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PdMo bimetallene for oxygen reduction catalysis

Author

Listed:
  • Mingchuan Luo

    (Peking University
    Peking University)

  • Zhonglong Zhao

    (California State University)

  • Yelong Zhang

    (Peking University)

  • Yingjun Sun

    (Peking University)

  • Yi Xing

    (Peking University)

  • Fan Lv

    (Peking University)

  • Yong Yang

    (Peking University)

  • Xu Zhang

    (California State University)

  • Sooyeon Hwang

    (Brookhaven National Laboratory)

  • Yingnan Qin

    (Peking University)

  • Jing-Yuan Ma

    (Chinese Academy of Sciences)

  • Fei Lin

    (Peking University)

  • Dong Su

    (Brookhaven National Laboratory)

  • Gang Lu

    (California State University)

  • Shaojun Guo

    (Peking University
    Peking University
    Peking University
    Peking University)

Abstract

The efficient interconversion of chemicals and electricity through electrocatalytic processes is central to many renewable-energy initiatives. The sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER)1–4 has long posed one of the biggest challenges in this field, and electrocatalysts based on expensive platinum-group metals are often required to improve the activity and durability of these reactions. The use of alloying5–7, surface strain8–11 and optimized coordination environments12 has resulted in platinum-based nanocrystals that enable very high ORR activities in acidic media; however, improving the activity of this reaction in alkaline environments remains challenging because of the difficulty in achieving optimized oxygen binding strength on platinum-group metals in the presence of hydroxide. Here we show that PdMo bimetallene—a palladium–molybdenum alloy in the form of a highly curved and sub-nanometre-thick metal nanosheet—is an efficient and stable electrocatalyst for the ORR and the OER in alkaline electrolytes, and shows promising performance as a cathode in Zn–air and Li–air batteries. The thin-sheet structure of PdMo bimetallene enables a large electrochemically active surface area (138.7 square metres per gram of palladium) as well as high atomic utilization, resulting in a mass activity towards the ORR of 16.37 amperes per milligram of palladium at 0.9 volts versus the reversible hydrogen electrode in alkaline electrolytes. This mass activity is 78 times and 327 times higher than those of commercial Pt/C and Pd/C catalysts, respectively, and shows little decay after 30,000 potential cycles. Density functional theory calculations reveal that the alloying effect, the strain effect due to the curved geometry, and the quantum size effect due to the thinness of the sheets tune the electronic structure of the system for optimized oxygen binding. Given the properties and the structure–activity relationships of PdMo metallene, we suggest that other metallene materials could show great promise in energy electrocatalysis.

Suggested Citation

  • Mingchuan Luo & Zhonglong Zhao & Yelong Zhang & Yingjun Sun & Yi Xing & Fan Lv & Yong Yang & Xu Zhang & Sooyeon Hwang & Yingnan Qin & Jing-Yuan Ma & Fei Lin & Dong Su & Gang Lu & Shaojun Guo, 2019. "PdMo bimetallene for oxygen reduction catalysis," Nature, Nature, vol. 574(7776), pages 81-85, October.
  • Handle: RePEc:nat:nature:v:574:y:2019:i:7776:d:10.1038_s41586-019-1603-7
    DOI: 10.1038/s41586-019-1603-7
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    Cited by:

