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d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine

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Journal of Energy Chemistry 2024年第2期89卷 216-225,I0006页

作者： Honggang Huang yao chen Hui Fu Cun chen Hanjun Li Zhe Zhang Feili Lai Shuxing Bai Nan Zhang Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122JiangsuChina Department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071ShandongChina

The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to ***,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing ***,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V *** hydrogen electrode,outperforming than those of FCC Pd Cu *** the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR *** work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.

关键词： d-d Orbital coupling Crystal-phase engineering Metallic aerogels Acetonitrile electroreduction reaction Ethylamine

Double casing warhead with sandwiched charge:The axial distribution of fragments velocities

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Defence Technology（防务技术） 2024年第4期34卷 201-216页

作者： Ping Ye Yongxiang dong Qitian Sun Peizhuo Shi Wang yao Yongnan Li Yujing Li Mingze Li State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing 100081China

The double casing warhead with sandwiched charge is a novel fragmentation warhead that can produce two groups of fragments with different velocity,and the previous work has presented a calculation formula to determine the maximum fragment *** current work builds on the published formula to further develop a formula for calculating the axial distribution characteristics of the fragment *** this type of warhead,the simulation of the dispersion characteristics of the detonation products at different positions shows that the detonation products at the ends have a much larger axial velocity than those in the middle,and the detonation products have a greater axial dispersion velocity when they are closer to the central *** loading process and the fragment velocity vary with the axial position for both casing layers,and the total velocity of the fragments is the vector sum of the radial velocity and the axial *** the same axial position,the acceleration time of the inner casing is greater than that of the outer *** the same casing,the fragments generated at the ends have a longer acceleration time than the fragments from the *** proposed formula is validated with the X-ray radiography results of the four warheads previously tested experimentally and the 3D smoothedparticle hydrodynamics numerical simulation results of several series of new warheads with different *** formula can accurately and reliably calculate the fragment velocity when the lengthto-diameter ratio of the charge is greater than 1.5 and the thickness of the casing is less than 20%its inner *** work thus provides a key reference for the theoretical analysis and the design of warheads with multiple casings.

关键词： Double casing warhead Sandwiched charge Fragment velocity Rarefaction wave Gurney formula Explosive loading

High-speed flexible near-infrared organic photodiode for optical communication

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National Science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin chen Ruiman Han Hao Qin Zhaoyang yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng chen The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University State Key Laboratory of Elemento-Organic Chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

The endogenous antioxidant ability of royal jelly in Drosophila is independent of Keap1/Nrf2 by activating oxidoreductase activity

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Insect Science 2024年第2期31卷 503-523页

作者： dongjing Wen Jiayu Xie yao Yuan Lirong Shen Yufeng Yang Wenfeng chen Institute of Life Sciences College of Biological Science and EngineeringFuzhou UniversityFuzhouChina School of Medicine Chongqing UniversityChongqingChina College of Biosystems Engineering and Food Science Zhejiang UniversityHangzhouChina

Royal jelly(RJ)is a biologically active substance secreted by the hypopharyngeal and mandibular glands of worker *** is widely claimed that RJ reduces oxidative ***,the antioxidant activity of RJ has mostly been determined by in vitro chemical detection methods or by external administration drugs that cause oxidative *** RJ can clear the endogenous production of reactive oxygen species(ROS)in cells remains largely ***,we systematically investigated the antioxidant properties of RJ using several endogenous oxidative stress models of *** found that RJ enhanced sleep quality of aging Drosophila,which is decreased due to an increase of oxidative damage with *** supplementation improved survival and suppressed ROS levels in gut cells of flies upon exposure to hydrogen peroxide or to the neurotoxic agent ***,RJ supplementation moderated levels of ROS in endogenous gut cells and extended lifespan after exposure of flies to heat *** deprivation leads to accumulation of ROS in the gut cells,and RJ attenuated the consequences of oxidative stress caused by sleep loss and prolonged ***,RJ prevented cell oxidative damage caused by heat stress or sleep deprivation,with the antioxidant activity in vivo independent of Keap1/Nrf2 *** supplementation activated oxidoreductase activity in the guts of flies,suggesting its ability to inhibit endogenous oxidative stress and maintain health,possibly in humans.

