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Combatting Pathogenic Bacteria with synthetic Immunotherapeutics from Chitosan:Antibody Recruiting at Engineered Bacterial Surface with Peptidoglycan Analogs

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CCS chemistry 2024年第6期6卷 1448-1457页

作者： Yuan Xu Shihao Song Hongwei Duan Yinyue Deng Xue-Wei Liu School of chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingapore 637371 key laboratory of Tropical Biological Resources of Ministry of Education School of Pharmaceutical SciencesHainan UniversityHaikou 570228 School of Pharmaceutical Sciences(Shenzhen) Shenzhen Campus of Sun Yat-sen UniversitySun Yat-sen UniversityShenzhen 518107

The emergence of microbial drug resistance,coupled with the paucity of new antibiotics poses an impending threat to public health.In this work,we drew inspiration from synthetic peptidoglycan oligomers and successfully constructed antibody-recruiting peptidoglycan analogs,2a-d,with excellent safety profiles and high efficiencies in recruiting antibodies across different conditions.Further,we demonstrated that these peptidoglycan analogs could be readily incorporated into bacteria cell walls,whereby both simple monoclonal and pooled human serum antibodies effectively congregated to the surfaceengineered bacteria,leading to the complete extermination of the engineered bacterial cells both in vitro and in vivo.Our peptidoglycan analog agents for recruiting endogenous antibodies to combat pathogenic bacteria enable further development of promising broad-spectrum immunotherapeutics.

关键词： chitosan bacterial infection endogenous antibodies bacterial surface engineering peptidoglycan analogs

Atomically Dispersed Dual‑Metal Sites Showing Unique Reactivity and Dynamism for Electrocatalysis

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Nano-Micro Letters 2023年第8期15卷 192-204页

作者： Jun‑Xi Wu Wen‑Xing Chen Chun‑Ting He Kai Zheng Lin‑Ling Zhuo Zhen‑Hua Zhao Jie‑Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275People’s Republic of China key Lab of Fluorine and Silicon for Energy Materials and chemistry of Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022People’s Republic of China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China

The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst.Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water splitting.More importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH groups.Density functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.

关键词： Metal-organic frameworks Atomically dispersed catalyst Hydrogen bond Overall water splitting

Acidic open-cage solution containing basic cage-confined nanospaces for multipurpose catalysis

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National Science Review 2022年第5期9卷 99-107页

作者： Kang Li Kai Wu Yan-Zhong Fan Jing Guo Yu-Lin Lu Yuan-Fan Wang Guillaume Maurin Cheng-Yong Su moe laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen University School of chemistry South China Normal University Institute Charles Gerhardt Montpellier Centre National de la Recherche Scientifiqueécole Nationale Supérieure de Chimie de MontpellierUniversité de Montpellier

The nanoscale chemical spaces inherent in porous organic/coordination cages or solid/liquid materials have been continuously explored for their nanoconfinement effect on selective adsorption and reaction of small gas or organic molecules.Herein,we aim to rationalize the unconventional chemical reactivities motivated by the cage-confined nanospaces in aqueous solutions,where the robust yet permeable nanospaces defined by the open cages facilitate dynamic guest exchange and unusual chemical reactions.The high positive charges on [(Pd/Pt)6(RuL3)8]28+nanocages drive imidazole-proton equilibrium to display a significantly perturbed pKashift,creating cage-defined nanospaces in solution with distinct intrinsic basicity and extrinsic acidity.The supramolecular cage effect plays pivotal roles in elaborating robust solution nanospaces,controlling ingress-and-egress molecular processes through open-cage portals and endowing nanocages with transition-state stabilization,amphoteric reactivities and the phase transfer of insoluble molecules,thus promoting chemical transformations in unconventional ways.Consequently,a wide range of application of cage-confined catalysis with anomalous reactivities maybe expected based on this kind of open-cage solution medium,which combines cage nanocavity,solution heterogeneity and liquid-phase fluidity to benefit various potential mass transfer and molecular process options.

关键词： open-cage solution supramolecular cage effect supramolecular catalysis cage-confined catalysis cage-confined nanospaces in solution

A Conductive Dinuclear Cuprous Complex Mimicking the Active Edge Site of the Copper(100)/(111)Plane for Selective Electroreduction of CO_(2) to C_(2)H_(4) at Industrial Current Density

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Research 2023年第2期2022卷 343-349页

作者： Jin-Meng Heng Hao-Lin Zhu Zhen-Hua Zhao Da-Shuai Huang Jun-Yi Li Pei-Qin Liao Xiao-Ming Chen moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Inorganic solids are a kind of important catalysts,and their activities usually come from sparse active sites,which are structurally different from inactive bulk.Therefore,the rational optimization of activity depends on studying these active sites.Copper is a widely used catalyst and is expected to be a promising catalyst for the electroreduction of CO_(2) to C_(2)H_(4).

