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Identifying the Active Site of Water Oxidation Catalyst Based on Defective Fe-Doped Ni Oxyhydroxide

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CCS Chemistry 2024年第2期6卷 365-376页

作者： Yunxuan Ding Jian Du Tao Wang Licheng sun Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024 Center of Artificial Photosynthesis for Solar Fuels Department of ChemistrySchool of ScienceWestlake UniversityHangzhou 310024

Electrochemical water splitting plays a crucial role in storing sustainable energy into h2 as an ideal fuel,in which the anodic oxygen evolution reaction(OER)is the ***,Fe-doped NiOOh(Ni_(1−x)Fe_(x)OOh)is a promising OER catalyst under alkaline ***,the specific active sites responsible for their good performances remain ***,we identify a nickel-oxygen radical(Ni–O·)and an iron-oxo(Fe=O)group as two essential states for adsorbed ***,both thermochemical O–O coupling and electrochemical OER elementary steps are considered on the Ni_(1−x)Fe_(x)OOh *** mechanistic studies with a combined density functional theory simulation and experimental analysis unravel that both the Ni and Fe centers can act as the active sites for the defective Ni_(1−x)Fe_(x)OOh to catalyze OER,depending on the nature of the *** presence of Fe can benefit the stabilization of the defective surface and influence the electronic property of the nearby Ni *** work not only identifies the intrinsic active sites of Ni_(1−x)Fe_(x)OOh,but also illustrates the essential roles of defects in catalysis,which sheds light on the design of more efficient OER catalysts in the future.

关键词： defect water nucleophilic attack oxygen evolution reaction heterogeneous catalysis density functional calculations

Enhancing Skin Cancer Diagnosis with Deep Learning:A hybrid CNN-RNN Approach

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Computers, Materials & Continua 2024年第4期79卷 1497-1519页

作者： Syeda Shamaila Zareen Guangmin sun Mahwish Kundi Syed Furqan Qadri Salman Qadri Faculty of Information Technology Beijing University of TechnologyBeijing100124China Computer Science International Engineering Collage Maynooth UniversityKildareW23 F2H6Irland Research Center for Data hub and Security Zhejiang LabHangzhou311121China Computer Science Department MNS University of AgricultureMultan59220Pakistan

Skin cancer diagnosis is difficult due to lesion presentation variability. Conventionalmethods struggle to manuallyextract features and capture lesions spatial and temporal variations. This study introduces a deep learning-basedConvolutional and Recurrent Neural Network (CNN-RNN) model with a ResNet-50 architecture which usedas the feature extractor to enhance skin cancer classification. Leveraging synergistic spatial feature extractionand temporal sequence learning, the model demonstrates robust performance on a dataset of 9000 skin lesionphotos from nine cancer types. Using pre-trained ResNet-50 for spatial data extraction and Long Short-TermMemory (LSTM) for temporal dependencies, the model achieves a high average recognition accuracy, surpassingprevious methods. The comprehensive evaluation, including accuracy, precision, recall, and F1-score, underscoresthe model’s competence in categorizing skin cancer types. This research contributes a sophisticated model andvaluable guidance for deep learning-based diagnostics, also this model excels in overcoming spatial and temporalcomplexities, offering a sophisticated solution for dermatological diagnostics research.

关键词： Skin cancer classification deep learning Convolutional Neural Network(CNN) RNN ResNet-50

Boosting zinc anode durability through synergistic inner helmholtz plane and interfacial electric field regulation

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Science Bulletin 2024年第13期69卷 2025-2029页

作者： hao Tan Chao Meng Tong sun Xing-Long Wu hong Liu Jian-Jun Wang State Key Laboratory of Crystal Materials Shandong UniversityJinan 250100China College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China MOE Key Laboratory for UV Light-Emitting Materials and Technology Department of PhysicsNortheast Normal UniversityChangchun 130024China Jinan Institute of Quantum Technology Jinan BranchHefei National LaboratoryJinan 250101China Shenzhen Research Institute Shandong UniversityShenzhen 518057China

