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Recent progress in single-atom nanozymes research

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Nano Research 2023年第2期16卷 1878-1889页

作者： Bing Jiang Zhanjun Guo Minmin Liang Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

single-atom nanozyme(SAzyme)is the hot topic of the current nanozyme research.Its intrinsic properties,such as high activity,stability,and low cost,present great substitutes to natural enzymes.Moreover,its fundamental characteristics,i.e.,maximized atom utilizations and well-defined geometric and electronic structures,lead to higher catalytic activities and specificity than traditional nanozymes.SAzymes have been applied in many biomedical areas,such as anti-tumor therapy,biosensing,antibiosis,and anti-oxidation therapy.Here,we will discuss a series of representative examples of SAzymes categorized by their biomedical applications in this review.In the end,we will address the future opportunities and challenges SAzymes facing in their designs and applications.

关键词： single-atom nanozymes natural enzymes enzyme-like activity biomedical applications

single-atom nanozymes towards central nervous system diseases

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Nano Research 2023年第4期16卷 5121-5139页

作者： Weichen Wei Department of Nanoengineering University of California San DiegoLa Jolla 92093USA

nanozymes have a similar catalytic mechanism to natural enzymes,with excellent performance,facile synthesis,and better stability.single-atom nanozymes are developed based on single-atom catalysts due to their advantages in coordination structure and electronic configuration,making them highly enzymatic-like biomimetic catalysts.Central nervous system(CNS)diseases have become one of the biggest killers of human health because they are difficult to diagnose and treat,expensive,and result in serious illness.single-atom nanozymes have been widely used for biomedical applications,especially in oxidative-stressinduced diseases and most CNS diseases which are closely related to oxidative stress.Therefore,single-atom nanozymes show promising application prospects for the treatment of CNS diseases.In addition,due to the outstanding material properties and sensitivity of single-atom nanozymes,they also exhibit great advantages in detecting various CNS disease markers for diagnosis.

关键词： single-atom nanozymes single-atom catalysis central nervous system diseases enzyme-like catalysts reactive oxygen species

single-atom nanozymes with axial ligand-induced self-adaptive conformation in alkaline medium boost chemiluminescence

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Science China Chemistry 2023年第3期66卷 904-912页

作者： Zhen Luo Liliang Tian Hengjia Wang Zhichao Wu Xin Luo Xiaosi Wang Lei Jiao Xiaoqian Wei Ying Qin Lirong Zheng Liuyong Hu Wenling Gu Le Shi Chengzhou Zhu Key Laboratory of Pesticides and Chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China State Key Laboratory of Electrical Insulation and Power Equipment Centre of Nanomaterials for Renewable EnergySchool of Electrical EngineeringXi’an Jiaotong UniversityXi’an 710049China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsWuhan Institute of TechnologyWuhan 430205China Fujian Shuikou Power Generation Group Corp. Fuzhou 350000China

Mimicking the structure of natural enzymes for designing advanced alternatives provides great opportunities to address the bottleneck of enzyme-involved chemiluminescence(CL). Herein, according to theoretical calculations, we found that an endogenous axial ligand of M-N-C single-atom nanozymes(SAzymes), originating from OH-spontaneously bonding to the metal center in an alkaline medium, can self-adaptively change its strength to facilitate intermediate steps. Furthermore, the lowest energy barrier of the rate-determining step and the strongest affinity and fastest electron transfer with luminol anion endow CoN-C with the highest peroxidase-like activity. Guided by the theoretical calculations, a series of M-N-C SAzymes(M=Fe, Co,Ni) were synthesized to boost CL, where Co-N-C SAzymes with superior catalytic activity and high selective generation of O_(2)·- were validated. As a proof-of-concept, Co-N-C SAzymes were employed for sensitive detection of acetylcholinesterase and organophosphorus pesticide.

关键词： single-atom nanozymes chemiluminescence hydrogen peroxide activation biosensing

Coordinatively unsaturated cobalt single-atom nanozymes for visual pesticides detection by smartphone-based platform

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Nano Research 2024年第4期17卷 2298-2307页

作者： Fangning Liu Zhe Li Hengya Wei Peng Xu Ge Kang Shicheng Zhu Tingting Wang Ruxue He Chuanxia Chen Yizhong Lu School of Materials Science and Engineering University of JinanJinan 250022China

By adjusting the coordination environment of single-atom catalysts,the enzyme-like activity can be finely tuned for highly sensitive biosensing.Herein,we demonstrated that coordinatively unsaturated cobalt-nitrogen sites doped within porous carbon(SA-CoN_(3))could serve as highly efficient oxidase mimic.Compared with the typical planar four-coordination structure(SA-CoN_(4)),the as-obtained single-atom Co nanozymes anchored by three nitrogen atoms are found to display much higher oxidase-like catalytic efficiency.Combined theoretical and experimental analysis revealed that the coordinatively unsaturated Co sites could facilitate adsorption and activation of O_(2) molecule and thus improve their oxidase-like activity.Based on the enhanced oxidase-like activity of SA-CoN_(3),a paper/smartphone sensor for organophosphorus pesticides(OPs)was successfully constructed and used to quantify glyphosate in environmental and food samples with a low detection limit of 0.66μM.This work not only highlights the important role of coordination unsaturation of SA nanozymes for promoting oxidase-like activity,but also provides an easy and cost-effective way to conduct effective quantification of OPs in the field.

