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Genome mining of sulfonated lanthipeptides reveals unique cyclic peptide sulfotransferases

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Acta Pharmaceutica Sinica B 2024年第6期14卷 2773-2785页

作者： Meng Wang Wen-Wei Li Zhe Cao Jianong Sun Jiang Xiong Si-Qin Tao Tinghong Lv Kun Gao Shangwen Luo Shi-Hui Dong State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China

Although sulfonation plays crucial roles in various biological processes and is frequently utilized in medicinal chemistry to improve water solubility and chemical diversity of drug leads,it is rare and underexplored in ribosomally synthesized and post-translationally modified peptides(RiPPs).Biosynthesis of RiPPs typically entails modification of hydrophilic residues,which substantially increases their chemical stability and bioactivity,albeit at the expense of reducing water *** explore sulfonated RiPPs that may have improved solubility,we conducted co-occurrence analysis of RiPP class-defining enzymes and sulfotransferase(ST),and discovered two distinctive biosynthetic gene clusters(BGCs)encoding both lanthipeptide synthetase(LanM)and *** expressing these BGCs,we characterized the structures of novel sulfonated lanthipeptides and determined the catalytic details of LanM and *** demonstrate that SslST-catalyzed sulfonation is leader-independent but relies on the presence of A ring formed by *** LanM and ST are promiscuous towards residues in the A ring,but ST displays strict regioselectivity toward *** recognition of cyclic peptide by ST was further *** evaluation underscores the significance of the ST-catalyzed *** study sets up the starting point to engineering the novel lanthipeptide STs as biocatalysts for hydrophobic lanthipeptides improvement.

关键词： Lanthipeptides Sulfotransferases Sulfonation Biosynthesis Genome mining

Structure regulating of metal clusters in carbonized metallic organic frameworks for high-efficient microwave absorption via tuning interaction strength between metals and ligands

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Nano Research 2024年第3期17卷 1699-1709页

作者： Chang Sun Kun-Yan Zhao Ming-Lu Huang Cheng-Long Luo Xu-Dong Chen Ming Wang School of chemistry and Chemical Engineering Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function ManufacturingSouthwest UniversityChongqing 400715China Jieyang Branch of chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China

Carbonized metallic organic frameworks(CMOF)have been attracting attention in microwave absorption(MA)research area because of their diverse structures,tunable compositions,and rich ***,structure regulation on metal clusters in CMOF is achieved by tuning the interaction strength between metals and ligands to enhance microwave absorption *** to relatively weak interaction among copper cations and ligands,copper nanoclusters(CuNC)can be uniformly formed and embedded within the cobalt/zinc(Co/Zn)***,copper cations are added to the Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs).Secondly,the CMOF composite particles with CuNCs(CuNCs/CoZn-CMOF)were developed by a pyrolysis *** CuNCs/CoZn-CMOF with an appropriate amount of CuNCs can harmonize both dielectric and magnetic *** a result,the minimum reflection loss(RLmin)reaches–45.1 dB at a matching thickness of 2.30 mm and the effective absorption bandwidth(EAB)is 8.80 GHz at a thickness of 3.10 *** broadband response to electromagnetic waves is attributed to interfacial polarization at CuNCs surface and heterogeneous interfaces,impedance matching and multiple scattering of electromagnetic *** study provides a feasible method to develop CMOF microwave absorption materials with high EAB values.

关键词： heterogeneous interface carbonized metallic organic frameworks microwave absorption interfacial polarization

Transition metal clusters with precise numbers of atoms anchored on graphdiyne as multifunctional electrocatalysts for OER/ORR/HER:a computational study

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Rare Metals 2024年第7期43卷 3107-3117页

作者： Xin-Yang Liu Jing-Wei Liu Gang Li Jing-Xiang Zhao College of chemistry and Chemical Engineering Harbin Normal University