As the need for energy storage devices escalates,aqueous zincion batteries(ZIBs)have risen as a promising alternative to the widely used Li-ion batteries,offering intrinsic safety,environmental compatibility,and cost advantages,positioning them as attractive energy storage systems for the future[1,2].however,challenges such as dendrite growth on Zn anodes,stemming from uneven electric fields on the surface and active water side reactions,compromise cycling stability and lifespan,posing significant hurdles for the practical application of ZIBs[3,4].To mitigate these issues,strategies like electrolyte optimization,artificial solid electrolyte interphase(SEI)layers,and current collector modifications have been proposed[5,6].Nevertheless,most long-cycle experiments are conducted at low current densities and deposition capacities,with high current density and capacity operations typically lasting less than 1000 h[7].

关键词： electrolyte durability offering

Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo_(2)C nanosheet

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Chinese Chemical Letters 2024年第8期35卷 319-323页

作者： Yue Zhang Xiaoya Fan Xun he Tingyu Yan Yongchao Yao Dongdong Zheng Jingxiang Zhao Qinghai Cai Qian Liu Luming Li Wei Chu Shengjun sun Xuping sun College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Institute for Advanced Study Chengdu UniversityChengdu 610106China College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJi’nan 250014China

Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production *** this communication,we report the application of Mo_(2)C nanosheets-decorated carbon sheets(Mo_(2)C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea *** CO_(2)-saturated 0.2 mol/L Na_(2)SO_(4)solution containing 0.05 mol/L NO_(3)^(-),the Mo_(2)C/C catalyst achieves an impres-sive urea yield of 579.13μg h^(-1)mg^(-1)with high Faradaic efficiency of 44.80%at-0.5 V versus the reversible hydrogen *** theoretical calculations reveal that the multiple Mo active sites enhance the formation of^(∗)CO and^(∗)Nh_(2)intermediates and facilitate their C-N *** research propels the use of Mo_(2)C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.

关键词： Mo_(2)C Multiple active sites C-N coupling Electrocatalysis Urea synthesis Density functional theory calculation

纳米光子结构软膜紫外光固化纳米压印(英文)

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纳米技术与精密工程 2006年第3期4卷 225-229页

作者： ShI J WANG Z M BAO K PEROZ C BELOTTI M XU L P LUO C X sun M h ZhANG B JI h OUYANG Q ChEN Y 北京大学物理学院北京100871 法国巴黎高等师范学院巴黎75005 法国国家科研中心光子与纳米结构实验室马库锡91460

紫外光固化纳米压印是实现纳米结构批量复制的一种新技术．其特点是低成本和高分辨,而且可以达到极高的套刻精度．为了得到大面积图案的均匀复制,可用聚二甲基硅氧烷(PDMS)制备透光的压印软模板．其母版图案可由高分辨率电子束曝光和反... 详细信息

紫外光固化纳米压印是实现纳米结构批量复制的一种新技术．其特点是低成本和高分辨,而且可以达到极高的套刻精度．为了得到大面积图案的均匀复制,可用聚二甲基硅氧烷(PDMS)制备透光的压印软模板．其母版图案可由高分辨率电子束曝光和反应离子刻蚀的方法在硅片基底上获得,然后用浇注的方法将图案转移到PDMS上．本实验特别发展了紫外光固化纳米压印适用于软膜压印的双层膜图型转移技术．该双层膜由廉价的光胶和聚甲基丙烯酸甲脂(PMMA)构成．对光胶层的压印可用普通的光学曝光仪实现．然后再将图案用反应离子刻蚀的方法转移到PMMA层中．为了证明方案的可行性,在两种不同材料的半导体基片上压印了三角晶格的光子晶体和准晶结构的图案,并用剥离的方法将它们转移到金属薄膜上,最后成功地进行了硅片刻蚀实验．相信这一纳米制做方法对大面积纳米光子结构和光学集成芯片的制造是普遍适用的．

关键词：纳米压印纳米加工纳米光子学

high Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

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Chinese Journal of Polymer Science 2024年第2期42卷 188-201,I0007页

