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Stabilizing MXene suspension with polyhydric alcohols

Journal of Materials Science & Technology 2023年第34期165卷 219-224页

作者： Renfei Cheng Junchao Wang Tao Hu Yiming Zhao Yan Liang Xiaohui Wang yanchun zhou Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China Institute of Materials Science and Devices School of Materials Science and EngineeringSuzhou University of Science and TechnologySuzhou 215009China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

MXenes have promises in myriad applications by virtue of two-dimensional nature and adjustable functional groups.To achieve the applications,MXenes are always first prepared in the form of aqueous suspension.However,fast degradation caused by the attack of dissolved oxygen and water molecules is the main obstacle to the application of MXenes.It has come to light that the degradation preferentially takes place at defective sites and edges where defects enrich.To tackle this problem and increase the stability,herein,using Ti_(3)C_(2)T_(x)MXene as a model material,we report a simple yet efficient strategy for long term storage of MXene suspension by introducing glycerol,a typical polyhydric alcohol.The effectiveness of the strategy is evidenced by structural compositional and morphological investigations.Glycerol protects the defective sites of MXene flakes through restricting water and/or oxygen molecules from reactive sites.This is supported by ab initio molecular dynamics simulations that form hydrogen bonds between MXene and glycerol molecules just over defective sites.Following this mechanism,other polyhydric alcohols,such as ethylene glycol and propylene glycol,are also effective in stabilizing Ti_(3)C_(2)T_(x)MXene suspension.The strategy based on polyhydric alcohols has the potential to be extended to other MXenes,solving the most urgent challenge in the field of MXene engineering.

关键词： MXene Stability Polyhydric alcohols Glycerol Ethylene glycol and propylene glycol

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High-entropy spinel ferrites MFe_(2)O_(4)(M=Mg,Mn,Fe,Co,Ni,Cu,Zn)with tunable electromagnetic properties and strong microwave absorption

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Journal of Advanced Ceramics 2022年第5期11卷 754-768页

作者： Jiabin MA Biao ZHAO Huimin XIANG Fu-Zhi DAI Yi LIU Rui ZHANG yanchun zhou Henan Key Laboratory of Aeronautical Materials and Application Technology School of Materials Science and EngineeringZhengzhou University of AeronauticsZhengzhou 450046China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China School of Material Science and Engineering Shaanxi University of Science and TechnologyXi'an 710021China School of Materials Science and Engineering Luoyang Institute of Science and TechnologyLuoyang 471023China

Ferrites are the most widely used microwave absorbing materials to deal with the threat of electromagnetic(EM)pollution.However,the lack of sufficient dielectric loss capacity is the main challenge that limits their applications.To cope with this challenge,three high-entropy(HE)spineltype ferrite ceramics including(Mg_(0.2)Mn_(0.2)Fe_(0.2)Co_(0.2)Ni_(0.2))Fe_(2)O_(4),(Mg_(0.2)Fe_(0.2)Co_(0.2)Ni_(0.2)Cu_(0.2))Fe_(2)O_(4),and(Mg_(0.2)Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2))Fe_(2)O_(4)were designed and successfully prepared through solid state synthesis.The results show that all three HE MFe_(2)O_(4) samples exhibit synergetic dielectric loss and magnetic loss.The good magnetic loss ability is due to the presence of magnetic components;while the enhanced dielectric properties are attributed to nano-domain,hopping mechanism of resonance effect and HE effect.Among three HE spinels,(Mg_(0.2)Mn_(0.2)Fe_(0.2)Co_(0.2)Ni_(0.2))Fe_(2)O_(4)shows the best EM wave absorption performance,e.g.,its minimum reflection loss(RL_(min))reaches-35.10 dB at 6.78 GHz with a thickness of 3.5 mm,and the optimized effective absorption bandwidth(EAB)is 7.48 GHz from 8.48 to 15.96 GHz at the thickness of 2.4 mm.Due to the easy preparation and strong EM dissipation ability,HE MFe_(2)O_(4) are promising as a new type of EM absorption materials.

