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Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation

Author

Listed:
  • Tingting Hou

    (Central South University)

  • Qiquan Luo

    (Anhui University
    University of Science and Technology of China)

  • Qi Li

    (Central South University)

  • Hualu Zu

    (Central South University)

  • Peixin Cui

    (the Chinese Academy of Sciences)

  • Siwei Chen

    (Central South University)

  • Yue Lin

    (University of Science and Technology of China)

  • Jiajia Chen

    (University of Science and Technology of China)

  • Xusheng Zheng

    (University of Science and Technology of China)

  • Wenkun Zhu

    (Southwest University of Science and Technology)

  • Shuquan Liang

    (Central South University)

  • Jinlong Yang

    (University of Science and Technology of China)

  • Liangbing Wang

    (Central South University)

Abstract

As a promising hydrogen carrier, formic acid (HCOOH) is renewable, safe and nontoxic. Although noble-metal-based catalysts have exhibited excellent activity in HCOOH dehydrogenation, developing non-noble-metal heterogeneous catalysts with high efficiency remains a great challenge. Here, we modulate oxygen coverage on the surface of Ti3C2Tx MXenes to boost the catalytic activity toward HCOOH dehydrogenation. Impressively, Ti3C2Tx MXenes after treating with air at 250 °C (Ti3C2Tx-250) significantly increase the amount of surface oxygen atoms without the change of crystalline structure, exhibiting a mass activity of 365 mmol·g−1·h−1 with 100% of selectivity for H2 at 80 °C, which is 2.2 and 2.0 times that of commercial Pd/C and Pt/C, respectively. Further mechanistic studies demonstrate that HCOO* is the intermediate in HCOOH dehydrogenation over Ti3C2Tx MXenes with different coverages of surface oxygen atoms. Increasing the oxygen coverage on the surface of Ti3C2Tx MXenes not only promotes the conversion from HCOO* to CO2* by lowering the energy barrier, but also weakens the adsorption energy of CO2 and H2, thus accelerating the dehydrogenation of HCOOH.

Suggested Citation

  • Tingting Hou & Qiquan Luo & Qi Li & Hualu Zu & Peixin Cui & Siwei Chen & Yue Lin & Jiajia Chen & Xusheng Zheng & Wenkun Zhu & Shuquan Liang & Jinlong Yang & Liangbing Wang, 2020. "Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18091-7
    DOI: 10.1038/s41467-020-18091-7
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    Cited by:

    1. Haifeng Shen & Huanyu Jin & Haobo Li & Herui Wang & Jingjing Duan & Yan Jiao & Shi-Zhang Qiao, 2023. "Acidic CO2-to-HCOOH electrolysis with industrial-level current on phase engineered tin sulfide," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Luyao Guo & Kaixuan Zhuge & Siyang Yan & Shiyi Wang & Jia Zhao & Saisai Wang & Panzhe Qiao & Jiaxu Liu & Xiaoling Mou & Hejun Zhu & Ziang Zhao & Li Yan & Ronghe Lin & Yunjie Ding, 2023. "Defect-driven nanostructuring of low-nuclearity Pt-Mo ensembles for continuous gas-phase formic acid dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Xiaoyang Pan & Xuhui Yang & Maoqing Yu & Xiaoxiao Lu & Hao Kang & Min-Quan Yang & Qingrong Qian & Xiaojing Zhao & Shijing Liang & Zhenfeng Bian, 2023. "2D MXenes polar catalysts for multi-renewable energy harvesting applications," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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