Wei Zhang & Wei Liu & Zeming Qi & Zheng Jiang & Jinlong Yang & Tao Yao, 2019. "Dynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    4. Yi Wang & Rong Yang & Yajun Ding & Bo Zhang & Hao Li & Bing Bai & Mingrun Li & Yi Cui & Jianping Xiao & Zhong-Shuai Wu, 2023. "Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Qian Dang & Haiping Lin & Zhenglong Fan & Lu Ma & Qi Shao & Yujin Ji & Fangfang Zheng & Shize Geng & Shi-Ze Yang & Ningning Kong & Wenxiang Zhu & Youyong Li & Fan Liao & Xiaoqing Huang & Mingwang Shao, 2021. "Iridium metallene oxide for acidic oxygen evolution catalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    6. Dafeng Zhang & Mengnan Li & Xue Yong & Haoqiang Song & Geoffrey I. N. Waterhouse & Yunfei Yi & Bingjie Xue & Dongliang Zhang & Baozhong Liu & Siyu Lu, 2023. "Construction of Zn-doped RuO2 nanowires for efficient and stable water oxidation in acidic media," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Zhaoping Shi & Ji Li & Yibo Wang & Shiwei Liu & Jianbing Zhu & Jiahao Yang & Xian Wang & Jing Ni & Zheng Jiang & Lijuan Zhang & Ying Wang & Changpeng Liu & Wei Xing & Junjie Ge, 2023. "Customized reaction route for ruthenium oxide towards stabilized water oxidation in high-performance PEM electrolyzers," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Qianqian Ji & Bing Tang & Xilin Zhang & Chao Wang & Hao Tan & Jie Zhao & Ruiqi Liu & Mei Sun & Hengjie Liu & Chang Jiang & Jianrong Zeng & Xingke Cai & Wensheng Yan, 2024. "Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Yu Shen & Xiao-Long Zhang & Ming-Rong Qu & Jie Ma & Sheng Zhu & Yu-Lin Min & Min-Rui Gao & Shu-Hong Yu, 2024. "Cr dopant mediates hydroxyl spillover on RuO2 for high-efficiency proton exchange membrane electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Xinyu Ping & Yongduo Liu & Lixia Zheng & Yang Song & Lin Guo & Siguo Chen & Zidong Wei, 2024. "Locking the lattice oxygen in RuO2 to stabilize highly active Ru sites in acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Chenhui Zhou & Jia Shi & Zhaoqi Dong & Lingyou Zeng & Yan Chen & Ying Han & Lu Li & Wenyu Zhang & Qinghua Zhang & Lin Gu & Fan Lv & Mingchuan Luo & Shaojun Guo, 2024. "Oxophilic gallium single atoms bridged ruthenium clusters for practical anion-exchange membrane electrolyzer," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Zhaoping Shi & Ji Li & Yibo Wang & Shiwei Liu & Jianbing Zhu & Jiahao Yang & Xian Wang & Jing Ni & Zheng Jiang & Lijuan Zhang & Ying Wang & Changpeng Liu & Wei Xing & Junjie Ge, 2023. "Customized reaction route for ruthenium oxide towards stabilized water oxidation in high-performance PEM electrolyzers," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    5. Lingxi Zhou & Yangfan Shao & Fang Yin & Jia Li & Feiyu Kang & Ruitao Lv, 2023. "Stabilizing non-iridium active sites by non-stoichiometric oxide for acidic water oxidation at high current density," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Jie Liang & Zhengwei Cai & Zixiao Li & Yongchao Yao & Yongsong Luo & Shengjun Sun & Dongdong Zheng & Qian Liu & Xuping Sun & Bo Tang, 2024. "Efficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    7. Wenxiang Zhu & Xiangcong Song & Fan Liao & Hui Huang & Qi Shao & Kun Feng & Yunjie Zhou & Mengjie Ma & Jie Wu & Hao Yang & Haiwei Yang & Meng Wang & Jie Shi & Jun Zhong & Tao Cheng & Mingwang Shao & Y, 2023. "Stable and oxidative charged Ru enhance the acidic oxygen evolution reaction activity in two-dimensional