关键词： high-entropy ceramics(HECs) spinel-type ferrite electromagnetic(EM)wave absorption dielectric loss magnetic loss

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Regulating the formation ability and mechanical properties of high-entropy transition metal carbides by carbon stoichiometry

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Journal of Materials Science & Technology 2022年第26期121卷 181-189页

作者： Juntao Song Guiqing Chen Huimin Xiang Fuzhi Dai Shun Dong Wenbo Han Xinghong Zhang yanchun zhou Science and Technology on Advanced Composite in Special Environments Laboratory Harbin Institute of TechnologyHarbin150080China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing100076China

Tremendous efforts have been dedicated to promote the formation ability of high-entropy transition metal carbides.However,the majority of methods for the synthesis of high-entropy transition metal carbides still face the challenges of high temperature,low efficiency,additional longtime post-treatment and uncontrollable properties.To cope with these challenges,high-entropy transition metal carbides with regulatable carbon stoichiometry(HE TMC)were designed and synthesized,achieving improved ability for single phase solid solutions formation,promoting of sintering and controllable mechanical properties.Two typical composition series,i.e.,easily synthesized(ZrHfTaNb)C(ZHTNC)and difficultly synthesized(Zr_(0.25)Hf_(0.25)Ta_(0.25)Ti_(0.25))C(ZHTTC)are selected to demonstrate the promoting formation ability of single phase solid solutions from carbon stoichiometry deviations.Single phase high-entropy ZHTTC,which has been proven difficult in forming a single phase solid solution,can be prepared with the decrease of C/TM ratio under 2000℃;while the high-entropy ZHTNC,which has been proven easy in forming a single phase solid solution,can be synthesized at lower temperatures with the decrease of C/TM ratio.The synergistic effect of entropy stabilization and reduced chemical bond strength gaining from carbon stoichiometry deviations is responsible for the formation of single phase solid solutions and the promoted sintering of HE TMC.For example,the relative density of bulk(ZrHfTaNb)C(SPS-ZHTNC)increases from 90.98%to 94.25%with decreasing the C/TM atomic ratio from 0.9 to 0.74.More importantly,the room temperature flexural strength,fracture toughness and brittleness index of SPS-ZHTNCcan be tuned in the range of 384 MPa–419 MPa,4.41 MPam–4.73 MPamand 3.679μm–4.083μm,respectively.Thus,the HE TMCprepared by adjusting the ratio of carbon to refractory transition metal oxides have great potential for achieving low temperature synthesis,promoted sintering and tunable properties.

关键词： Carbon stoichiometry High-entropy ceramics Transition metal carbide Low temperature synthesis Tunable mechanical properties

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Tunnel-structured willemite Zn_(2)SiO_(4):Electronic structure,elastic,and thermal properties

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Journal of Advanced Ceramics 2022年第8期11卷 1249-1262页

作者： Ruqiao DAI Renfei CHENG Jiemin WANG Chao ZHANG Cuiyu LI Hailong WANG Xiaohui WANG yanchun zhou Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China Advanced Computing East China Sub-center Suma Technology Company LimitedKunshan 215300China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China

Willemite Zn_(2)SiO_(4)crystallizes in such a way that Zn and Si are tetrahedrally coordinated with O in an ionic–covalent manner to form ZnO_(4)and SiO_(4)tetrahedra as the building units.The tetrahedra are corner-sharing,of which one SiO_(4)tetrahedron connects eight ZnO_(4)tetrahedra,and one ZnO_(4)tetrahedron links four ZnO_(4)tetrahedra and four SiO_(4)tetrahedra.The unique crystallographic configuration gives rise to parallel tunnels with a diameter of 5.7Åalong the c-axis direction.The tunnel structure of Zn_(2)SiO_(4)definitely correlates with its interesting elastic and thermal properties.On the one hand,the elastic modulus,coefficient of thermal expansion(CTE),and thermal conductivity are low.Zn_(2)SiO_(4)has low Vickers hardness of 6.6 GPa at 10 N and low thermal conductivity of 2.34 W/(m·K)at 1073 K.On the other hand,the elastic modulus and CTE along the c-axis are significantly larger than those along the a-and b-axes,showing obvious elastic and thermal expansion anisotropy.Specifically,the Young’s modulus along the z direction(Ez=179 GPa)is almost twice those in the x and y directions(Ex=Ey=93 GPa).The high thermal expansion anisotropy is ascribed to the empty tunnels along the c-axis,which are capable of more accommodating the thermal expansion along the a-and b-axes.The striking properties of Zn_(2)SiO_(4)in elastic modulus,hardness,CTE,and thermal conductivity make it much useful in various fields of ceramics,such as low thermal expansion,thermal insulation,and machining tools.

