Defective Carbon Catalysts with Graphitic N-Modified Adjacent Pentagons as Active Sites for Boosted Oxygen Reduction Reaction in Seawater (2025)

    Energy, Environmental, and Catalysis Applications

    • Lei Wang

      Lei Wang

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

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    • Xuan Liu

      Xuan Liu

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

      More by Xuan Liu

    • Mengting Huang

      Mengting Huang

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

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    • Yun Han

      Yun Han

      School of Engineering and Built Environment, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Brisbane, Queensland 4111, Australia

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    • Panjie Guo

      Panjie Guo

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

      More by Panjie Guo

    • Run Huang

      Run Huang

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

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    • Ying Chen

      Ying Chen

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

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    • Helong Wu

      Helong Wu

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

      More by Helong Wu

    • Jinyan Zhang

      Jinyan Zhang

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

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    • Shuangming Chen

      Shuangming Chen

      National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China

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    • Aijun Du

      Aijun Du

      School of Chemistry and Physics and Centre for Materials Science, Queensland University of Technology, Brisbane, QLD 4000, Australia

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    • Xin Wang*

      Xin Wang

      College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

      *Email: [emailprotected]

      More by Xin Wang

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX

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    https://pubs.acs.org/doi/10.1021/acsami.5c01475

    Published April 24, 2025

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    Defective Carbon Catalysts with Graphitic N-Modified Adjacent Pentagons as Active Sites for Boosted Oxygen Reduction Reaction in Seawater (6)

    Seawater electrocatalysis is highly desired for various energy storage and conversion systems, such as water splitting using seawater as an electrolyte and metal fuel cells. However, the adsorption of chloride ions (Cl) on the active sites of cathodes would worsen the oxygen reduction reaction (ORR) activity and stability, thus lowering the battery performance. Herein, the coupling active sites of graphitic N-regulated adjacent pentagon defects in carbon nanosheets (GAP/CN) were first synthesized by a low-boiling-point metal-mediated partial N-removal strategy. Experimental and theoretical results affirm the advantageous cooperative effect between adjacent pentagons and graphitic N toward the ORR in a harsh seawater environment, where adjacent pentagons act as the authentic highly effective ORR active sites and surrounding graphitic N site serves as the structural regulator to weaken the binding strength of harmful Cl to prevent catalyst poisoning. As a result, GAP/CN delivers excellent ORR activities in diverse electrolytes, including 0.1 M KOH (half-wave potential of 0.87 V), alkaline artificial seawater (half-wave potential of 0.87 V), and natural seawater (half-wave potential of 0.71 V), and also good long-term stability, which can be comparable to commercial Pt/C. This study provides valuable guidance for the rational design of ORR electrocatalysts for seawater-related energy-conversion devices.

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    • Catalysts
    • Defects
    • Electrolytes
    • Redox reactions
    • Seawater

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2025, XXXX, XXX, XXX-XXX

    Click to copy citationCitation copied!

    Published April 24, 2025

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    • Revised

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      online

    © 2025 American Chemical Society

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