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<p>Despite of the progress in cathode catalysts for lithium oxygen Li-O<sub>2</sub> batteries (LOBs) development, significant challenges persist, mainly due to the slow kinetics of the redox reactions due to insulating and insoluble discharge products. Dual-atom catalysts (DACs), perfectly inheriting the advantages of single atom catalysts (SACs), can exhibit better catalytic performance than simple SACs and thus have gradually gained researchers’ attention. Herein, integrated adjacent Ni/Co atoms were designed <i>via</i> a scalable pre-constrained metal twin’s strategy. Utilizing a click chemistry-derived approach, cross-linked polyphthalocyanine frameworks (TMPPc-XL) were synthesized. This design prevented metal aggregation during pyrolysis, enriched nitrogen, and stabilized well-defined Ni/Co-N<sub><i>x</i></sub> coordination sites. The resulting dual-atom catalysts exhibited exceptional oxygen reduction reaction (ORR) performance, including high activity, stability, and capacity, driven by the synergistic electronic interplay between neighboring Ni-Co sites. It is expected that Ni optimizes intermediate adsorption, while Co tailored <i>d</i>-band positioning and lowers energy barriers, collectively enhancing charge redistribution and multi-step reaction stabilization. The modular synthesis, compatible with diverse transition metal phthalocyanines, offers a versatile platform for designing ideal electrocatalysts for realizing high-performance LOBs.</p>

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Ni/Co Dual Atom Catalysts with Synergistic Bifunctionality for High-efficiency Lithium Oxygen Battery

  • 期刊论文

  • 发表日期：

    2025年7月8日

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  • Zeinab Mohamed,
  • Joseph Peter Chimtali,
  • Wei Jiang,
  • Hanchen Xu,
  • Changda Wang,
  • Li Song

摘要

Despite of the progress in cathode catalysts for lithium oxygen Li-O2 batteries (LOBs) development, significant challenges persist, mainly due to the slow kinetics of the redox reactions due to insulating and insoluble discharge products. Dual-atom catalysts (DACs), perfectly inheriting the advantages of single atom catalysts (SACs), can exhibit better catalytic performance than simple SACs and thus have gradually gained researchers’ attention. Herein, integrated adjacent Ni/Co atoms were designed via a scalable pre-constrained metal twin’s strategy. Utilizing a click chemistry-derived approach, cross-linked polyphthalocyanine frameworks (TMPPc-XL) were synthesized. This design prevented metal aggregation during pyrolysis, enriched nitrogen, and stabilized well-defined Ni/Co-Nx coordination sites. The resulting dual-atom catalysts exhibited exceptional oxygen reduction reaction (ORR) performance, including high activity, stability, and capacity, driven by the synergistic electronic interplay between neighboring Ni-Co sites. It is expected that Ni optimizes intermediate adsorption, while Co tailored d-band positioning and lowers energy barriers, collectively enhancing charge redistribution and multi-step reaction stabilization. The modular synthesis, compatible with diverse transition metal phthalocyanines, offers a versatile platform for designing ideal electrocatalysts for realizing high-performance LOBs.