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Dramatic Difference Between Cu_(20)H_(8)and Cu_(20)H_(9)Clusters in Catalysis

CCS Chemistry 2024年第6期6卷 1581-1590页

作者： Chun-Yu Liu Tong-Yu Liu Zong-Jie Guan song Wang yuan-yuan Dong Feng hu De-en Jiang Quan-Ming Wang Department of Chemistry Engineering Research Center of Advanced Rare Earth Materials(Ministry of Education)Tsinghua UniversityBeijing 100084 Jiangsu Engineering Research Centre for Digital Textile Inkjet Printing Key Laboratory of Eco-Textile Jiangnan UniversityMinistry of EducationWuxiJiangsu 214122 Department of Chemical and Biomolecular Engineering Vanderbilt UniversityNashvilleTennessee 37235 Department of Chemistry Vanderbilt UniversityNashvilleTennessee 37235 College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082 Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefeiAnhui 230026

Sensitivity to structure and composition is very challenging to establish in nanocatalysis due to inadequate definition of structures that are very close in *** synthesized a pair of atomically precise copper clusters that are very close in composition,[Cu_(20)H_(9)(Tf-dpf)_(10)]·BF4(Cu_(20)H_(9))and[Cu_(20)H_(8)(Tf-dpf)_(10)]·(BF_(4))_(2)(Cu_(20)H_(8)),by using a pyridyl-functionalized flexible amidinate ligand,N,N′-di(5-trifluoromethyl-2-pyridyl)*** one-hydride difference in their composition leads to significant variation in geometric and electronic structures and,consequently,distinctly different optical and catalytic ***_(20)H_(8)exhibits 25 times higher catalytic activity than Cu_(20)H_(9)(96.7%vs 3.7%in yield)in the selective hydrogenation of anα,β-unsaturated aldehyde(cinnamaldehyde)to saturated aldehyde(3-phenylpropanal).Electrospray ionization mass spectrometry combined with density functional theory calculations reveal that the greater ease of dissociation of one Tf-dpf ligand compared to Cu_(20)H_(8)is the key to its higher *** work demonstrates a clear case of structure and composition sensitivity in nanocatalysis and that one hydride,out of∼330 atoms in the nanoclusters,can make a huge difference in the catalytic *** insights will be useful in the design and synthesis of atomically precise nanocatalysts.

关键词： copper cluster hydride amidinate ligand structural transformation hydrogenation catalysis

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Atomistic understanding of rough surface on the interfacial friction behavior during the chemical mechanical polishing process of diamond

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Friction 2024年第6期12卷 1119-1132页

作者： song yuan Xiaoguang GUO Hao WANG Renke KANG Shang GAO State Key Laboratory of High-performance Precision Manufacturing Dalian University of TechnologyDalian 116024China

The roughness of the contact surface exerts a vital role in *** is still a significant challenge to understand the microscopic contact of the rough surface at the atomic ***,the rough surface with a special root mean square(RMS)value is constructed by multivariate Weierstrass–Mandelbrot(W–M)function and the rubbing process during that the chemical mechanical polishing(CMP)process of diamond is mimicked utilizing the reactive force field molecular dynamics(ReaxFF MD)*** is found that the contact area A/A0 is positively related with the load,and the friction force F depends on the number of interfacial bridge *** the surface roughness will increase the friction force and friction *** model with low roughness and high lubrication has less friction force,and the presence of polishing liquid molecules can decrease the friction force and friction *** RMS value and the degree of damage show a functional relationship with the applied load and lubrication,i.e.,the RMS value decreases more under larger load and higher lubrication,and the diamond substrate occurs severer damage under larger load and lower *** work will generate fresh insight into the understanding of the microscopic contact of the rough surface at the atomic level.

