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| 1 | Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase‑Like Activity for Sensitive Biosensing显示文摘Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges.Herein,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites.Benefiting from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like activity.As a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1.Moreover,the detection of organophosphorus pesticides was also achieved.This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors. | Weiqing Xu Yikun Kang Lei Jiao Yu Wu Hongye Yan Jinli Li Wenling Gu Weiyu Song Chengzhou Zhu | 2020 | Nano-Micro Letters2020，12，12： | 4 |
| 2 | Atomically dispersed N-coordinated Fe-Fe dual-sites with enhanced enzyme-like activities显示文摘Replacement of enzymes with nanomaterials such as atomically dispersed metal catalysts is one of the most crucial steps in addressing the challenges in biocataiysis.Despite the breakthroughs of single-atom catalysts in enzyme-mimicking,a fundamental investigation on the development of an instructional strategy is still required for mimicking biatomic/multiatomic active sites in natural enzymes and constructing synergistically enhanced metal atom active sites.Herein,Fe_(2)NC catalysts with atomically dispersed Fe-Fe dual-sites supported by the metal-organic frameworks-derived nitrogen-doped carbon are employed as biomimetic catalysts to perform proof-of-concept investigation.The effect of Fe atom number toward typical oxidase(cytochrome C oxidase,NADH oxidase,and ascorbic acid oxidase)and peroxidase(NADH peroxidase and ascorbic acid peroxidase)activities is systematically evaluated by experimental and theoretical investigations.A peroxo-like O_(2) adsorption in Fe_(2)NC nanozymes could accelerate the O-O activation and thus achieve the enhanced enzyme-like activities.This work achieves the vivid simulation of the enzyme active sites and provides the theoretical basis for the design of high-performance nanozymes.As a concept application,a colorimetric biosensor for the detection of S^(2-) in tap water is established based on the inhibition of enzyme-like activity of Fe_(2)NC nanozymes. | Lei Jiao Wei Ye Yikun Kang Yu Zhang Weiqing Xu Yu Wu Wenling Gu Weiyu Song Yujie Xiong Chengzhou Zhu | 2022 | Nano Research2022，15，2： | 1 |
| 3 | Defect-rich and ultrathin nitrogen-doped carbon nanosheets with enhanced peroxidase-like activity for the detection of urease activity and fluoride ion显示文摘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. | Yu Zhang Lei Jiao Weiqing Xu Yifeng Chen Yu Wu Hongye Yan Wenling Gu Chengzhou Zhu | 2022 | Chinese Chemical Letters2022，33，3： | 1 |
| 4 | Metal atom doping-induced S-scheme heterojunction boosts the photoelectric response显示文摘Carrier migration path and driving forces are two crucial factors for charge separation of heterojunction with efficient photoelectric response from the thermodynamic and kinetic perspectives,respectively.Constructing the S-scheme heterojunction and achieving an efficient migration path for space charge separation have aroused great interest,while a thorough insight into tuning interfacial band bending for S-scheme heterojunction is absent.Herein,we report a class of Zn atom-doped CeO_(2)/g-C_(3)N_(4) heterostructure for achieving a new carrier migration path conversion from inferior type-II to advanced S-scheme.Zn-dependent volcano-type plot for Zn-CeO_(2) is established to tune the Fermi level of CeO_(2).The built-in electric field for carrier flow dynamics strengthens when coupling with g-C_(3)N_(4),which significantly boosts the photoelectric response.Based on the intrinsic enzymelike activity of Zn-CeO_(2),we further demonstrate that the Zn-CeO_(2)/g-C_(3)N_(4) S-scheme heterojunction can be explored for constructing a sensitive nanozymatic photoelectrochemical biosensor for the detection of acetylcholinesterase. | Mingwang Liu Jing Wen Ying Qin Jinli Li Yinjun Tang Lei Jiao Yu Wu Qie Fang Lirong Zheng Xiaowen Cui Wenling Gu Chengzhou Zhu Liuyong Hu Shaojun Guo | 2023 | Science China Chemistry2023，66，4： | 0 |
