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N-doped hollow carbon nanospheres embedded in N-doped graphene forming a three-dimensional interconnected layered porous support loaded with palladium nanoparticles as an efficient electrocatalyst for formic acid oxidation

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新型炭材料(中英文) 2024年

作者： FANG Yue YANG Fu-kai QU Wei-li DENG Chao WANG Zhen-bo Key laboratory of Photochemical Biomaterials and Energy Storage materials Shenzhen Key laboratory of Special Functional materials Shenzhen Engineering Laboratory for Advance Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University MIIT Key laboratory of Critical materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Lab of Urban Water Resource and Environment Harbin Institute of Technology College of Chemistry and Chemical Engineering Harbin Normal University No.1 Normal University South Road

The efficient electrocatalysts with low cost, high activity and good durability plays a crucial role in the application of direct formic acid fuel cells. Herein, Pd nanoparticles supported on N-doped hollow carbon nanospheres (NHCN) embedded in Ndoped graphene (NG) with three-dimensional (3D) layered porous configuration by a simple and economical method were investigated as direct formic acid fuel cell catalysts. Owing to the unique 3D interconnected layered porous configuration doped with nitrogen atoms, Pd/NHCN@NG catalyst with smaller Pd nanoparticle size shows large catalytic active surface area, superior electrocatalyticactivity,highsteady-statecurrentdensity,strongabilitytoresistCOpoisoning,farsurpassingthoseofconventionalPd/C,Pd/NG,andPd/***/GOratio,itisfoundthatwhenthe HCN/GO mass ratio is 1∶1, Pd/NHCN@NG catalyst has the most outstanding performance in catalytic oxidation of formic acid,with an activity 4.21 times that of Pd/C. This work has developed a superior carbon-based support material for electrocatalysts, which brings broad application prospects for the development of fuel cells.

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D-type neuropeptide decorated AIEgen/RENP hybrid nanoprobes with light-driven ROS generation ability for NIR-Ⅱ fluorescence imaging-guided through-skull photodynamic therapy of gliomas

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Aggregate 2024年第1期5卷 185-195页

作者： Xuelu He Yuan Luo Yanying Li Yuanbo Pan Ryan T.K.Kwok Lulu He Xiaolin Duan Pengfei Zhang Aiguo Wu Ben Zhong Tang Juan Li Ningbo Key laboratory of Biomedical Imaging Probe materials and Technology Zhejiang International Cooperation Base of Biomedical Materials Technology and ApplicationChinese Academy of Sciences(CAS)Key Laboratory of Magnetic Materials and DevicesNingbo Cixi Institute of Biomedical EngineeringZhejiang Engineering Research Center for Biomedical MaterialsNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingboP.R.China Guangdong Key laboratory of Nanomedicine Shenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS-HK Joint Lab for BiomaterialsResearch Laboratory for Biomedical Optics and Molecular ImagingShenzhen Key Laboratory for Molecular ImagingCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhenP.R.China Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced StudyThe Hong Kong University of Science and Technology(HKUST)KowloonP.R.China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhenP.R.China

Glioma is one of the most common malignant tumors of the central nervous system,leading high mortality rates in ***-induced emission(AIE)photosensitizers-based photodynamic therapy(PDT)has emerged as a promising therapeutic strategy for least-invasive treatment of glioma,which involves local irradiation of the tumor using an external near-infrared(NIR)***,most AIE photosensitizers suffered from poorly penetration of the visible light excitation,bad spatiotemporal resolution in deep tissues and low efficient blood-brain barrier(BBB)crossing ability,which greatly limited the clinical practice of AIE photosensitizers for especially deep-seated brain tumor *** this work,we developed a multifunctional NIR-driven theranostic agent through hybrid of AIE photosensitizers TIND with rare-earth doping nanoparticles(RENPs)NaGdF4:Nd/Yb/Tm with up/down dual-mode conversion *** theranostic agent was further decorated with D-type neuropeptide DNPY for crossing BBB and targeting *** the 808-nm light irradiation,the down-conversion NIR-II luminescence could indicate the position glioma and the upconversion NIR-I luminescence could trigger the AIE photosensitizers producing reactive oxygen species to inhibit orthotopic glioma tumor growth in *** results demonstrate that the integration of Dtype neuropeptide,AIE photosensitizers and RENPs could be promising candidates for in vivo NIR-II fluorescence image-guided through-skull PDT treatments of brain tumors.

