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Interfacial charge effects of supported-metal-cluster heterostructures on azo hydrogenation catalyzation

Nano Research 2024年第5期17卷 3853-3862页

作者： Zhenhua Gu Jingli Zhang Zijun Zhang Qingxue Mu Liangchong Yu Taolei Sun Lei Shen Guanbin Gao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases School of ChemistryChemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070China

The impact of interfacial charge on catalytic performance of supported-metal-cluster(SMC)heterostructures remains unclear,hindering efforts to develop high-performance SMC *** we systematically investigated interfacial charge effects of SMCs using a model system of graphene-supported gold-nanoclusters(AuNCs/rGO)for azo *** types of SMCs with different interfacial charges were synthesized by anchoring electropositive 2-aminoethanethiol(CSH),amphoteric cysteine(Cys),and electronegative 3-mercaptopropionic-acid(MPA)onto AuNCs/rGO,*** three SMCs exhibited high and selective catalytic activity to azo-hydrogenation in four representative azo *** catalytic activity of Cys@AuNCs/rGO was lower than that of CSH@AuNCs/rGO but higher than that of MPA@AuNCs/***,the cyclic stability of Cys@AuNCs/rGO was inferior to that of both CSH@AuNCs/rGO and MPA@AuNCs/*** mechanistic studies revealed that amino ligands modified CSH@AuNCs and Cys@AuNCs agglomerated into large-size gold nanoparticles on rGO surface during catalytic reaction under NaBH_(4) action,leading to reduced efficiency and cyclic ***,non-amino ligand modified MPA@AuNCs only partially detached from rGO surface without agglomeration,resulting in better cyclic *** of amino groups in ligands such as modifying-NH_(3)^(+)group in Cys into imine to form N-isobutyryl-L-cysteine(NIBC)substantially improved the cyclic stability while maintaining the high activity in the NIBC@AuNCs/rGO catalyst *** work provides an approach for developing a highly-active and stable SMC heterostructure catalyst via manipulating interfacial charges in SMC.

关键词： interfacial charge effect supported-metal-cluster catalyst azo hydrogenation graphene supported gold nanoclusters

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Photo-responsive Carboxymethyl Chitosan/Laponite Hydrogel as a Potential Spinal Cord Injury Scaffold:Characterization and Cytocompatibility Study

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Journal of Wuhan University of technology(materials Science) 2024年第6期39卷 1628-1636页

作者： Jayanti Parajuli LI Yongtao CHANG Likun YE Liyuan HAN Yingchao YIN Yixia State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Biomedical Materials and Engineering Research Center of Hubei Province Wuhan University of TechnologyWuhan 430070China

We synthesized photo-responsive carboxymethyl chitosan(CMC-MA)via free radical polymerization and utilized nanoclay laponite(LAP)as an inorganic crosslinking agent to develop an injectable and 3D-printable CMC-MA/LAP *** determined the optimal ratio of 2.5 w/v%CMC-MA/7.5 w/v%LAP based on injection molding,compression modulus,swelling properties,rheological properties,and 3D printing properties of the hydrogel ***-vitro cytocompatibility experiments showed that both CMC-MA and CMC-MA/LAP hydrogel had no inhibitory effect on cell proliferation and can promote cell growth when cultured on the surface of the hydrogel ***,the hydrogel containing LAP particles significantly facilitated cell adhesion(>60%)compared with the hydrogel without LAP(20%).Our findings demonstrate that the CMC-MA/LAP hydrogel has great potential for tissue repair in neural tissue engineering.

