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Tribological properties and tribomechanism of nickel nanoparticles in-situ synthesized in rapeseed oil

Friction 2024年第3期12卷 474-489页

作者： Wenya XU Guangbin YANG Shengmao ZHANG Jun XU Yujuan ZHANG Tianhua SUN Ningning SONG Laigui YU Pingyu ZHANG Engineering research Center for nanomaterials Henan UniversityKaifeng 475004China State Key laboratory of Tribology in Advanced Equipment Tsinghua UniversityBeijing 100084China

Nickel(Ni)nanoparticles can be enriched on the surface of iron-based frictional pairs,which provides the possibility to get rid of the competitive adsorption between the polar species of vegetable oil and the surface-active nano-additives *** this paper,nickel acetylacetonate was used as a precursor to in-situ synthesize nickel nanoparticles with an average diameter of about 12 nm in rapeseed oil(RO)as the reducing agent,surface modifier,and solvent as *** tribological properties of the as-synthesized Ni nanoparticles were evaluated with a four-ball tribometer,and their tribomechanism was investigated based on the characterizations of the tribofilm on rubbed steel surfaces by the scanning electron microscopy(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).It was found that the Ni nanoparticles in-situ prepared in the RO with a mass fraction of 0.3%can reduce the wear scar diameter(WSD)of the steel ball by 36%.This is because,on the one hand,the Ni nanoparticles are adsorbed on the rubbed steel surfaces to repair or fill up the micro-pits and grooves *** the other hand,Ni nanoparticles participate in tribochemical reactions with atmospheric O and steel substrate to form the tribochemical reaction film on the rubbed steel surfaces with the assistance of friction-induced heat and applied normal *** addition,an amorphous carbon film is formed on the rubbed surface via the carbonization of base oil under the catalysis of Ni *** adsorbed Ni layer,the tribochemical reaction film,and the carbon layer comprise a composite tribofilm composed of amorphous carbon,polar fatty acid,metallic nickel,iron oxides,and nickel oxides on the rubbed steel surfaces,which contributes to significantly improving the antiwear ability and load-carrying capacity of the RO for the steel-steel sliding pair.

关键词： nickel(Ni)nanoparticles rapeseed oil(RO) in-situ synthesis tribological properties tribomechanism

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2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density toward a self-sufficient integrated microsystem

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Fundamental research 2024年第2期4卷 307-314页

作者： Yuanyuan Zhu Shuanghao Zheng Jieqiong Qin Jiaxin Ma Pratteek Das Feng Zhou Zhong-Shuai Wu State Key laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China College of Science Henan Agricultural UniversityZhengzhou 450002China Dalian National laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China Key laboratory of Spin Electron and nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors(MSCs)catering to integrated ***,the narrow electrochemical voltage windows of conventional aqueous electrolytes(≤1.23 V)and symmetric MXene MSCs(typically≤0.6 V)substantially limit their output voltage and energy *** concentrated aqueous electrolytes exhibit lower water molecule activity,which inhibits water splitting and consequently widens the operating voltage ***,we report ultrahigh-voltage aqueous planar asymmetric MSCs(AMSCs)based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene(Ti3C2Tx)as the negative electrode and MnO_(2) nanosheets as the positive electrode(MXene//MnO_(2)-AMSCs).The MXene//MnO_(2)-AMSCs exhibit a high voltage of up to 2.4 V,attaining an ultrahigh volumetric energy density of 53 mWh cm−***,the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our ***,the MXene//MnO_(2)-AMSC-based integrated microsystem,in conjunction with solar cells and consumer electronics,could efficiently realize simultaneous energy harvesting,storage,and *** findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.