关键词： Zn_(2)SiO_(4) electronic structure elastic properties thermal expansion thermal conductivity

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Improved thermal stability and infrared emissivity of high-entropy REMgAl_(11)O_(19)and LaMAl_(11)O_(19)(RE=La,Nd,Gd,Sm,Pr,Dy;M=Mg,Fe,Co,Ni,Zn)

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Journal of Materials Science & Technology 2022年第9期104卷 131-144页

作者： Haolin Zhu Ling Liu Huimin Xiang Fu-Zhi Dai Xiaohui Wang Zhuang Ma Yanbo Liu yanchun zhou School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China National Key Laboratory of Science and Technology on Materials under Shock and Impact Beijing 100081China Beijing Institute of Technology Chongqing Innovation Center Chongqing 401120China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China

LaMgAl_(11)O_(19)(LMA),characterized by high melting point,low density and thermal conductivity as well as good infrared emissivity,is regarded as a potential candidate for the thermal protection of hypersonic vehicles.Nevertheless,the unsatisfied phase stability at high temperature results in declining of the emissivity below 6μm,which limits the extensive applications of LaMgAl_(11)O_(19).In order to overcome this obstacle,three dense bulk high-entropy ceramics,(La_(0.2)Nd_(0.2)Gd_(0.2)Sm_(0.2)Pr_(0.2))MgAl_(11)O_(19)(HE LMA-1),(La_(0.2)Nd_(0.2)Gd_(0.2)Sm_(0.2)Dy_(0.2))Mg Al_(11)O_(19)(HE LMA-2)and La(Mg_(0.2)Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2))Al_(11)O_(19)(HE LMA-3),were designed and successfully prepared through solid state reaction at 1700℃for 4 h in one step.XRD analyses show that the phase compositions of HE LMA-1,HE LMA-2 and HE LMA-3 are single-phase solid solutions with the relative density of 95.61%,95.49%and 94.31%,respectively.Heat treatment experiments demonstrate that the phase composition of HE LMA-1 remains a single phase after high-temperature heating,while second phase appears in other two samples.The stability of HE LMA-1 is attributed to small average size differenceδ(~4%)of constitute elements.Intriguingly,the average emissivity of HE LMA-1 in the range of 3-6μm reaches 0.9,which is significantly higher than that of LMA and other two HE LMA samples.The emissivity of all samples remains above 0.95 from 6 to 10μm.In the far infrared region(10-14μm),although the emissivity of these specimens decreases slightly,it still exceeds 0.85.The UV-Vis absorption spectra indicate that the formation of many discrete impurity energy levels with small intervals in HE LMA-1 promotes the f electrons to transit between adjacent impurity energy levels and conduction band,which enhances the infrared emission of HE LMA-1 below 6μm.In a word,with improved phase stability and thermal emissivity in infrared range,high-entropy REMgAl_(11)O_(19),especially(La_(0.2)Nd_(0.2)Gd_(0.2)Sm_(0.2)Pr_(0.2))MgAl_(11)O_(19)(HE LMA-

关键词： High-entropy ceramics LaMgAl_(11)O_(19) Thermal stability Infrared emissivity UV-Vis absorption

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Single droplet formation by controlling the viscoelasticity of polymer solutions during inkjet printing

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Chinese Chemical Letters 2024年第6期35卷 244-248页

作者： Dong Lv Xuelei Liu Wei Li Qiang Zhang Xinhong Yu yanchun Han State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Inkjet printing has emerged as a potential solution processing method for large-area patterned films.During inkjet printing,a single droplet without satellite droplet is required for high-quality film.Herein,we propose a strategy for obtaining a single droplet by adjusting the reduced concentration(c/c^(*),where c^(*)is the critical overlap concentration)in the range of 1.0-1.5.Droplet formation can be categorized into three distinct regimes:(1)c/c^(*)2.0,no droplet.Furthermore,an inertial-capillary balance led to the 2/3-power scaling of the minimum radius with time for the solutions of c/c^(*)<1.0.However,for the solutions of c/c^(*)=1.0-1.5,the ligament radius decreased exponentially with time.Moreover,the Weissenberg number was higher than the critical value of 0.5,indicating that the polymer chains underwent coil-stretch transition.The viscoelastic-capillary balance dominated instead of the inertial-capillary balance.The resulting viscoelastic resistance reduced the length of the ligament and increased the velocity difference between the satellite and main droplets.Consequently,a single droplet was formed.In addition,the law can be successfully generalized to various molecular weights,molecular structures and solvents.

