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Active Template Synthesis of Protein[n]Catenanes Using Engineered Peptide–Peptide Ligation Tools

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CCS chemistry 2024年第2期6卷 377-389页

作者： Fan Zhang Yajie Liu Yu Shao Wen-Bin Zhang Beijing National laboratory for molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 Beijing Academy of Artificial Intelligence Beijing 100084

The expansion of protein topological diversity requires new and efficient synthetic ***,we report the second and third generations of the SpyStapler-mediated SpyTag/BDTag ligation system for the efficient synthesis of 4-arm star proteins and the repurposing of the third generation as an active template to enable the synthesis of higher-order protein[n]catenanes(n=3,4,and 5).SpyStapler003 has a higher affinity to its cognate SpyTag and BDTag reactive pairs relative to the original ***,it can overcome much more profound steric hindrance in protein ligation and improve the efficiency of the resulting active template tool to facilitate the construction of radial protein[n]*** proteins of interest,such as dihydrofolate reductase and the nanobody KN035,can be modularly incorporated into the[n]catenanes with intact *** of passive and active template strategies gives rise to linear protein[4]catenanes,which further expands the current topological ***,higher-order protein catenation not only leads to enhanced thermal stability and proteolytic resistance but also higher affinity of the nanobody via multivalent *** study provides tools useful for bioconjugation and new topological protein scaffolds for the multivalent display of enzymes and antibodies.

关键词： SpyTag SpyCatcher catenane topology active template ligation

Palladium-catalyzed multi components oxy-aminofluorination and aminofluorination of gem-difluoroalkenes

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Chinese Chemical Letters 2024年第2期35卷 420-425页

作者： Fen Wu Xin Li Junbiao Chang Dachang Bai State key laboratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative DrugKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringPingyuan LaboratoryHenan Normal UniversityXinxiang 453007China State key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Organofluorine compounds are widely used in the realm of drug discovery and material ***,we developed palladium catalyzed intermolecular aminofluorination and oxy-aminofluorination of gem‑difluoroalkenes with N-fluorobenzenesulfonimide(NFSI),in which NFSI was used as the nitrogen source and *** reaction provides an efficient and straightforward synthesis route of a series ofα-trifluoromethyl benzylic ***,three/four components oxy-aminofluorination processes were realized to giveα-trifluoromethyl benzylic ether with a terminal amino group,which proceed through C(sp^(3))-O bond cleavage of easily available ether and simultaneous introduced a fluorine,an amino and an oxy substituent in one pot with excellent *** divergent reactivity not only included the incorporation of one ether molecular,but also much more challenged two ether insertion with excellent selectivity through succession C(sp^(3))-O bonds *** protocol allows for concise synthesis of high value amines with fluoroalkyl-substituents and selectively transformation of easily available ethers by high-valent palladium catalysis.

关键词： Palladium Multi components Aminofluorination Oxy-aminofluorination C(sp^(3))-O bond cleavage

Toward Selective Synthesis of Protein Olympiadanes via Orthogonal Active Templates in One Step

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CCS chemistry 2024年第4期6卷 1047-1059页

作者： Fan Zhang Yajie Liu Xiao-Di Da Wen-Bin Zhang Beijing National laboratory for molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871 Beijing Academy of Artificial Intelligence Beijing 100084

Unlike small molecules,the topological complexity of macromolecules remains largely unexplored due to the huge synthetic ***,we report the development of orthogonal active templates for concise and selective synthesis of protein[n]heterocatenanes toward protein *** active template(AT-Snoop)was first developed based on the isopeptide-bond-forming RrgA domain with comparable efficiency and excellent orthogonality to the previously reported active template(AT-Spy)based on the CnaB2 *** combination facilitated the selective synthesis of protein[n]catenanes from multiple components in one step and the resulting structures were verified by sodium dodecyl sulfate-polyacrylamide gel electrophoresis,size exclusion chromatography,liquid chromatography-mass spectrometry,and proteolytic digestion *** results offered a promising solution to tackling the daunting challenge of precision synthesis of protein olympiadane with five distinct ring *** only did the success provide new tools for proteintopology engin eering but alsospurred and fueled the future exploitation of topology-related functional benefits in protein science.