关键词： diamond random roughness reactive force field molecular dynamics(ReaxFF MD) friction Weierstrass-Mandelbrot(W-M)function chemical mechanical polishing(CMP)

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CSCO guidelines for colorectal cancer version 2024:Updates and discussions

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Chinese Journal of Cancer Research 2024年第3期36卷 233-239页

作者： Liubo Chen Hanguang hu Ying yuan Shanshan Weng Department of Medical Oncology(Key Laboratory of Cancer Prevention and Intervention China National Ministry of EducationKey Laboratory of Molecular Biology in Medical SciencesZhejiang ProvinceChina)the Second Affiliated HospitalZhejiang University School of MedicineHangzhou 310009China Zhejiang Provincial Clinical Research Center for CANCER Hangzhou 310009China Cancer Center Zhejiang UniversityHangzhou 310058China

According to the latest global cancer statistics,colorectal cancer(CRC)is the most common malignancy of the digestive system and the second most lethal among all cancer types(1).In China,CRC is the second most prevalent cancer,following only after lung cancer(2).The first version of the Chinese Society of Clinical Oncology(CSCO)guideline was launched in 2017 and has been updated annually based on the latest findings of clinical research,drug accessibility and expert consensus(3-8).Here,we present the main updates of the 2024 version compared to the 2023 version.

关键词： CSCO colorectal cancer

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Chemico-biological conversion of carbon dioxide

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Journal of Energy Chemistry 2024年第2期89卷 371-387,I0009页

作者： Liangwei hu Junzhu Yang Qi Xia Jin Zhang Hongxin Zhao yuan Lu Zhejiang Province Key Laboratory of Plant Secondary Metabolism and Regulation College of Life Sciences and MedicineZhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Department of Chemical Engineering Tsinghua UniversityBeijing 100084China College of Biological and Chemical Engineering Jiaxing UniversityJiaxing 314000ZhejiangChina

The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse *** address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and *** cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical *** innovative strategy offers several advantages,including environmental friendliness,high efficiency,and *** study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis *** also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and *** both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in ***,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of *** also explored the biocompatibility of the electrode materials and developed novel *** materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of ***,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this *** novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic ***,it offers exciting prospects for utilizing CO_(2)in synthesizing

关键词： Carbon dioxide Bioelectric synthesis Artificial photosynthesis Synthetic product

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Transfer matrix method for free and forced vibrations of multi-level functionally graded material stepped beams with different boundary conditions

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Applied Mathematics and Mechanics(English Edition) 2024年第6期45卷 983-1000页

作者： Xiaoyang SU Tong hu Wei ZHANG Houjun KANG Yunyue CONG Quan yuan School of Civil Engineering and Architecture Guangxi UniversityNanning 530004China Scientific Research Center of Engineering Mechanics Guangxi UniversityNanning 530004China State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite Structures Guangxi UniversityNanning 530004China

Functionally graded materials(FGMs)are a novel class of composite materials that have attracted significant attention in the field of engineering due to their unique mechanical *** study aims to explore the dynamic behaviors of an FGM stepped beam with different boundary conditions based on an efficient solving *** the assumptions of the Euler-Bernoulli beam theory,the governing differential equations of an individual FGM beam are derived with Hamilton’s principle and decoupled via the separation-of-variable ***,the free and forced vibrations of the FGM stepped beam are solved with the transfer matrix method(TMM).Two models,i.e.,a three-level FGM stepped beam and a five-level FGM stepped beam,are considered,and their natural frequencies and mode shapes are *** demonstrate the validity of the method in this paper,the simulation results by ABAQUS are also *** this basis,the detailed parametric analyses on the frequencies and dynamic responses of the three-level FGM stepped beam are carried *** results show the accuracy and efficiency of the TMM.