关键词： neural injectable hydrogels spinal cord injury CMC-MA/LAP hydrogel cytocompatibility

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Hierarchically Macroporous Zeolite ZSM-5 Microspheres for Efficient Catalysis

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Chemical Research in Chinese Universities 2024年第4期40卷 704-711页

作者： ZHENG Mingdan CHEN Ya LIU Zhan LYU Jiamin YE Bo SUN Ming-Hui CHEN Li-Hua SU Bao-Lian State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070P.R.China Laboratory of Inorganic Materials Chemistry(CMI) University of Namur5000NamurWalloniaBelgium

Hollow zeolite microspheres have recently attracted much attention for their applications in catalysis,microreactors and ***,we present hierarchically structured zeolite ZSM-5 microspheres with unique,abundant macropores that allow more efficient use for *** hierarchically macroporous zeolite ZSM-5 microspheres are synthesized under the assistance of water/oil emulsions and using polystyrene nanospheres as *** zeolite microsphere is assembled by uniform hollow zeolite *** large inner cavities and thin zeolite shells lead to smaller diffusion channel and higher improved accessibility to active sites,contributing to high catalytic performance in the catalytic conversion of benzyl alcohol in *** novel zeolite microspheres with impressive performance will be applied to numerous other industrial catalytic reactions.

关键词： Hierarchically porous structure Hollow structure Microsphere Zeolite ZSM-5 Alkylation

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Bottom-up synthesis of 2D heterostructures enables effective polysulfides inhibition and conversion

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Nano Research 2023年第6期16卷 8488-8496页

作者： Ge Zhang Cheng Zhou Juncai Long Yan Li Lei Lv Kaijian Yan Xinhui Chen Chenxu Dong Xu Xu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

Due to the high theoretical capacity and energy density,lithium-sulfur(Li-S)batteries have good commercial ***,shuttle effect of soluble lithium polysulfides(LiPSs)formed by sulfur reduction has severely limited the further development of Li-S *** this work,the two-dimensional(2D)MXene-metal-organic framework(MOF)(Ti_(3)C_(2)T_(x)-CoBDC(BDC:1,4-benzenedicarboxylate))heterostructures were employed to modify the separator to inhibit the shuttle effect and facilitate the conversion of the soluble ***,a bottom-up synthesis strategy was adopted to synthesize the 2D MXene-MOF heterogeneous layered *** high specific surface area,in which the catalytic metal atoms not only restrain the shuttle effect of polysulfides but also exhibit excellent redox electrocatalytic *** cell with Ti_(3)C_(2)T_(x)-CoBDC@PP(PP:polypropylene)separator has a high initial capacity of 1255 mAh·g^(−1)at 0.5 *** the current density is 2 C,the battery has a capacity retention rate of 94.4%after 600 cycles,with the fading rate of only 0.01%per ***,with a sulfur loading of 7.5 mg·cm^(−2),the battery shows the discharge capacity of 1096 mAh·g^(−1)at 0.2 C and exhibits excellent cycling *** work offers novel insights into the application of MOF and MXene heterostructures in Li-S batteries.

关键词： nanosheets lithium-sulfur batteries MXenes modified separators shuttle inhibition

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Energy-dispersive X-ray Spectroscopy for the Quantitative Analysis of Pyrite Thin Specimens

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Journal of Wuhan University of technology(materials Science) 2023年第6期38卷 1304-1310页

作者： LUO Tingting GUO Yi DENG Zhao LIU Xiaoqing SUN Zhenya QI Yanyuan YANG Meijun Center for Materials Research and Analysis Testing Wuhan University of Technology Wuhan 430070China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070Wuhan

To explore ways to improve the accuracy of quantitative analysis of samples in the micrometer to nanometer range of magnitudes,we adopted analytical transmission electron microscopy(AEM/EDS)for qualitative and quantitative analysis of pyrite ***,the k factor of pyrite is calculated *** develop an appropriate non-standard quantitative analysis model for pyrite materials,the experimentally calculated k factor is compared with that estimated from the non-standard quantitative analytical model of the instrument *** experimental findings demonstrate that the EDS attached to a TEM can be employed for precise quantitative analysis of micro-and nanoscale regions of pyrite ***,it serves as a reference for improving the results of the EDS quantitative analysis of other sulfides.