关键词： aggregation-induced emission D-type neuropeptide glioma photodynamic therapy rare-earth doping nanoparticles

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Macroporous Directed and Interconnected Carbon Architectures Endow Amorphous Silicon Nanodots as Low‑Strain and Fast‑Charging Anode for Lithium‑Ion Batteries

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Nano-Micro Letters 2024年第5期16卷 333-351页

作者： Zhenwei Li Meisheng Han Peilun Yu Junsheng Lin Jie Yu Guangdong Provincial Key laboratory of Semiconductor Optoelectronic materials and Intelligent Photonic Systems Shenzhen Engineering Lab for Supercapacitor MaterialsSchool of Material Science and EngineeringHarbin Institute of TechnologyShenzhenUniversity TownShenzhen 518055People’s Republic of China Songshan Lake materials laboratory Dongguan Dongguan 523808GuangdongPeople’s Republic of China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055People’s Republic of China

Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion ***,we report a unique silicon-carbon composite fabricated by uniformly dis-persing amorphous Si nanodots(SiNDs)in carbon nanospheres(SiNDs/C)that are welded on the wall of the macroporous carbon framework(MPCF)by vertical graphene(VG),labeled as MPCF@VG@SiNDs/*** high dispersity and amor-phous features of ultrasmall SiNDs(~0.7 nm),the flexible and directed electron/Li+transport channels of VG,and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites,rapid Li+transport path,and unique low-strain property during Li+***,the MPCF@VG@SiNDs/C exhibits high cycle stability(1301.4 mAh g^(-1) at 1 A g^(-1) after 1000 cycles without apparent decay)and high rate capacity(910.3 mAh g^(-1),20 A g^(-1))in half cells based on industrial electrode *** assembled pouch full cell delivers a high energy density(1694.0 Wh L^(-1);602.8 Wh kg^(-1))and an excellent fast-charging capability(498.5 Wh kg^(-1),charging for 16.8 min at 3 C).This study opens new possibilities for preparing advanced silicon-carbon com-posite anodes for practical applications.

关键词： Amorphous Si nanodots Low-strain Fast-charging Lithium-ion batteries

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Coupling Co-Ni phosphides for energy-saving alkaline seawater splitting

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Nano research 2024年第6期17卷 4797-4806页

作者： Weijia Liu Wenxian Liu Tong Hou Junyang Ding Zhigui Wang Ruilian Yin Xingyuan San Ligang Feng Jun Luo Xijun Liu State Key laboratory of Featured Metal materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Nonferrous Metals and Featured MaterialsMOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China College of materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Hebei Key laboratory of Optic-electronic Information and materials the College of Physics Science and TechnologyHebei UniversityBaoding 071002China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China ShenSi lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion ***,the fabrication of efficient multifunctional catalysts for this promising technology is of great ***,a heterostructured catalyst comprising CoP and Ni_(2)P on nickel foam(CoP/Ni_(2)P@NF)is reported for hydrazine oxidation(HzOR)-assisted alkaline seawater *** coupling of CoP and Ni_(2)P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and ***,the two-electrode HzOR-assisted alkaline seawater splitting(OHzS)cell based on the CoP/Ni_(2)P@NF required only 0.108 V to deliver 100 mA·cm^(−2),much lower than 1.695 V for alkaline seawater electrolysis ***,the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm^(−2).Furthermore,the CoP/Ni_(2)P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation,methanol oxidation,and urea oxidation in alkaline seawater *** work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H_(2) production.

