Plant alkaloids,renowned for their structural diversity and bioactivity,are prominent in both modern and traditional medicine[1].Unraveling the intricacies of plant alkaloid biosynthesis could pave the way for the dis...Plant alkaloids,renowned for their structural diversity and bioactivity,are prominent in both modern and traditional medicine[1].Unraveling the intricacies of plant alkaloid biosynthesis could pave the way for the discovery of new natural products and pathways.It may also shed light on the roles of existing pathways in host biology and provide valuable tools for metabolic engineering in plants and microbes[2].Unlike other major classes of plant natural products,such as terpenoids and polyketides,the formation of alkaloid scaffolds does not conform to a uniform chemical theme or depend on a singular enzyme class[3].A case in point is the Lycopodium alkaloids in the Lycopodiaceae family,where the enzymes responsible for their core scaffold construction remain unidentified[4].展开更多
Nanozymes are nanomaterials with enzyme-like properties that have attracted significant interest owing to their capability to address the limitations of traditional enzymes such as fragility,high cost,and impossible m...Nanozymes are nanomaterials with enzyme-like properties that have attracted significant interest owing to their capability to address the limitations of traditional enzymes such as fragility,high cost,and impossible mass production.Over the past decade,a broad variety of nanomaterials have been found to mimic the enzyme-like activity by engineering the active centers of natural enzymes or developing multivalent elements within nanostructures.Carbon nanomaterials with well-defined electronic and geometric structures have served as favorable surrogates of traditional enzymes by mimicking the highly evolved catalytic center of natural enzymes.In particular,by combining the unique electronic,optical,thermal,and mechanical properties,carbon nanomaterials-based nanozymes can offer a variety of multifunctional platforms for biomedical applications.In this review,we will introduce the enzymatic characteristics and recent advances of carbon nanozymes,and summarize their significant applications in biomedicine.展开更多
Pathogenic bacteria pose a devastating threat to public health.However,because of the growing bacterial antibiotic resistance,there is an urgent need to develop alternative antibacterial strategies to the established ...Pathogenic bacteria pose a devastating threat to public health.However,because of the growing bacterial antibiotic resistance,there is an urgent need to develop alternative antibacterial strategies to the established antibiotics.Herein,iron-doped carbon dots(Fe-CDs,~3 nm)nanozymes with excellent photothermal conversion and photoenhanced enzyme-like properties are developed through a facile one-pot pyrolysis approach for synergistic efficient antibacterial therapy and wound healing.In particular,Fe doping endows CDs with photoenhanced peroxidase(POD)-like activity,which lead to the generation of heat and reactive oxygen species(ROS)for Gram-positive and Gram-negative bacteria killing.This study demonstrates Fe-CDs have significant wound healing efficiency of Fe-CDs by preventing infection,promoting fibroblast proliferation,angiogenesis,and collagen deposition.Furthermore,the ultrasmall size of Fe-CDs possesses good biocompatibility favoring clinical translation.We believe that the nanozyme-mediated therapeutic platform presented here is expected to show promising applications in antibacterial.展开更多
Nanozymes are nanomaterials with enzyme-like activities that efficiently overcome the drawbacks of natural enzymes in biosensing,detection,and biomedical fields,and they are the most widely used artificial enzymes.Owi...Nanozymes are nanomaterials with enzyme-like activities that efficiently overcome the drawbacks of natural enzymes in biosensing,detection,and biomedical fields,and they are the most widely used artificial enzymes.Owing to their excellent catalytic characteristics,biocompatibility,and environmental favorability,carbondots-based(CDs) nanozymes have inspired a research upsurge.However,no review focusing on CDs nanozymes has been published,even though substantial advances have been achieved.Herein,the advances,catalytic activities,and applications of CDs nanozymes are highlighted and summarized.In addition,the critical issues and challenges of researching nanozymes are discussed.We hope that this review will broaden the horizons of nanozymes and CDs nanozymes,as well as promote their development.展开更多
It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design o...It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design of nanomaterials as enzyme mimics.Hereby,N,S-rich carbonized wool nanosheets(CWs)were synthesized at different pyrolysis temperatures.As expected,only CWs treated with high-temperature possess intrinsic oxidase-and peroxidase-like activities.Meanwhile,density functional theory(DFT)calculations demonstrate that graphitic nitrogen and the co-existence of nitrogen and sulfur in the carbon matrix serve as the active sites for the enzyme-like process.More importantly,combining theoretical calculations and experimental observations,the high-temperature triggered catalytic mechanism can be ascribed to the fact that an appropriate high-temperature maximizes the graphitization degree to a certain extent,at which most of the catalytic active sites are well retained rather than evaporating.Moreover,coupling with excellent photothermal conversion efficiency and catalytic performance,CWs can be applied to photothermal-catalytic cancer therapy under near-infrared region(NIR)light irradiation.We believe this work will contribute to understanding the catalytic mechanism of carbon-based nanozymes and promote the development of new biomedical and pharmaceutical applications.展开更多