关键词： catenane topology active template SnoopTag SnoopCatcher SpyTag SpyCatcher

A robust indium-organic framework with open tubular channels for efficient separation of acetylene

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Nano Research 2024年第4期17卷 3139-3146页

作者： Yong-Zhi Li Gang-Ding Wang Fan Xu Qing Yin Danyang Zhao Jiqiu Qi Yanwei Sui Lei Hou Yao-Yu Wang School of Materials and Physics China University of Mining and TechnologyXuzhou 221116China key laboratory of Synthetic and Natural Functional Molecule of the ministry of education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi’an 710069China

Considering the tremendous applications and purification requirement of acetylene(C_(2)H_(2)),seeking appropriate adsorbents with high capacity and selectivity is a vital task and remains an enduring ***,we designed and synthesized a robust three-dimensional(3D)indium-organic framework([(Me)_(2)NH_(2)][In(L6)_(0.5)(IPA)_(0.5)]·DMA·2H_(2)O(In-L6-IPA,DMA=dimethylammonium,IPA=isopropyl alcohol))featuring two types of one-dimensional(1D)tubular *** activated In-L6-IPA displayed high loading for C_(2)H_(2)(104.4 cm^(3)·g^(-1),the second highest value among all reported indium-based metal-organic frameworks(MOFs))and simultaneously selective adsorption for C_(2)H_(2) over CO_(2),C_(2)H_(6),and ethylene(C_(2)H_(4))at 298 K under 100 *** modelling revealed that the porous wall of In-L6-IPA provides more and stronger multiple interactions for C_(2)H_(2) than CO_(2),C_(2)H_(6),and C_(2)H_(4) containing C–H···π,C–H···O,and O···π*** experiments validated the actual separation ability for various ratios of binary C_(2)H_(2)/C_(2)H_(4) and C_(2)H_(2)/CO_(2) mixtures as well as equimolar ternary C_(2)H_(2)/C_(2)H_(4)/CO_(2) and C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6) mixtures with excellent reusability.

关键词： indium-organic framework crystal structure gas adsorption acetylene(C_(2)H_(2))separation

Recent progress in lanthanide ions doped inorganic metal halide perovskites

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Journal of Rare Earths 2024年第2期42卷 237-250,I0001页

作者： Yiyan Zhang Tianyu Zhao Guanying Chen MIIT key laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringState Key Laboratory of Urban Water Resource and EnvironmentKey Laboratory of Micro-systems and Micro-structuresMinistry of EducationHarbin Institute of TechnologyHarbin150001China

Benefiting from their large molar extinction coefficient,high carrier mobility,narrow and tunable emissions,inorganic metal halide perovskites(IMHPs) demonstrate great potential in various optoelectrical devices including solar cells,light emitting diodes and photodetectors in the past few *** ions doping,well-known as a modification method of semiconductors,has been extensively applied in IMHPs as *** metal ions have been doped in IMHPs including alkali metals,alkali earth metals,transition metals and lanthanide metals,which either improve their optical performances or induce intriguing brand-new *** them,lanthanide metals feature plentiful energy levels and stable optical properties and are one of the most noteworthy *** we review recent progress in lanthanide ions doped *** summarize Yb,Eu or Er ions singly doping in detail,which was the most investigated species in *** lanthanide ions are also reviewed ***,we introduce lanthanide ions multi-doped IMHPs and at last we put forward several potential development *** the interests in lanthanide ions doped IMHPs rise,researchers have made some achievements in the *** though,there are more unexplored *** there are review articles focusing on metal ions doped IMHPs or lanthanide ions doped perovskites,this review aims to provide an overall introduction of lanthanide ions doped *** review may help researchers learn about lanthanide ions doped IMHPs and is to inspire researchers to make further promotion in this field.

关键词： Halide perovskite Lanthanide Doping Rare earths

Synergism of solar-driven interfacial evaporation and photo-Fenton Cr(Ⅵ) reduction by sustainable Bi-MOF-based evaporator from waste polyester

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Journal of Energy chemistry 2024年第7期94卷 527-540页

作者： Zifen Fan Jie Liu Huajian Liu Lijie Liu Yan She Xueying Wen Huiyue Wang Guixin Hu Ran Niu Jiang Gong key laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHuazhong University of Science andTechnologyWuhan430074HubeiChina

The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade ***,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is ***,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater ***,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic *** to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of *** integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced *** the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.

