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Moderate Fields, Maximum Potential: Achieving High Records with Temperature‑Stable Energy Storage in lead‑free BNT‑Based Ceramics

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Nano-Micro Letters 2024年第5期16卷 184-200页

作者： Wenjing Shi Leiyang Zhang Ruiyi Jing Yunyao Huang Fukang Chen Vladimir Shur Xiaoyong Wei Gang Liu Hongliang Du Li Jin Electronic Materials Research Laboratory Key Laboratory of the Ministry of EducationSchool of Electronic Science and EngineeringXi’an Jiaotong UniversityXi’an 710049People’s Republic of China School of Materials and Energy Southwest UniversityChongqing 400715People’s Republic of China School of Natural Sciences and Mathematics Ural Federal UniversityEkaterinburg 620000Russia Multifunctional Electronic Ceramics Laboratory College of EngineeringXi’an International UniversityXi’an 710077People’s Republic of China

The increasing awareness of environmental concerns has prompted a surge in the exploration of leadfree,high-power ceramic capacitors.Ongoing efforts to develop leadfree dielectric ceramics with exceptional energystorage performance(ESP)have predominantly relied on multicomponent composite strategies,often accomplished under ultrahigh electric fields.However,this approach poses challenges in insulation and system downsizing due to the necessary working voltage under such conditions.Despite extensive study,bulk ceramics of(Bi_(0.5)Na_(0.5))TiO_(3)(BNT),a prominent lead-free dielectric ceramic family,have seldom achieved a recoverable energy-storage(ES)density(Wrec)exceeding 7 J cm^(−3).This study introduces a novel approach to attain ceramic capacitors with high ESP under moderate electric fields by regulating permittivity based on a linear dielectric model,enhancing insulation quality,and engineering domain structures through chemical formula optimization.The incorporation of SrTiO_(3)(ST)into the BNT matrix is revealed to reduce the dielectric constant,while the addition of Bi(Mg_(2/3)Nb_(1/3))O_(3)(BMN)aids in maintaining polarization.Additionally,the study elucidates the methodology to achieve high ESP at moderate electric fields ranging from 300 to 500 kV cm^(−1).In our optimized composition,0.5(Bi_(0.5)Na_(0.4)K_(0.1))TiO_(3)–0.5(2/3ST-1/3BMN)(B-0.5SB)ceramics,we achieved a Wrec of 7.19 J cm^(−3) with an efficiency of 93.8%at 460 kV cm^(−1).Impressively,the B-0.5SB ceramics exhibit remarkable thermal stability between 30 and 140℃ under 365 kV cm^(−1),maintaining a Wrec exceeding 5 J cm^(−3).This study not only establishes the B-0.5SB ceramics as promising candidates for ES materials but also demonstrates the feasibility of optimizing ESP by modifying the dielectric constant under specific electric field conditions.Simultaneously,it provides valuable insights for the future design of ceramic capacitors with high ESP under constraints of limited electric field.

关键词： BNT Energy storage lead-free Relaxor ferroelectrics Capacitors

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lead-free hybrid two-dimensional double perovskite with switchable dielectric phase transition

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Chinese Chemical Letters 2024年第6期35卷 176-179页

作者： Tian Yang Yi Liu Lina Hua Yaoyao Chen Wuqian Guo Haojie Xu Xi Zeng Changhao Gao Wenjing Li Junhua Luo Zhihua Sun College of Chemistry Fuzhou UniversityFuzhou 350108China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Molecular dielectric switches constitute a type of intelligent materials that are highly coveted for their distinctive advantages of switchable dielectric responses,lightweight,and mechanical flexibility.Twodimensional(2D)hybrid perovskites have demonstrated excellent promise for assembling dielectric switches,in which the dynamic motions of organic moieties afford driving force to trigger switchable dielectric phase transition.Here,we successfully assembled a new lead-free hybrid double perovskite,(CHA)4Cu Bi Br8(1,CHA=cyclohexylammonium),adopting a typical 2D structural motif,which shows dielectric anisotropy and bistable behaviors during the reversible phase transition near T_(c)=378 K(the Curie temperature).That is,its dielectric constants could be switched and tuned between high-dielectric and low-dielectric states.Structure analyses reveal that the ordered-disordered transformation of the organic CHA+moiety and distortion of inorganic framework account for its phase transition.This result will stimulate further exploration of molecular dielectric switches in this 2D environmentally friendly family.

