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Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution

Author

Listed:
  • Jie Dai

    (Nanjing Tech University)

  • Yinlong Zhu

    (Monash University)

  • Hassan A. Tahini

    (Australian National University)

  • Qian Lin

    (Monash University)

  • Yu Chen

    (Monash University)

  • Daqin Guan

    (Nanjing Tech University)

  • Chuan Zhou

    (Nanjing Tech University)

  • Zhiwei Hu

    (Max Planck Institute for Chemical Physics of Solids)

  • Hong-Ji Lin

    (National Synchrotron Radiation Research Center)

  • Ting-Shan Chan

    (National Synchrotron Radiation Research Center)

  • Chien-Te Chen

    (National Synchrotron Radiation Research Center)

  • Sean C. Smith

    (Australian National University)

  • Huanting Wang

    (Monash University)

  • Wei Zhou

    (Nanjing Tech University)

  • Zongping Shao

    (Nanjing Tech University
    Curtin University)

Abstract

The state-of-the-art active HER catalysts in acid media (e.g., Pt) generally lose considerable catalytic performance in alkaline media mainly due to the additional water dissociation step. To address this issue, synergistic hybrid catalysts are always designed by coupling them with metal (hydro)oxides. However, such hybrid systems usually suffer from long reaction path, high cost and complex preparation methods. Here, we discover a single-phase HER catalyst, SrTi0.7Ru0.3O3-δ (STRO) perovskite oxide highlighted with an unusual super-exchange effect, which exhibits excellent HER performance in alkaline media via atomic-scale synergistic active centers. With insights from first-principles calculations, the intrinsically synergistic interplays between multiple active centers in STRO are uncovered to accurately catalyze different elementary steps of alkaline HER; namely, the Ti sites facilitates nearly-barrierless water dissociation, Ru sites function favorably for OH* desorption, and non-metal oxygen sites (i.e., oxygen vacancies/lattice oxygen) promotes optimal H* adsorption and H2 desorption.

Suggested Citation

  • Jie Dai & Yinlong Zhu & Hassan A. Tahini & Qian Lin & Yu Chen & Daqin Guan & Chuan Zhou & Zhiwei Hu & Hong-Ji Lin & Ting-Shan Chan & Chien-Te Chen & Sean C. Smith & Huanting Wang & Wei Zhou & Zongping, 2020. "Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19433-1
    DOI: 10.1038/s41467-020-19433-1
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    Cited by:

    1. Jiaxi Zhang & Longhai Zhang & Jiamin Liu & Chengzhi Zhong & Yuanhua Tu & Peng Li & Li Du & Shengli Chen & Zhiming Cui, 2022. "OH spectator at IrMo intermetallic narrowing activity gap between alkaline and acidic hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Jie Dai & Yawen Tong & Long Zhao & Zhiwei Hu & Chien-Te Chen & Chang-Yang Kuo & Guangming Zhan & Jiaxian Wang & Xingyue Zou & Qian Zheng & Wei Hou & Ruizhao Wang & Kaiyuan Wang & Rui Zhao & Xiang-Kui , 2024. "Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Xiangyu Meng & Chuntong Zhu & Xin Wang & Zehua Liu & Mengmeng Zhu & Kuibo Yin & Ran Long & Liuning Gu & Xinxing Shao & Litao Sun & Yueming Sun & Yunqian Dai & Yujie Xiong, 2023. "Hierarchical triphase diffusion photoelectrodes for photoelectrochemical gas/liquid flow conversion," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    4. Jie Dai & Yinlong Zhu & Yu Chen & Xue Wen & Mingce Long & Xinhao Wu & Zhiwei Hu & Daqin Guan & Xixi Wang & Chuan Zhou & Qian Lin & Yifei Sun & Shih-Chang Weng & Huanting Wang & Wei Zhou & Zongping Sha, 2022. "Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    5. Luqi Wang & Yixin Hao & Liming Deng & Feng Hu & Sheng Zhao & Linlin Li & Shengjie Peng, 2022. "Rapid complete reconfiguration induced actual active species for industrial hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    6. Dongpeng Zhang & Yanxiao Li & Pengfei Wang & Jinyong Qu & Yi Li & Sihui Zhan, 2023. "Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    7. Sheng Zhao & Sung-Fu Hung & Liming Deng & Wen-Jing Zeng & Tian Xiao & Shaoxiong Li & Chun-Han Kuo & Han-Yi Chen & Feng Hu & Shengjie Peng, 2024. "Constructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    8. Jiawei Zhu & Yu Zhang & Zitao Chen & Zhenbao Zhang & Xuezeng Tian & Minghua Huang & Xuedong Bai & Xue Wang & Yongfa Zhu & Heqing Jiang, 2024. "Superexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO2 electromethanation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    9. Kamran Dastafkan & Xiangjian Shen & Rosalie K. Hocking & Quentin Meyer & Chuan Zhao, 2023. "Monometallic interphasic synergy via nano-hetero-interfacing for hydrogen evolution in alkaline electrolytes," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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