关键词： transfer matrix method(TMM) free vibration forced vibration functionally graded material(FGM) stepped beam

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Simultaneously enhanced electrochemical performance and air stability of Ni-rich cathode with a modified washing process

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Rare Metals 2024年第1期43卷 87-97页

作者： Ben-Rui hu Ying-Yi yuan Yu-Cheng Wang Xun-hui Xiong School of Environment and Energy Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640China

Water washing has been regarded as one of the most effective strategies to remove surface residual lithium of nickel-rich layered oxides for lithium-ion batteries(LIBs).However,the loss of lattice lithium during the water washing process deteriorates the electrochemical performances and air ***,washing the LiNi_(0.90)Co_(0.05)Al_(0.02)O_(2)(NCA) with ammonium dihydrogen phosphate(NH_(4)H_(2)PO_(4)) solution has been proposed to simultaneously enhance electrochemical performances and air stability,in which in-situ generated Li_(3)PO_(4) coating layer on surface of NCA can suppress the loss of lattice ***,as a fast ionic conductor,Li_(3)PO_(4) coating layer on NCA can prevent the direct contact with electrolyte/*** a result,the NH_(4)H_(2)PO_(4) solution washed NCA cathode can deliver a high capacity of131.9 mAh·g^(-1) at 10.0C rate as well as impressive cycle stability with a capacity retention of 83.1% after 100 cycles at 1.0C,much higher than those of water washed NCA(WS-NCA) *** exposed in air for 7 days,the NH_(4)H_(2)PO_(4) solution washed NCA electrode can more effectively maintain the structural integrity as well as the electrochemical performances than water-washed *** work provides a simple and effective approach to enhance the cycle stability and air stability of Nickel-rich cathode materials.

关键词： Layered Ni-rich cathode Residual lithium Li_(3)PO_(4)coating Rate performance Air stability

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Buried interface management via bifunctional NH_(4)BF_(4)towards efficient CsPbI_(2)Br solar cells with a V_(oc)over 1.4 V

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Journal of Energy Chemistry 2024年第2期89卷 364-370,I0009页

作者： Fazheng Qiu Ming-hua Li Jinpeng Wu Jin-song hu School of Materials Science and Engineering NingboTech UniversityNingbo 315100ZhejiangChina Beijing National Laboratory for Molecular Sciences(BNLMS) Institute of ChemistryChinese Academy of SciencesBeijing 100190China College of Chemical Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China

CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar ***,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(V_(oc))output and stability much lower than ***,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI_(2)Br defects by introducing ammonium tetrafluoroborate(NH_(4)BF_(4)),thereby resulting in both high CsPbI_(2)Br crystallization and minimized interfacial energy ***,NH_(4)^(+)ions could preferentially heal hydroxyl groups on the SnO_(2)surface and balance energy level alignment between SnO_(2)and CsPbI_(2)Br,enhancing charge transport efficiency,while BF_(4)^(-)anions as a quasi-halogen regulate crystal growth of CsPbI_(2)Br,thus reducing perovskite ***,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI_(2)Br for strengthening the phase *** a result,the optimized CsPbI_(2)Br PSCs realize a remarkable efficiency of 17.09%and an ultrahigh V_(oc)output of 1.43 V,which is one of the highest values for CsPbI_(2)Br PSCs.

关键词： Inorganic perovskite Buried interface Defect Stability Open-circuit voltage loss

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Experimental and numerical study on ignition and combustion characteristics of boron-magnesium composite powders

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Particuology 2024年第1期84卷 12-29页

作者： Shuyuan Liu Luyang Han Hongmei Liu Yingkai song Linlin Liu songqi hu Science and Technology on Combustion Internal Flow and Thermo-Structure LaboratoryNorthwestern Polytechnical UniversityXi'an710072China School of Mechanical Engineering and Rail Transit Changzhou UniversityChangzhou213164China Shanghai Institute of Space Propulsion Shanghai201112China Shanghai Engineering Research Center of Space Engine Shanghai201112China

A high-pressure laser ignition and combustion system with adjustable oxidizer gas atmosphere is established to investigate the ignition and combustion characteristics of boron-magnesium(BM)com-posite *** ignition and combustion model of BM powders is established and validated in the present *** results show that increasing water content,O_(2) content and Mg content all result in shorter ignition delay time of BM powders,among which the effect of water content is the most ***,ignition delay time increases as pressure *** combustion time decreases with increasing Mg content and ambient pressure but increases with water *** the increase of O_(2) content,combustion time of BM powders first increases and then decreases,which means a critical O_(2) content exists above which combustion time *** results show that there exists a trade-off between ignition and combustion performance of BM composite powders.