关键词： Copper catalyst rational

Flexibility of Metal-Organic Framework Tunable by Crystal Size at the Micrometer to Submillimeter Scale for Efficient Xylene Isomer Separation

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Research 2019年第1期2019卷 433-441页

作者： Xiao Yang Hao-Long Zhou Chun-Ting He Zong-Wen Mo Jia-Wen Ye Xiao-Ming Chen Jie-Peng Zhang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Understanding,controlling,and utilizing the flexibility of adsorbents are of great importance and difficulty.Analogous with conventional solid materials,downsizing to the nanoscale is emerging as a possible strategy for controlling the flexibility of porous coordination polymers(or metal-organic frameworks).We report a unique flexibility controllable by crystal size at the micrometer to submillimeter scale.Template removal transforms[Cu_(2)(pypz)_(2)]·0.5p-xylene(MAF-36,Hpypz=4-(1H-pyrazol-4-yl)pyridine)with one-dimensional channels toα-[Cu_(2)(pypz)_(2)]with discrete small cavities,and further heating gives a nonporous isomerβ-[Cu_(2)(pypz)_(2)].Both isomers can adsorb p-xylene to give[Cu_(2)(pypz)_(2)]·0.5p-xylene,meaning the coexistence of guest-driven flexibility and shape-memory behavior.The phase transition temperature fromα-[Cu_(2)(pypz)_(2)]toβ-[Cu_(2)(pypz)_(2)]decreased from~270℃ to~150℃ by increasing the crystal size from the micrometer to the submillimeter scale,ca.2-3 orders larger than those of other size-dependent behaviors.Single-crystal X-ray diffraction showed coordination bond reconstitution and chirality inversion mechanisms for the phase transition,which provides a sufficiently high energy barrier to stabilize the metastable phase without the need of downsizing to the nanoscale.By virtue of the crystalline molecular imprinting and gate-opening effects,α-[Cu_(2)(pypz)_(2)]andβ-[Cu_(2)(pypz)_(2)]show unprecedentedly high p-xylene selectivities of 16 and 51,respectively,as well as ultrafast adsorption kinetics(<2 minutes),for xylene isomers.

关键词： isomers coordination adsorbent

构建三元WO_(3)/CsPbBr_(3)/ZIF-67异质结用于高效光催化CO_(2)还原

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Science China Materials 2022年第6期65卷 1550-1559页

作者：董玉杰江勇廖金凤陈洪燕匡代彬苏成勇 moe key laboratory of bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于... 详细信息

近年来,卤素钙钛矿纳米材料以其优异的光电性能在光催化等领域引起了关注.然而,光生载流子严重的复合反应和较差的反应动力学也极大地限制了其光催化性能.本论文设计合成了一种三元WO_(3)/CsPbBr_(3)/ZIF-67异质光催化剂,并将其应用于有效的CO_(2)光还原反应.研究表明,WO_(3)与CsPbBr_(3)之间构建的Z型电荷转移路径能够保证光生载流子的有效转移和分离.此外,在表面修饰具有活性Co中心的ZIF-67壳层作为助催化剂有利于改善复合材料的CO_(2)的吸附和活化能力.因此,电荷分离和CO_(2)吸附性能的增强大大提高了WO_(3)/CsPbBr_(3)/ZIF-67的光催化活性,还原产物中CO产率达到99.38μmol g_(−1),是单一CsPbBr_(3)的6.8倍.这项工作有望为开发高效的卤素钙钛矿基光催化剂及其在CO_(2)还原和其他复杂光催化反应中的应用提供参考.

关键词： Z-scheme heterojunction halide perovskite CO_(2)photoreduction heterostructure charge separation

Modulating hydrothermal condition to achieve carbon dots-zeolite composites with multicolor afterglow

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Nano Research 2023年第5期16卷 7761-7769页

作者： Jiali Wen Zhifeng Zeng Bolun Wang Junyu Hong Yingyuan Chen Jianyu Zhang Jiyang Li Jiuxing Jiang moe key laboratory of bioinorganic and synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510006China State key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Department of chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and ReconstructionThe Hong Kong University of Science and TechnologyKowloonHong Kong 999077China Guangdong Provincial key laboratory of Optical Chemicals XinHuaYue GroupMaoming 525000China

Responsive luminescence materials with prolonged lifetime and multicolor emission have drawn great attention due to their attractive optical property and potential applications.Herein,two responsive carbon dots(CDs)based composites:CD_(1)@MCM-22P and CD_(2)@ZSM-12 were achieved by a one-step hydrothermal method.By adjusting the hydrothermal condition,CD_(1)@MCM-22P owns temperature-dependent afterglow,while CD_(2)@ZSM-12 is equipped with excitation-dependent room-temperature phosphorescence.The photoluminescence mechanisms of CD1@MCM-22P and CD_(2)@ZSM-12 were investigated and proposed,and the composites were applied in multi-mode anti-counterfeiting.This work provides an insight as well as a feasible method for the development of multi-emissive CDs@zeolite composite.

