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<p>The integration of artificial nanozymes with photoelectrochemical (PEC) biosensing remains underexplored, primarily due to challenges in balancing catalytic efficiency, material stability, and interfacial charge dynamics. Herein, we present a novel split-type PEC biosensor that leverages Au@CeO<sub>2</sub> yolk-shell nanozymes with robust phosphatase-mimicking activity and staggered band structure of WO<sub>3</sub>/BiVO<sub>4</sub> heterojunction for ultrasensitive detection of the breast cancer biomarker HER-2. Unlike conventional nanoenzymes, the yolk-shell architecture encases Au NPs within a CeO<sub>2</sub> shell, synergistically enhancing catalytic efficiency by maximizing the active surface area while simultaneously preventing nanoparticle aggregation and leaching through a protective barrier. Density functional theory (DFT) calculations reveal that the CeO<sub>2</sub>(111)/Au(111) interface drastically reduces the energy barrier for phosphate ester bond cleavage (-16.94 eV vs. 5.69&#xa0;eV for free molecules), thereby enabling rapid hydrolysis of ascorbic acid 2-phosphate (AAP) into ascorbic acid. This catalytic amplification strategy, when integrated with a visible-light-responsive semiconductor substrate, enables zero-bias detection and while effectively eliminating interference from high-voltage operations. The biosensor achieves a detection limit of 41&#xa0;fg/mL (<i>S/N</i> = 3) for HER-2 across a linear range of 0.0001 − 100 ng/mL, surpassing existing methods. Remarkable selectivity, reproducibility (RSD = 3.9%), and recovery rates (95.1%–102.4%) in serum further validate its clinical applicability. This work establishes a universal platform for nanozyme-driven PEC biosensing, presenting significant promise for future use in pathological diagnostics.</p>

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Multi-Level Engineering of Staggered Band Alignment Heterojunctions and Au@CeO2 Yolk-Shell Nanozyme for Photoelectrochemical Biosensing Under Zero-Bias Conditions

  • 期刊论文

  • 发表日期：

    2025年11月13日

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  • Yu Du,
  • Rui Feng,
  • Tingting Wu,
  • Xue Dong,
  • Hongying Jia,
  • Dongquan Leng,
  • Huangxian Ju,
  • Qin Wei

摘要

The integration of artificial nanozymes with photoelectrochemical (PEC) biosensing remains underexplored, primarily due to challenges in balancing catalytic efficiency, material stability, and interfacial charge dynamics. Herein, we present a novel split-type PEC biosensor that leverages Au@CeO2 yolk-shell nanozymes with robust phosphatase-mimicking activity and staggered band structure of WO3/BiVO4 heterojunction for ultrasensitive detection of the breast cancer biomarker HER-2. Unlike conventional nanoenzymes, the yolk-shell architecture encases Au NPs within a CeO2 shell, synergistically enhancing catalytic efficiency by maximizing the active surface area while simultaneously preventing nanoparticle aggregation and leaching through a protective barrier. Density functional theory (DFT) calculations reveal that the CeO2(111)/Au(111) interface drastically reduces the energy barrier for phosphate ester bond cleavage (-16.94 eV vs. 5.69 eV for free molecules), thereby enabling rapid hydrolysis of ascorbic acid 2-phosphate (AAP) into ascorbic acid. This catalytic amplification strategy, when integrated with a visible-light-responsive semiconductor substrate, enables zero-bias detection and while effectively eliminating interference from high-voltage operations. The biosensor achieves a detection limit of 41 fg/mL (S/N = 3) for HER-2 across a linear range of 0.0001 − 100 ng/mL, surpassing existing methods. Remarkable selectivity, reproducibility (RSD = 3.9%), and recovery rates (95.1%–102.4%) in serum further validate its clinical applicability. This work establishes a universal platform for nanozyme-driven PEC biosensing, presenting significant promise for future use in pathological diagnostics.