关键词： single-atom nanozymes asymmetric organophosphorus pesticides oxygen adsorption smartphone

Dual-active-site Fe/Cu single-atom nanozymes with multifunctional specific peroxidase-like properties for S^(2-)detection and dye degradation

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Chinese Chemical Letters 2023年第6期34卷 267-272页

作者： Xiaofang Chen Ya Wang Min Feng Die Deng Xiaoyi Xie Caixia Deng Kashif Nawaz Khattak Xiupei Yang College of Chemistry and Chemical Engineering Chemical Synthesis and Pollution Control Key Laboratory of Sichuan ProvinceChina West Normal UniversityNanchong 637000China College of Environmental Science and Engineering China West Normal UniversityNanchong 637000China

Designing single-atom nanozymes with densely exposed metal atom active sites and enhancing catalytic activity to detect pollutants remain a serious challenge.Herein,we reported a single-atom nanozyme with layered stacked Fe/Cu dual active sites(Fe/Cu-NC SAzyme)synthesized via hydrothermal and hightemperature pyrolysis using folic acid as a template.Compared with Fe-NC and Cu-NC SAzyme,Fe/Cu-NC SAzyme has higher peroxidase-like activity,which indicates that the doping of synthesized Fe/Cu bimetals can improve the catalytic activity and that the atomic loading of Fe and Cu in Fe/Cu-NC is 5.5 wt%and 2.27 wt%,respectively.When S^(2-)is added to the Fe/Cu-NC catalytic system,a high-sensitivity and high-selectivity S^(2-)colorimetric sensing platform can be established,with a wide linear range(0.09-6μmol/L)and a low detection limit(30 nmol/L),which can be used to detect S^(2-)in environmental water samples.What’s more,the Fe/Cu-NC SAzyme can activate peroxymonosulfate(PMS)to degrade 99.9%of rhodamine B(Rh B)within 10 min with a degradation kinetics of 0.5943 min^(-1).This work details attractive applications in Fe/Cu-NC SAzyme colorimetric sensing and dye degradation.

关键词： single-atom nanozymes Dual active sites Peroxidase-like catalyst Colorimetric detection Dye degradation

Diatomic active sites nanozymes:Enhanced peroxidase-like activity for dopamine and intracellular H2O2 detection

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Nano Research 2022年第5期15卷 4266-4273页

作者： Shan Wang Zunfu Hu Qiulian Wei Huimin Zhang Weina Tang Yunqiang Sun Haiqiang Duan Zhichao Dai Qingyun Liu Xiuwen Zheng Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China School of Materials Science and Engineering Linyi UniversityLinyi 276000China

Considering intracellular hydrogen peroxide(H_(2)O_(2))plays pivotal roles in the regulation of serial biological processes,the in-situ detection of intracellular H2O2 has attracted an extensive attention.In the present work,an atomically dispersed diatomic active sites nanozymes(FeN_(3)/PtN_(4)-single-atom nanozymes(SAzyme))was prepared exhibiting enhanced peroxidase-like activity.The obvious synergistic effect between Fe-Pt heteronuclear diatomic active sites was confirmed by series of characterization and density functional theory(DFT).The peroxidase-like activity of Fe-sites could be substantially enhanced by the bonded Pt-sites via the modulation effect.As a consequence,the gap between the d-band centre(εd)of Fe 3d orbitals and the Fermi energy level was narrowed and the electronic interaction could be strengthened,leading to a lower free energy barrier and a lower activation energy as well as fortified metal-O bonding in the kinetic pathway.Therefore,the constructed FeN3/PtN4-SAzyme exhibited higher peroxidase-like activity than that of FeN4-SAzyme.The FeN3/PtN4-SAzyme-assisted oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)facilitated the colorimetric detection of dopamine(DA),an important biomolecule.The linear detection range and limit of detection(LOD)of DA and H_(2)O_(2) were 1-10 μM,0.01-1.0 mM and 0.109 μM,7.97 μM,respectively.In addition,the constructed SAzymes were also applied for the in-situ detection of intracellular H2O2,expanding the application scope of the newborn SAzymes.

关键词： single-atom nanozymes heteronuclear diatomic active sites peroxidase-like dopamine intracellular H_(2)O_(2)