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Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene

Author

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  • Yan Jiao

    (School of Chemical Engineering, The University of Adelaide)

  • Yao Zheng

    (School of Chemical Engineering, The University of Adelaide)

  • Kenneth Davey

    (School of Chemical Engineering, The University of Adelaide)

  • Shi-Zhang Qiao

    (School of Chemical Engineering, The University of Adelaide)

Abstract

The hydrogen evolution reaction (HER) is a fundamental process in electrocatalysis and plays an important role in energy conversion through water splitting to produce hydrogen. Effective candidates for HER are often based on noble metals or transition metal dichalcogenides, while carbon-based metal-free electrocatalysts generally demonstrate poorer activity. Here we report evaluation of a series of heteroatom-doped graphene materials as efficient HER electrocatalysts by combining spectroscopic characterization, electrochemical measurements, and density functional theory calculations. Results of theoretical computations are shown to be in good agreement with experimental observations regarding the intrinsic electrocatalytic activity and the HER reaction mechanism. As a result, we establish a HER activity trend for graphene-based materials, and explore their reactivity origin to guide the design of more efficient electrocatalysts. We predict that by rationally modifying particular experimentally achievable physicochemical characteristics, a practically realizable graphene-based material will have the potential to exceed the performance of the metal-based benchmark for HER.

Suggested Citation

  • Yan Jiao & Yao Zheng & Kenneth Davey & Shi-Zhang Qiao, 2016. "Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene," Nature Energy, Nature, vol. 1(10), pages 1-9, October.
    • Handle: RePEc:nat:natene:v:1:y:2016:i:10:d:10.1038_nenergy.2016.130
    DOI: 10.1038/nenergy.2016.130
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    Cited by:

    1. Bohua Ren & Guobin Wen & Rui Gao & Dan Luo & Zhen Zhang & Weibin Qiu & Qianyi Ma & Xin Wang & Yi Cui & Luis Ricardez–Sandoval & Aiping Yu & Zhongwei Chen, 2022. "Nano-crumples induced Sn-Bi bimetallic interface pattern with moderate electron bank for highly efficient CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. Zengyao Wang & Jiyi Chen & Erhong Song & Ning Wang & Juncai Dong & Xiang Zhang & Pulickel M. Ajayan & Wei Yao & Chenfeng Wang & Jianjun Liu & Jianfeng Shen & Mingxin Ye, 2021. "Manipulation on active electronic states of metastable phase β-NiMoO4 for large current density hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. 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.
    4. Wenyao Chen & Yao Shi & Changwei Liu & Zhouhong Ren & Zikun Huang & Zhou Chen & Xiangxue Zhang & Shanshan Liang & Lei Xie & Cheng Lian & Gang Qian & Jing Zhang & Xi Liu & De Chen & Xinggui Zhou & Weik, 2024. "Restructuring the interfacial active sites to generalize the volcano curves for platinum-cobalt synergistic catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Lee, Seung Jun & Theerthagiri, Jayaraman & Nithyadharseni, Palaniyandy & Arunachalam, Prabhakarn & Balaji, Dhandapani & Madan Kumar, Arumugam & Madhavan, Jagannathan & Mittal, Vikas & Choi, Myong Yong, 2021. "Heteroatom-doped graphene-based materials for sustainable energy applications: A review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 143(C).
    6. Chao Ye & Huanyu Jin & Jieqiong Shan & Yan Jiao & Huan Li & Qinfen Gu & Kenneth Davey & Haihui Wang & Shi-Zhang Qiao, 2021. "A Mo5N6 electrocatalyst for efficient Na2S electrodeposition in room-temperature sodium-sulfur batteries," Nature Communications, Nature, vol. 12(1), pages 1-11, December.

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