关键词： Dielectric switch lead-free Double perovskite Phase transition Symmetry breaking

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A novel lead-free relaxor with endotaxial nanostructures for capacitive energy storage

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SusMat 2024年第1期4卷 116-125页

作者： Xiaoyan Dong Tengfei Hu XiaojunWu Jie Yin Zhengqian Fu Jiagang Wu College of Materials Science and Engineering Sichuan UniversityChengduP.R.China Analysis and Testing Center for Inorganic Materials Shanghai Institute of CeramicsChinese Academy of SciencesShanghaiP.R.China

Dielectric capacitors with a fast charging/discharging rate,high power density,and long-term stability are essential components in modern electrical devices.However,miniaturizing and integrating capacitors face a persistent challenge in improving their energy density(W_(rec))to satisfy the specifications of advanced electronic systems and applications.In this work,leveraging phase-field simulations,we judiciously designed a novel lead-free relaxor ferroelectric material for enhanced energy storage performance,featuring flexible distributed weakly polar endotaxial nanostructures(ENs)embedded within a strongly polar fluctuation matrix.The matrix contributes to substantially enhanced polarization under an external electric field,and the randomly dispersed ENs effectively optimize breakdown phase proportion and provide a strong restoring force,which are advantageous in bolstering breakdown strength and minimizing hysteresis.Remarkably,this relaxor ferroelectric system incorporating ENs achieves an exceptionally high W_(rec)value of 10.3 J/cm^(3),accompanied by a large energy storage efficiency(η)of 85.4%.This work introduces a promising avenue for designing new relaxor materials capable of capacitive energy storage with exceptional performance characteristics.

关键词： endotaxial nanostructure energy storage lead-free relaxor ferroelectric

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Large Energy Capacitive High-Entropy lead-free Ferroelectrics

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Nano-Micro Letters 2023年第5期15卷 69-82页

作者： Liang Chen Huifen Yu Jie Wu Shiqing Deng Hui Liu Lifeng Zhu He Qi Jun Chen Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical ChemistryUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China School of Mathematics and Physics University of Science and Technology BeijingBeijing 100083People’s Republic of China School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China

Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market.Here,an ultrahigh energy storage density of~13.8 J cm^(-3)and a large efficiency of~82.4%are achieved in high-entropy lead-free relaxor ferroelectrics by increasing configuration entropy,named high-entropy strategy,realizing nearly ten times growth of energy storage density compared with low-entropy material.Evolution of energy storage performance and domain structure with increasing configuration entropy is systematically revealed for the first time.The achievement of excellent energy storage properties should be attributed to the enhanced random field,decreased nanodomain size,strong multiple local distortions,and improved breakdown field.Furthermore,the excellent frequency and fatigue stability as well as charge/discharge properties with superior thermal stability are also realized.The significantly enhanced comprehensive energy storage performance by increasing configuration entropy demonstrates that high entropy is an effective but convenient strategy to design new high-performance dielectrics,promoting the development of advanced capacitors.

关键词： High-entropy Energy storage lead-free Relaxor ferroelectrics Capacitors

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Metal–organic framework wafer enabled fast response radiation detection with ultra-low dark current

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Nano Research 2024年第4期17卷 2988-2993页

作者： Meng Xu Jianxi Liu Wei Wu Yang Chen Donghao Ma Sixin Chen Wanqi Jie Menghua Zhu Yadong Xu State Key Laboratory of Solidification Processing MIIT Key Laboratory of Radiation Detection Materials and Devices&School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

Semiconductive metal–organic frameworks(MOFs)have attracted great interest for the electronic applications.However,dark currents of present hybrid organic–inorganic materials are 1000–10,000 times higher than those of commercial inorganic detectors,leading to poor charge transportation.Here,we demonstrate a ZIF-8(Zn(mim)_(2),mim=2-methylimidazolate)wafer with ultra-low dark current of 1.27 pA·mm^(-2) under high electric fields of 322 V·mm^(-1).The isostatic pressing preparation process provides ZIF-8 wafers with good transmittance.Besides,the presence of redox-active metals and small spatial separation between components promotes the charge hopping.The ZIF-8-based semiconductor detector shows promising X-ray detection sensitivity of 70.82μC·Gy^(-1)·cm^(-2) with low doses exposures,contributing to superior X-ray imaging capability with a relatively high spatial resolution of 1.2 lp·mm^(-1).Simultaneously,good peak discrimination with the energy resolution of~43.78%is disclosed when the detector is illuminated by uncollimated 241Am@5.48 MeVα-particles.These results provide a broad prospect of MOFs for future radiation detection applications.