关键词： seawater splitting heterostructure electrocatalysis hydrazine oxidation reaction hydrogen evolution reaction

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Dynamic lithium-compensation mechanism for densification of garnet-type Li_(7)La_(3)Zr_(2)O_(12)electrolyte by Li_(2)O atmosphere buffer pair

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Nano research 2024年第7期17卷 6184-6191页

作者： Chujun Zheng Ya Chen Haoxin Dong Yan Lu Jun Jin Zhaoyin Wen CAS Key laboratory of materials for Energy Conversion Shanghai Institute of CeramicsChinese Academy of ScienceShanghai 200050China State Key lab High Performance Ceram and Superfine Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Solid-state lithium metal batteries are one of the most promising options for next-generation batteries pursuing high-energy density and ***,the inevitable volatilization of lithium compounds during sintering leads to low relative density and low ionic conductivity of solid-state ***,the dynamic lithium-compensation mechanism is proposed to facilitate the densification of Ta-substituted garnet-type electrolyte(Li_(6.5)La_(3)Zr_(1.5)Ta_(0.5)O_(12)(LLZT))through the reversible manipulating of Li_(2)O ***_(2)ZrO_(3)is used as mother powder additive,which reacts with Li_(2)O in sintering atmosphere and forms Li_(6)Zr_(2)O_(7).Li_(2)ZrO_(3)/Li_(6)Zr_(2)O_(7)buffer pair manipulates the sintering Li_(2)O atmosphere,which is vital for LLZT,within the Li_(2)O partial pressure range corresponding to Li_(2)ZrO_(3)and Li_(6)Zr_(2)O_(7).Furthermore,the reversibility mechanism of buffer pair for Li_(2)O absorption and release is *** obtained LLZT exhibits a relative density of over 96%and an ionic conductivity exceeding 7×10^(−4)S·cm^(−1)with no abnormal grain *** symmetric cell demonstrates an excellent lithium dendrite suppressing ability(stable cycling at a current density of 0.3 mA·cm^(−2)for over 1000 h).Such dynamic lithium-compensation strategy has been successfully applied in atmosphere manipulation of LLZT sintering process,which reduces the dependence of LLZT on the Li_(2)O atmosphere,making it conducive to large-scale preparation of electrolyte ceramics.

关键词： solid-state batteries garnet-type electrolyte high-density electrolyte dynamic lithium-compensation buffer pair

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Synthesis,chemical bonding and reactivity of new medium-sized polyarsenides

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Chinese Chemical Letters 2024年第7期35卷 497-501页

作者： Xu-Hui Yue Xiang-Wen Zhang Hui-Min He Lei Qiao Zhong-Ming Sun State Key laboratory of Element-Organic Chemistry Tianjin Key Lab for Institution Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of Physics Institute of Computational and Applied PhysicsTaiyuan Normal UniversityJinzhong 030619China

Gaining an understanding of the growth mechanism from single atoms to clusters and bulk materials continues to present a ***,it is important to explore the evolving trends of clusters in the structure and properties during the size *** this work,we report the synthesis and characterization of two medium-sized chain-like polyarsenic anions.[As_(21)]^(3-)represents a trimeric example of polyarsenic anion assembled through oxidative coupling of As_(7)^(3-)*** anion As_(18)^(4-)included in[As_(18)MO_(2)(CO)_(8)]^(4-)is regarded as formed by two realgar-type As_(8)subunits connected by a dinuclear AsAs *** As_(18)cluster was previously predicted by theory,and this is the first time successfully synthesized using wet chemistry ***,small-sized polyarsenides As_(2)^(2-)and As_(10)^(2-)were found in compound[K(18-crown-6)]_(3)[As_(10)]_(0.5)[As_(4){Mo(CO)_(3)}_(2)]_(0.5)·*** these,the former exhibits coordination with metal ***-crystal X-ray diffraction combined with quantum chemical calculations revealed the formation of double bonded As_(2)^(2-)stabilized by metal carbonyl *** work demonstrates a novel synthetic approach for the preparation of new polyarsenides and highlights their intriguing bonding characteristics,laying the foundation for the synthesis of such compounds and paving the way for their potential applications.