关键词： carbon dots zeolitic matrices responsive photoluminescence room-temperature phosphorescence thermally activated delayed fluorescence

Construction of cobalt vacancies in cobalt telluride to induce fast ionic/electronic diffusion kinetics for lithium-ion half/full batteries

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Journal of Materials Science & Technology 2022年第32期127卷 124-132页

作者： Lei Hu Lin Li Yuyang Zhang Xiaohong Tan Hao Yang Xiaoming Lin Yexiang Tong Anhui laboratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China moe of the key laboratory of bioinorganic and synthetic chemistry The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China Guangxi key laboratory of Electrochemical Energy Materials School of Chemistry&Chemical EngineeringGuangxi UniversityNanning 530004China key laboratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006China

Designing novel electrode materials with unique structures is of great significance for improving the performance of lithium ion batteries(LIBs).Herein,copper-doped Co_(1-x)Te@nitrogen-doped carbon hollow nanoboxes(Cu-Co_(1-x)Te@NC HNBs)have been fabricated by chemical etching of Cu Co-ZIF nanoboxes,followed by a successive high-temperature tellurization process.The as-synthesized Cu-Co_(1-x)Te@NC HNBs composite demonstrated faster ionic and electronic diffusion kinetics than the pristine Co Te@NC HNBs electrode.The existence of Co-vacancy promotes the reduction of Gibbs free energy change(ΔG_(H^(*)))and effectively improves the Li~+diffusion coefficient.XPS and theoretical calculations show that performance improvement is ascribed to the electronic interactions between Cu-Co_(1-x)Te and nitrogen-doped carbon(NC)that trigger the shift of the p-band towards facilitation of interfacial charge transfer,which in turn helps boost up the lithium storage property.Besides,the proposed Cu-doping-induced Co-vacancy strategy can also be extended to other conversion-type cobalt-based material(CoSe_(2))in addition to asobtained Cu-Co_(1-x)Se_(2)@NC HNBs anodes for long-life and high-capacity LIBs.More importantly,the fabricated LiCoO_(2)//Cu-Co_(1-x)Te@NC HNBs full cell exhibits a high energy density of 403 Wh kg^(-1)and a power density of 6000 W kg^(-1).We show that the energy/power density reported herein is higher than that of previously studied cobalt-based anodes,indicating the potential application of Cu-Co_(1-x)Te@NC HNBs as a superior electrode material for LIBs.

关键词： MOF-derived material Cobalt telluride Cobalt vacancy Diffusion kinetics Lithium storage

Spherical lanthanide nanoclusters toward white-light emission and cell membrane imaging

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Nano Research 2023年第8期16卷 11495-11502页

作者： Hai-Ling Wang Zhiqiang Ni Ze-Yu Ruan Zhong-Hong Zhu Pei-Yu Liao Guangxue Feng Jian-Hua Jia Ming-Liang Tong key laboratory of bioinorganic and synthetic chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou 510006China State key laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSchool of Materials Science and EngineeringSouth China University of TechnologyGuangzhou 510640China

Lanthanide doping is an effective strategy for modulating the emission of emitters.Herein,by changing the cluster composition to control the energy transfer pathway,the application potential of high-nuclearity lanthanide cluster(HLC)as white-light emitter has been confirmed for the first time.Specifically,by precisely controlling the proportion of GdIII,TbIII,and EuIII ions in reactants,we obtained a spherical heterotrimetallic nanocluster Gd_(10)Tb_(12)Eu_(10),a white-light emitter with quantum yield(QY)of 12.58%and lifetime of 327.14μs.High-resolution electrospray ionization mass spectrometry(HRESI-MS)demonstrates that homometallic nanoclusters Ln_(32)(Ln=Gd,Tb,and Eu)are tetracationic clusters and are highly stable in solution.The peripheral dense organic ligands provide a protective layer for the cluster core,which improves the stability of Ln_(32) in aqueous solution,avoids the contact between metal centers and bioactive molecules,and greatly reduces the biological toxicity.In cell imaging experiments,cationic clusters Ln_(32) are mainly localized on the cell membrane with negative charge distribution.As far as we know,this is the first time that spherical lanthanide nanoclusters have been used for membrane imaging of living cell,opening the door for the application of HLCs in biological imaging.

关键词： spherical lanthanide clusters white-light emission high stability low toxicity cell membrane imaging