关键词： Boron magnesium powder Laser ignition Ignition and combustion model Reaction mechanism Numerical model

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ZIF-8-functionalized polymer electrolyte with enhanced performance for high-temperature solid-state lithium metal batteries

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Rare Metals 2024年第3期43卷 984-994页

作者： Jin-Fang Zhang yuan-yuan Wang Xiao-Feng Li Gen-Yan Zhang Ying Li Rong Liu Sheng-Liang hu Tuo-Ping hu Ruth Knibbe Qing-Bing Xia School of Materials Science and Engineering North University of ChinaTaiyuan030051China School of Energy and Power Engineering North University of ChinaTaiyuan030051China School of Chemistry and Chemical Engineering North University of ChinaTaiyuan030051China School of Mechanical and Mining Engineering The University of QueenslandBrisbaneQLD4072Australia

Solid polymer electrolytes(SPEs)with high ionic conductivity are desirable for solid-state lithium metal batteries(SSLMBs)to achieve enhanced safety and energy *** nanofillers into a polymeric matrix to develop nanocomposite solid electrolytes(NCSEs)has become a promising method for improving the ionic conductivity of the ***,a novel ZIF-8-functionalized NCSE was prepared for high-temperature S SLMB s using an in situ radical polymerization *** is found that the ZIF-8 nanoparticles could reduce the crystallinity of polymer segments and offer a Lewis acid surface that promotes the dissociation of lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)and stabilizes the TFSI^(-) anion ***,the as-prepared NCSE exhibits an outstanding ionic conductivity of 1.63×10^(-3)S·cm^(-1),an electrochem ical stability window of 5.0 V at 80℃,and excellent interface compatibility with lithium metal anode with a stable polarization over 2000 ***,the assembled SSLMBs with LiFePO_(4)cathode show dendrite-free Li-metal surface,good rate capability,and stable cycling stability with a capacity retention of 70%over 1000 cycles at a high temperature of 80℃.This work provides valuable insights into promoting the ionic conductivity of SPEs.

关键词： Lithium metal batteries Metal-organic frameworks Solid polymer electrolytes Lithium metal anode Interfacial compatibility

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Deep learning-based inpainting of saturation artifacts in optical coherence tomography images

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Journal of Innovative Optical Health Sciences 2024年第3期17卷 1-10页

作者： Muyun hu Zhuoqun yuan Di Yang Jingzhu Zhao Yanmei Liang Institute of Modern Optics Nankai UniversityTianjin Key Laboratory of Micro-scale Optical Information Science and TechnologyTianjin 300350China Department of Thyroid and Neck Tumor Tianjin Medical University Cancer Institute and Hospital National Clinical Research Center for CancerKey Laboratory of Cancer Prevention and TherapyTianjin 300060China

Limited by the dynamic range of the detector,saturation artifacts usually occur in optical coherence tomography(OCT)imaging for high scattering *** available methods are difficult to remove saturation artifacts and restore texture completely in OCT *** proposed a deep learning-based inpainting method of saturation artifacts in this *** generation mechanism of saturation artifacts was analyzed,and experimental and simulated datasets were built based on the *** super-resolution generative adversarial networks were trained by the clear–saturated phantom image *** perfect reconstructed results of experimental zebrafish and thyroid OCT images proved its feasibility,strong generalization,and robustness.

关键词： Optical coherence tomography saturation artifacts deep learning image inpainting.

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