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Rare Metals 2024年第2期43卷 588-598页

作者： Fei Wang Han Gao Zhao-Yu Niu Yao-Peng Zheng Ming-Yan Chuai Jia-Nan Xu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China

In the current situation where the practical application of silicon anode materials encounters great challenges,silicon oxide(SiO_(x),0≤x≤2)has attracted the attention of researchers due to its relatively small volume expansion,stable cycling performance,and low cost,which is possible to realize commercial applications earlier than silicon ***,it remains a challenge to prepare SiO_(x)materials with long-term stable cycling performance and high Coulombic efficiency using low-cost *** this work,SiO_(x)anode material with high Coulombic efficiency and good long-term cycling stability was prepared at a low cost by hydrolysis of siloxane and in situ polymerization of phenolic *** hydrolysis of siloxane was further regulated by different silane coupling agents to regulate the size and microstructure of prepared SiO_(x)materials,which displayed the substantially improved electrochemical *** excellent electrochemical performance of SiO_(x)prepared by regulated hydrolysis of siloxane with silane coupling agents is attributed to the effect of silane coupling agent on size and microstructure of SiO_(x),revealing that the strategy of modulating the hydrolysis of siloxane by silane coupling agent is a potential method to prepare high-performance SiO_(x)materials.

关键词： Hydrolysis Silane coupling agent Long cycle SiO_(x) anode Lithium-ion battery(LIB)

Organo-electroreduction enables arylcarboxylation of styrenes

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Science China chemistry 2024年第11期67卷 3825-3832页

作者： Yanwei Wang Qian Wang Zile Zhu Weikang Qi Youai Qiu State Key Laboratory and institute of Elemento-Organic chemistry Frontiers Science Center for New Organic Matter Haihe Laboratory of Sustainable Chemical Transformations College of Chemistry Nankai University

Electroreduction offers an alternative to generate high active intermediates from electrophiles(halides, alkenes, etc.) in organic synthesis. However, it still remains challenge to enable the transformations in controlled fashion for substrates with similar reduction potentials. Herein, an electroreductive arylcarboxylation of styrenes with aryl halides and CO2promoted by an organomediator has been developed. The reaction exhibits the remarkable reactivity control between styrenes and aryl halides bearing very similar reduction potentials, which is enabled by the addition of a simple organic mediator. The mediated process for different kinds of aryl halides(iodides and bromides) could be achieved by simply tuning the electronic effect of the skeleton of naphthalene. This protocol displays a broad substrate scope and the extension to late-stage modification of biorelevant molecules and their derivatives showed a bright prospect. Moreover, density functional theory(DFT) calculations and mechanistic studies have been conducted and provide solid support to rationalize the selectivity and reactivity control observed.

关键词： CO2 utilization reductive organo-mediator carboxylation electroreduction aryl halides

Aggregation-induced T_(1)/T_(2) contrast enhancement for magnetic resonance imaging-guided intraoperative surgery

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Science China chemistry 2024年第6期67卷 2046-2055页

作者： Wenbo Sun Bin Yu Dianshuai Huang Chunhuan Jiang Wei Wang Jianhua Liu Zonghua Wang Lehui Lu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China College of chemistry and Chemical Engineering Shandong Sino-Japanese Center for Collaborative Research of Carbon NanomaterialsQingdao Application Technology Innovation Center of Photoelectric Biosensing for Clinical Diagnosis and TreatmentQingdao UniversityQingdao266071China Department of Radiology Second Hospital of Jilin UniversityChangchun130041China

Magnetic resonance imaging(MRI)plays an important role in precision medicine that is hampered by the lack of contrast agents with high efficiency and the ability to translate diagnostic accuracy into therapeutic ***,we demonstrate a DNA-based MRI probe that overcomes previous single-mode enhancement and provides a mechanism of action for aggregationinduced dual-modal MRI signal enhancement.A facile method is developed to produce aggregated T_(1)/T_(2)dual-modal NaGdF_(4):Dy@PDA-DNA(PDA=polydopamine)MRI *** aggregated,this probe can further amplify MRI signal intensity and exhibit improved geometrical and positional stability in *** performance of the NaGdF_(4):Dy@PDA-DNA MRI probe toward MRI-guided preoperative planning and visualization-guided surgery is verified using an orthotopic tumor-bearing mouse *** result shows that the rapid metabolism of the degraded probe leads to the mitigation of long-term toxic ***,the developed high-performance MRI probe is of great significance for enhancing MRI diagnostic accuracy into precision medical therapeutic interventions.