作者： Chantsalnyam Bariashir Qiu-Yue Zhang Bayasgalan Ulambayar Gregory A.Solan Tong-Ling Liang Wen-hua sun Institute of Chemistry and Chemical Technology Mongolian Academy of SciencesUlaanbaatar13330Mongolia Key Laboratory of Engineering Plastics and Beijing National Laboratory for Molecular Science Institute of ChemistryChinese Academy of SciencesBeijing100190China Department of Chemistry University of LeicesterUniversity RoadLeicesterLE17RHUK State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China

The N,N,N'-ferrous chloride complexes,[2-{CMeN(2,4-(ChPh)_(2)-6-FC_(6)h_(2))}-6-(CMeNAr)C_(5)h_(3)N]FeCl_(2)(Ar=2,6-Me_(2)C_(6)h_(3) Fe1,2,6-Et_(2)C_(6)h_(3)Fe2,2,6-^(i)Pr_(2)C_(6)h_(3) Fe3,2,4,6-Me_(3)C_(6)h_(2) Fe4 and 2,6-Et_(2)-4-MeC_(6)h_(2) Fe5),each possessing one N-2,4-dibenzhydryl-6-fluorophenyl group,were readily synthesized from their respective unsymmetrical bis(imino)pyridines,*** identification of Fe2 highlighted the variation in the steric properties provided by the dissimilar N-aryl *** pre-treatment with either MAO or MMAO,complexes Fe1-Fe5 all displayed,at an operating temperature of 80℃,high activities for ethylene polymerization with levels falling in the order:Fe4> Fe1> Fe5> Fe2> ***,Fe4/MAO displayed the highest activity of 1.94×10^(7) g_(PE)·mol_(Fe)^(-1)·h^(-1) of the study with only a modest loss in performance at 90℃.Generally,the resulting polyethylenes were highly linear(T_(m) range:122-132℃),narrowly disperse and of low molecular weight(M_(w) range:6.73-46.04kg·mol^(-1)),with the most sterically hindered Fe3 forming the highest molecular weight polymer of the ***-group analysis by ^(1)h-and ^(13)CNMR spectroscopy revealed saturated alkyl(n-propyl and i-propyl) and unsaturated vinyl chain ends indicative of the role of both β-h elimination and chain transfer to aluminum as termination *** comparison with previou sly reported iron precatalysts with similar tridentate ligand skeletons,it is evident that the introduction of a large benzhydryl group in combination with a fluorine as the ortho-substituents of one N-aryl group has the effect of enhancing thermal stability of the iron polymerization catalyst whilst maintaining appreciable polymer molecular weight.

关键词： Iron catalyst Ethylene polymerization Linear polyethylene Fluoride effect Thermal stability

Correlation between hydration properties and electrochemical performances on Ln cation size effect in layered perovskite for protonic ceramic fuel cells

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Journal of Energy Chemistry 2024年第1期88卷 1-9,I0001页

作者： Inhyeok Cho Jiwon Yun Boseok Seong Junseok Kim sun hee Choi ho-Il Ji Sihyuk Choi Department of Mechanical Engineering Kumoh National Institute of TechnologyGumi 39177GyeongbukRepublic of Korea Department of Aeronautics Mechanical and Electronic Convergence EngineeringKumoh National Institute of TechnologyGumi 39177GyeongbukRepublic of Korea Center for Energy Materials Research Korea Institute of Science and Technology(KIST)Seoul 02792Republic of Korea Center for hydrogen and Fuel Cell Research Clean Technology Research DivisionKorea Institute of Science and Technology(KIST)Seoul 02792Republic of Korea Department of Energy and Environmental Engineering University of Science and TechnologySeoul 02792Republic of Korea Nanomaterials Science and Engineering Korea University of Science and Technology(UST)KIST CampusSeoul 02792Republic of Korea

PrBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(PrBSCF) has attracted much research interest as a potential triple ionic and electronic conductor(TIEC) electrode for protonic ceramic fuel cells(PCFCs). The chemical formula for Pr BSCF is AA'B_(2)O_(5+δ), with Pr(A-site) and Ba/Sr(A'-site) alternately stacked along the c-axis. Due to these structural features, the bulk oxygen ion diffusivity is significantly enhanced through the disorder-free channels in the PrO layer;thus, the A site cations(lanthanide ions) play a pivotal role in determining the overall electrochemical properties of layered perovskites. Consequently, previous research has predominantly focused on the electrical properties and oxygen bulk/surface kinetics of Ln cation effects,whereas the hydration properties for PCFC systems remain unidentified. here, we thoroughly examined the proton uptake behavior and thermodynamic parameters for the hydration reaction to conclusively determine the changes in the electrochemical performances depending on LnBa_(0.5)Sr_(0.5)Co_(1.5)Fe_(0.5)O_(5+δ)(LnBSCF,Ln=Pr, Nd, and Gd) cathodes. At 500 ℃, the quantitative proton concentration of PrBSCF was 2.04 mol% and progressively decreased as the Ln cation size decreased. Similarly, the Gibbs free energy indicated that less energy was required for the formation of protonic defects in the order of Pr BSCF he close relationship between hydration properties and electrochemical performances in LnBSCF cathodes, PCFC single cell measurements and analysis of the distribution of relaxation time were further investigated.

关键词： Protonic ceramic fuel cell Cathode Triple ionic and electronic conductor hydration property Proton uptake Gibbs free energy

Ultrathin Zincophilic Interphase Regulated Electric Double Layer Enabling highly Stable Aqueous Zinc‑Ion Batteries

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Nano-Micro Letters 2024年第5期16卷 285-299页

作者： Yimei Chen Zhiping Deng Yongxiang sun Yue Li hao Zhang Ge Li hongbo Zeng Xiaolei Wang Department of Chemical and Materials Engineering University of Alberta9211‑116 Street NWEdmontonAB T6G 1H9Canada Department of Mechanical Engineering University of Alberta9211‑116 Street NWEdmontonAB T6G 1H9Canada

The practical application of aqueous zinc-ion batteries for large-grid scale systems is still hindered by uncontrolled zinc dendrite and side *** the elec-trical double layer via the electrode/electrolyte interface layer is an effective strategy to improve the stability of Zn ***,we report an ultrathin zincophilic ZnS layer as a model *** a given cycling current,the cell with Zn@ZnS electrode displays a lower potential drop over the helmholtz layer(stern layer)and a suppressed diffuse layer,indicating the regulated charge distribution and decreased electric double layer repulsion *** zinc adsorption sites are also expected as proved by the enhanced electric double-layer ***,the symmetric cell with the ZnS protection layer can stably cycle for around 3,000 h at 1 mA cm^(-2) with a lower overpotential of 25 *** coupled with an I2/AC cathode,the cell demonstrates a high rate performance of 160 mAh g^(-1) at 0.1 A g^(-1) and long cycling stability of over 10,000 cycles at 10 A g^(-1).The Zn||MnO_(2) also sustains both high capacity and long cycling stability of 130 mAh g^(-1) after 1,200 cycles at 0.5 A g^(-1).

关键词： Zinc anode Electric double-layer regulation Multifunction SEI layer Inhibited side reactions and dendrite Rapid kinetics

A gel polymer electrolyte based on IL@Nh_(2)-MIL-53(Al)for high-performance all-solid-state lithium metal batteries

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Chinese Journal of Chemical Engineering 2024年第5期69卷 47-55页

作者： Sijia Wang Ye Liu Liang he Yu sun Qing huang Shoudong Xu Xiangyun Qiu Tao Wei School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China College of Materials Science and Engineering Nanjing Forestry UniversityNanjing 210037China College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China Power&Energy Storage System Research Center College of Mechanical and Electrical EngineeringQingdao UniversityQingdao 266071China

Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage ***,a new gel polymer electrolyte(GPE)containing Nh_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-hFP was prepared using a simple method of solution *** effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(Nh_(2)-MIL-53(Al))on the electrochemical properties were ***,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were *** GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 *** work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.

关键词： Metal-organic frameworks(MOFs) All solid-state lithium batteries(ASSLBs) Ionic liquid Nh_(2)-MIL-53(Al) Solid-state electrolytes(SSEs)