关键词： Asymmetric micro-supercapacitors MXene MnO_(2) Aqueous electrolyte High voltage Integrated microsystem

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Synergic catalysis of W and Ni originating from substitution of trivacant phosphotungstate for the selective oxidation of aniline to azoxybenzene

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Chinese Chemical Letters 2024年第2期35卷 558-563页

作者： Sheng Cai Xiao-Yuan Wu Weiming Wu Sa-Sa Wang Can-Zhong Lu CAS Key laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China Xiamen Institute of Rare Earth Materials Chinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China

Partial substitution of polyoxometalate(POM)is an efficient route to modulate the catalytic property of maternal *** this work,a new Keggin type POM involving{Ni 6}cluster,{[Ni(H_(2) O)_(2)(Dach)_(2)][Ni(Dach)_(2)]_(2)}{[Ni_(6)Cl(μ-OH)_(3)(H_(2) O)(Dach)_(3)(WO_(4))(PW9 O_(3)_(4))][Ni_(6)(μ-OH)_(3)(H_(2) O)_(2)(Dach)_(3)(WO_(4))(PW9 O_(3)_(4))]}Cl·27H_(2) O,(1,Dach=1,2-diaminocyclohexane)was *** 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene(AOB)in *** apparently different results from that with the matrix{PW 9 O_(3)_(4)}({PW9})suggest the successful regulation of the catalytic property of{PW9}by the introduction of the{Ni6}cluster into the *** experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites,which are respectively responsible for the oxidation and condensation steps in the production of *** good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites,respectively.

关键词： Polyoxometalate {Ni6}cluster Modulated catalytic property Aniline oxidation Azoxybenzene

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Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries

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Chinese Chemical Letters 2024年第5期35卷 434-440页

作者： Haodong Wang Xiaoxu Lai Chi Chen Pei Shi Houzhao Wan Hao Wang Xingguang Chen Dan Sun CAS Key laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key laboratory of nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Fujian Normal UniversityFuzhou 350007China Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China School of Microelectronics Hubei UniversityWuhan 430062China Xiamen Key laboratory of Rare Earth Photoelectric Functional Materials Xiamen 361021China

The detrimental“shuttle effect”of lithium polysulfides(LiPSs)together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur(Li-S)batteries from commercial ***,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical *** this work,a two-dimensional(2D)rare-earth-based composite constructed by the layered gadolinium hydroxy chloride[Gd_(2)(OH)_(5)(H_(2)O)_(n)]Cl nanoplates(LGdH NPs)and graphene oxide(GO)was designed as a sulfur immobilizer for Li-S *** the experimental results and density functional theory(DFT)calculations,it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling,but also acts as an effective catalyst to accelerate the liquid-solid conversion of *** Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C,as well as excellent cycle stability with a decay rate of 0.087%over 500 cycles at 2 *** study provided a deep understanding of the mechanism to suppress the“shuttle effect”by the LREHs,and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.

关键词： Lithium-sulfur batteries Functional separator Layered rare-earth hydroxides Shuttle effect Adsorption catalysis

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Supported Atomically Dispersed Pd Catalyzed Direct Alkoxylation and Allylic Alkylation

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Chinese Journal of Chemistry 2024年第7期42卷 719-724页

作者： Ruixuan Qin Ziwen Chen Qingyuan Wu Nanfeng Zheng Pengxin Liu New Cornerstone Science laboratory State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenFujian 361005China Innovation Laboratry for Scences and Technoogies of Energy Materials of Fujan Province(IKKM) Xiamen Fujian 361102China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Fujian Key laboratory of Rare-earth Functional Materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyanFujian 366300China

A new approach to allylic alkylation is realized using an atomically dispersed palladium catalyst(Pd1/TiO2-EG).Unlike conventional methods that require derivation of substrates and utilization of additives,this method allows for direct allylic alkylation from allylic alcohols,producing H2O as the sole *** catalyst's high efficiency is attributed to the local hydrogen bonding at the or-ganic-inorganic interface(Pd-EG interface),facilitating hydroxyl group activation forη3π-allyl complex *** system demonstrates successful direct C—O and C—C coupling reactions with high selectivity,requiring no *** study highlights the potential of supported atomically dispersed catalysts for greener and more efficient catalysis,meanwhile,offers unique insights into the distinct behavior of atomically dispersed catalysts in comparison to homogeneous or nanoparticle-based catalysts.