关键词： analytical transmission electron microscopy(AEM) energy dispersive X-ray spectroscopy(EDS) pyrite thin specimen quantitative analysis

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Cr-doped Na_(3)V_(2)(PO_(4))_(3)@C enables high-capacity with V^(2+)/V^(5+)reaction and stable sodium storage

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Journal of materials Science & technology 2023年第34期165卷 1-7页

作者： Bo Mai Boyu Xing Yunfan Yue Nianyao Cai Congcong Cai Sitian Lian Hao Fan Mengyu Yan Ting Zhu Ping Hu Xuewen Wang Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong LaboratoryFoshan 528216China

Due to its abundant sodium content and low cost,sodium-ion battery(SIB)has become an effective substitute and supplement for lithium-ion batteries,which has a broad development prospect in largescale energy storage ***-super-ionic conductor(NASICON)structural materials have stable 3D skeleton structures and open Na+transport channels,which is a very promising SIB cathode *** in the typical NASICON material Na_(3)V_(2)(PO_(4))_(3)(NVP),the number of electrons involved in NVP per formula unit is less than 2 at the stable voltage window,which limits the further improvement of battery *** this work,we report another NASICON structured Na_(3)V_(4/3)Cr_(2/3)(PO_(4))_(3)@C(NVCP@C),which is obtained by Cr-doped NVP through spray *** taking full advantage of the voltage platforms of V^(5+/4+),V^(4+/3+),and V^(3+/2+)in the window of 1.5-4.4 V,NVCP@C delivered a high discharge capacity(175 mAh g^(-1))and durable cyclability(86%capacity retention for 2000 cycles).In-situ X-ray diffraction results demonstrate that the reversible structural evolution accompanies by solid-solution reaction and two-phase reaction mechanisms co-exist during charge/discharge *** coupled with Na^(+)preembedded hard carbon(HC),the assembled NVCP@C//HC full cell delivers a high capacity(105 mAh g^(-1))and long cycling performance(70%after 1000 cycles).This Cr-doped NVP method offers new insights into the design of high-energy NASICON-structured cathode materials.

关键词： Sodium-ion batteries NASICON Na_(3)V_(4/3)Cr_(2/3)(PO_(4))_(3)@C Spray drying V^(2+)/V^(5+)reaction

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Constructing a stable cobalt-nitrogen-carbon air cathode from coordinatively unsaturated zeolitic-imidazole frameworks for rechargeable zinc-air batteries

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Nano Research 2022年第7期15卷 5895-5901页

作者： Tingting Wang Meng Liu Somboon Chaemchuen Jichao Wang Ye Yuan Cheng Chen Ang Qiao Francis Verpoort Zongkui Kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Zeolitic-imidazole frameworks(ZIFs)derivations have widely emerged as an efficient air cathode of zinc-air batteries(ZABs)due to excellent bifunctional oxygen electrocatalysis ***,they are not stable enough for long-term operation of rechargeable ZABs because of weak association with current collector,especially under bending conditions for flexible ZAB ***,we show that by purposely designing coordinatively unsaturated ZIFs via a facile morphology regulation,which can be chemically linked on acid-treated carbon cloth,a stable Co-N-C air cathode is therefore derived where Co nanoparticles(NPs)are uniformly confined within the Co-N-C matrix on carbon cloth(Co/Co-N-C/CC).Specifically,when without being stabilized from carbon cloth,the pyrolysis of ZIFs with different unsaturated coordination levels has a negligible impact on the bifunctional oxygen-catalyzed *** optimal Co/Co-N-C/CC catalyst assembled ZAB possesses a large open circuit voltage of 1.415 V and a high peak power density of 163 mW·cm^(−2) as well as excellent cycling durability upon 630 discharge–charge cycles with 61%voltage efficiency remained,largely exceeding those of a benchmark Pt/C-IrO_(2) catalyst assembled *** synergy between Co NPs and active Co-N-C sites via electronic interaction induces the outstanding bifunctional oxygen-catalyzed activity and cathode *** present work highlights the importance of unsaturated coordination structures in ZIFs precursors for the performance of derived nanostructures in integrated electrodes.

