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Chinese Chemical Letters 2024年第4期35卷 382-388页

作者： Shiyu Hou Maolin sun Liming Cao Chaoming liang Jiaxin Yang Xinggui Zhou Jinxing Ye Ruihua Cheng School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China School of Pharmacy East China University of Science and TechnologyShanghai 200237China

Microchannels enable the fast and efficient mixing of multiphase *** this study, a millimeter-scale three-dimensional(3D) circular cyclone-type microreactor was designed for the *** flow characteristics and mixing intensity were simulated by computational fluid dynamics simulations at a flow rate range of 12–96 m L/min using a water/ethyl acetate *** the 3D variable-diameter structure,the microreactor induced paired opposite vortices and abruptly changed the local pressure to achieve a stable turbulent effect within the theoretical range of laminar *** injection simulations indicated that sufficient mixing units successfully promote fluid ***-coupling experiments showed a segregation index of X_S= 0.00,039 within a residence time of 9 *** experiments on the nbutanol/succinic acid/water system showed that the 3D circular cyclone-type microreactor achieved 100%extraction efficiency(E) in 4.25 s, and the overall volume mass transfer coefficient(K_La) reached 0.05–1.5s^(-1) in 12–96 m L/*** isolated yield of the phase transfer alkylation and oxidation reactions in the 3D circular cyclone-type microreactor achieved 99% within 36 s, which was superior to the coil microreactor and batch reactor.

关键词： Microfluidics Passive microreactor CFD simulation Extraction Liquid-liquid biphase reaction

Facile preparation of a SiC@SiO_(2)nanowire-toughened ZrB_(2)-SiC/SiC bilayer coating with good interfacial bonding,high toughness,and excellent cyclic ablation resistance on C/CA composites

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Journal of Advanced Ceramics 2024年第4期13卷 486-495页

作者： Meng Yan Chenglong Hu Jian Li Shengyang Pang Bohui sun Rida Zhao Bin liang Rui Luo Sufang Tang Shi-Changxu Innovation Center for Advanced Materials Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China

Preparing antioxidant coatings to address the inherent oxidation sensitivity of carbon fiber-reinforced carbon aerogel(C/CA)composites is a feasible way to promote their application in oxidizing environments as thermal insulation ***,preparing the coatings with excellent oxidation and ablation resistance while avoiding evident damage to the C/CA substrate still remains a ***,a SiC@SiO_(2)nanowire-toughened ZrB2–SiC/SiC bilayer coating with a large thickness of 500μm was prepared on C/CA using a one-step low-temperature reaction sintering method,which simultaneously formed a sintered outer layer with even-distributed nanowires and a siliconized gradient inner *** courtesy of the synergic thermal response of the layers and the crack deflection induced by the nanowires,the resulting coating has moderate residual compressive stress of 0.08–1.22 GPa in the interface,high interfacial bonding strength of 6.02 MPa,and good fracture toughness of 4.36 MPa·m^(1/2).Benefited from the optimum components and improved structure,the coating shows excellent cyclic ablation resistance with linear ablation rates of 0.1μm/s at 1650℃for 1500 s(300 s×5 cycles)and 0.4μm/s at 1850℃for 900 s(300 s×3 cycles).The one-step preparation strategy contributes to little damage to the substrate,thus showing the well-preserved mechanical and thermal insulation properties.

关键词： coating carbon fiber reinforced carbon aerogel(C/CA)composites toughness interface residual stress

Enzymatic self-assembly/disassembly turns “ON”/“OFF” the mimetic hydrolytic activity of histidine nanofibers

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Science China Chemistry 2024年第2期67卷 517-522页

作者： Xianbao sun Manli Wang Xiaoyang Liu Wenjun Zhan Guangqiong Xu Qiaochu Jiang Hai-Dong Xu Fuqiang Wang Gaolin liang State Key Laboratory of Digital Medical Engineering School of Biological Science and Medical EngineeringSoutheast UniversityNanjing210096China Analysis Center Nanjing Medical UniversityNanjing210029China