| 5 | Knockdown of PGC1α suppresses dysplastic oral keratinocytes proliferation through reprogramming energy metabolism显示文摘Oral potentially malignant disorders(OPMDs)are precursors of oral squamous cell carcinoma(OSCC).Deregulated cellular energy metabolism is a critical hallmark of cancer cells.Peroxisome proliferator-activated receptor-gamma coactivator-1 alpha(PGC1α)plays vital role in mitochondrial energy metabolism.However,the molecular mechanism of PGC1αon OPMDs progression is less unclear.Therefore,we investigated the effects of knockdown PGC1αon human dysplastic oral keratinocytes(DOKs)comprehensively,including cell proliferation,cell cycle,apoptosis,xenograft tumor,mitochondrial DNA(mtDNA),mitochondrial electron transport chain complexes(ETC),reactive oxygen species(ROS),oxygen consumption rate(OCR),extracellular acidification rate(ECAR),and glucose uptake.We found that knockdown PGC1αsignificantly inhibited the proliferation of DOKs in vitro and tumor growth in vivo,induced S-phase arrest,and suppressed PI3K/Akt signaling pathway without affecting cell apoptosis.Mechanistically,downregulated of PGC1αdecreased mtDNA,ETC,and OCR,while enhancing ROS,glucose uptake,ECAR,and glycolysis by regulating lactate dehydrogenase A(LDHA).Moreover,SR18292(an inhibitor of PGC1α)induced oxidative phosphorylation dysfunction of DOKs and declined DOK xenograft tumor progression.Thus,our work suggests that PGC1αplays a crucial role in cell proliferation by reprograming energy metabolism and interfering with energy metabolism,acting as a potential therapeutic target for OPMDs. | Yunkun Liu Nengwen Huang Xianghe Qiao Zhiyu Gu Yongzhi Wu Jinjin Li Chengzhou Wu Bo Li Longjiang Li | 2023 | International Journal of Oral Science2023，15，3： | 0 |
| 6 | Single-atom nanozymes with axial ligand-induced self-adaptive conformation in alkaline medium boost chemiluminescence显示文摘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. | 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 | 2023 | Science China Chemistry2023，66，3： | 0 |
| 7 | Fine-Tuning Pyridinic Nitrogen in Nitrogen-Doped Porous Carbon Nanostructures for Boosted Peroxidase-Like Activity and Sensitive Biosensing显示文摘Carbon materials have been widely used as nanozymes in bioapplications,attributing to their intrinsic enzyme-like activities.Nitrogen(N)-doping has been explored as a promising way to improve the activity of carbon material-based nanozymes(CMNs).However,hindered by the intricate N dopants,the real active site of N-doped CMNs(N-CMNs)has been rarely investigated,which subsequently retards the further progress of high-performance N-CMNs.Here,a series of porous N-CMNs with well-controlled N dopants were synthesized,of which the intrinsic peroxidase(POD)like activity has a positive correlation with the pyridinic N content.Density functional theory calculations also reveal that pyridinic N boosts the intrinsic POD-like activity of N-CMNs.Pyridinic-N dopant can effectively promote the first H_(2)O desorption process in comparison with the graphitic and pyrrolic N,which is the key endothermic reaction during the catalytic process.Then,utilizing the optimized nanozymes with high pyridinic N content(NP-CMNs)and superior POD-like activity,a facile total antioxidant capacity(TAC)assay was developed,holding great promise in the quality assessment of medicine tablets and antioxidant food for healthcare and healthy diet. | Hongye Yan Linzhe Wang Yifeng Chen Lei Jiao Yu Wu Weiqing Xu Wenling Gu Weiyu Song Dan Du Chengzhou Zhu | 2020 | Research2020，，1： | 0 |
| 8 | Protein trap-engineered metal-organic frameworks for advanced enzyme encapsulation and mimicking显示文摘Immobilizing enzymes within metal-organic frameworks(MOFs)enables enzymes to against extreme environments.However,these MOF shells are just like armors,protective but heavy,which shield the enzymes from threats while locking them in the cage.The exploitation of immobilization strategy and intrinsic property of MOFs themselves is of great significance.Here,we proposed a functional protein trap strategy for efficient enzyme encapsulation.The ferrocenedicarboxylic acid(Fc)was used to induce the formation of defect-rich Co-based MOFs(CoBDC-Fc).As result,the engineered protein trap can not only improve the enzyme loading but also accelerate catalytic efficiency.Specifically,the atomically dispersed Fc sites serve as cocatalysts/cofactors and even change the conformation of enzymes in the construed microenvironment.Furthermore,the obtained CoBDC-Fc/enzyme exhibits excellent recyclability and tolerance to inhospitable conditions.Benefited by these,the CoBDC-Fc/enzyme/antigen composites were further prepared for cascade enzyme-linked immunosorbent assay of prostate-specific antigen with satisfactory sensitivity. | Weiqing Xu Yu Wu Lei Jiao Meng Sha Xiaoli Cai Yating Wen Yifeng Chen Wenling Gu Chengzhou Zhu | 2023 | Nano Research2023，16，2： | 0 |
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