关键词： antioxidant biological oxidations Drosophila oxidative stress royal jelly sleep loss

The synthesis of fluorescent nanoclusters based on the etching reaction

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Nano Research 2024年第5期17卷 4631-4638页

作者： Hongbin Lin Yitao Cao Qiaofeng yao Tiankai chen Huiting Shan Jianping Xie Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)and Key Laboratory of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Key Laboratory of Integrated Organic CircuitsMinistry of EducationDepartment of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic ***,fluorescent NCs present extraordinary practical values in biosensing and bioimaging research ***,restricted by the types of fluorescent NCs,there are great difficulties in promoting the development of NCs in fluorescent research *** a result,it is of significant necessity for researchers to develop new synthetic pathways to produce high-quality fluorescent *** to the analysis about the structural characteristics of fluorescent NCs,some general features like longer motif and higher ligand-to-metal ratio can be found,consistent to some presented regularities in etching ***,in this work,we used Au_(25)(MHA)_(18)(MHA=6-mercaptohexanoic acid)as a model nanocluster and utilized the etching reaction to systematically explore etching products and their corresponding luminescent ***,we also identified three main reaction processes in the entire etching reaction process,which can generate new metal nanocluster species with various fluorescent ***,the etching reaction will provide a good platform to produce new luminescent metal NC species.

关键词： etching reaction metal nanoclusters fluorescent properties fluorescent conversion

Reinforced Lewis covalent bond by twinborn nitride heterostructure for lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第1期88卷 363-372,I0009页

作者： yaochen Song Pengkai Tang Yanjie Wang Yi Wang Linnan Bi Qi Liang Liang He Qingyu Xie Yiyong Zhang Peng dong Yingjie Zhang yao yao Jiaxuan Liao Sizhe Wang Yangtze Delta Region Institute(QuZhou) University of Electronic Science and Technology of ChinaQinzhou 324000ZhejiangChina School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina National and Local Joint Engineering Laboratory for Lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science&TechnologyXi’an 710021ShaanxiChina School of Environmental Science and Engineering North China Electric Power UniversityBaoding 071003HebeiChina

The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox ***,a tungsten and molybdenum nitride heterostructure functionalized with hollow metal-organic framework-derived carbon(W_(2)N/Mo_(2)N)was proposed as the sulfur *** hollow spherical structure provides storage space for sulfur,enhances electrical conductivity,and inhibits volume *** metal atoms in the nitrides bonded with lithium polysulfides(Li PSs)through Lewis covalent bonds,enhancing the high catalytic activity of the nitrides and effectively reducing the energy barrier of Li PSs redox ***,the high intrinsic conductivity of nitrides and the ability of the heterostructure interface to accelerate electron/ion transport improved the Li+*** leveraging the combined properties of strong adsorption and high catalytic activity,the sulfur host effectively inhibited the shuttle effect and accelerated the redox kinetics of Li ***-efficiency Li+transmission,strong adsorption,and the efficient catalytic conversion activities of Li PSs in the heterostructure were experimentally and theoretically *** results indicate that the W_(2)N/Mo_(2)N cathode provides stable,and long-term cycling(over 2000 cycles)at 3 C with a low attenuation rate of 0.0196%per *** design strategy of a twinborn nitride heterostructure thus provides a functionalized solution for advanced Li-S batteries.

关键词： Heterostructure Adsorption Redox kinetics

Atomic tailoring-induced deficiency in tungsten oxides for high-performance energy-related devices

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Tungsten 2024年第2期6卷 269-277页

作者： Jing-Huang Lin yao-Tian Yan Jun-Lei Qi chen-Yang Zha Institute of Applied Physics and Materials Engineering Zhuhai UM Science and Technology Research InstituteUniversity of MacaoTaipaMacao SAR 999078China State Key Laboratory of Advanced Welding and Joining Harbin Institute of TechnologyHarbin 150001China Jiangmen Laboratory of Carbon Science and Technology Hong Kong University of Science and Technology(Guangzhou)Jiangmen 529199China Key Laboratory of Flexible Electronics School of Flexible Electronics(Future Technologies)Institute of Advanced MaterialsNanjing Tech UniversityNanjing 211816China

Nowadays,tungsten oxides,as a typical transition metal oxide,are widely and intensively investigated owing to their excellent material properties and device *** oxygen defi ciency in tungsten oxides is typically the key to enhance their performances for a variety of critical technological *** a gradual increase of oxygen defi ciency,various non-stoichiometric tungsten oxides can be formed by re-adjustment of the atomic arrangement,which exhibits superior performances than their traditional stoichiometric *** review mainly focuses on the recent advances in oxygen-defi cient tungsten oxides from the point of atomic structures,including the forming mechanism of non-stoichiometric tungsten oxides and the superiority of these oxygen-defi cient tungsten oxides in energy-related ***,the challenge and perspective of oxygen-defi cient tungsten oxides are also discussed.