Mimetic enzymes are devised as alternates or supplements of natural enzymes in broad fields but regulating their activities in a switchable manner remains ***,we proposed an enzymatic self-assembly/disassembly strategy to address this issue.A peptide molecule Nap FFEYIH(YH) was rationally designed which,after self-assembling into nanofibers,lined up the histidine moieties to form active hydrolysis centers for mimicking hydrolase *** dephosphorylation of Nap FFEYp IH(Yp H) by alkaline phosphatase to yield YH also turned “ON” the hydrolase *** turn,phosphorylation of YH by phosphokinase epidermal growth factor receptor to yield Yp H disassembled the nanofibers and thus turned the activity “OFF”.As such,the “ON”/“OFF” of the mimetic hydrolase activities could be regulated under physiological conditions through ALP/EGFR-mediated self-assembly/disassembly of histidine *** work provides a feasible strategy for the on-demand fabrication of artificial enzymes with controllable and superior activities.

关键词： disassembly hydrolytic activity mimetic enzyme phosphorylation self-assembly

Mechanistic investigation on Ag-Cu_(2)O in electrocatalytic CO_(2) to CH_(4) by in situ/operando spectroscopic and theoretical analysis

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Journal of Energy Chemistry 2024年第1期88卷 521-531,I0012页

作者： Min sun Luxiao Zhang Fuli Tian Jiaxin Li Yanqiu Lei heng Zhang Lifeng Han Zhihua Guo Yonghui Gao Fenrong Liu Yan Wang Luhui Wang Shanghong Zeng School of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina Key Laboratory of Medicinal and Edible Plants Resources of Hainan Province Hainan Vocational University of Science and TechnologyHaikou 571126HainanChina State Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030Inner MongoliaChina Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control Zhejiang Ocean UniversityZhoushan 316022ZhejiangChina

Silver-copper electrocatalysts have demonstrated effectively catalytic performance in electroreduction CO_(2) toward CH_(4),yet a revealing insight into the reaction pathway and mechanism has remained ***,we construct chemically bonded Ag-Cu_(2)O boundaries,in which the complete reduction of Cu_(2)O to Cu has been strongly impeded owing to the presence of surface Ag *** interfacial confinement effect helps to maintain Cu^(+)sites at the Ag-Cu_(2)O *** in situ/operando spectroscopy and theoretical simulations,it is revealed that CO_(2) is enriched at the Ag-Cu_(2)O boundaries due to the enhanced physisorption and chemisorption to CO_(2),activating CO_(2) to form the stable intermediate^(*)*** boundaries between Ag shell and the Cu_(2)O mediate local^(*)CO coverage and promote^(*)CHO intermediate formation,consequently facilitating CO_(2)-to-CH_(4) *** work not only reveals the structure-activity relationships but also offers insights into the reaction mechanism on Ag-Cu catalysts for efficient electrocatalytic CO_(2) reduction.

关键词： Ag shell Interfacial confinement effect Cu~+ Local*CO coverage CO_(2)reduction

X-ray excited Mn^(2+)-doped persistent luminescence materials with biological window emission for in vivo bioimaging

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Journal of Rare Earths 2024年第1期42卷 28-35,I0001页

作者： Hanrun Zheng Lin Liu Yi’ang Li Rui Rong liang Song Junpeng Shi Jing Teng Xia sun Yun Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of the Chinese Academy of Sciences Beijing100049China Xiamen Hospital of Traditional Chinese Medicine Xiamen361015China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China

In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity *** metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window ***,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence *** excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 *** *** can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence *** addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in *** LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be *** the persistent luminescence decays,LYGM can be re-excited for repeated ***,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.

