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Nano Research 2024年第8期17卷 7027-7038页

作者： Wenan Cai Yuichiro Tanaka Xing Zhu Teruhisa Ohno department of applied chemistry Faculty of EngineeringKyushu Institute of TechnologyKitakyushu 804-8550Japan College of Bioresources Chemical and Materials Engineering Shaanxi University of Science&TechnologyXi’an 710021China

Polymer carbon nitride(PCN)is widely used in ***,pristine PCN has disadvantages such as insufficient visible light absorption and low photogenerated carrier separation efficiency that greatly limited the photocatalytic *** a non-toxic metal,gallium has the potential to solve the defects of *** ions coordinated with nitrogen in carbon nitride to form Ga-N active sites and improved the photocatalytic *** doped potassium ions form a transmission channel for charge redistribution and transfer between adjacent layers,which is beneficial for better separation of photoexcited *** this study,a series of PCN co-doped with gallium and potassium(Ga-K-PCN)were *** experimental results indicated photocatalytic generation of hydrogen peroxide proceeds through the 2e−oxygen reduction reaction ***,Nyquist plots and photocurrent results further proved that the presence of Ga-N sites and potassium ion doping could significantly improve the separation/transfer of intra-planar and interlayer charge carriers and thus enhance photocatalytic *** Ga10-K3-PCN photocatalysts promoted yield of H_(2)O_(2),with reactivity at 28.2μmol/(g·h)and solar-to-chemical conversion efficiency at 0.64%,surpassed that of a typical photo-catalyst based on PCN(0.18%).

关键词： photocatalysis gallium oxygen reduction reaction H_(2)O_(2) production

Sequential enantioselective Ugi-4CR/post-Ugi transformation strategy:a precise construction of structurally diverse azaspiro polycyclic scaffolds

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Science China chemistry 2024年第2期67卷 576-586页

作者： Xiao-Bao Wu Jun-Xiu Shi Yi-Ming Ou Hua-Jie Jiang Yi-Jun Fang Qi-Ming Wang Quan Gao Jie Yu department of applied chemistry Anhui Province Engineering Laboratory for Green Pesticide Development and ApplicationAnhui Province Key Laboratory of Crop Integrated Pest ManagementAnhui Agricultural UniversityHefei230036China

A privileged strategy has been developed for the precise construction of enantioenriched azaspiro polycyclic *** diverse azaspiro polycycles bearing multiple contiguous stereocenters are obtained with excellent results(up to 99:1 e.r.,>95:5 d.r.) via sequential enantioselective four-component Ugi reactions/post-Ugi transformations with substrates containing prerequisite functional groups in the presence of anionic stereogenic-at-cobalt(Ⅲ) complexes.

关键词： asymmetric catalysis post-Ugi transformation anionic stereogenic-at-cobalt(Ⅲ)complex azaspiro polycyclic scaffold one-pot synthesis

Thermal transports in the MXenes family:Opportunities and challenges

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Nano Research 2024年第8期17卷 7700-7716页

作者： Yurui Liu Yue Wu Xinwei Wang department of Chemical and biological Engineering Iowa State University618 Bissell AmesIA 50011USA department of Mechanical Engineering 271 Applied Science Complex II1915 Scholl RoadIowa State UniversityAmesIA 50011USA

The carbides and nitrides of transition metals known as“MXenes”refer to a fast-growing family of two-dimensional materials discovered in *** to their unique nanolayer structure,superior electrical,mechanical,and thermal properties,MXenes have shown great potential in addressing the critical overheating issues that jeopardize the performance,stability,and lifetime of high-energy-density components in modern devices such as microprocessors,integrated circuits,and capacitors,*** outstanding intrinsic thermal conductivity of MXenes has been proved by experimental and theoretical *** MXenes-enabled high thermal conductivity composites incorporated with polymer matrix have also been reported and widely used as thermal management *** the booming heat dissipation demands,MXenes-enabled thermal management material is an extremely valuable and scalable option for modern electronics ***,the fundamental thermal transport mechanisms behind the MXenes family remain *** MXene thermal conductivity disparities between the theoretical prediction and experimental results are still *** better understand the thermal conduction in MXenes and provide more insights for engineering high-performance MXene thermal management materials,in this article,we summarize recent progress on thermal conductive *** essential factors that affect MXenes intrinsic thermal conductivities are tackled,selected MXenes-polymer composites are highlighted,and prospects and challenges are also discussed.

关键词： transition metal carbide(MXene) thermal transport two-dimensional materials thermally conductive composites

Charting the course to solid-state dual-ion batteries

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Carbon Energy 2024年第3期6卷 132-177页

作者： Habtom D.Asfaw Antonia Kotronia Nuria Garcia-Araez Kristina Edström Daniel Brandell department of chemistry Ångström LaboratoryUppsala UniversityUppsalaSweden department of chemistry University of SouthamptonSouthamptonUK

An electrolyte destined for use in a dual-ion battery(DIB)must be stable at the inherently high potential required for anion intercalation in the graphite electrode,while also protecting the Al current collector from anodic dissolution.A higher salt concentration is needed in the electrolyte,in comparison to typical battery electrolytes,to maximize energy density,while ensuring acceptable ionic conductivity and operational *** recent years,studies have demonstrated that highly concentrated organic electrolytes,ionic liquids,gel polymer electrolytes(GPEs),ionogels,and water-in-salt electrolytes can potentially be used in *** can help reduce the use of solvents and thus lead to a substantial change in the Coulombic efficiency,energy density,and long-term cycle life of ***,GPEs are suited to manufacture compact DIB designs without separators by virtue of their mechanical strength and electrical *** this review,we highlight the latest advances in the application of different electrolytes in DIBs,with particular emphasis on GPEs.

