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| 1 | Secondary-Atom-Doping Enables Robust Fe-N-C Single-Atom Catalysts with Enhanced Oxygen Reduction Reaction显示文摘Single-atom catalysts(SACs) with nitrogen-coordinated nonprecious metal sites have exhibited inimitable advantages in electrocatalysis.However,a large room for improving their activity and durability remains.Herein,we construct atomically dispersed Fe sites in N-doped carbon supports by secondary-atom-doped strategy.Upon the secondary doping,the density and coordination environment of active sites can be efficiently tuned,enabling the simultaneous improvement in the number and reactivity of the active site.Besides,structure optimizations in terms of the enlarged surface area and improved hydrophilicity can be achieved simultaneously.Due to the beneficial microstructure and abundant highly active FeN_5 moieties resulting from the secondary doping,the resultant catalyst exhibits an admirable half-wave potential of 0.81 V versus 0.83 V for Pt/C and much better stability than Pt/C in acidic media.This work would offer a general strategy for the design and preparation of highly active SACs for electrochemical energy devices. | Xin Luo Xiaoqian Wei Hengjia Wang Wenling Gu Takuma Kaneko Yusuke Yoshida Xiao Zhao Chengzhou Zhu | 2020 | Nano-Micro Letters2020,12,11: | 5 |
| 2 | Self-supported ternary Co0.5Mn0.5P/carbon cloth (CC) as a high-performance hydrogen evolution electrocatalyst显示文摘可伸缩的生产地球丰富,为氢进化反应的 easy-to-prepare,和划算的 electrocatalysts (她的) 为持续基于精力的系统是必要的。此处,我们系统地学习了 electrocatalytic 她 self-supported 的性能第三的公司 0.5 Mn 0.5 用热水的反应和 phosphorization 过程准备的 P/carbon 布(CC ) nanomaterial。电气化学的测试证明第三的公司 0.5 Mn 0.5 P/CC nanomaterial 能是在酸的媒介的高度活跃的 electrocatalyst 与仅仅 41 和 89 mV 的过电位,吗负担得起 10 和 100 妈的当前的密度?????昭汵敬敲敮愠汤祡牥????????????? 洠捡潲祣汣 吗?? | Xiaoyan Zhang Wenling Gu Erkang Wang | 2017 | Nano Research2017,10,3: | 5 |
| 3 | Genetic basis of high aroma and stress toleranee in the oolong tea cultivar genome显示文摘Tea plants(Camellia sinensis)are commercially cultivated in>60 countries,and their fresh leaves are processed into tea,which is the most widely consumed beverage in the world.Although several chromosome-level tea plant genomes have been published,they collapsed the two haplotypes and ignored a large number of allelic variations that may underlie important biological functions in this species.Here,we present a phased chromosome-scale assembly for an elite oolong tea cultivar,'Huangdan',that is well known for its high levels of aroma.Based on the two sets of haplotype genome data,we identi fi ed numerous genetic variations and a substantial proportion of allelic imbalance related to important traits,including aroma-and stress-related alleles.Comparative genomics revealed extensive structural variations as well as expansion of some gene families,such as terpene synthases(TPSs),that likely contribute to the high-aroma characteristics of the backbone parent,underlying the molecular basis for the biosynthesis of aroma-related chemicals in oolong tea.Our results uncovered the genetic basis of special features of this oolong tea cultivar,providing fundamental genomic resources to study evolution and domestication for the economically important tea crop. | Pengjie Wang Jiaxin Yu Shan Jin Shuai Chen Chuan Yue Wenling Wang Shuilian Gao Hongli Cao Yucheng Zheng Mengya Gu Xuejin Chen Yun Sun Yuqiong Guo Jiangfan Yang Xingtan Zhang Naixing Ye | 2021 | Horticulture Research2021,8,1: | 4 |
| 4 | 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 |
| 5 | Intestinal dysbiosis exacerbates the pathogenesis of psoriasis-like phenotype through changes in fatty acid metabolism显示文摘The intestinal microbiota has been associated with host immunity as well as psoriasis;however,the mechanism of intestinal microbiota regulating psoriasis needs to be demonstrated systematically.Here,we sought to examine its role and mechanism of action in the pathogenesis of psoriasis.We found that the severity of psoriasis-like skin phenotype was accompanied by changes in the composition of the intestinal microbiota.We performed co-housing and fecal microbial transplantation(FMT)experiments using the K14-VEGF transgenic mouse model of psoriasis and demonstrated that the transfer of intestinal microbiota from mice with severe psoriasis-like skin phenotype exacerbated psoriasiform skin inflammation in mice with mild symptoms,including increasing the infiltration and differentiation of Th17,and increased the abundance of Prevotella,while decreasing that of Parabacteroides distasonis,in the colon.These alterations affected fatty acid metabolism,increasing the abundance of oleic and stearic acids.Meanwhile,gentamicin treatment significantly reduced the