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Manipulating guest-responsive spin transition to achieve switchable fluorescence in a Hofmann-type framework

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Science China Chemistry 2024年第10期67卷 3339-3346页

作者： Xue-Ru wu Shu-Qi wu Zhi-Kun Liu Ming-Xing Chen Jun tao Osamu Sato Hui-Zhong Kou Engineering Research Center of Advanced Rare Earth Materials(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China Institute for Materials Chemistry and Engineering&IRCCS Kyushu University744 MotookaNishi-kuFukuoka 819-0395Japan Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Analytical Instrumentation Center College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The change of fluorescence emission manipulated by spin state transition attracts considerable attention owing to its potential applications in magneto-optical switching ***,we report two two-dimensional(2D)Hofmann-type spin crossover(SCO)metal-organic frameworks(MOFs)[Fe^(Ⅱ)(PNI)_(2){Ag^(Ⅰ)(CN)_(2)}_(2)]·CHCl_(3)(3Ag·CHCl_(3))and[FeⅡ(PNI)_(2){AuⅠ(CN)_(2)}_(2)]·CHCl_(3)(3Au·CHCl_(3))based on the fluorescent ligand N-(4-pyridylmethyl)-1,8-naphthalimide(PNI).Both complexes exhibit interesting SCO behaviors switched by guest solvent molecules,namely three-step transitions for the solvated complexes and complete onestep hysteretic SCO for the desolvated ones,verified by temperature-dependent magnetic susceptibility measurements,Mossbauer spectra,structural analyses,and differential scanning calorimetry ***,temperature-dependent fluorescence spectra exhibit double peaks(monomer and excimer emission)with both emission peaks change consistent with the change in SCO properties during the solvent molecule *** this study,we integrated guest-responsive SCO behavior into MOFs to manipulate the multistability of spin state and fluorescence switching,providing a rational strategy for the development of stimuli-responsive multifunctional materials.

关键词： spin crossover fluorescence multifunctional materials metal-organic frameworks Hofmann-type

Reduced magma generation and its implications for the Pulang giant porphyry Cu-polymetallic deposit in Northwest Yunnan,China

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Acta Geochimica 2024年第4期43卷 802-813页

作者： Jingwei Guan tao Ren Lei Wang Shenjin Guan Lianrong wu Baosheng Shi Faculty of Land Resources Engineering Kunming University of Science and TechnologyKunming 650093People’s Republic of China Diqing Nonferrous Metals Co. LtdShangri-La 674400People’s Republic of China

The Pulang giant porphyry Cu-Mo polymetallic deposit is located in the Zhongdian area in the center of the Sanjiang Tethys tectonic domain,which was formed by the westward subduction of the Garze-Litang oceanic slab beneath the Zhongza ***-pyrrhotite-pyritemolybdenite occurs as disseminations,veins,veinlets,and stockworks distributed in the K-silicate alteration zone in the monzonite porphyry,which is superimposed by *** chemical compositions of biotite and amphibole analyzed by electron probe microanalysis(EPMA)indicate that the ore-forming magma and exsolved fluids experienced a continuous decrease in the oxygen fugacity(fO_(2)).Primary amphibolite and biotite(type I)crystallized at relatively high temperatures(744-827°C)and low fO_(2)(log fO_(2)=−12.26 to−11.91)during the magmatic *** fluids exsolved from the magma have a relatively lower temperature(621-711°C)and fO_(2)(log fO_(2)=−14.36 to−13.32)than the original *** addition,the presence of a high abundance of pyrrhotite and an insufficiency of primary magnetite and sulfate in the ore(i.e.,anhydrite and gypsum)indicate that the deposit may be a reduced porphyry *** and fluid fO_(2)results,combined with previous research on magmatic fO_(2)at the Pulang deposit,indicate that the magma associated with the reduced Pulang ore assemblages was initially generated as a highly oxidized magma that was subsequently reduced by sedimentary rocks of the Tumugou Formation.

关键词： Porphyry deposit Oxygen fugacity(fO_(2)) Contamination of surrounding rock Pulang Zhongdian arc

Metal-organic frameworks and their composites for advanced lithium-ion batteries:Synthesis,progress and prospects

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Journal of Energy Chemistry 2024年第2期89卷 449-470,I0011页

作者： Chengcai Liu Borong wu tao Liu Yuanxing Zhang Jingwen Cui Lingjun Huang Guoqiang Tan Ling Zhang Yuefeng Su Feng wu School of Material Science and Engineering Beijing Institute of TechnologyBeijing 100081China Chonging Innovation Center Beijing Institute of TechnologyChongqing 401120China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing 100081China

Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical *** instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery *** the chemical composition of MOF can introduce more active sites for electrochemical ***,MOFs and their related composites have been extensively and thoroughly explored for ***,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery *** review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.