关键词： anion intercalation concentrated electrolytes dual-ion battery graphite ionic liquids polymer electrolyte

Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key Laboratory of Electroanalytical chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

MicroED as a powerful technique for the structure determination of complex porous materials

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Chinese Journal of Structural chemistry 2024年第3期43卷 41-54页

作者： Chao Ma Cong Lin Jian Li State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China department of applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityKowloonHong Kong China

Porous materials have garnered significant attention in recent *** the intrinsic relationship between their structures and properties requires precise knowledge of their atomic ***-crystal X-ray diffraction(SCXRD)has traditionally been the primary method for elucidating such structures,but it demands large,high-quality crystals,often exceeding 5μm in *** growth of these crystals can be a time-consuming process,especially for one-and two-dimensional *** explore structures at the nanoscale,MicroED(microcrystal electron diffraction(ED))offers unprecedented insights into the realm of *** revolutionary technique enables researchers to uncover intricate details within nanoscale structures,promising to reshape our fundamental understanding of *** this review,we delve into the applications of MicroED in the study of various porous materials,including zeolites,metal-organic frameworks(MOFs),and covalent organic frameworks(COFs).We emphasize the pivotal role of MicroED in nanomaterial characterization,enabling precise crystallographic analysis and phase identification.

关键词： Atomic structure MicroED Porous materials Three-dimensional electron diffraction

Opto-fluidically multiplexed assembly and micro-robotics

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Light(Science & Applications) 2024年第3期13卷 544-554页

作者： Elena Erben Weida Liao Antonio Minopoli Nicola Maghelli Eric Lauga Moritz Kreysing Max Planck Institute of Molecular Cell Biology and Genetics Dresden 01307Germany Center for Systems Biology Dresden 01307Germany Institute of biological and Chemical Systems–biological Information Processing.Karlsruhe Institute of Technology(KIT) Eggenstein-Leopoldshafen 76344Germany department of applied Mathematics and Theoretical Physics University of CambridgeCambridge CB30WAUK

Techniques for high-definition micromanipulations,such as optical tweezers,hold substantial interest across a wide range of ***,their applicability remains constrained by material properties and laser *** while microfluidic manipulations have been suggested as an alternative,their inherent capabilities are limited and further hindered by practical challenges of implementation and *** we show that the iterative application of laser-induced,localized flow fields can be used for the relative positioning of multiple micro-particles,irrespectively of their material *** to the standing theoretical proposal,our method keeps particles mobile,and we show that their precision manipulation is non-linearly accelerated via the multiplexing of temperature stimuli below the heat diffusion *** resulting flow fields are topologically rich and mathematically *** represent unprecedented microfluidic control capabilities that are illustrated by the actuation of humanoid micro-robots with up to 30 degrees of freedom,whose motions are sufficiently well-defined to reliably communicate personal characteristics such as gender,happiness and *** results constitute high-definition micro-fluidic manipulations with transformative potential for assembly,micro-manufacturing,the life sciences,robotics and optohydraulically actuated micro-factories.

关键词： manipulation fluid assembly

Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu department of applied chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen *** extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still ***,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox *** entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction *** a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts *** encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine

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Journal of Energy chemistry 2024年第2期89卷 216-225,I0006页

作者： Honggang Huang Yao Chen Hui Fu Cun Chen Hanjun Li Zhe Zhang Feili Lai Shuxing Bai Nan Zhang Tianxi Liu Key Laboratory of Synthetic and biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122JiangsuChina department of chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium College of chemistry and Chemical Engineering Qingdao UniversityQingdao 266071ShandongChina

The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to ***,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing ***,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V *** hydrogen electrode,outperforming than those of FCC Pd Cu *** the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR *** work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.

关键词： d-d Orbital coupling Crystal-phase engineering Metallic aerogels Acetonitrile electroreduction reaction Ethylamine

DPY19L3 promotes vasculogenicmimicry by its C-mannosyltransferase activity

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Oncology Research 2024年第4期32卷 607-614页

作者： HASSAN BAYDOUN YUJI KATO HIROKI KAMO ANNA HÜSCH HAYATO MIZUTA RYOTA KAWAHARA SIRO SIMIZU department of applied chemistry Faculty of Science and TechnologyKeio UniversityYokohama223-8522Japan department of Pharmacy and Biochemistry Faculty of ScienceUniversity of TübingenTübingen72074Germany

C-mannosylation is a post-translational modification that occurs intracellularly in the endoplasmic *** humans,biosynthesis of C-mannosylation in proteins containing thrombospondin type 1 repeat is catalyzed by the DPY19 family;nonetheless,biological functions of protein C-mannosylation are not yet fully understood,especially in tumor *** mimicry(VM)is the formation of fluid-conducting channels by highly invasive and genetically deregulated tumor cells,enabling the tumors to form matrix-embedded vasculogenic structures,containing plasma and blood cells to meet the metabolic demands of rapidly growing *** this study,we focused on DPY19L3,a C-mannosyltransferase,and aimed to unravel its role in *** of DPY19L3 inhibited the formation of VM in HT1080 human fibrosarcoma ***-expression of wild-type DPY19L3 recovered VM formation;however,DPY19L3 isoform2,an enzymatic activity-defect mutant,did not restore it,suggesting that the C-mannosyltransferase activity of DPY19L3 is crucial to its ***,the knockdown of DPY19L3 in MDA-MB-231 breast cancer cells hindered its network formation ***,our findings suggest that DPY19L3 is required for VM formation and stipulate the relevance of C-mannosylation in oncogenesis.

关键词： C-mannosylation Vasculogenic mimicry DPY19L3