Carbon-based nanozymes with multifunctional applications have attracted enormous attention,however,there is still a lack of an effective strategy for inexpensive preparation of high-active carbon-based nanozyme.We her...Carbon-based nanozymes with multifunctional applications have attracted enormous attention,however,there is still a lack of an effective strategy for inexpensive preparation of high-active carbon-based nanozyme.We herein report a waste paperderived CoFe_(2)O_(4)/porous carbon nanozyme for the colorimetric detection of glucose and glutathione(GSH)in biofluids.The hybrid CoFe_(2)O_(4)/porous carbon material was successfully prepared via a combined impregnation,hydrolysis and carbonization method.Newly constructed CoFe_(2)O_(4)/porous carbon material with enhanced peroxidase-like activity could oxidize colorless tetramethylbenzidine(TMB)to blue oxidized TMB with adding H_(2)O_(2).A sensitive colorimetric analysis platform for monitoring the levels of glucose and GSH in biofluids was respectively developed.The proposed analytical method possessed predominant features such as low limit of detections(LODs)(0.16μmol/L for glucose and 120 nmol/L for GSH),broad linear ranges(1-200μmol/L for glucose and 1-50μmol/L for GSH),and excellent practical potential.This multipurpose platform not only provides a promising strategy for transforming waste paper into valuable carbon-based nanozyme,but also paves the way for excavating the potential biomedical and environmental applications from waste paper.展开更多
Although carbon nanozymes have attracted great interest due to their good biocompatibility, low cost,and high stability, designing high-active carbon nanozymes still faces great challenges. Herein, ultrathin nitrogen-...Although carbon nanozymes have attracted great interest due to their good biocompatibility, low cost,and high stability, designing high-active carbon nanozymes still faces great challenges. Herein, ultrathin nitrogen-doped carbon nanosheets with rich defects(d-NC) were prepared through a high-temperature annealing process, using potassium chloride and ammonium chloride as templates. Owing to the large specific surface area, rich defects and the high exposure of active sites, the proposed d-NC nanozymes exhibited excellent peroxidase-like activity. The d-NC nanozymes possess maximal reaction velocity and their specific activity is 9.4-fold higher than that of nitrogen-doped carbon nanozymes, indicating that the induced defects can boost the catalytic performance. Benefited from the good peroxidase-like activities of d-NC nanozymes, the colorimetric sensing platforms were constructed for the detection of urease activity and fluoride ion, exhibiting satisfactory stability and selectivity. This study not only offers a way to synthesize carbon nanozymes with improved enzyme-like activities but also broadens their applications in colorimetric biosensing.展开更多
Nanozymes have become attractive in analytical and biomedical fields,mainly because of their low cost,long shelf life,and less environmental sensitivity.Particularly,nanozymes formed from nanomaterials having high sur...Nanozymes have become attractive in analytical and biomedical fields,mainly because of their low cost,long shelf life,and less environmental sensitivity.Particularly,nanozymes formed from nanomaterials having high surface area and rich active sites are interesting since their activities can be tuned through carefully controlling their size,morphology,and surface properties.This review article focuses on preparation of carbon dots(C dots)possessing peroxidase-like activity and their analytical applications.We highlight the important roles of the oxidation states and surface residues of C dots and their nanocomposites with metal,metal oxides,or metal sulfides playing on determining their specificity and sensitivity toward H2O2.Examples of C dot nanozymes(CDzymes)for developing sensitive and selective absorption,fluorescence,and elec-trochemical sensing systems in the presence of substrates are presented to show their potential in analytical applications.For example,CDzymes couple with glucose oxidase and cholesterol oxidase are specific and sensitive for quantitation of glucose and cholesterol,separately,when using 3,3′,5,5′-tetramethylbenzidine(TMB)as the signal probe.This review article concludes with possible strategies for enhancing and tuning the catalytic activity of CDzymes.展开更多
文摘Plant alkaloids,renowned for their structural diversity and bioactivity,are prominent in both modern and traditional medicine[1].Unraveling the intricacies of plant alkaloid biosynthesis could pave the way for the discovery of new natural products and pathways.It may also shed light on the roles of existing pathways in host biology and provide valuable tools for metabolic engineering in plants and microbes[2].Unlike other major classes of plant natural products,such as terpenoids and polyketides,the formation of alkaloid scaffolds does not conform to a uniform chemical theme or depend on a singular enzyme class[3].A case in point is the Lycopodium alkaloids in the Lycopodiaceae family,where the enzymes responsible for their core scaffold construction remain unidentified[4].
