Single-atom rhodium mimicking the oxidase and peroxidase for NADH cascade oxidation

IF 9.6 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Rare Metals Pub Date : 2025-03-03 DOI:10.1007/s12598-024-03221-7

Hong-Jin Xue, Meng Zhang, Yong-Qing Li, Chao-Ran Liu, Xin-Yu Ma, Qin-Bin He, Yin-Chuan Wang, Jin-Xing Chen, Jian-Feng Qiu

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Abstract

Constructing high-performance nanozymes for specific biomolecules is crucial but challenging for practical applications and fundamental research. Herein, through the examination of the catalytic reaction paths of natural nicotinamide adenine dinucleotide (NADH) oxidase (NOX), a novel and efficient single-atom rhodium catalyst (Rh₁/NC) was developed to mimic NOX. The Rh₁/NC demonstrated the ability to catalyze the dehydrogenation of NADH and transfer electrons to O₂ to generate H₂O₂ through the typical two-electron pathway. Furthermore, our findings revealed that Rh₁/NC exhibits the ability to catalyze the conversion of produced H₂O₂ into OH under mildly acidic conditions. This process amplifies the oxidation of NADH, showcasing NADH peroxidase-like activity (NPx-like). As a paradigm, this unique dual enzyme-like property of Rh₁/NC with a positive feedback effect holds significance in disrupting cancer cellular homeostasis. Rh₁/NC can effectively consume NADH via cascade biocatalytic reactions within cancer cells, further triggering the elevation of reactive oxygen species (ROS), leading to impaired oxidative phosphorylation and decreased mitochondrial membrane potential, thus damaging the adenosine triphosphate (ATP) synthesis. The resulting 'domino effect' interferes with the energy metabolism homeostasis of cancer cells, ultimately promoting cell apoptosis. This study provides potential guidance for the rational design of materials with greater capabilities.

Graphical abstract

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单原子铑模拟NADH级联氧化的氧化酶和过氧化物酶

构建针对特定生物分子的高性能纳米酶对于实际应用和基础研究来说至关重要，但具有挑战性。本文通过对天然烟酰胺腺嘌呤二核苷酸（NADH）氧化酶（NOX）催化反应途径的考察，研制了一种新型高效的单原子铑催化剂（Rh1/NC）来模拟NOX。Rh1/NC通过典型的双电子途径催化NADH脱氢并将电子转移到O2生成H2O2。此外，我们的研究结果表明，Rh1/NC显示出在弱酸性条件下催化H2O2转化为OH的能力。这个过程放大了NADH的氧化，显示出NADH过氧化物酶样活性（npx样）。作为一个范例，Rh1/NC这种独特的双酶样特性具有正反馈效应，在破坏癌细胞稳态方面具有重要意义。Rh1/NC可通过癌细胞内的级联生物催化反应有效消耗NADH，进而触发活性氧（ROS）升高，导致氧化磷酸化受损，线粒体膜电位降低，从而破坏三磷酸腺苷（adenosine triphosphate， ATP）合成。由此产生的“多米诺骨牌效应”干扰了癌细胞的能量代谢稳态，最终促进细胞凋亡。本研究为高性能材料的合理设计提供了潜在的指导。图形抽象

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来源期刊

Rare Metals 工程技术-材料科学：综合

CiteScore

12.10

自引率

12.50%

发文量

2919

审稿时长

2.7 months

期刊介绍： Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.