关键词： MRI probe DNA aggregation-induced T_(1)/T_(2)contrast enhancement precision medicine degradable probe

Effect of Ta_(2)O_(5)nanoparticles on bioactivity,composition,structure,in vitro and in vivo behavior of PEO coatings on Mg-alloy

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Journal of Magnesium and Alloys 2024年第6期12卷 2360-2379页

作者： D.V.Mashtalyar I.M.Imshinetskiy V.V.Kashepa K.V.Nadaraia M.A.Piatkova A.I.Pleshkova K.A.Fomenko A.Yu.Ustinov S.L.Sinebryukhov S.V.Gnedenkov institute of chemistry Far Eastern BranchRussian Academy of SciencesVladivostok690022Russia Far Eastern Federal University Vladivostok690950Russia Regional clinical Dermatovenerological Dispensary Vladivostok690033Russia

The present study investigates the physical and chemical characteristics,behavior in vitro and in vivo,and biocompatibility of coatings containing Ta_(2)O_(5),which are obtained by plasma electrolytic oxidation(PEO)on MA8 magnesium *** obtained coatings demonstrate in vivo biocompatibility and in vitro *** to the base PEO coating,the layers containing Ta_(2)O_(5)facilitate the development of apatite in simulated body fluid,suggesting that the inclusion of nanoparticles improves bioactivity of the *** was found that incorporation of Ta_(2)O_(5)nanoparticles increases roughness and porosity of the formed layers by increasing particle concentration in electrolytes for the PEO process contributing to sufficient soft tissue ingrowth in *** on in vivo studies,these coatings also provide favorable tissue response and minimal inflammatory reaction in comparison with the bare magnesium alloy due to protection of living tissues from deleterious corrosion events of magnesium implant such as local alkalization and intense hydrogen *** results obtained in the present study concluded biocompatibility,tissue integration of the PEO coatings containing Ta_(2)O_(5)nanoparticles making them a promising protective layer for biodegradable magnesium implants.

关键词： Plasma electrolytic oxidation Bioactive coatings Tantalum pentoxide Simulated body fluid(SBF) Apatite formation Histology

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

Introducing hydroxyl groups to tailor the d-band center of Ir atom through side anchoring for boosted ORR and HER

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Journal of Energy chemistry 2024年第3期90卷 144-151,I0005页

作者： Qing Lv Meiping Li Xiaodong Li Xingru Yan Zhufeng Hou Changshui Huang Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100ShandongChina institute of chemistry Chinese Academy of ScienceBeijing 100191China State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina

Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic ***,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination ***,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline *** from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical *** those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.

关键词： Oxygen reduction reaction D-band center Graphdiyne Hydroxyl group Electrocatalysis

Anion-induced differential assembly and structural transformation of supramolecular coordination cages

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Chinese Chemical Letters 2024年第3期35卷 268-272页

作者： Shao-Ping Zheng Yao-Wei Xu Pei-Yang Su Chen-Hui Liu Yin-Hui Huang Yu-Lin Lu Zhang-Wen Wei Zhiwei Jiao Hai-Sen Xu Cheng-Yong Su MOE Laboratory of Bioinorganic and Synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China institute of Environmental Research at Greater Bay Area Guangzhou UniversityGuangzhou 510006China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The intimate host-anion interactions will regulate thermodynamics and kinetics in the self-assembly of cationic cages mimicking biological ***,we report construction and transformation of three Pd(Ⅱ)-based metal-organic cages(MOCs)depending on different *** conversions of the lantern-shaped MOC-34 into either octahedral MOC-35 or tricapped trigonal prism MOC-36 are induced by BF_(4)^(–)or NO_(3)^(–),***-36 is kinetically favored and can undergo quantitative conversion to the thermodynamically preferred MOC-35 upon heating,accelerated by excess BF_(4)^(–)to motivate dissociative dynamics of Pd-vertices and lower activation barrier of cage *** guest encapsulation behaviors of MOC-35 and MOC-36 have also been *** results manifest a significance of host-anion dynamics beyond complementary anion template,shedding light on the understanding of intricate anion recognition in nature.