基金This work was supported by China Postdoctoral Science Foundation(Nos.2019T120754 and 2018M633229)Sanming Project of Medicine in Shenzhen(No.SZSM201612031)+4 种基金Natural Science Foundation of Guangdong Province of China(Nos.2018A030310665 and 2018A0303130295)Shenzhen Science and Technology Innovation Committee(Nos.ZDSYS201707281114196,JCYJ20170306091657539,JCYJ20170413162242627,JCYJ20190806163814395,JCYJ-20170306091452714,and GJHZ20170313172439851)Development and Reform Commission of Shenzhen Municipality(No.S2016005470013)National Key R&D Program of China(No.2017YFA0205501)the National Natural Science Foundation of China(Nos.81722024 and 81571728).
文摘Nanozymes are nanomaterials with enzyme-like properties that have attracted significant interest owing to their capability to address the limitations of traditional enzymes such as fragility,high cost,and impossible mass production.Over the past decade,a broad variety of nanomaterials have been found to mimic the enzyme-like activity by engineering the active centers of natural enzymes or developing multivalent elements within nanostructures.Carbon nanomaterials with well-defined electronic and geometric structures have served as favorable surrogates of traditional enzymes by mimicking the highly evolved catalytic center of natural enzymes.In particular,by combining the unique electronic,optical,thermal,and mechanical properties,carbon nanomaterials-based nanozymes can offer a variety of multifunctional platforms for biomedical applications.In this review,we will introduce the enzymatic characteristics and recent advances of carbon nanozymes,and summarize their significant applications in biomedicine.
基金supported by the National Natural Science Foundation of China(NO.21822802,51772018,and 22061130205)National Key Research and Development Program of China(NO.2016YFA0201500 and 2018YFC1200100)Fundamental Research Funds for the Central Universities(NO.XK1802-8 and buctrc201915).
文摘Pathogenic bacteria pose a devastating threat to public health.However,because of the growing bacterial antibiotic resistance,there is an urgent need to develop alternative antibacterial strategies to the established antibiotics.Herein,iron-doped carbon dots(Fe-CDs,~3 nm)nanozymes with excellent photothermal conversion and photoenhanced enzyme-like properties are developed through a facile one-pot pyrolysis approach for synergistic efficient antibacterial therapy and wound healing.In particular,Fe doping endows CDs with photoenhanced peroxidase(POD)-like activity,which lead to the generation of heat and reactive oxygen species(ROS)for Gram-positive and Gram-negative bacteria killing.This study demonstrates Fe-CDs have significant wound healing efficiency of Fe-CDs by preventing infection,promoting fibroblast proliferation,angiogenesis,and collagen deposition.Furthermore,the ultrasmall size of Fe-CDs possesses good biocompatibility favoring clinical translation.We believe that the nanozyme-mediated therapeutic platform presented here is expected to show promising applications in antibacterial.
基金supported by the National Natural Science Foundation of China (Nos.21974125, 21708035)the Collaborative Innovation Project of Zhengzhou (Zhengzhou University)(No.18XTZX12002)the 111 Project (No.D20003)。
文摘Nanozymes are nanomaterials with enzyme-like activities that efficiently overcome the drawbacks of natural enzymes in biosensing,detection,and biomedical fields,and they are the most widely used artificial enzymes.Owing to their excellent catalytic characteristics,biocompatibility,and environmental favorability,carbondots-based(CDs) nanozymes have inspired a research upsurge.However,no review focusing on CDs nanozymes has been published,even though substantial advances have been achieved.Herein,the advances,catalytic activities,and applications of CDs nanozymes are highlighted and summarized.In addition,the critical issues and challenges of researching nanozymes are discussed.We hope that this review will broaden the horizons of nanozymes and CDs nanozymes,as well as promote their development.
基金funded by the National Natural Science Foundation of China(Nos.12274356,22275081)Key Laboratory of Pharmaceutical Analysis and Laboratory Medicine(Putian University)(No.PALM 202206)+1 种基金Fujian Province University,the Fundamental Research Funds for the Central Universities(No.20720220022)the 111 Project(No.B16029)。
文摘It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design of nanomaterials as enzyme mimics.Hereby,N,S-rich carbonized wool nanosheets(CWs)were synthesized at different pyrolysis temperatures.As expected,only CWs treated with high-temperature possess intrinsic oxidase-and peroxidase-like activities.Meanwhile,density functional theory(DFT)calculations demonstrate that graphitic nitrogen and the co-existence of nitrogen and sulfur in the carbon matrix serve as the active sites for the enzyme-like process.More importantly,combining theoretical calculations and experimental observations,the high-temperature triggered catalytic mechanism can be ascribed to the fact that an appropriate high-temperature maximizes the graphitization degree to a certain extent,at which most of the catalytic active sites are well retained rather than evaporating.Moreover,coupling with excellent photothermal conversion efficiency and catalytic performance,CWs can be applied to photothermal-catalytic cancer therapy under near-infrared region(NIR)light irradiation.We believe this work will contribute to understanding the catalytic mechanism of carbon-based nanozymes and promote the development of new biomedical and pharmaceutical applications.