关键词： Polyarsenide Zintl anions Chain-like cluster DFT calculations AdNDP

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A strategy based on water soluble coal tar pitches to construct MnO_(2)@C composite materials with high electrochemical performance

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Science China(Technological Sciences) 2024年第1期67卷 311-320页

作者： LIU Bo WANG Kun GUO ZhaoQi HAN BeiBei XU GuiYing JU DongYing AN BaiGang LI YongCheng NI ZhenYong ZHOU WeiMin Key laboratory of Energy materials and Electrochemistry research Liaoning Province University of Science and Technology LiaoningAnshan 114051China Advanced Science research laboratory Saitama Institute of TechnologyFusaiji 1690Japan Liaoning Starry Sky Sodium Battery Co. Ltd.Anshan 114051China Sinosteel Anshan research Institute of Thermo-Energy Co. Ltd.Anshan 114051China State Key laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228China Key laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China

The water soluble coal tar pitches(WS-CTPs)were successfully prepared and used to construct the MnO_(2)@C composite materials by a hydrothermal *** is interestingly observed that the structures and morphologies of MnO_(2)@C materials can be controlled by controlling the dosages of WS-CTPs and ***,it is aware that MnO_(2)exists in the MnO_(2)@C materials in an amorphous *** with MnO_(2),MnO_(2)@C materials output a remarkable improvement in electrochemical *** instance,MnO_(2)@C-0.3 shows the storage capacity at 965.7 mA h g^(−1)after 300 cycles at a current density of 0.1 A g^(−1).In addition,after 600 cycles at a current density of 1.0 A g^(−1),the storage capacity of MnO_(2)@C-0.3 still keeps 450.3 mA h g^(−1),indicating that MnO_(2)@C-0.3 owns tremendous cycle stability at a high current *** view of the fact that the coal tar pitches possess great cost advantages,the strategy of using WS-CTPs as a carbon source to cover the metal oxides is a competitive way to expand the application of metal oxides in the fabrication of electrodes of LIBs.

关键词： water soluble coal tar pitches MnO_(2) composite materials lithium ion batteries(LIBs) energy storage systems(ESSs) coal tar pitches

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Structural Elucidation of the Polymeric Condensed Tannins of Acacia nilotica Subspecies by ^(13)C NMR, MALDI-TOF and TMA as Sources of Bioadhesives

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Journal of Renewable materials 2024年第7期12卷 1291-1310页

作者： Zeinab Osman Antonio Pizzi Bertrand Charrier Institute of Engineering research and materials Technology National Center for ResearchP.O.Box 2404KhartoumSudan ENSTIB-LERMAB University of Lorraine27 rue Philippe SeguinEpinal88000France Department of materials Science and Engineering Institute of Analytical Sciences and Physico-Chemistry for the Environment and Materials-Xylomat(IPREM-UMR5254)University of Pau and the Adour RegionE2S UPPACNRSMont de Marsan40004France