关键词： MOFs lead-free α-particles X-ray detection and imaging dark current fast response

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Sodium lithium niobate lead-free piezoceramics for high-power applications:Fundamental,progress,and perspective

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Journal of Advanced Ceramics 2023年第1期12卷 1-23页

作者： Chen-Bo-Wen LI Zhao LI Juan WANG Yi-Xuan LIU Jing-Tong LU Ze XU Pak-Sheng SOON Ke BI Chuan CHEN Ke WANG State Key Laboratory of Information Photonics and Optical Communications School of ScienceBeijing University of Posts and TelecommunicationsBeijing 100876China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Department of Stomatology Beijing Jishuitan HospitalBeijing 100035China Department of Electric Power Sensing Technology State Grid Smart Grid Research Institute Co.Ltd.Beijing 102211China

With the capability of interconversion between electrical and mechanical energy,piezoelectric materials have been revolutionized by the implementation of perovskite-piezoelectric-ceramic-based studies over 70 years.In particular,the market of piezoelectric ceramics has been dominated by lead zirconate titanate for decades.Nowadays,the research on piezoelectric ceramics is largely driven by cutting-edge technological demand as well as the consideration of a sustainable society.Hence,environmental-friendly lead-free piezoelectric materials have emerged to replace lead-based Pb(Zr,Ti)O_(3)(PZT)compositions.Owing to the inherent high mechanical quality factor(Q_(m))and low energy loss,(Li,Na)NbO_(3)(LNN)materials have recently drawn increasing attention and brought advantages to high-power piezoelectric applications.Although the crystallographic structures of LNN materials were intensively investigated for decades,the technical strategies for electrical performance are still limited.As a result,the property enhancement appears to have approached a plateau.This review traces the progress in the development of LNN materials,starting from the polymorphism in terms of the crystal structures,phase transitions,and local structural distortions.Then,the key milestone works on the functional tunability of LNN are reviewed with emphasis on involved engineering approaches.The exceptional performance at a large vibration velocity makes LNN ceramics promising for high-power applications,such as ultrasonic welding(UW)and ultrasonic osteotomes(UOs).The remaining challenges and some strategic insights for synergistically engineering the functional performance of LNN piezoceramics are also suggested.

关键词： sodium lithium niobate lead-free piezoelectric performance high-power applications

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(K,Na)NbO_(3)-based lead-free ceramics with enhanced temperature-stable piezoelectricity and efficient red luminescence

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Journal of Advanced Ceramics 2023年第2期12卷 373-385页

作者： Qing LIU Er PAN Fucai LIU Jing-Feng LI School of Optoelectronic Science and Engineering University of Electronic Science and Technology of ChinaChengdu 610054China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China

There has been a surge of research interest in the promising lead-free potassium-sodium niobate(KNN)-based ceramics,applications of which could be significantly promoted by improving thermal stability of piezoelectricity.Besides,endowing the KNN-based ceramics with photoluminescence property by rare-earth-ion doping can make them more completive lead-free counterparts in potential applications such as novel multifunctional sensing devices.Herein,a novel KNN-based ceramic material doped with Eu was elaborately designed to simultaneously obtain enhanced temperaturestable piezoelectricity and good luminescence property.By the introduction of diffused phase transition and the modulation of unit cell distortion,a large piezoelectric strain coefficient(d^(*)_(33))with a small variation(590±59 pm/V)over a wide temperature range(from room temperature to 110℃)was realized.The optimal composition also exhibited a considerable piezoelectric coefficient(d_(33))with small fluctuation(330±33 pC/N)from 20 to 80℃.In addition to the enhanced temperature-stable piezoelectricity,the luminescence of these ceramics was slightly enhanced with the elevation of BaZrO_(3)(BZ)doping contents,which could be attributed to the increased compositional disorder and the decreased unit cell distortion of the matrix material.Moreover,an optical characteristic was more prominent at ultra-low temperatures.This work unprecedentedly provides a novel paradigm for the design of multifunctional KNN-based ceramics with enhanced temperature-stable piezoelectricity and good luminescence property,revealing the great potential of the rare-earth-element-doped KNN material for future applications in the novel multifunctional devices.

关键词： piezoelectric thermal stability rare-earth lead-free potassium-sodium niobate(KNN)

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Ultrahigh strain in textured BCZT-based lead-free ceramics with CuO sintering agent

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Journal of Materials Science & Technology 2022年第22期117卷 207-214页

作者： Yingchun Liu Hongjun Zhang Wenming Shi Qian Wang Guicheng jiang Bin Yang Wenwu Cao Jiubin Tan Functional Materials and Acoustooptic Instruments Institute School of Instrumentation Science and EngineeringHarbin Institute of TechnologyHarbin 150080China Department of Mathematics and Materials Research Institute The Pennsylvania State Ultra-precision Optical&Electronic Instrument Engineering Center Harbin Institute of TechnologyHarbin 150001China