abundance of Prevotella and alleviated the psoriasis-like symptoms in both K14-VEGF mice and imiquimod(IMQ)-induced psoriasis-like mice.Indeed,administration of oleic and stearic acids exacerbated psoriasis-like symptoms and increased Th17 and monocyte-derived dendritic cell infiltration in the skin lesion areas in vivo,as well as increased the secretion of IL-23 by stimulating DCs in vitro.At last,we found that,treatment of PDE-4 inhibitor alleviated psoriasis-like phenotype of K14-VEGF mice accompanied by the recovery of intestinal microbiota,including the decrease of Prevotella and increase of Parabacteroides distasonis.Overall,our findings reveal that the intestinal microbiota modulates host metabolism and psoriasis-like skin inflammation in mice,suggesting a new target for the clinical diagnosis and treatment of psoriasis. | Qixiang Zhao Jiadong Yu Hong Zhou Xiaoyan Wang Chen Zhang Jing Hu Yawen Hu Huaping Zheng Fanlian Zeng Chengcheng Yue Linna Gu Zhen Wang Fulei Zhao Pei Zhou Haozhou Zhang Nongyu Huang Wenling Wu Yifan Zhou Jiong Li | 2023 | Signal Transduction and Targeted Therapy2023,8,2: | 2 |
| 6 | 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 |
| 7 | 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 |
| 8 | Enhancement of the hydrogen evolution performance by finely tuning the morphology of Co-based catalyst without changing chemical composition显示文摘Transition-metal phosphides, as the promising alternatives to noble metal catalysts, have been widely used as efficient electrocatalysts for hydrogen evolution reaction (HER). In this work, three kinds of cobalt-8-hydroxyquinoline (Coqx) with different size and nanostructures are synthesized by varying the hydrothermal conditions, which was named as Coqx-L, Coqx-M and Coqx-S according to the decreased size. Accordingly, the CoxP/NC with three different size nanostructures (CoxP/NC-L, CoxP/NC-M and CoxP/NC-S) are obtained by the sequential carbonization and phosphidation of Coqx. The X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results imply the identical chemical composition in these catalysts with different morphologies. Thus, systematic study is carried out to reveal the relationship between catalytic performance and morphologies of materials with the same chemical composition. The experimental result indicates that the morphology of Cc)xP/NC plays a crucial role on the surface area and electron transfer. Finally, the catalyst of CoxP/NC-S with the smallest size nanostructrue exhibits the best HER performance with a low overpotential at current density of 10 mA/cm^2 (n = 56.9 and 115.6 mV) and a small Tafel slope (52.3 and 69.3 mV/dec) in both 0.1 M HCIO4 and 1.0M KOH as well as long-term stability. | Wenling Gu Liuyong Hu Changshuai Shang Jing Li Erkang Wang | 2019 | Nano Research2019,12,1: | 1 |
| 9 | 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 |
| 10 | 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 |
| 11 | 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 |
| 12 | Two antibodies show broad,synergistic neutralization against SARS-CoV-2 variants by inducing conformational change within the RBD显示文摘Continual evolution of the severe acute respiratory syndrome coronavirus(SARS-CoV-2)virus has allowed for its gradual evasion of neutralizing antibodies(nAbs)produced in response to natural infection or vaccination.The rapid nature of these changes has incited a need for the development of superior broad nAbs(bnAbs)and/or the rational design of an antibody cocktail that can protect against the mutated virus strain.Here,we report two angiotensin-converting enzyme 2 competing nAbs—8H12 and 3E2—with synergistic neutralization but evaded by some Omicron subvariants.Cryo-electron microscopy reveals the two nAbs synergistic neutralizing virus through a rigorous pairing permitted by rearrangement of the 472-489 loop in the receptor-binding domain to avoid steric clashing.Bispecific antibodies based on these two nAbs tremendously extend the neutralizing breadth and restore neutralization against recent variants including currently dominant XBB.1.5.Together,these findings expand our understanding of the potential strategies for the neutralization of SARS-CoV-2 variants toward the design of broad-acting antibody therapeutics and vaccines. | Hui Sun Tingting Deng Yali Zhang Yanling Lin Yanan Jiang Yichao Jiang Yang Huang Shuo Song Lingyan Cui Tingting Li Hualong Xiong Miaolin Lan Liqin Liu Yu Li Qianjiao Fang Kunyu Yu Wenling Jiang Lizhi Zhou Yuqiong Que Tianying Zhang Quan Yuan Tong Cheng Zheng Zhang Hai Yu Jun Zhang Wenxin Luo Shaowei Li Qingbing Zheng Ying Gu Ningshao Xia | 2024 | Protein & Cell2024,15,2: | 0 |
| 13 | 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 |