关键词： Metal-organic frameworks Electrodes Electrolytes Separators Lithium-ion batteries

Preparation and Structure-Property Regulation Mechanism of Reversible Thermochromic Polydiacetylene

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Chinese Journal of Polymer Science 2024年第8期42卷 1111-1121页

作者： Zhi-Qing Ge Shuo Yan zu-Xiong Pan Shan Lei Xuan-Zhi Mao Chu Zhao Mo-Zhen Wang Xue-wu Ge Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Marshall Laboratory of Biomedical Engineering International Cancer CenterLaboratory of Evolutionary Theranostics(LET)School of Biomedical EngineeringShenzhen University Medical SchoolShenzhen UniversityShenzhen 518055China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China University of Chinese Academy of Sciences Beijing 100049China

The thermochromic mechanism and the structure-property regulation principle of reversible thermochromic polydiacetylene(PDA)materials have always been a challenging *** this work,a series of diacetylene monomers(m-PCDA)containing phenyl and amide or carboxyl groups were synthesized from 10,12-pentacosadiynoic acid(PCDA)through the esterification or amidation *** effects of the number and the distribution of the functional groups in m-PCDA molecules on their solid-state polymerization capability,and the thermochromic mechanism of their corresponding polymers(m-PDA)were investigated and discussed in *** results show that the m-PCDA monomers containing both benzene ring and groups that can form hydrogen bonding interactions have strong intermolecular interaction,and are easy to carry out the solid phase polymerization under 254-nm UV irradiation to obtain the corresponding new thermochromic m-PDA *** thermochromic behavior of m-PDA depends on its melting *** initial color-change temperature(blue to red)is determined by the onset melting tem perature,and the temperature range in which reversible color recovery can be achieved by repeat heating-cooling treatment is determined by its melting *** to the proposed thermochromic mechanism of PDA,various new PDA materials with precise thermochromic temperatu res and reversible thermochromic temperature ra nges can be designed and synthesized through the appropriate introduction of benzene ring and groups that can form hydrogen bonding interactions into the molecular structure of linear diacetylene *** work provides a perspective to the precise molecular structure design and the property regulation of the reversible thermochromic PDA materials.

关键词： Polydiacetylene Thermochromism Hydrogen bonding Chemical modification

Unraveling colorectal cancer prevention:The vitamin D-gut flora-immune system nexus

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World Journal of Gastrointestinal Oncology 2024年第6期16卷 2394-2403页

作者： Zhi-Song Zhan zu-Shun Zheng Jing Shi Juan Chen Si-Yi wu Shi-Yan Zhang Department of Dentistry Fuding HospitalFujian University of Traditional Chinese MedicineFuding 355200Fujian ProvinceChina Department of Physical Examination Fuding HospitalFujian University of Traditional Chinese MedicineFuding 355200Fujian ProvinceChina Department of Anesthesiology Fuding HospitalFujian University of Traditional Chinese MedicineFuding 355200Fujian ProvinceChina Department of Clinical Laboratory Fuding HospitalFujian University of Traditional Chinese MedicineFuding 355200Fujian ProvinceChina Department of Surgery Fuding HospitalFujian University of Traditional Chinese MedicineFuding 355200Fujian ProvinceChina

Colorectal cancer(CRC)is one of the most common cancers diagnosed in the *** environmental and genetic factors play a major role in the pathogenesis of CRC,extensive research has suggested that vitamin D may play a pivotal role in the development of *** D,primarily obtained through sunlight exposure,dietary sources,and supplements,has long been recognized for its essential functions in maintaining health,including immune *** article delves into the intricate relationship between vitamin D,the immune system,gut flora,and the prevention of *** presents a synthesis of epidemiological data,experimental studies,and clinical trials,highlighting the mechanisms by which vitamin D influences immune cell function,cytokine production,and *** enhancing the immune system’s surveillance and antitumor activity,vitamin D may offer a promising avenue for CRC ***,this comprehensive review delves into the prospective clinical applications of vitamin D supplementation and delineates the forthcoming avenues of research in this dynamic ***,the paper tentatively outlines a spectrum of prophylactic impacts of vitamin D on CRC,emphasizing its significant potential in reducing CRC risk through shedding light on its mechanisms,encompassing antineoplastic mechanisms,influences on the immune system,and modulation of the gut microbiome.

关键词： Colorectal cancer Vitamin D Immune system Gut flora Immunomodulation Microbial dysbiosis Cancer prevention

Improvements in energy saving and thermal comfort for electric vehicles in summer through coupled electrochromic and radiative cooling smart windows

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Building Simulation 2024年第8期17卷 1231-1251页

作者： Zhoujie Duan Shuangdui wu Hongli Sun Borong Lin Pei Ding tao Cui Jeremy To Xi Zhang College of Architectureand Environment Sichuan UniversityChengdu610065China Department of Building Science Tsinghua UniversityBejing 100084China KeyLaboratoryofEco Planning&Green Building MinistryofEducationTsinghua UniversityBeijing100084China State Key Laboratory of Hydraulics and Mountain River Engineering Sichuan UniversityChengdu 610065China School of EmergencyManagement Xihua UniversityChengdu 610039China Department of PSVD Mercedes-benz Group China Ltd.Beijing 100102China