关键词： Persistent luminescence X-ray Biological window In vivo imaging Rare earths

Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable Li metal batteries

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Nano Research 2024年第6期17卷 5216-5223页

作者： Guocheng Li Kang liang Yuanjian Li Xiangrui Duan Lin Fu Zhao Cai Zhaofu Zhang Jiangnan Dai Yongming sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China The Institute of Technological Sciences Wuhan UniversityWuhan 430074China Faculty of Materials Science and Chemistry China University of Geoscience(Wuhan)Wuhan 430074China

Employing quasi-solid-state gel polymer electrolyte(GPE)instead of the liquid counterpart has been regarded as a promising strategy for improving the electrochemical performance of Li metal ***,the poor and uneven interfacial contact between Li metal anode and GPE could cause large interfacial resistance and electrochemical Li stripping/plating inhomogeneity,deteriorating the electrochemical ***,we proposed that the functional component of composite anode could work as the catalyst to promote the in situ polymerization reaction,and we experimentally realized the integration of polymerized-dioxolane electrolyte and Li/Li_(22)Sn_(5)/LiF composite electrode with low interfacial resistance and good stability by in situ catalyzation ***,the reaction kinetics and stability of metallic Li anode were significantly *** a demonstration,symmetric cell using such a GPE-Li/Li_(22)Sn_(5)/LiF integration achieved stable cycling beyond 250 cycles with small potential hysteresis of 25 mV at 1 mA·cm^(−2)and 1 mAh·cm^(−2),far outperforming the counterpart regular GPE on pure *** with LiNi0.5Co0.3Mn0.2O2,the full cell with the GPE-Li/Li_(22)Sn_(5)/LiF integration maintained 85.7%of the original capacity after 100 cycles at 0.5 C(1 C=200 mA·g^(−1)).Our research provides a promising strategy for reducing the resistance between GPE and Li metal anode,and realizes Li metal batteries with enhance electrochemical performance.

关键词： catalyzation polymerization interface resistance interfacial stability Li metal batteries electrochemical performance

Optical Fibre Communication Feature Analysis and Small Sample Fault Diagnosis Based on VMD-FE and Fuzzy Clustering

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Energy Engineering 2024年第1期121卷 203-219页

作者： Xiangqun Li Jiawen liang Jinyu Zhu Shengping Shi Fangyu Ding Jianpeng sun Bo Liu Gannan Power Supply Company of State Grid Gansu Electric Power Supply Company Hezuo747000China Digital Communication Department Gannan Power Supply Company of State Grid Gansu Electric Power Supply CompanyHezuo747000China

To solve the problems of a few optical fibre line fault samples and the inefficiency of manual communication optical fibre fault diagnosis,this paper proposes a communication optical fibre fault diagnosis model based on variational modal decomposition(VMD),fuzzy entropy(FE)and fuzzy clustering(FC).Firstly,based on the OTDR curve data collected in the field,VMD is used to extract the different modal components(IMF)of the original signal and calculate the fuzzy entropy(FE)values of different components to characterize the subtle differences between *** fuzzy entropy of each curve is used as the feature vector,which in turn constructs the communication optical fibre feature vector matrix,and the fuzzy clustering algorithm is used to achieve fault diagnosis of faulty optical *** VMD-FE combination can extract subtle differences in features,and the fuzzy clustering algorithm does not require sample *** experimental results show that the model in this paper has high accuracy and is relevant to the maintenance of communication optical fibre when compared with existing feature extraction models and traditional machine learning models.

关键词： Optical fibre fault diagnosis OTDR curve variational mode decomposition fuzzy entropy fuzzy clustering

Interactions of phenol and benzaldehyde in electrocatalytic upgrading process

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Chinese Chemical Letters 2024年第2期35卷 464-468页

作者： Lan liang Chuanbin Wang Xukai Lu Yunan sun Beibei Yan Ning Li Guanyi Chen Li'an Hou School of Environmental Science and Engineering Tianjin Key Lab of Biomass/Wastes UtilizationTianjin UniversityTianjin 300350China School of Mechanical Engineering Tianjin University of CommerceTianjin 300134China Georgia Tech Shenzhen Institute Tianjin UniversityShenzhen 518071China High Tech Inst Beijing Beijing 100085China

