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Green Synthesized Liquid-like Dynamic Polymer Chains with Decreased Nonspecific Adhesivity for High-Purity Capture of Circulating Tumor Cells

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CCS Chemistry 2024年第2期6卷 507-517页

作者： Feng Wu Xiaofeng Chen Shuli Wang Ruimin Zhou Chunyan Wang Lejian Yu Jing Zheng Chaoyong Yang Xu Hou state Key laboratory of Physical Chemistry of solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamenFujian 361005 College of Physical Science and Technology Xiamen UniversityXiamenFujian 361005 College of physics and New Energy Xuzhou University of TechnologyXuzhouJiangsu 221018 Fujian Engineering Research Center for solid-state Lighting Department of Electronic ScienceSchool of Electronic Science and EngineeringXiamen UniversityXiamenFujian 361005 Institute of Artificial Intelligence Xiamen UniversityXiamenFujian 361005 Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) XiamenFujian 361102 state Key laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdaoShandong 266071

The capture of circulating tumor cells(CTCs)is of great significance in reducing cancer mortality and ***,the nonspecific binding of proteins and white blood cells(WBCs)weakens the targeting capabilities of the capture surfaces,which critically hampers the efficiency and purity of the captured ***,we propose a liquid-like interface design strategy that consists of liquid-like polymer chains and anti-EpCAM modification processes for high-purity and high-efficiency capture of *** dynamic flexible feature of the liquid-like chains endows the modified surfaces with excellent antiadhesion property for proteins and blood *** liquid-like surfaces can capture the target CTCs and show high cell viability due to the environmentfriendly surface modification *** liquid-like surface designs were introduced in the deterministic lateral displacement(DLD)-patterned microfluidic chip,the nonspecific adhesion rate of WBCs was reduced by more than fivefold compared to that in the DLD chip without liquid-like interface design,while maintaining comparable capture ***,this strategy provides a novel perspective on surface design for achieving high purity and efficient capture of CTCs.

关键词： green synthesis dynamic polymer chains liquid-like interface nonspecific adsorption capture of circulating tumor cells microfluidics

Concerted Steric and Electronic Strategy in Thermostable Salicylaldiminato Nickel Catalysts for Ethylene(Co)polymerization

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Chinese Journal of Polymer Science 2024年第8期42卷 1085-1092页

作者： Hong-Yu Ji Hong-Liang Mu Chun-Feng Tang Yu-Xing Zhang Yue Chi Zhong-Bao Jian Key laboratory of Advanced Structural Materials Ministry of EducationSchool of Materials Science and EngineeringChangchun University of TechnologyChangchun 130012China state Key laboratory of Polymer physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Olefin polymerization is one of the most im portant chemical reactions in *** work presents a strategy that emphasizes the synergistic meta/poro-steric hindrance of N-aryl groups and electronic effects in newly synthesized neutral salicylaldiminato nickel *** nickel(Ⅱ)catalysts exhibit exceptional thermostability,ranging from 30℃to 130℃,demonstrating enhanced catalytic activities and broadly regulated polyethylene molecular weights(3-341 kg·mol^(-1))and controlled polymer branch density(2-102 brs/1000C).The preferred catalyst Ni3 with concerted steric and electronic effects enables the production of solid-state semi-crystalline polyethylene materials at temperatures below 90℃.Notably,Ni3 exhibits an impressive tolerance of 110℃and can withstand even the challenging polymerization temperature of 130℃,leading to the production of polyethylene wax and ***,functionalized polyethylene is produced.

关键词： Polyolefin Salicylaldiminato ligand Nickel catalyst Oil Wax

Viability of all-solid-state lithium metal battery coupled with oxide solid-state electrolyte and high-capacity cathode

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Journal of Energy Chemistry 2024年第4期91卷 122-131页

作者： Xingxing Jiao Xieyu Xu Yongjing Wang Xuyang Wang Yaqi Chen Shizhao Xiong Weiqing Yang Zhongxiao Song Yangyang Liu Research Institute of Frontier Science Southwest Jiaotong UniversityChengdu 610031SichuanChina state Key laboratory for Mechanical Behavior of Materials Xi'an Jiaotong UniversityXi'an 710049ShaanxiChina department of physics Chalmers University of TechnologyGöteborgSE 41296Sweden

Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and ***,its applications are still challenged by plenty of technical and scientific *** this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of ***,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak ***,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.