关键词： Interfacial solar steam generation Cr(VI)reduction Photo-Fenton reaction Metal-organic framework Waste plastic upcycling

Solution-processed all-inorganic lead halide perovskite/layered double hydroxides superlattices

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Science China chemistry 2024年第9期67卷 2904-2910页

作者： Deyu Li Mingming Zhang Lulu Wei Shubing Tian Mingze Sun Kang Liu Jixiang Xu Lei Wang Jun Xing key laboratory of Eco-chemical Engineering Ministry of Education College of Chemistry and Molecular Engineering Qingdao University of Science & Technology College of Sino-German Science and Technology Qingdao University of Science & Technology

Quantum wells and superlattices are key building blocks in the semiconductor industry, normally fabricated using epitaxial growth techniques, such as vapor phase epitaxy, metalorganic chemical vapor deposition and molecular beam epitaxy. However,these complicated preparation processes, as well as their high cost, limit their extensive applications. It is essential to develop a simple solution process for building superstructures. Here, we demonstrate an ion exchange strategy for synthesizing an allinorganic superlattice cesium lead bromide/layered double hydroxides（CsPbBr3/LDH） in solution. At room temperature, the perovskite ions diffuse into the interlayer of LDH and assemble into layered perovskite with various thicknesses. Compared with traditional organic-inorganic hybrid perovskite superlattice, the all-inorganic perovskite superlattice CsPbBr3/LDH has weak quantum confinement, which exhibits narrow emission line-widths of 20 nm, high quantum yields of 55%, and radiative lifetimes of several ns. Our findings offer a new route to synthesize novel perovskite superlattices and enrich the perovskite supercrystal platform for electronics, photonics and optoelectronics devices.

关键词： halide perovskite superlattice layered double hydroxides 2D

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Dimethylamine oxalate manipulating CsPbI_(3) perovskite film crystallization process for high efficiency carbon electrode based perovskite solar cells

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Journal of Energy chemistry 2024年第6期93卷 221-228,I0006页

作者： Wenran Wang Xin Peng Jianxin Zhang Jiage Lin Rong Huang Guizhi Zhang Huishi Guo Zhenxiao Pan Xinhua Zhong Huashang Rao key laboratory for Biobased Materials and Energy of ministry of education College of Materials and EnergySouth China Agricultural UniversityGuangzhou 510642GuangdongChina College of chemistry and Civil Engineering Shaoguan UniversityShaoguan 512005GuangdongChina Guangdong Provincial key laboratory of Utilization and Conservation of Food and medicinal Resources in Northern Region Shaoguan UniversityShaoguan 512005GuangdongChina

Crystallization process determines the quality of perovskite films and the performances of resultant perovskite solar cells(PSCs).Dimethylamine oxalate has been proven as a multifunctional modulator,and is explored as an efficient additive in manipulating the crystallization process of CsPbI_(3) perovskite *** one hand,oxalate serves as the precipitator that facilitates the nucleation process of *** larger size of intermediate is conductive to the larger size and smaller grain boundaries of resultant *** the other hand,in subsequent annealing process,the phase conversion and growth process of transient perovskite can be decelerated due to the strong interactions of oxalate with both dimethylamine cation(DMA^(+))and Pb^(2+).Due to the optimized crystallization kinetics,the morphology and quality of CsPbI_(3) perovskite films are comprehensively improved with lower defect concentrations,and charge recombination loss is effectively *** from the optimized crystal quality of perovskite films,the carbon electrode-based CsPbI_(3) PSCs exhibit a champion efficiency of 18.48%.This represents one of the highest levels among all hole transport layer-free inorganic perovskite solar cells.

关键词： Solar cells Perovskite CsPbI_(3) Carbon electrodes Oxalate

From charge storage mechanism to performance:A strategy toward boosted lithium/sodium storage through heterostructure optimization

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Journal of Energy chemistry 2024年第1期88卷 112-124,I0003页

作者： Xiaoke Zhang Guangfa Deng Mianying Huang Zhaohui Xu Jianlin Huang Xuan Xu Zhiguang Xu Maochan Li Lei Hu Xiaoming Lin key laboratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Anhui laboratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000AnhuiChina National Engineering Research Center for Carbohydrate Synthesis Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022JiangxiChina

Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent *** this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and *** optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active ***_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in *** functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical *** heterostructure building technique may pave the way for the development of high-performance LIBs and ***,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.

关键词： Metal-organic framework Heterostructure Lithium-ion batteries Sodium-ion batteries DFT calculation