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Subtle tuning of nanodefects actuates highly efficient electrocatalytic oxidation

Author

Listed:
  • Yifan Gao

    (Tsinghua University)

  • Shuai Liang

    (Beijing Forestry University)

  • Biming Liu

    (Tsinghua University)

  • Chengxu Jiang

    (Tsinghua University)

  • Chenyang Xu

    (Tsinghua University)

  • Xiaoyuan Zhang

    (Tsinghua University)

  • Peng Liang

    (Tsinghua University)

  • Menachem Elimelech

    (Yale University)

  • Xia Huang

    (Tsinghua University)

Abstract

Achieving controllable fine-tuning of defects in catalysts at the atomic level has become a zealous pursuit in catalysis-related fields. However, the generation of defects is quite random, and their flexible manipulation lacks theoretical basis. Herein, we present a facile and highly controllable thermal tuning strategy that enables fine control of nanodefects via subtle manipulation of atomic/lattice arrangements in electrocatalysts. Such thermal tuning endows common carbon materials with record high efficiency in electrocatalytic degradation of pollutants. Systematic characterization and calculations demonstrate that an optimal thermal tuning can bring about enhanced electrocatalytic efficiency by manipulating the N-centered annulation–volatilization reactions and C-based sp3/sp2 configuration alteration. Benefiting from this tuning strategy, the optimized electrocatalytic anodic membrane successfully achieves >99% pollutant (propranolol) degradation during a flow-through (~2.5 s for contact time), high-flux (424.5 L m−2 h−1), and long-term (>720 min) electrocatalytic filtration test at a very low energy consumption (0.029 ± 0.010 kWh m−3 order−1). Our findings highlight a controllable preparation approach of catalysts while also elucidating the molecular level mechanisms involved.

Suggested Citation

  • Yifan Gao & Shuai Liang & Biming Liu & Chengxu Jiang & Chenyang Xu & Xiaoyuan Zhang & Peng Liang & Menachem Elimelech & Xia Huang, 2023. "Subtle tuning of nanodefects actuates highly efficient electrocatalytic oxidation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37676-6
    DOI: 10.1038/s41467-023-37676-6
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    References listed on IDEAS

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    1. Yiou Wang & Xu Liu & Xiaoyu Han & Robert Godin & Jialu Chen & Wuzong Zhou & Chaoran Jiang & Jamie F. Thompson & K. Bayazit Mustafa & Stephen A. Shevlin & James R. Durrant & Zhengxiao Guo & Junwang Tan, 2020. "Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Yong Zhao & Ryuhei Nakamura & Kazuhide Kamiya & Shuji Nakanishi & Kazuhito Hashimoto, 2013. "Nitrogen-doped carbon nanomaterials as non-metal electrocatalysts for water oxidation," Nature Communications, Nature, vol. 4(1), pages 1-7, December.
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