关键词： All-solid-state lithium metal battery LiNi_(0.5C)o_(0.2)Mn_(0.3)O_(2)-Li7La_(3)Zr_(2)O_(12)composite cathode Co-sintering Lithium metal anode Electro-chemo-mechanical failure

LATP-coated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode with compatible interface with ultrathin PVDF-reinforced PEO-LLZTO electrolyte for stable solid-state lithium batteries

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Journal of Materiomics 2024年第3期10卷 682-693页

作者： Xiao Chen Yinda Li Yunhao Lu Jian Xie Cheng Huang Xiongwen Xu Jian Tu Xinbing Zhao Tiejun Zhu state Key laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou310058China department of physics Zhejiang UniversityHangzhou310058China LI-FUN Technology Corporation Limited Zhuzhou412000China

LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)is considered as a promising cathode for high-energy-density solid-sate Li metal battery for its high theoretical ***,the high oxidizability and structural instability during charge limit its practical *** this work,1%(in mass)of nanosized Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)(LATP)was coated on NCM811 to enhance its electrochemical stability with a ceramic/polymer com-posite electrolyte.A robust,ultrathin(11 mm)composite electrolyte film was prepared by combining poly(vinylidene fluoride)(PVDF)with polyethylene oxide(PEO)-Li_(6.5)La_(3)Zr_(1.5)Ta_(0.5)O_(12)(LLZTO).An in-situ polymerization process was used to enhance the interface between the PVDF/PEO-LLZTO(PPL)com-posite electrolyte and the LATP-coated NCM811(LATP-NCM811).Coin-type Li|LATP-NCM811 cell with the PPL electrolyte exhibits stable cycling with an 81%capacity retention after 100 cycles at 0.5 ***-type cell was also fabricated,which can be stably cycled for 70 cycles at 0.5 C/1.0 C(80%retention),and withstand abuse tests of bending,cutting and nail *** work provides an applicable method to fabricate solid-state Li metal batteries with high performance.

关键词： Ultrathin electrolyte film LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)coating In-situ polymerization Li metal battery

Air-stable Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)solid-state electrolyte with high ionic conductivity and lithium anode compatibility toward high-performance all-solid-state lithium metal batteries

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SusMat 2024年第4期4卷 39-49页

作者： Daokuan Jin Haodong Shi Yuxin Ma Yangyang Liu Yang Wang Yanfeng Dong Mingbo Wu Zhong-Shuai Wu state Key laboratory of Heavy Oil Processing Institute of New EnergyCollege of Chemistry and Chemical EngineeringChina University of Petroleum(East China)QingdaoChina state Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina University of Chinese Academy of Sciences BeijingChina College of New Energy China University of Petroleum(East China)QingdaoChina department of Chemistry College of SciencesNortheastern UniversityShenyangChina Dalian national laboratory for Clean Energy Chinese Academy of SciencesDalianChina

Sulfide solid-state electrolytes(SSEs)with superior ionic conductivity and processability are highly promising candidates for constructing all-solid-state lithium metal batteries(ASSLMBs).However,their practical applications are limited by their intrinsic air instability and serious interfacial ***,a novel glass-ceramic electrolyte Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)was synthesized by co-doping Li_(3)PS_(4)with Bi and I for high-performance *** to the strong Bi-S bonds that are thermodynamically stable to water,increased unit cell volume and Li+concentration caused by P5+substitution with Bi3+,and the in situ formed robust solid electrolyte interphase layer LiI at lithium surface,the as-prepared Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)SSE achieved excellent air stability with a H2S concentration of only 0.205 cm^(3)g^(-1)(after 300 min of air exposure),outperform-ing Li_(3)PS_(4)(0.632 cm^(3)g^(-1))and the most reported sulfide SSEs,together with high ionic conductivity of 4.05 mS cm^(-1).Furthermore,the Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)effectively improved lithium metal *** this SSE,an ultralong cyclabil-ity of 700 h at 0.1 mA cm^(-2)was realized in a lithium symmetrical ***,the Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)-based ASSLMBs with LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)cathode achieved ultrastable capacity retention rate of 95.8%after 300 cycles at 0.1 *** work provides reliable strategy for designing advanced sulfide SSEs for commercial applications in ASSLMBs.