关键词： Atomically dispersed catalyst Alkylation C—C coupling Organic-inorganic Interface Hydrogen bond Tsuji-Trost reaction Green catalysis

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Surface Ligand Evolution:Sulfur-Directed Covalent Bonding of PPh_(3) on Pd_(4)S with Improved Semi-hydrogenation of Terminal Alkynes

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Precision Chemistry 2024年第5期2卷 200-207页

作者： Wentong Jing Shiguang Mo Weijie Zhang Wenting Zhou Kunlong Liu Jie Wei Ruixuan Qin Nanfeng Zheng New Cornerstone Science laboratory State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China China Resources Cement Technology R&D(Guangxi)Co Ltd. Nanning 530008China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Surface modification of metallic nanocatalysts with organic ligands has emerged as an effective strategy to enhance catalytic selectivity,although offten at the expense of catalytic *** this study,we demonstrate a compelling approach by surface modifying Pd2S nanocrystals with PPhz ligands,resulting in a catalyst with excellent catalytic activity and durable selectivity for the semi-hydrogenation of terminal *** and theoretical investigations reveal that the presence of S sites on the Pd surface directs PPh_(3) ligands to preferentially form covalent bonds with S,creating distinctive surface S=PPh_(3) *** configuration induces a partial positive charge on Pd,facilitating hydrogen transfer and thus promoting catalytic ***,the covalent bond between the ligand and catalyst surface forms a robust network,ensuring ligand stability and increasing the hydrogenation energy barrier of ***,the Pd_(4)S@PPhz catalyst exhibits an improved catalytic selectivity with durability in terminal alkyne *** study introduces an effective strategy for designing selective hydrogenation catalysts with an enhanced performance.

关键词： Pd nanocatalysts surface modification selective hydrogenation catalytic stability alkyne semi-hydrogenation

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An Integrated Carbon Dioxide Capture and Methanation Process

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CCS Chemistry 2024年第5期6卷 1174-1183页

作者： Xiaochen Zhang Mengzhu Li Xingwu Liu Ang Li Yuchen Deng Mi Peng Yu Zhang Charlotte Vogt Matteo Monai Junxian Gao Xuetao Qin Yao Xu Qiaolin Yu Meng Wang Guofu Wang Zheng Jiang Xiaodong Han Casper Brady Wei-Xue Li Wu Zhou Jin-Xun Liu Bingjun Xu Bert M.Weckhuysen Ding Ma Beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 China Academy of Aerospace Science and Innovation Beijing 100088 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Beijing 101400 Beijing Key laboratory of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing Inorganic Chemistry and catalysis group Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials ScienceFaculty of ScienceUtrecht University3584 CG Utrecht State Key laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001 Shanghai Synchrotron Radiation Facility Zhangjiang LadShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210 Center for Catalytic Science and Technology University of DelawareNewarkDelaware 19716 Key laboratory of Precision and Intelligent Chemistry School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefeiAnhui 230026 Hefei National laboratory University of Science and Technology of ChinaHefei 230088 School of Physical Sciences CAS Key Laboratory of Vacuum PhysicsUniversity of Chinese Academy of SciencesBeijing 100049

Reducing the ever-growing level of CO_(2)in the atmosphere is critical for the sustainable development of human society in the context of global *** of the capture and upgrading of CO_(2)is,therefore,highly desirable since each process step is costly,both energetically and ***,we report a CO_(2)direct air capture(DAC)and fixation process that produces *** concentrations of CO_(2)(∼400 ppm)in the air are captured by an aqueous solution of sodium hydroxide to form *** carbonate is subsequently hydrogenated to methane,which is easily separated from the reaction system,catalyzed by TiO2-supported Ru in the aqueous phase with a selectivity of 99.9%among gas-phase *** concurrent regenerated hydroxide,in turn,increases the alkalinity of the aqueous solution for further CO_(2)capture,thereby enabling this one-ofits-kind continuous CO_(2)capture and methanation *** simulations demonstrate the energy feasibility of this CO_(2)DAC and methanation process,highlighting its promise for potential largescale applications.