关键词： Inkjet printing Single droplet Satellite droplet Viscoelasticity Coil-stretch

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Zr_(2)SeB and Hf_(2)SeB:Two new MAB phase compounds with the Cr_(2)AlC-type MAX phase(211 phase)crystal structures

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Journal of Advanced Ceramics 2022年第11期11卷 1764-1776页

作者： Qiqiang ZHANG yanchun zhou Xingyuan SAN Wenbo LI Yiwang BAO Qingguo FENG Salvatore GRASSO Chunfeng HU Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China Hebei Key Lab of Optic–Electronic Information and Materials College of Physics Science and TechnologyHebei UniversityBaoding 071002China State Key Laboratory of Green Building Materials China Building Materials AcademyBeijing 100024China

The ternary or quaternary layered compounds called MAB phases are frequently mentioned recently together with the well-known MAX phases.However,MAB phases are generally referred to layered transition metal borides,while MAX phases are layered transition metal carbides and nitrides with different types of crystal structure although they share the common nano-laminated structure characteristics.In order to prove that MAB phases can share the same type of crystal structure with MAX phases and extend the composition window of MAX phases from carbides and nitrides to borides,two new MAB phase compounds Zr_(2)SeB and Hf_(2)SeB with the Cr_(2)AlC-type MAX phase(211 phase)crystal structure were discovered by a combination of first-principles calculations and experimental verification in this work.First-principles calculations predicted the stability and lattice parameters of the two new MAB phase compounds Zr_(2)SeB and Hf_(2)SeB.Then they were successfully synthesized by using a thermal explosion method in a spark plasma sintering(SPS)furnace.The crystal structures of Zr_(2)SeB and Hf_(2)SeB were determined by a combination of the X-ray diffraction(XRD),scanning electron microscopy(SEM),and high-resolution transmission electron microscopy(HRTEM).The lattice parameters of Zr_(2)SeB and Hf_(2)SeB are a=3.64398Å,c=12.63223Åand a=3.52280Å,c=12.47804Å,respectively.And the atomic positions are M at 4f(1/3,2/3,0.60288[Zr]or 0.59889[Hf]),Se at 2c(1/3,2/3,1/4),and B at 2a(0,0,0).And the atomic stacking sequences follow those of the Cr_(2)AlC-type MAX phases.This work opens up the composition window for the MAB phases and MAX phases and will trigger the interests of material scientists and physicists to explore new compounds and properties in this new family of materials.

关键词： Zr_(2)SeB and Hf_(2)SeB MAB phase MAX phase first-principles calculations thermal explosion synthesis

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Curing the vulnerable heterointerface via organic-inorganic hybrid hole transporting bilayers for efficient inverted perovskite solar cells

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Chinese Chemical Letters 2024年第6期35卷 254-257页

作者： Kangrong Yan Ziqiu Shen yanchun Huang Benfang Niu Hongzheng Chen Chang-Zhi Li State Key Laboratory of Silicon and Advanced Semiconductor Materials Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

To promote the practices of perovskite photovoltaics,it requires to develop efficient perovskite solar cells(PVSCs)standing long-time operation under the adverse environments.Herein,we demonstrate that the tailor-made conjugated polymers as conductive adhesives stabilized the originally redox-reactive heterointerface between perovskite and metal oxide,facilitating the access of efficient and stable inverted PVSCs.It was revealed that bithiophene and phenyl alternating conjugated polymers with partial glycol chains atop of the metal oxide layer has resulted in effective organic-inorganic hybrid hole transporting bilayers,which allow maintaining efficient hole extraction and transport,meanwhile preventing halide migration to directly contact with the nickel oxide(NiO_(x))layer.As a result,the corresponding inverted PVSCs with the organic-inorganic hole transporting bilayers have achieved an excellent power conversion efficiency of 23.22%,outperforming 20.65% of bare NiO_(x)-based devices.Moreover,the encapsulated PVSCs with organic-inorganic bilayers exhibited the excellent photostability with 91% of the initial efficiency after 1000-h one-sun equivalent illumination in ambient conditions.Overall,this work provides new insights into stabilizing the vulnerable heterointerface for perovskite solar cells.