关键词： air stability all-solid-state lithium metal battery glass-ceramic lithium metal compatibility sulfide solid-state electrolyte

High-Performance H_(2) Photosynthesis from Pure Water over Ru−S Charge Transfer Channels

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Precision Chemistry 2024年第9期2卷 471-479页

作者： Huiping Peng Mingzi Sun Fei Xue Xiaozhi Liu Shangheng Liu Tang Yang Lin Sun Hongbo Geng Dong Su Bolong Huang Yong Xu Xiaoqing Huang state Key laboratory of Physical Chemistry of solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityKowloonHong Kong SAR 999077China Beijing national laboratory for Condensed Matter physics Institute of physics Chinese Academy of SciencesBeijing 100190China School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China i-lab Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO)Chinese Academy of Sciences(CAS)Suzhou 215123China

As a versatile energy carrier,H_(2) is considered as one of the most promising sources of clean energy to tackle the current energy crisis and environmental concerns,which can be produced from photocatalytic water ***,solar-driven photocatalytic H_(2) production from pure water in the absence of sacrificial reagents remains a great ***,we demonstrate that the incorporation of Ru single atoms(SAs)into ZnIn_(2)S_(4)(Ru-ZIS)can enhance the light absorption,reduce the energy barriers for water dissociation,and construct a channel(Ru-S)for separating photogenerated electron−hole pairs,as a result of a significantly enhanced photocatalytic water splitting ***,the productivity of H_(2) reaches 735.2μmol g^(-1) h^(-1) under visible light irradiation in the absence of sacrificial *** apparent quantum efficiency(AQE)for H_(2) evolution reaches 7.5% at 420 nm,with a solarto-hydrogen(STH)efficiency of 0.58%,which is much higher than the value of natural synthetic plants(~0.10%).Moreover,Ru-ZIS exhibits steady productivity of H_(2) even after exposure to ambient conditions for 330 *** work provides a unique strategy for constructing charge transfer channels to promote the separation of photogenerated electron−hole pairs,which may motivate the fundamental researches on catalyst design for photocatalysis and beyond.

关键词： Ru single atom charge channel ZnIn_(2)S_(4) photocatalytic pure water splitting

Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese Chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping Zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu Haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state Key laboratory of Physical Chemistry of solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS Key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

A Polyvinyl Alcohol/Acrylamide Hydrogel with Enhanced Mechanical Properties Promotes Full-Thickness Skin Defect Healing by Regulating Immunomodulation and Angiogenesis Through Paracrine Secretion

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Engineering 2024年第6期37卷 138-151页

作者： Peng Wang Liping Qian Huixin Liang Jianhao Huang Jing Jin Chunmei Xie Bin Xue Jiancheng Lai Yibo Zhang Lifeng Jiang Lan Li Qing Jiang state Key laboratory of Pharmaceutical Biotechnology Division of Sports Medicine and Adult Reconstructive SurgeryDepartment of Orthopedic SurgeryNanjing Drum Tower HospitalThe Affiliated Hospital of Nanjing University Medical SchoolNanjing UniversityNanjing 210008China Jiangsu Engineering Research Center for 3D Bioprinting Nanjing 210008China Institute of Medical 3D Printing Nanjing UniversityNanjing 210093China Centre for Experimental Animals Nanjing Drum Tower HospitalThe Affiliated Hospital of Nanjing University Medical SchoolNanjing UniversityNanjing 210008China College of Aeroplane Engineering Nanjing University of Aeronautics and AstronauticsNanjing 210016China national laboratory of solid state Microstructures Department of PhysicsNanjing UniversityNanjing 210093China department of Chemical Engineering Stanford UniversityStanfordCA 94305USA department of Orthopedic Surgery The Second Affiliated Hospital Zhejiang University School of MedicineOrthopedic Research Institute of Zhejiang UniversityKey Laboratory of Motor System Disease Research and Precision Therapy of Zhejiang ProvinceHangzhou 310009China