关键词： CO_(2)capture and methanation process sodium hydroxide carbonate Ru/TiO_(2) catalytic mechanism CO_(2)activation and hydrogenation

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MXene@c-MWCNT Adhesive Silica Nanofiber Membranes Enhancing Electromagnetic Interference Shielding and Thermal Insulation Performance in Extreme Environments

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Nano-Micro Letters 2024年第10期16卷 82-98页

作者： Ziyuan Han Yutao Niu Xuetao Shi Duo Pan Hu Liu Hua Qiu Weihua Chen Ben Bin Xu Zeinhom MEl-Bahy Hua Hou Eman Ramadan Elsharkawy Mohammed AAmin Chuntai Liu Zhanhu Guo Key laboratory of Materials Processing and Mold(Zhengzhou University) Ministry of EducationNational Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou 450002People's Republic of China School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefei 230026People's Republic of China Key laboratory of Multifunctional nanomaterials and Smart Systems Advanced Materials DivisionSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123People's Republic of China Shaanxi Key laboratory of Macromolecular Science and Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi'an 710072People's Republic of China College of Chemistry&Green catalysis Center Zhengzhou UniversityZhengzhou 450001People's Republic of China Mechanical and Construction Engineering Faculty of Engineering and EnvironmentNorthumbria UniversityNewcastle Upon Tyne NE18UK Department of Chemistry Faculty of ScienceAl-Azhar UniversityNasr City 11884CairoEgypt Department of Chemistry Faculty of ScienceNorthern Border UniversityArarSaudi Arabia Department of Chemistry College of ScienceTaif UniversityP.O.Box 1109921944 TaifSaudi Arabia

A lightweight flexible thermally stable composite is fabricated by com-bining silica nanofiber membranes(SNM)with MXene@c-MWCNT hybrid *** flexible SNM with outstanding thermal insulation are prepared from tetraethyl orthosilicate hydrolysis and condensation by electrospinning and high-temperature calcination;the MXene@c-MWCNT_(x:y)films are prepared by vacuum filtration *** particular,the SNM and MXene@c-MWCNT_(6:4)as one unit layer(SMC_(1))are bonded together with 5 wt%polyvinyl alcohol(PVA)solution,which exhibits low thermal conductivity(0.066 W m^(-1)K^(-1))and good electromagnetic interference(EMI)shielding performance(average EMI SE_(T),37.8 dB).With the increase in func-tional unit layer,the overall thermal insulation performance of the whole composite film(SMC_(x))remains stable,and EMI shielding performance is greatly improved,especially for SMC_(3)with three unit layers,the average EMI SET is as high as 55.4 *** addition,the organic combination of rigid SNM and tough MXene@c-MWCNT_(6:4)makes SMC_(x)exhibit good mechanical tensile ***,SMC_(x)exhibit stable EMI shielding and excellent thermal insulation even in extreme heat and cold ***,this work provides a novel design idea and important reference value for EMI shielding and thermal insulation components used in extreme environmental protection equipment in the future.

关键词： SiO_(2)nanofiber membranes MXene@c-MWCNT Composite film Thermal insulation Electromagnetic interference shielding

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具有骨样微环境的压电催化可控矿化支架实现内源性骨再生

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Science Bulletin 2024年第12期69卷 1895-1908页

作者：崔希胥玲玲单义珠李佳宣吉健颖汪恩贵张葆堃文晓舟白源罗聃陈春英李舟 Beijing Key laboratory of Micro-nano Energy and Sensor Beijing Institute of Nanoenergy and NanosystemsChinese Academy of SciencesBeijing 101400China School of Nanoscience and Engineering University of Chinese Academy of SciencesBeijing 100049China New Cornerstone Science laboratory CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety and CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China