关键词： Oxygen defi ciency Tungsten oxide Atomic structures Catalyst Storage

Tool Wear State Recognition with Deep Transfer Learning Based on Spindle Vibration for Milling Process

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Computer Modeling in Engineering & Sciences 2024年第3期138卷 2825-2844页

作者： Qixin Lan Binqiang chen Bin yao Wangpeng He School of Aerospace Engineering Xiamen UniversityXiamen361005China School of Aerospace Science and Technology Xidian UniversityXi’an710126China

The wear of metal cutting tools will progressively rise as the cutting time goes on. Wearing heavily on the toolwill generate significant noise and vibration, negatively impacting the accuracy of the forming and the surfaceintegrity of the workpiece. Hence, during the cutting process, it is imperative to continually monitor the tool wearstate andpromptly replace anyheavilyworn tools toguarantee thequality of the *** conventional tool wearmonitoring models, which are based on machine learning, are specifically built for the intended cutting ***, these models require retraining when the cutting conditions undergo any changes. This method has noapplication value if the cutting conditions frequently change. This manuscript proposes a method for monitoringtool wear basedonunsuperviseddeep transfer learning. Due to the similarity of the tool wear process under varyingworking conditions, a tool wear recognitionmodel that can adapt to both current and previous working conditionshas been developed by utilizing cutting monitoring data from history. To extract and classify cutting vibrationsignals, the unsupervised deep transfer learning network comprises a one-dimensional (1D) convolutional neuralnetwork (CNN) with a multi-layer perceptron (MLP). To achieve distribution alignment of deep features throughthe maximum mean discrepancy algorithm, a domain adaptive layer is embedded in the penultimate layer of thenetwork. A platformformonitoring tool wear during endmilling has been constructed. The proposedmethod wasverified through the execution of a full life test of end milling under multiple working conditions with a Cr12MoVsteel workpiece. Our experiments demonstrate that the transfer learning model maintains a classification accuracyof over 80%. In comparisonwith the most advanced tool wearmonitoring methods, the presentedmodel guaranteessuperior performance in the target domains.

关键词： Multi-working conditions tool wear state recognition unsupervised transfer learning domain adaptation maximum mean discrepancy(MMD)

Strong metal-support interaction between AuPd nanoparticles and oxygen-rich defect ZrO_(2) for enhanced catalytic 5-hydroxymethylfurfural oxidation

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Chinese Chemical Letters 2024年第2期35卷 507-511页

作者： Yunlei Zhang Yiran Liu Wen Guan Mengxue Cao yao chen Pengwei Huo Institute of Green Chemistry and Chemical Technology School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China School of the Environment and Safety Jiangsu UniversityZhenjiang 212013China

The unique properties of metal oxide surfaces,crystal surfaces and defects play vital roles in biomass upgrading *** this work,hierarchical porous bowl-shaped ZrO_(2)(HB-ZrO_(2))with mixed crystal phase was designed and employed as the support for loading AuPd bimetal with different proportions to synthesize AuPd/HB-ZrO_(2) *** effects of surface chemistry,oxygen defects,bimetal interaction and metal-support interaction of AuPd/HB-ZrO_(2) on catalytic performance for the selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA)were systematically *** Au 2 Pd1/HB-ZrO_(2) catalyst afforded a satisfactory FDCA yield of 99.9%from HMF oxidation using O_(2) as the oxidant in water,accompanied with an excellent FDCA productivity at 97.6 mmol g^(−1) h^(−1).This work offers fresh insights into rationally designing efficient catalysts with oxygen-rich defects for the catalytic upgrading of biomass platform chemicals.

关键词： 5-Hydroxymethylfurfural oxidation 2,5-Furandicarboxylic acid Oxygen-rich defect ZrO_(2) AuPd bimetal Bowl-shaped structure