    1. Yueshan Xu & Daoxiong Wu & Qinghua Zhang & Peng Rao & Peilin Deng & Mangen Tang & Jing Li & Yingjie Hua & Chongtai Wang & Shengkui Zhong & Chunman Jia & Zhongxin Liu & Yijun Shen & Lin Gu & Xinlong Ti, 2024. "Regulating Au coverage for the direct oxidation of methane to methanol," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Lu Tao & Kai Wang & Fan Lv & Hongtian Mi & Fangxu Lin & Heng Luo & Hongyu Guo & Qinghua Zhang & Lin Gu & Mingchuan Luo & Shaojun Guo, 2023. "Precise synthetic control of exclusive ligand effect boosts oxygen reduction catalysis," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. 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.
    4. Wanlin Zhou & Baojie Li & Xinyu Liu & Jingjing Jiang & Shuowen Bo & Chenyu Yang & Qizheng An & Yuhao Zhang & Mikhail A. Soldatov & Huijuan Wang & Shiqiang Wei & Qinghua Liu, 2024. "In situ tuning of platinum 5d valence states for four-electron oxygen reduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. Lin He & Menggang Li & Longyu Qiu & Shuo Geng & Yequn Liu & Fenyang Tian & Mingchuan Luo & Hu Liu & Yongsheng Yu & Weiwei Yang & Shaojun Guo, 2024. "Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Yinghao Li & Chun-Kuo Peng & Huimin Hu & San-Yuan Chen & Jin-Ho Choi & Yan-Gu Lin & Jong-Min Lee, 2022. "Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Qichen Wang & Qingguo Feng & Yongpeng Lei & Shuaihao Tang & Liang Xu & Yu Xiong & Guozhao Fang & Yuchao Wang & Peiyao Yang & Jingjing Liu & Wei Liu & Xiang Xiong, 2022. "Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    8. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    9. Zhongzhe Wei & Zijiang Zhao & Chenglong Qiu & Songtao Huang & Zihao Yao & Mingxuan Wang & Yi Chen & Yue Lin & Xing Zhong & Xiaonian Li & Jianguo Wang, 2023. "Tripodal Pd metallenes mediated by Nb2C MXenes for boosting alkynes semihydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    10. Shan Lei & Jing Zhang & Nicholas Thomas Blum & Meng Li & Dong-Yang Zhang & Weimin Yin & Feng Zhao & Jing Lin & Peng Huang, 2022. "In vivo three-dimensional multispectral photoacoustic imaging of dual enzyme-driven cyclic cascade reaction for tumor catalytic therapy," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    11. Yifeng Hou & Fengyan Wang & Chichu Qin & Shining Wu & Mengyang Cao & Pengkun Yang & Lu Huang & Yingpeng Wu, 2022. "A self-healing electrocatalytic system via electrohydrodynamics induced evolution in liquid metal," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    12. Jinfa Chang & Guanzhi Wang & Xiaoxia Chang & Zhenzhong Yang & Han Wang & Boyang Li & Wei Zhang & Libor Kovarik & Yingge Du & Nina Orlovskaya & Bingjun Xu & Guofeng Wang & Yang Yang, 2023. "Interface synergism and engineering of Pd/Co@N-C for direct ethanol fuel cells," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    13. Geng Wu & Xiao Han & Jinyan Cai & Peiqun Yin & Peixin Cui & Xusheng Zheng & Hai Li & Cai Chen & Gongming Wang & Xun Hong, 2022. "In-plane strain engineering in ultrathin noble metal nanosheets boosts the intrinsic electrocatalytic hydrogen evolution activity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    14. Xingkun Wang & Liangliang Xu & Cheng Li & Canhui Zhang & Hanxu Yao & Ren Xu & Peixin Cui & Xusheng Zheng & Meng Gu & Jinwoo Lee & Heqing Jiang & Minghua Huang, 2023. "Developing a class of dual atom materials for multifunctional catalytic reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    15. Pu Wang & Xingyu Zhang & Run Shi & Jiaqi Zhao & Geoffrey I. N. Waterhouse & Junwang Tang & Tierui Zhang, 2024. "Photocatalytic ethylene production by oxidative dehydrogenation of ethane with dioxygen on ZnO-supported PdZn intermetallic nanoparticles," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    16. Zhiqiang Zheng & Lu Qi & Xiaoyu Luan & Shuya Zhao & Yurui Xue & Yuliang Li, 2024. "Growing highly ordered Pt and Mn bimetallic single atomic layers over graphdiyne," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    17. Qiqi Mao & Xu Mu & Wenxin Wang & Kai Deng & Hongjie Yu & Ziqiang Wang & You Xu & Liang Wang & Hongjing Wang, 2023. "Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    18. Dongping Xue & Yifang Yuan & Yue Yu & Siran Xu & Yifan Wei & Jiaqi Zhang & Haizhong Guo & Minhua Shao & Jia-Nan Zhang, 2024. "Spin occupancy regulation of the Pt d-orbital for a robust low-Pt catalyst towards oxygen reduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    19. Zhe Jiang & Xuerui Liu & Xiao-Zhi Liu & Shuang Huang & Ying Liu & Ze-Cheng Yao & Yun Zhang & Qing-Hua Zhang & Lin Gu & Li-Rong Zheng & Li Li & Jianan Zhang & Youjun Fan & Tang Tang & Zhongbin Zhuang &, 2023. "Interfacial assembly of binary atomic metal-Nx sites for high-performance energy devices," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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