关键词： Supramolecular coordination cage Dynamic host-anion interactions Structural transformation Anion receptor Guest inclusion

Selective oxygen electroreduction to hydrogen peroxide in acidic media:The superiority of single-atom catalysts

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Nano Research 2024年第6期17卷 4668-4681页

作者： Ergui Luo Tongtong Yang Jingyi Liang Yuhong Chang Junming Zhang Tianjun Hu Junjie Ge Jianfeng Jia Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China School of chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Two-electron oxygen reduction reaction(2e-ORR)provides an environmentally friendly direction for the on-site production of hydrogen peroxide(H_(2)O_(2)).Central to this technology is the exploitation of efficient,economical,and safe 2e-ORR *** overview starts with the fundamental chemistry of ORR to highlight the decisive role of adsorbing intermediates on the reaction pathway and activity,followed by a comprehensive survey of the tuning strategies to favor 2e-ORR on traditional precious *** latest achievements in designing efficient and selective precious-metal-based single-atom catalysts(SACs)and metal-nitrogen-carbon(M-Nx/C)catalysts,from the aspects of material synthesis,theoretical calculations,and mass transport promotion,are systematically *** introductions on the evaluation metrics for 2e-ORR catalysts and the primary reactor designs for cathodic H_(2)O_(2)synthesis are also *** conclude this review with an outlook on the challenges and direction of efforts to advance electrocatalytic 2e-ORR into realistic H_(2)O_(2)production.

关键词： oxygen reduction reaction H_(2)O_(2)production single-atom catalysts selectivity

A Highly Efficient Ni/Al_(2)O_(3)-LaO_(x) Catalyst for the Reductive Amination of Furfural to Furfurylamine:the Promoting Effect of La

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Chemical Research in Chinese Universities 2024年第1期40卷 36-46页

作者： YANG Yinze ZHANG Liyan ZHOU Leilei CHENG Haiyang ZHAO Fengyu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied chemistry and Engineering University of Science Technology of ChinaHefei 230026P.R.China Jilin Province Key Laboratory of Green chemistry and Process Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China

The reductive amination of furfural to furfurylamine is an important and still challenging topic in the field of biomass conversion. In this work, we prepared a series of Ni/Al_(2)O_(3)-LaO_(x) catalysts by co-precipitation method, the role of La played in promoting the catalytic performances of reductive amination furfural was discussed based on the changes in the electronic state of Ni species, acidity, and Ni particle size. The catalytic activity and the selectivity of furfurylamine are highly dependent on the surface properties and the structure of the catalyst. The addition of La promoted the amount of strong acidic sites and the H2dissociation and spillover on the surface, thus inducing the improvement of the catalytic activity and furfurylamine selectivity. The Ni/Al_(2)O_(3)-0.5LaO_(x)catalyst with suitable acid sites gave a high yield of furfurylamine (94.9%) under mild reaction conditions. Moreover, the catalyst could be recycled five times without significant loss in activity. The Ni/Al_(2)O_(3)-LaO_(x) catalyst is of great promise in the production of amines via reductive amination reaction.

关键词： Reductive amination Furfural Nickel catalyst Furfurylamine Lanthanum

Decarboxylative cyanation and thiocyanation via catalytic electron donor-acceptor complex with copper catalysis

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Science China chemistry 2024年第9期67卷 3019-3028页

作者： Hongping Zhao Xiaoxiang Xi Tianbao Wu Zimin Chen Minyan Wang Weiming Yuan Key Laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Bioinorganic Chemistry and Materia MedicaSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Huazhong University of Science and Technology Research institute Shenzhen 518000China

A new catalytic decarboxylative cyanation and thiocyanation via a synergistic Na I/Cu catalysis is *** photoexcited electron donor-acceptor complex by assembly of Na I,R3P,and N-acyloxy-phthalimide ester(NHPI ester)triggers the generation of alkyl radical species,which then engages in Cu-catalyzed radical coupling *** to success of this dual catalytic transformation is the reliable charge transfer between I·and Cu(I).This dual catalytic platform can eliminate the use of expensive iridium-based photocatalyst or synthetically elaborate organic dyes.A series of primary,secondary,and tertiary alkyl nitriles and thiocyanates are easily ***,an asymmetric decarboxylative cyanation by applying a chiral Cu catalyst is also developed to afford chiral nitriles in high *** mechanistic details and the origin of the high enantioselectivity are further investigated by the mechanistic experiments and the density functional theory calculations.

关键词： electron donor-acceptor catalysis copper catalysis cyanation thiocyanation asymmetric synthesis