Biomass pyrolysis oil can be improved effectively by electrocatalytic hydrogenation(ECH).However,the unclear interactions among different components lead to low bio-oil upgrading efficiency in the conversion ***,benzaldehyde and phenol,as common compounds in bio-oil,were chosen as model *** interactions between the two components were explored in the ECH process by combining experiments and theoretical *** showed that phenol could accelerate the conversion of benzaldehyde in the *** selectivity of benzyl alcohol was increased from 60.9%of unadded phenol to 99.1%with 30 mmol/L phenol concentration at 5 *** inhibited the ECH of *** the presence of benzaldehyde,the conversion rate of phenol was below 10.0%with no cyclohexanone and cyclohexanol formation at 5 *** density functional theory(DFT)calculations revealed that the phenol could promote the adsorption of benzaldehyde and facilitate the targeted conversion of benzaldehyde on the active site by lowering the reaction energy *** research on the interaction between phenol and benzaldehyde in the ECH provides a theoretical basis for the application of ECH in practical bio-oil upgrading.

关键词： Interaction Bio-oil Electrocatalytic hydrogenation Phenol Benzaldehyde

A Fluorine-Functionalized 3D Covalent Organic Framework with Entangled 2D Layers

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Chinese Journal of Polymer Science 2024年第8期42卷 1210-1216页

作者： Li-Bang Xiao Zi-Han Wu Jun-Jie Xin Yuan-Peng Cheng Bo Gui Jun-liang sun Cheng Wang College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China College of Chemistry and Molecular Engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing 100871China

Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped ***,we report the design and synthesis of a fluorine functionalized 3DCOF(3D-An-COF-F)formed by entangled 2D sql *** structure of 3D-An-COF-F was determined by the combination of continuous rotation electron diffraction technique and modelling based on the chemical information from real ***,compared to the isostructural 3D-An-COF without F atom s,3DAn-COF-F showed an improved CO_(2)sorption ability and higher CO_(2)/N_(2)*** study not only demonstrated the generality of constructing 3D COFs with entangled 2D nets by introducing bulky groups vertically in planar building blocks,but also will expand the diversity of 3D COFs for various applications.

关键词： 3D covalent organic frameworks Fluorine Entangled 2D layers Electron diffraction CO_(2)adsorption

Optimizing the power conversion processes in diluted donor/acceptor heterojunctions towards 19.4%efficiency all-polymer solar cells

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Journal of Energy Chemistry 2024年第9期96卷 345-350页

作者： liang Wang Chen Chen Zirui Gan Chenhao Liu Chuanhang Guo Weiyi Xia Wei sun Jingchao Cheng Yuandong sun Jing Zhou Zexin Chen Dan Liu Wei Li Tao Wang School of Materials Science1nd Engineering Wuhan University of TechnologyWuhan 430070HubeiChina School of Materials1nd Microelectronics Wuhan University of TechnologyWuhan 430070HubeiChina

All polymer solar cells(all-PSCs)promise mechanically-flexible and morphologically-stable organic photovoltaics and have aroused increased interests very ***,due to their disorderly conformation structures within the photoactive film,inefficient charge generation and carrier transport are observed which lead to inferior photovoltaic performance compared to smaller molecular acceptor-based ***,by diluting PM6 with a cutting-edge polymeric acceptor PY-IT and diluting PY-IT with PM6 or D18,donor-dominating or acceptor-dominating heterojunctions were *** X-ray and multiple spectrometer techniques reveal that the diluted heterojunctions receive increased structural order,translating to enhanced carrier mobility,improved exciton diffusion length,and suppressed non-radiative recombination loss during the power *** the results,the corresponding PM6+1%PY-IT/PY-IT+1%D18 and PM6+1%PY-IT/PY-IT+1%PM6 devices fabricated by layer-by-layer deposition received superior power conversion efficiency(PCE)of 19.4%and 18.8%respectively,along with enhanced operational lifetimes in air,outperforming the PCE of 17.5%in the PM6/PY-IT reference device.

关键词： All-polymer solar cells Power conversion efficiency Structural order Charge generation