基金supported by the Science and Technology Innovation Special Fund of Xuzhou,China(KC21292)Special fund for Science and Technology Project of Jiangsu Province,China(BE2022715)+1 种基金Outstanding Talents Research Start-up Fund of Xuzhou Medical University,China(D2021003)Integrated Innovation Project of Xuzhou Medical University,China(XYRHCX2021017)
文摘Carbon-based nanozymes with multifunctional applications have attracted enormous attention,however,there is still a lack of an effective strategy for inexpensive preparation of high-active carbon-based nanozyme.We herein report a waste paperderived CoFe_(2)O_(4)/porous carbon nanozyme for the colorimetric detection of glucose and glutathione(GSH)in biofluids.The hybrid CoFe_(2)O_(4)/porous carbon material was successfully prepared via a combined impregnation,hydrolysis and carbonization method.Newly constructed CoFe_(2)O_(4)/porous carbon material with enhanced peroxidase-like activity could oxidize colorless tetramethylbenzidine(TMB)to blue oxidized TMB with adding H_(2)O_(2).A sensitive colorimetric analysis platform for monitoring the levels of glucose and GSH in biofluids was respectively developed.The proposed analytical method possessed predominant features such as low limit of detections(LODs)(0.16μmol/L for glucose and 120 nmol/L for GSH),broad linear ranges(1-200μmol/L for glucose and 1-50μmol/L for GSH),and excellent practical potential.This multipurpose platform not only provides a promising strategy for transforming waste paper into valuable carbon-based nanozyme,but also paves the way for excavating the potential biomedical and environmental applications from waste paper.
基金financial support of the National Natural Science Foundation of China (Nos. 22074049 and22004042)the Fundamental Research Funds for the Central Universities (Nos. CCNU20QN007 and CCNU20TS013)the Program of Introducing Talents of Discipline to Universities of China (111program, No. B17019)。
文摘Although carbon nanozymes have attracted great interest due to their good biocompatibility, low cost,and high stability, designing high-active carbon nanozymes still faces great challenges. Herein, ultrathin nitrogen-doped carbon nanosheets with rich defects(d-NC) were prepared through a high-temperature annealing process, using potassium chloride and ammonium chloride as templates. Owing to the large specific surface area, rich defects and the high exposure of active sites, the proposed d-NC nanozymes exhibited excellent peroxidase-like activity. The d-NC nanozymes possess maximal reaction velocity and their specific activity is 9.4-fold higher than that of nitrogen-doped carbon nanozymes, indicating that the induced defects can boost the catalytic performance. Benefited from the good peroxidase-like activities of d-NC nanozymes, the colorimetric sensing platforms were constructed for the detection of urease activity and fluoride ion, exhibiting satisfactory stability and selectivity. This study not only offers a way to synthesize carbon nanozymes with improved enzyme-like activities but also broadens their applications in colorimetric biosensing.
基金We are grateful to the Ministry of Science and Technology(MOST)of Taiwan for providing financial support for this study under contracts 107-2113-M-002-015-MY3,and MOST 107-2113-M-018-005.
文摘Nanozymes have become attractive in analytical and biomedical fields,mainly because of their low cost,long shelf life,and less environmental sensitivity.Particularly,nanozymes formed from nanomaterials having high surface area and rich active sites are interesting since their activities can be tuned through carefully controlling their size,morphology,and surface properties.This review article focuses on preparation of carbon dots(C dots)possessing peroxidase-like activity and their analytical applications.We highlight the important roles of the oxidation states and surface residues of C dots and their nanocomposites with metal,metal oxides,or metal sulfides playing on determining their specificity and sensitivity toward H2O2.Examples of C dot nanozymes(CDzymes)for developing sensitive and selective absorption,fluorescence,and elec-trochemical sensing systems in the presence of substrates are presented to show their potential in analytical applications.For example,CDzymes couple with glucose oxidase and cholesterol oxidase are specific and sensitive for quantitation of glucose and cholesterol,separately,when using 3,3′,5,5′-tetramethylbenzidine(TMB)as the signal probe.This review article concludes with possible strategies for enhancing and tuning the catalytic activity of CDzymes.