In hot climates,the large amount of cooling load in electric vehicle(EV)results in a lot of battery energy consumption,leading the decrease of driving *** the widespread application of windows in EV,the electrochromic glass(EC)shows great prospect in lowering the cooling ***,researches on the application of EC in EV lack the consideration of both passive cooling measures and passenger comfort,which limits the further application of *** this paper,we proposed an idea combining the novel techniques of both electrochromism and radiative *** fluid dynamics(CFD)is modeled to simulate the application of electrochromic and radiative cooling coupled smart windows in hot parking conditions,exploring the improvement effect of the window on the thermal environment,comfort and energy saving of the *** results indicate that,under the intense sunlight with an outdoor temperature of 33℃,activating the air conditioning to maintain an average interior temperature of 26℃,the coupled windows reduced the cooling capacity of the air conditioning by 762 W compared to regular windows,which can further increase the range of ***,compared to simple electrochromic fully colored glass,the integration of radiative cooling technology can lower the window surface temperature by up to 10.7℃.Moreover,compared to regular windows,the coupled windows lowered the standard effective temperature(SET*)for passengers by approximately 7℃,significantly improving *** research findings are expected to provide guidance for optimizing window design and enhancing the performance of EV.

关键词： electrochromism radiative cooling smart windowel ectric vehicle cabin thermal comfort energy saving

Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis

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Green Energy & Environment 2024年第4期9卷 695-701页

作者： Jianjun Tian Changsheng Cao Yingchun He Muhammad Imran Khan Xin-tao wu Qi-Long Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences(CAS)Fuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China University of Chinese Academy of Sciences Beijing100049China Research Institute of Sciences and Engineering(RISE) University of SharjahSharjah27272United Arab Emirates

Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical ***,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary ***,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical *** NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of *** work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.

关键词： Hierarchical superstructures Metal–organic frameworks Layered double hydroxides Urea oxidation reaction Hydrogen evolution reaction

Synergistic effects of multiscale TiC and dual-phase structure on tensile properties of particle-reinforced steel

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Journal of Iron and Steel Research International 2024年第5期31卷 1232-1245页

作者： Ye Jia Xiang-tao Deng Qi Wang Cheng-ru Li Hao wu Zhao-dong Wang State Key Laboratory of Rolling and Automation Northeastern UniversityShenyang110819LiaoningChina

The conventional melting methods were used to obtain in situ TiC particle-reinforced dual-phase steel,followed by hot rolling and heat treatment *** aim was to investigate the effect of TiC particles on the fracture behavior of dual-phase steel at different annealing temperatures,by analyzing the microstructure and tensile behavior of the multiscale TiC particle-reinforced dual-phase *** results showed that TiC particles precipitated in the as-cast microstructure of dual-phase steel were distributed along the grain *** hot rolling,the grain boundary-like morphology of the micron-sized TiC particles was disrupted,and the particles became more refined and evenly distributed in the *** tensile tests revealed that the strength of the TiC particle-reinforced dual-phase steel increased with increasing martensite content,while the elongation *** results were similar to those of conventional *** addition of 1 vol.%multiscale TiC particles improved the strength of the dual-phase steel but did not affect elongation of the *** and holes were primarily concentrated around the TiC particles rather than at the interface of martensite and *** main causes of crack sprouting were TiC particle interface cracking and TiC particle internal ***,the study demonstrated the potential of multiscale TiC particle-reinforced dual-phase steel as a strong and tough *** refined distribution of TiC particles in the matrix improved the strength of the material without compromising its *** results also highlighted the importance of careful selection of reinforcement particles to avoid detrimental effects on the fracture behavior of the material.

关键词： TiC particle Dual-phase structure TiC-reinforced dual-phase steel Tension Fracture behavior

Strategic regulation of nitrogen-containing intermediates for enhanced nitrate reduction over Co_(3)O_(4)/SiC catalyst having multiple active centers

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Journal of Energy Chemistry 2024年第9期96卷 291-299页

作者： Ming-Hao Guan Hao-Nan Xu Jin Liu tao wu An-Hui Lu State Key Laboratory of Fine Chemicals Liaoning Key Laboratory for Catalytic Conversion of Carbon ResourcesSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina

Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction ***,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the ***,a family of n%-Co_(3)O_(4)/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co^(2+)and Co^(3+)were prepared for NO_(3)*** found that Co^(3+)primarily acts as the active site for NO_(3)^(−)reduction to NO_(2)^(−),while Co^(2+)is responsible for the conversion of NO_(2)^(−)to NH_(3).Moreover,the conversion of these intermediates over the active sites is autonomous and separately *** processes synergistically accomplish the reduction of nitrate ions to synthesize *** the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(^(*)NHO→^(*)NHOH→^(*)NH_(2)OH→^(*)NH_(2)→^(*)NH_(3))is more favorable due to the lowerΔG value(0.25 eV)for the rate-limiting step(^(*)NO→^(*)NHO).The NH_(3)yield rate of 8%-Co_(3)O_(4)/SiC reached 1.08 mmol/(cm^(2)h)with a Faradaic efficiency of 96.4%at−0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO_(3)RR *** strategy not only provides an efficient catalyst for NO_(3)RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.

关键词： Electrocatalysis Nitratereduction Co_(3)O_(4)/SiC catalysts Intermediates control