关键词： coordinatively unsaturated zeolitic-imidazole frameworks(ZIFs) cobalt-nitrogen-carbon bifunctional air electrodes zincair battery flexible electrode

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Donor-acceptor conjugated copolymer with high thermoelectric performance:A case study of the oxidation process within chemical doping

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Chinese Physics B 2022年第2期31卷 80-88页

作者： Liangjun Chen Wei Wang Shengqiang Xiao Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

The doping process and thermoelectric properties of donor-acceptor(D-A)type copolymers are investigated with the representative poly([2,6-4,8-di(5-ethylhexylthienyl)benzo[1,2-b;3,3-b]dithiophene]3-fluoro-2-[(2-ethylhexyl)-carbonyl]thieno[3,4-b]thiophenediyl))(PTB7-Th).The PTB7-Th is doped by Fe Cl;and only polarons are induced in its doped *** results reveal that the electron-rich donor units within PTB7-Th lose electrons preferentially at the initial stage of the oxidation and then the acceptor units begin to be oxidized at a high doping *** energy levels of polarons and the Fermi level of the doped PTB7-Th remain almost unchange with different doping ***,the morphology of the PTB7-Th films could be deteriorated as the doping levels are improved,which is one of the main reasons for the decrease of electrical conductivity at the later stage of *** best electrical conductivity and power factor are obtained to be 42.3 S·cm^(-1);and 33.9μW·mK^(-1),respectively,in the doped PTB7-Th film at room *** power factor is further improved to 38.3μW·mK^(-1);at 75℃.This work may provide meaningful experience for development of D-A type thermoelectric copolymers and may further improve the doping efficiency.

关键词： donor-acceptor copolymer doping oxidization process thermoelectric performance

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Improving Cyclic Stability and Rate Performance of Lithium Ion Batteries Using La^(3+)Modified LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)Cathode materials

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Journal of Wuhan University of technology(materials Science) 2023年第4期38卷 735-742页

作者：杜玉喆 RUAN Zhefei ZHANG Ruiming 张海宁 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Foshan528200China

La_(4)NiLiO_(8)-coated NCM622 samples were prepared through a sol-gel method,and the electrochemical performance as cathode materials was *** is revealed that part of the introduced La^(3+)ions produce a coating layer on the surface of NCM622 particles,while the rest occupy the 3b position of the *** optimized sample exhibits a capacity retention of 96.54%after 100 cycles under 1C rate with a discharge specific capacity of 117.54 mAh·g^(-1)under 5C rate,much higher than those of the unmodified *** results show that the addition of La^(3+)ion can greatly improve the cyclic stability and the rate performance of NCM622.

关键词： lithium ion batter La^(3+)doping NCM622 cycling stability rate performance

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Quantum dots boost large-view NIR-II imaging with high fidelity for fluorescence-guided tumor surgery

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Chinese Chemical Letters 2024年第12期35卷 497-502页

作者： Biao Huang Tao Tang Fushou Liu Shi-Hui Chen Zhi-Ling Zhang Mingxi Zhang Ran Cui College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Owing to the high spatiotemporal resolution,the second near-infrared(NIR-II)imaging window can provide high imaging contrast with diminished tissue autofluorescence and suppressed photon scattering to pinpoint the locations for tumor *** to the unique optical properties and excellent fluorescence performance,quantum dots(QDs)are regarded as ideal nanoprobes for fluorescence-guided surgery(FGS).Moreover,QDs can be excited by a variety of light sources owing to the continuous and wide absorption ***,light-emitting diode(LED)was used as the excitation source of QDs-based nanoprobes to realize FGS of tumor with high *** the LED light could irradiate a large region with consistent light intensity,signal distortion at the edge of imaging field was *** signal intensity of the view edges under LED excitation can be improved by about 5 times compared to laser ***,more micro-vessels and smaller tumors(Vtumor<5 mm^(2))could be detected,thus providing more precise guidance for tumor resection surgery.

关键词： NIR-II imaging Fluorescence-guided surgery Quantum dots Light-emitting diode Tumor imaging

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