Hydrogel-based tissue-engineered skin has attracted increased attention due to its potential to restore the structural integrity and functionality of ***,the mechanical properties of hydrogel scaffolds and natural skin are substantially ***,we developed a polyvinyl alcohol(PVA)/acrylamide based interpenetrating network(IPN)hydrogel that was surface modified with polydopamine(PDA)and termed *** Dopa-gel exhibited mechanical properties similar to native skin tissue and a superior ability to modulate paracrine ***,a tough scaffold with tensile resistance was fabricated using this hydrogel by three-dimensional *** results showed that the interpenetration of PVA,alginate,and polyacrylamide networks notably enhanced the mechanical properties of the *** modification with PDA endowed the hydrogels with increased secretion of immunomodulatory and proangiogenic *** an in vivo model,Dopa-gel treatment accelerated wound closure,increased vascularization,and promoted a shift in macrophages from a proinflammatory M1 phenotype to a prohealing and anti-inflammatory M2 phenotype within the wound ***,the focal adhesion kinase(FAK)/extracellular signal-related kinase(ERK)signaling pathway may mediate the promotion of skin defect healing by increasing paracrine secretion via the ***,proangiogenic factors can be induced through Rho-associated kinase-2(ROCK-2)/vascular endothelial growth factor(VEGF)-mediated paracrine secretion under tensile stress *** together,these findings suggest that the multifunctional Dopa-gel,which has good mechanical properties similar to those of native skin tissue and enhanced immunomodulatory and angiogenic properties,is a promising scaffold for skin tissue regeneration.

关键词： Polyvinyl alcohol/acrylamide hydrogel Mechanical property enhancement Paracrine effect Skin regeneration Signaling pathways

Free-electron crystals for enhanced X-ray radiation

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Light(Science & Applications) 2024年第7期13卷 1299-1309页

作者： Lee Wei Wesley Wong Xihang Shi Aviv Karnieli Jeremy Lim Suraj Kumar Sergio Carbajo Ido Kaminer Liang Jie Wong School of Electrical and Electronic Engineering Nanyang Technological University50 Nanyang AvenueSingapore 639798Singapore. solid state Institute and Faculty of Electrical and Computer Engineering Technion–Israel Institute of TechnologyHaifa 3200003Israel. School of Electrical Engineering Fleischman Faculty of EngineeringTel Aviv UniversityTel Aviv 69978Israel department of Applied physics Stanford UniversityStanfordCA 94305USA. Science Mathematics and TechnologySingapore University of Technology and Design8 Somapah RoadSingapore 487372Singapore. Electrical and Computer Engineering department UCLA420 WestwoodLos AngelesCA 90095USA. physics and Astronomy department UCLA475 Portola PlazaLos AngelesCA 90095USA. SLAC national Accelerator laboratory Stanford University2575 Sand Hill RoadMenlo ParkCA 94025USA

Bremsstrahlung—the spontaneous emission of broadband radiation from free electrons that are deflected by atomic nuclei—contributes to the majority of X-rays emitted from X-ray tubes and used in applications ranging from medical imaging to semiconductor chip ***,we show that the bremsstrahlung intensity can be enhanced significantly—by more than three orders of magnitude—through shaping the electron wavefunction to periodically overlap with atoms in crystalline ***,we show how to shape the bremsstrahlung X-ray emission pattern into arbitrary angular emission profiles for purposes such as unidirectionality and ***,we find that these enhancements and shaped emission profiles cannot be attributed solely to the spatial overlap between the electron probability distribution and the atomic centers,as predicted by the paraxial and nonrecoil theory for free electron light *** work highlights an unprecedented regime of free electron light emission where electron waveshaping provides multi-dimensional control over practical radiation processes like *** results pave the way towards greater versatility in table-top X-ray sources and improved fundamental understanding of quantum electron-light interactions.

关键词： overlap attributed arbitrary