ruthenium-iridium oxide," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    8. Qianqian Ji & Bing Tang & Xilin Zhang & Chao Wang & Hao Tan & Jie Zhao & Ruiqi Liu & Mei Sun & Hengjie Liu & Chang Jiang & Jianrong Zeng & Xingke Cai & Wensheng Yan, 2024. "Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. Haoyin Zhong & Qi Zhang & Junchen Yu & Xin Zhang & Chao Wu & Hang An & Yifan Ma & Hao Wang & Jun Zhang & Yong-Wei Zhang & Caozheng Diao & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin Xue, 2023. "Key role of eg* band broadening in nickel-based oxyhydroxides on coupled oxygen evolution mechanism," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    10. Wang, Mingkai & Pei, Pucheng & Xu, Yiming & Fan, Tengbo & Ren, Peng & Zhu, Zijing & Chen, Dongfang & Fu, Xi & Song, Xin & Wang, He, 2024. "CO-tolerance behaviors of proton exchange membrane fuel cell stacks with impure hydrogen fuel," Applied Energy, Elsevier, vol. 366(C).
    11. Kun Du & Lifu Zhang & Jieqiong Shan & Jiaxin Guo & Jing Mao & Chueh-Cheng Yang & Chia-Hsin Wang & Zhenpeng Hu & Tao Ling, 2022. "Interface engineering breaks both stability and activity limits of RuO2 for sustainable water oxidation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    12. Guokang Han & Xue Zhang & Wei Liu & Qinghua Zhang & Zhiqiang Wang & Jun Cheng & Tao Yao & Lin Gu & Chunyu Du & Yunzhi Gao & Geping Yin, 2021. "Substrate strain tunes operando geometric distortion and oxygen reduction activity of CuN2C2 single-atom sites," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    13. Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    14. Yanrong Xue & Jiwu Zhao & Liang Huang & Ying-Rui Lu & Abdul Malek & Ge Gao & Zhongbin Zhuang & Dingsheng Wang & Cafer T. Yavuz & Xu Lu, 2023. "Stabilizing ruthenium dioxide with cation-anchored sulfate for durable oxygen evolution in proton-exchange membrane water electrolyzers," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    15. Huanyu Jin & Xinyan Liu & Pengfei An & Cheng Tang & Huimin Yu & Qinghua Zhang & Hong-Jie Peng & Lin Gu & Yao Zheng & Taeseup Song & Kenneth Davey & Ungyu Paik & Juncai Dong & Shi-Zhang Qiao, 2023. "Dynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    16. Jie Wei & Hua Tang & Li Sheng & Ruyang Wang & Minghui Fan & Jiale Wan & Yuheng Wu & Zhirong Zhang & Shiming Zhou & Jie Zeng, 2024. "Site-specific metal-support interaction to switch the activity of Ir single atoms for oxygen evolution reaction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    17. Zhe Chen & Jili Li & Lingshen Meng & Jianan Li & Yaming Hao & Tao Jiang & Xuejing Yang & Yefei Li & Zhi-Pan Liu & Ming Gong, 2023. "Ligand vacancy channels in pillared inorganic-organic hybrids for electrocatalytic organic oxidation with enzyme-like activities," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Zhirong Zhang & Chuanyi Jia & Peiyu Ma & Chen Feng & Jin Yang & Junming Huang & Jiana Zheng & Ming Zuo & Mingkai Liu & Shiming Zhou & Jie Zeng, 2024. "Distance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    19. Shixuan Zhao & Bin Liu & Kailang Li & Shujie Wang & Gong Zhang & Zhi-Jian Zhao & Tuo Wang & Jinlong Gong, 2024. "A silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    20. Pengcheng Ye & Keqing Fang & Haiyan Wang & Yahao Wang & Hao Huang & Chenbin Mo & Jiqiang Ning & Yong Hu, 2024. "Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49281-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.