Subnanometer metal clusters play an increasingly important role in heterogeneous catalysis due to their high catalytic activity and *** this work,by means of the density functional theory（DFT） calculations,the catalytic activities of transition metal clusters with precise numbers of atoms supported on graphdiyne(TM1-4@GDY,TM=V,Cr,Mn,Fe,Co,Ni,Cu,Ru,Rh,Pd,Ir,Pt) were investigated for oxygen evolution reactions（OER）,oxygen reduction reactions（ORR） and hydrogen evolution reactions（HER）.The computed results reveal that the Pd2,Pd4and Pt1anchored graphdiyne can serve as trifunctional catalysts for OER/ORR/HER with the overpotentials of 0.49/0.37/0.06,0.45/0.33/0.12 and 0.37/0.43/0.01 V,respectively,while Pd1and Pt2@graphdiyne can exhibit excellent catalytic performance for water splitting（OER/HER） with the overpotentials of 0.55/0.17 and 0.43/0.03 *** addition,Ni1and Pd3anchored GDY can perform as bifunctional catalysts for metal-air cells（OER/ORR） and fuels cells（ORR/HER） with the overpotentials of 0.34/0.32 and 0.42/0.04 V,***,by precisely controlling the numbers of atoms in clusters,the TM1-4anchored graphdiyne can serve as promising multifunctional electrocatalysts for OER/ORR/HER,which may provide an instructive strategy to design catalysts for the energy conversation and storage devices.

关键词： Density functional theory Graphdiyne Single-cluster catalysts Multifunctional electrocatalysts Overpotential

Inorganic ionic polymerization:From biomineralization to materials manufacturing

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Nano Research 2024年第2期17卷 550-569页

作者： Yanhua Sang Kexin Qin Ruikang Tang Zhaoming Liu Department of chemistry Zhejiang UniversityHangzhou 310058China

Biomineralization process regulates the growth of inorganic minerals by complex molecules,proteins,and cells,endowing bio-materials with marvels structures and excellent *** intricate structures and compositions found in biominerals have inspired scientists to design and synthesize numerous artificial biomimetic *** methodology for controlling the formation of inorganics plays a pivotal role in achieving biomimetic structures and ***,the current approach predominantly relies on the classical nucleation theory,which hinders the precise preparation of inorganic materials by replicating the biomineralization ***,the development of“inorganic ionic polymerization”strategy has enabled us to regulate the arrangement of inorganic ions from solution to solid phase,which establishes an artificial way to produce inorganic materials analogous to the biomineralization *** on inorganic ionic polymerization,a series of achievements have been realized for the biomimetic preparation,including moldable construction of inorganic materials,hard tissue regeneration,and high-performance biomimetic ***,the utilization of inorganic ionic polymerization has also facilitated the production of numerous advanced materials,including novel structures that exceed the current knowledge of materials *** inorganic ionic polymerization system provides new artificial strategies and methodologies for the controllable synthesis of inorganics,which mimics the biomineralization process,paving the way for the future development of more high-performance materials.

关键词： biomineralization inorganic ionic polymerization biomimetic materials crystal growth synthetic methodology

Particle Distribution Informed by Chain Rigidity in Diblock Copolymer Melts: The Effect of Entropy

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Chinese Journal of Polymer Science 2024年第3期42卷 388-399,I0009页

作者： Yuguo Chen Shuanhu Qi Ying Jiang School of chemistry Beihang UniversityBeijing 100191China

We study the effect of chain rigidity on tailoring the nanoparticle locations for neutral and selective particles embedded in the lamellar morphology formed by semiflexible diblock copolymer chains using self-consistent field calculations. The nanoparticles are modeled through a cavity function, and the semiflexible chains are represented by the continuous Kratsky-Porod chain model. In general situation, the nanoparticles prefer to stay at the interface in order to reduce the interface areas and thus the system free energy. However, the particle distribution at the domain center is subtle, and the underlying physics is intrinsically different depending on the polymer flexibility. In the case of flexible chains, the entropy just contributes a constant shift to the free energy when the nanoparticles move around the domain center indicating that the local metastable state if appears at the domain center is wholly attributed to the local minimum in the enthalpy. If the polymers are rigid, the variation of the particle distribution at the domain center has a close relation with the polymer rigidity and nanoparticle size. In the case of strongly rigid polymers with small nanoparticles, a nearly uniform particle distribution at the domain center is observed, while in other cases, a local enhancement of particle distribution there is found. In contrast to the case of flexible chains, further analysis reveals the crucial role of entropy in controlling the shape of particle distributions at the phase domain. Specifically, the local metastable state appears in the domain center is determined by the large entropy there which arises from the weak coupling of bond orientations that allows the polymer chains to be relatively relaxed. When the particle becomes selective, its distribution in the phase domain exhibits a shift almost uniformly rather than changes its profile, and the underlying physics still holds. In all, our study establishes a strong coupling between the chain rigi