Orderly hierarchical structure with balanced mechanical,chemical,and electrical properties is the basis of the natural bone *** by nature,we developed a piezocatalytically-induced controlled mineralization strategy using piezoelectric polymer poly-L-lactic acid(PLLA)fibers with ordered micro-nano structures to prepare biomimetic tissue engineering scaffolds with a bone-like microenvironment(pcm-PLLA),in which PLLA-mediated piezoelectric catalysis promoted the in-situ polymerization of dopamine and subsequently regulated the controllable growth of hydroxyapatite crystals on the fiber *** fibers,as analogs of mineralized collagen fibers,were arranged in an oriented manner,and ultimately formed a bone-like interconnected pore structure;in addition,they also provided bone-like piezoelectric *** uniformly sized HA nanocrystals formed by controlled mineralization provided a bone-like mechanical strength and chemical *** pcm-PLLA scaffold could rapidly recruit endogenous stem cells,and promote their osteogenic differentiation by activating cell membrane calcium channels and PI3K signaling pathways through ultrasound-responsive piezoelectric *** addition,the scaffold also provided a suitable microenvironment to promote macrophage M2 polarization and angiogenesis,thereby enhancing bone regeneration in skull defects of *** proposed piezocatalytically-induced controllable mineralization strategy provides a new idea for the development of tissue engineering scaffolds that can be implemented for multimodal physical stimulation therapy.

关键词： Piezoelectric catalysis Controllable mineralization Biomimetic Bone repair Biodegradable

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NIR-Ⅱ成像引导的精准光动力治疗通过干扰糖代谢重编程增强肿瘤饥饿治疗

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Science Bulletin 2024年第9期69卷 1263-1274页

作者：吴夏维凡勇王楷若缪云秋常永亮明江王欣月陆晟威刘芮池张凡张扬秦环龙施剑林 Nanomedicine and Intestinal Microecology research Center Shanghai Tenth People’s HospitalSchool of MedicineTongji UniversityShanghai 200072China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsState Key Laboratory of Molecular Engineering of Polymers and iChemFudan UniversityShanghai 200433China State Key laboratory of High Performance Ceramics and Superﬁne Microstructure Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China

Metabolic reprogramming is a mechanism by which cancer cells alter their metabolic patterns to promote cell proliferation and growth, thereby enabling their resistance to external stress. 2-Deoxy-Dglucose(2DG) can eliminate their energy source by inhibiting glucose glycolysis, leading to cancer cell death through starvation. However, a compensatory increase in mitochondrial metabolism inhibits its efficacy. Herein, we propose a synergistic approach that combines photodynamic therapy(PDT) with starvation therapy to address this challenge. To monitor the nanodrugs and determine the optimal triggering time for precise tumor therapy, a multifunctional nano-platform comprising lanthanide-doped nanoparticle(Ln NP) cores was constructed and combined with mesoporous silicon shells loaded with2DG and photosensitizer chlorin e6(Ce6) in the mesopore channels. Under 980 nm near-infrared light excitation, the downshifted 1550 nm fluorescence signal in the second near-infrared(NIR-II, 1000–1700 nm) window from the Ln NPs was used to monitor the accumulation of nanomaterials in ***, upconverted 650 nm light excited the Ce6 to generate singlet oxygen for PDT, which damaged mitochondrial function and enhanced the efficacy of 2DG by inhibiting hexokinase 2 and lactate dehydrogenase A expressions. As a result, glucose metabolism reprogramming was inhibited and the efficiency of starvation therapy was significantly enhanced. Overall, the proposed NIR-II bioimaging-guided PDT-augmented starvation therapy, which simultaneously inhibited glycolysis and mitochondria, facilitated the effects of a cancer theranostic system.

关键词： Metabolic reprogramming Colorectal cancer Glycolytic inhibition Photodynamic therapy NIR-II imaging

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