Tannin was extracted from different subspecies of Acacia nilotica,Acacia nilotica nilotica(Ann),Acacia nilotica tomentosa(Ant)and Acacia nilotica adansonii(Ana).The aim was to elucidate their structure and evaluate their reactivity as bioadhesives in the wood *** extracts were prepared by hot water extraction(90°C tem-perature).Their gel time with paraformaldehyde was used atﬁrst to compare their *** tannin contents and the percentage of total polyphenolic materials in different solutions of the extracts spray dried powder were determined by the hide powder *** solutions(47%)were tested by both MALDI ToF,*** thermomechanical analysis(TMA)was performed to evaluate their modulus of elasticity(MOE)at different *** gel times of all the three tannin extracts showed that their reactivity and it was com-parable to other known procyanidin/prodelphinidin tannin extract ***,Ann and Ant showed highest per-cent of total polyphenolic materials at 70%,64%,and 57%,*** 13CNMR spectra showed that the three subspecies of condensed tannins were mainly constituted of procyanidins(PC)and prodelphinidins(PD)in slightly different ***(56.5%PC and 43.4%PD),Ant(57%PC and 43%PD)and Ana(58%PC and 42%PD).MALDI–TOF spectra showed the presence ofﬂavonoid monomers,and oligomers some of which linked to short carbohydrates monomers or *** revealed that the three types of tannins had high MOE at their initial pH(5).

关键词： Acacia nilotica condensed tannins procyanidins prodelphinidins 13C NMR MALDI-ToF

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Emerging hierarchical mesoporous materials of covalent organic frameworks

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Science China Chemistry 2024年第9期67卷 2796-2802页

作者： Lingyan Huang Wenda Li Hongyi Zhang Shanzhe Ke Hao Chen Jianwei Fu Chengbin Jing Jiangong Cheng Shaohua Liu State Key laboratory of Precision Spectroscopy Engineering research Center of Nanophotonics & Advanced Instrument (Ministry of Education) School of Physics and Electronic Science East China Normal University School of materials Science and Engineering Zhengzhou University State Key lab of Transducer Technology Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences

Benefiting from abundant exposed active sites, minimized diffusion resistance of guest molecules, facilitated mass transfer process and enhanced storage capacity, covalent organic frameworks (COFs) have gained widespread scientific attention [1–4]. Further construction of mesopores regarding pore engineering (pore size, pore geometry, pore volume, and framework compositions) in COFs can improve mass transport, accessibility as well as size-selectivity of the special guest moieties, thus exhibiting potential in catalysis,energy storage and separation and so on [5,6].

关键词： FABRICATION COMPOSITE

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低温热循环加速非晶合金剪切带在室温的结构弛豫

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Science China materials 2024年第3期67卷 974-982页

作者：魏玉锋潘杰孙永昊李宁张诚汪卫华柳林 School of materials Science and Engineering State Key Lab for Materials Processing and Die&Mold TechnologyHuazhong University of Science and TechnologyWuhan 430074China Shenyang National laboratory for materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Institute of Physics Chinese Academy of SciencesBeijing 100190China Songshan Lake materials laboratory Dongguan 523808China

低温热循环是实现非晶合金结构回春的一种简单有效方法,但某些非晶合金在低温热循环处理后发生弛豫而不是回春.本研究通过在非晶合金中引入剪切带,在同一块样品上获得了不同区域初始能量不同的非晶合金,系统地研究了不同初始状态对低温... 详细信息

低温热循环是实现非晶合金结构回春的一种简单有效方法,但某些非晶合金在低温热循环处理后发生弛豫而不是回春.本研究通过在非晶合金中引入剪切带,在同一块样品上获得了不同区域初始能量不同的非晶合金,系统地研究了不同初始状态对低温热循环处理效果的影响.研究结果发现,在经过低温热循环处理后,同一试样中的剪切带发生结构弛豫,而基体发生结构回春.类似的双向变化趋势还可以从显微硬度、纳米压痕曲线以及压痕形状的变化上得到验证.经历了100次低温热循环处理后,剪切带和基体的焓和硬度均收敛到一个平衡值.低温热循环能够加速剪切带的结构弛豫,实现了在低温热循环的上限温度上做长时间退火所达不到的状态.文中还采用自由体积模型对实验结果进行分析,阐明了非晶合金的初始状态影响其结构演化方向的机理.本研究为低温热循环处理非晶合金提供了新见解,阐明非晶合金初始状态在其焓变方向上的关键作用.

关键词： metallic glasses cryogenic thermal-cycling rejuvenation relaxation energy state

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