关键词： Semiflexible diblock copolymer Nanoparticle distribution Self-consistent field theory Entropic effect

Asymmetric reversible structural switching of a diene coordination polymer promoted by UV-visible light

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Science China chemistry 2024年第2期67卷 536-541页

作者： Yong Wang Qiaoqiao Zhang Yong-Yong Cao Qi Liu Brendan F.Abrahams Jian-Ping Lang College of chemistry Chemical Engineering and MaterialsSoochow UniversitySuzhou215123China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China College of Biological Chemical Science and EngineeringJiaxing UniversityJiaxing314001China School of chemistry University of MelbourneVictoria3010Australia

In natural and artificial systems,reversible reactions are commonly asymmetric with respect to the time scale and nature of the stimuli which drive the forward and backward *** applications for which switching behavior is required,it is desirable that the reversible reaction goes as close to symmetric as possible;however,such systems are ***,we report an example of ultraviolet(UV)-visible light-regulated asymmetric reversible structural switching involving a diene-based coordination polymer,CP1 and its monocyclobutane product,*** is possible to cycle at least ten times through a forward [2+2] photocycloaddition reaction and the reverse,photocleavage reaction.A single cycle can be completed within a few *** transformation is accompanied by fast and distinct fluorescence changes,arising from optimisation of the reaction *** functional theory calculations allow rationalisation of the asymmetric reversible transformation between CP1 and CP1a rather than between CP1 and its dicyclobutane product *** work provides a clear illustration of reversible structural switching which approaches symmetric behaviour with respect to reaction rate and *** insights gained from this work also assist in the design of fast,reversible switching materials.

关键词： asymmetrical reversible structural switching coordination polymer photocycloaddition UV-visible light-controlled fluorescence switching

Syntheses of new di-nuclear and tetra-nuclear lanthanide 9-anthracenecarboxylates:Magnetocaloric effect,slow magnetic relaxation and luminescent properties

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Journal of Rare Earths 2024年第6期42卷 1101-1109,I0004页

作者： Xing Liu Ruonan Yang Lu Zhang Jian Zhou Chunmei Huang Huahong Zou Zunhong Xiao Chongqing Key Laboratory of Inorganic Functional Materials College of ChemistryChongqing Normal UniversityChongqing401331China Key Laboratory for the chemistry and Molecular Engineering of Medicinal Resources(Ministry of Education of China) School of Chemistry and Chemical Engineering of Guangxi Normal UniversityGuilin541004China School of chemistry and Materials Guizhou Normal UniversityGuiyang550025China

