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<p>Enhancing cathodic luminol electrochemiluminescence (ECL) relies critically on the efficient generation of reactive oxygen species (ROS) via the oxygen reduction reaction (ORR). However, under weakly alkaline conditions for biological and environmental applications, ORR performance is markedly constrained by the sluggish ORR kinetics, leading to unfavorable ROS yields and weak ECL intensity. Herein, we introduce an innovative hydrogen spillover-mediated ORR mechanism that circumvents this limitation by drastically reducing the activation energy for O–O dissociation. This strategy is achieved through the rational design of dual-active-site catalysts (Ni-N<sub>2</sub>O<sub>2</sub>-Pd), comprising palladium nanoclusters (Pd NCs) and nickel single-atom sites (Ni SASs) co-anchored on a carbon matrix. During catalysis, adsorbed hydrogen generated at Pd NCs migrates to adjacent Ni SASs, where it synergistically promotes the cleavage of the O–O bond. The hydrogen spillover-mediated ORR process significantly boosts the production of ROS and achieves an 83-fold increase in the cathodic ECL intensity notably in weakly alkaline aqueous solutions, in comparison to the conventional single-site ORR pathway. Consequently, an ECL biosensing platform is successfully constructed and applied for chlorpyrifos detection.</p>

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H*-mediated oxygen reduction on Ni-Pd dual sites boosts electrochemiluminescence

  • 期刊论文

  • 发表日期：

    2026年3月3日

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  • Juan He,
  • Hengjia Wang,
  • Jingshuai Li,
  • Mengzhen Xi,
  • Liuyong Hu,
  • Chengzhou Zhu,
  • Wenling Gu

摘要

Enhancing cathodic luminol electrochemiluminescence (ECL) relies critically on the efficient generation of reactive oxygen species (ROS) via the oxygen reduction reaction (ORR). However, under weakly alkaline conditions for biological and environmental applications, ORR performance is markedly constrained by the sluggish ORR kinetics, leading to unfavorable ROS yields and weak ECL intensity. Herein, we introduce an innovative hydrogen spillover-mediated ORR mechanism that circumvents this limitation by drastically reducing the activation energy for O–O dissociation. This strategy is achieved through the rational design of dual-active-site catalysts (Ni-N2O2-Pd), comprising palladium nanoclusters (Pd NCs) and nickel single-atom sites (Ni SASs) co-anchored on a carbon matrix. During catalysis, adsorbed hydrogen generated at Pd NCs migrates to adjacent Ni SASs, where it synergistically promotes the cleavage of the O–O bond. The hydrogen spillover-mediated ORR process significantly boosts the production of ROS and achieves an 83-fold increase in the cathodic ECL intensity notably in weakly alkaline aqueous solutions, in comparison to the conventional single-site ORR pathway. Consequently, an ECL biosensing platform is successfully constructed and applied for chlorpyrifos detection.