关键词： Perovskite solar cells Conjugated polymer Hole transporting bilayer Charge extraction Heterointerface degradation

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Synthesis and mechanical and elevated temperature tribological properties of a novel high-entropy(TiVNbMoW)C_(4.375) with carbon stoichiometry deviation

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Journal of Advanced Ceramics 2023年第2期12卷 242-257页

作者： Jicheng LI yanchun zhou Yunfeng SU Shuna CHEN Qiuan SUN Hengzhong FAN Junjie SONG Litian HU Yongsheng ZHANG State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Science and Technology on Advanced Functional Composite Laboratory Aerospace Research Institute of Materials&Processing TechnologyBeijing 100076China

High-entropy carbides are a nascent group of ceramics that are promising for high-temperature applications due to the combination of good stability,high hardness(H),high strength,and superior creep resistance that they display.Due to high melting points and low lattice diffusion coefficients,however,the high-entropy carbides are usually difficult to consolidate to a nearly full density.To cope with this challenge,herein,binary carbides including TiC,V_(8)C_(7),NbC,Mo_(2)C,and WC with different carbon stoichiometry were used to prepare dense high-entropy(TiVNbMoW)C_(4.375),and the influence of carbon vacancy on formation ability and mechanical properties of carbon-deficient high-entropy(TiVNbMoW)C_(4.375) were investigated.Intriguingly,although the starting binary carbides have different crystal structures and carbon stoichiometry,the as-prepared high-entropy material showed a rock-salt structure with a relatively high density(98.1%)and good mechanical properties with hardness of 19.4±0.4 GPa and fracture toughness(KIC)of 4.02 MPa·m^(1/2).More importantly,the high-entropy(TiVNbMoW)C_(4.375) exhibited low coefficient of friction(COF)at room temperature(RT)and 800℃.Wear rate(W)gradually increased with the temperature rising,which were attributed to the formation of low-hardness oxidation films at high temperatures to aggravate wear.At 800℃,lubricating films formed from sufficient oxidation products of V_(2)O_(5) and MoO_(3) effectively improved tribological behavior of the high-entropy(TiVNbMoW)C_(4.375).Wear mechanisms were mainly abrasive wear resulting from grain pullout and brittle fracture as well as oxidation wear generated from high-temperature reactions.These results are useful as valuable guidance and reference to the synthesis of high-entropy ceramics(HECs)for sliding parts under high-temperature serving conditions.

关键词： high-entropy ceramics(HECs) transition metal(TM)carbides carbon stoichiometry deviation tribological performances wear

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Electron-irradiation-facilitated production of chemically homogenized nanotwins in nanolaminated carbides

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Journal of Advanced Ceramics 2023年第6期12卷 1288-1297页

作者： Hui Zhang Qianqian Jin Tao Hu Xiaochun Liu Zezhong Zhang Chunfeng Hu yanchun zhou Yu Han Xiaohui Wang Electron Microscopy Center South China University of TechnologyGuangzhou 510640China School of Emergent Sof Mater South China University of TechnologyGuangzhou 510640China Center for the Structure of Advanced Matter School of Electronic EngineeringGuangxi University of Science and TechnologyLiuzhou 545006China Institute of Materials Science and Devices School of Materials Science and EngineeringSuzhou University of Science and TechnologySuzhou 215009China Institute of Metals Changsha University of Science&TechnologyChangsha 410004China Electron Microscopy for Materials Research(EMAT) University of AntwerpAntwerp 2020Belgium Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China School of Materials Science&Engineering Zhengzhou UniversityZhengzhou 4501China Advanced Membranes and Porous Materials Center Physical Sciences and Engineering DivisionKing Abdullah University of Science and TechnologyThuwal 23955-6900Saudi Arabia Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China

Twin boundaries have been exploited to stabilize ultrafine grains and improve mechanical properties of nanomaterials.The production of the twin boundaries and nanotwins is however prohibitively challenging in carbide ceramics.Using a scanning transmission electron microscope as a unique platform for atomic-scale structure engineering,we demonstrate that twin platelets could be produced in carbides by engineering antisite defects.The antisite defects at metal sites in various layered ternary carbides are collectively and controllably generated,and the metal elements are homogenized by electron irradiation,which transforms a twin-like lamellae into nanotwin platelets.Accompanying chemical homogenization,α-Ti_(3)AlC_(2) transforms to unconventionalβ-Ti_(3)AiC_(2).The chemical homogeneity and the width of the twin platelets can be tuned by dose and energy of bombarding electrons.Chemically homogenized nanotwins can boost hardness by~45%.Our results provide a new way to produce ultrathin(<5 nm)nanotwin platelets in scientifically and technologically important carbide materials and showcase feasibility of defect engineering by an angstrom-sized electron probe.

关键词： electron-irradiation MAX phases carbides antisite defects crystal-structure engineering

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