Lanthanide complex-based materials with magnetic and luminescent properties have received a great deal of attention,owing to their importantly potential applications in diverse *** this work,the 9-anthracenecarboxylic acid(9-Haca)as bridging ligand was applied in combination with optically activeπ-conjugated 2,4,6-tri(2-pyridyl)-1,3,5-triazine(tptz)to construct a series of new di-nuclear and tetranuclear lanthanide 9-anthracenecarboxylates[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]·0.25H_(2)O(1),[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]·0.5AQ·CH_(3)COOH_(2)H_(2)O[Ln=Sm(2a),Eu(2b),Gd(2c),Tb(2d),Dy(2e),Tm(2f);AQ=9,10-anthracenedione]and[Ln_(4)(9-aca)_(10)(tptz)_(2)(CH3COO)2]·H_(2)O[Ln=Eu(3a),Gd(3b),Dy(3c)].1 displays a di-nuclear centrosymmetric moiety[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]built up from two complex[La(9-aca)_(2)(tptz)]groups bridged by one H_(2)O molecule and two syn-syn-μ2-η1:η1-9-aca-bridging ligands,while 2a-2f are isostructural and co mprise another di-nuclear centrosymmetric moieties[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]based on two complex[Ln(9-aca)_(2)(tptz)(H_(2)O)]groups connected by two syn-syn-μ2-η1:η1-9-aca-bridging ligands,3a-3c are isostructural and show tetra-nuclear centro symmetric moieties[Ln4(9-aca)10(tptz)2(CH3COO)2]containing three types of coordination modes of *** present compounds offer the only examples of lanthanide 9-anthracenecarboxylates decorated by optically active *** investigations of 2a,2c-2f,and 3b-3c indicate that 3c is typical of slow relaxation of the magnetization,while 2c and 3b show significant magnetocaloric effect(MCE)with the value of-ΔSm of 5.26 J/(kg·K)at 4 K and 15.65 J/(kg·K)at 2 K(ΔH=7 T),*** luminescent properties were also studied and reveal that the characteristic luminescent properties of the 7r-conjugated aromatic ligands are introduced into magnetic lanthanide 9-anthracenecarboxylates,simultaneously exhibiting slow magnetic relaxation(or MCE)and luminescen

关键词： Lanthanide complexes Luminescence Magnetic properties Magnetocaloric effect Slow magnetic relaxation Rare earths

Highly reversible Zn anode enabled by anticatalytic carbon layer with suppressed hydrogen evolution

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Rare Metals 2024年第7期43卷 3044-3054页

作者： Wen-Duo Zhang Chuang Sun Yu-Xuan Zhu Feng Gao Chao Lai School of chemistry and Materials Science Jiangsu Normal University

Aqueous zinc-ion batteries（AZIBs） have emerged as a promising high-efficiency energy storage system due to the high energy density,low-cost and environmental ***,the practical application of AZIBs is severely restricted by the challenges faced by the Zn anode,which include uncontrollable dendrite growth,corrosion and hydrogen evolution ***,a simple and convenient physical vapor deposition（PVD）method is reported for fabricating uniform graphite as a protection layer on the surface of Zn *** high conductivity graphite layer on Zn anode（denoted as Zn@C） not only benefits the uniform distribution of the electric field,but also provides numerous Zn nucleation sites to regulate and navigate Zn-ion stripping/plating ***,the graphite layer with a poor catalytic activity endows the Zn@C anode with a highly suppressed hydrogen ***,a hydrogen and dendrite free anode is achieved with artificial anticatalytic carbon layer on Zn anode,exhibiting a high reversibility and excellent cycling stability over 2600 h at the current density of 5 mA·cm-2with a capacity of 2.5 mAh·cm-2and longtime cycling stability for assembled full *** work strategically designs the properties of the artificial interface layer to effectively address various challenges simultaneously,which presents insights for the future development of high-performance rechargeable AZIBs.

关键词： Zn metal anode Artificial anticatalytic layer Hydrogen suppression Dendrite free

Atomically dispersed materials:Ideal catalysts in atomic era

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Nano Research 2024年第1期17卷 18-38页

作者： Tao Gan Dingsheng Wang Department of chemistry Tsinghua UniversityBeijing 100084China

Catalysts can accelerate the chemical reaction rate and effectively promote the molecules transformation,which is of great significance in the research of chemical industry and material *** extreme utilization of reactive sites has led to the emergence and development of atomically dispersed materials(ADMs).The highly active coordination unsaturated metal sites and fully utilized metal atoms make ADMs show great potential in catalytic *** adjustment of coordination environment and electronic structure provides more possibilities for constructing reactive centers with different *** review summarized the application and research progress of ADMs in different *** design strategy and structure–activity relationship of ADMs for specific reactions were summarized and ***,we also provided advices for the challenges and opportunities faced by ADMs in catalytic reactions.

关键词： atomically dispersed materials catalysis organic synthesis battery sensor enzyme