Textured BaTiO_(3)(BT)-based lead-free ceramics have gained significant attention due to their high piezoelectric coefficient(d)and very large field induced strain(S).However,costly nano-size raw materials,excessively high sintering temperature and low Curie temperature(T_(c))hinder their device applications.In this work,highly[001]_(c)-oriented(Ba_(0.95)Ca_(0.05))(Zr_(0.04)Ti_(0.96))O_(3) ceramics with x mol%CuO(x=0.25,0.5,1.0,2.5)denoted as BCZT-x were synthesized by templated grain growth using micro-sized raw powders.The introduction of CuO sintering agent lowered the sintering temperature by 125℃ to 1450℃,and the BCZT-1.0 achieved a high texture degree of∼99%.In addition,the CuO-based liquid phases eliminated boundaries between BT templates and BCZT matrix powders.Such liquid-phase sintering reduced sintering stresses,decreased the average grain size of BCZT-1.0 from 16μm down to 13μm,and increased the dielectric dispersion coefficientγto 1.63.The almost smoothed out T_(O-T) anomaly in the temperature dependence of dielectric permittivity and comparably high T_(c)(>102℃)lead to better temperature stability.The narrower grain orientation distribution with full width at half maximum(FWHM)of∼5.9°and smaller domains with the size of 0.1–0.5μm in width and 3–8μm in length were obtained,a high field induced maximum strain S_(max) of 0.38%and low H_(s) of 5.2%have been achieved in BCZT-1.0 textured ceramics together with a high and homogeneous piezoelectric stress coefficient d_(33)∼780 pC/N and very large d_(33)∗∼2950 pm/V.

关键词： lead-free BCZT Textured ceramics Piezoelectric Strain hysteresis

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Defects and doping engineering towards high performance lead-free or lead-less perovskite solar cells

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Journal of Energy Chemistry 2022年第5期31卷 420-438页

作者： Wenying Cao Zhaosheng Hu Zhenhua Lin Xing Guo Jie Su Jingjing Chang Yue Hao State Key Discipline Laboratory of Wide Band Gap Semiconductor Technology School of MicroelectronicsXidian UniversityXi’an 710071ShaanxiChina Advanced Interdisciplinary Research Center for Flexible Electronics Xidian UniversityXi’an 710071ShaanxiChina

Up to now, perovskite solar cells(PSCs) have reached a certified 25.5% efficiency. As a promising photo-electric material, the metal halide perovskite possesses many outstanding properties such as tunable bandgap, long diffusion length, high absorption coefficient and carrier mobility. In spite of these remarkable properties, defects are inevitable during the solution processing. Therefore, many efforts have been made to reduce defects in perovskite films and thus improve the performance of devices. Among them,substitution or doping engineering is one of the most studied methods. Meanwhile, due to the poor stability of the organic-inorganic hybrid perovskite and the toxicity of Pb-based perovskite materials, all inorganic perovskite and lead-less or lead-free perovskite have emerged as promising materials. Here,we focus on the defect engineering especially substitutions on different sites in an ABX_(3) structure. The particular attention is devoted towards lead-less or lead-free perovskites, and we discuss several common elements or groups used to partially replace Pb^(2+). It is noted that proper elemental doping at different sites is an important guarantee for obtaining high-performance lead-less or lead-free PSCs.

关键词： Perovskite Defects Doping engineering lead-free lead-less Solar cells

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Exploring centimeter-sized crystals of bismuth-iodide perovskite toward highly sensitive X-ray detection

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Chinese Chemical Letters 2024年第6期35卷 185-188页

作者： Xin Dong Jing Liang Zhijin Xu Huajie Wu Lei Wang Shihai You Junhua Luo Lina Li College of Chemistry Fuzhou UniversityFuzhou 350116China State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China

lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility,large atomic number,and long carrier lifetime,but the toxicity of lead is regarded as the major factor hindering their development.Here,we introduce organic molecule(R)-(-)-2-methylpiperazine(R-MPz)into the bismuth-based structure to synthesize lead-free(R)-(H_(2)MPz)BiI_(5)(R-MBI).The high-quality centimeter-sized single crystals have been obtained,which show a low dark current and superior environmental stability.Particularly,the single-crystal device of R-MBI exhibits a highμτproduct up to 1.88×10^(-4)cm^(2)/V and a low trap density of 1.21×10^(10)cm^(-3).Further,the detector displays excellent detection sensitivity of 263.58μC Gy_(air)^(-1)cm^(-2)and a favorable low detection limit of 4.35μGyair/s,both of which meet the requirement for medical diagnostics.These findings shed light on the exploration of innovative bismuth-based hybrid perovskites for high-performance X-ray detection.

关键词： Perovskite lead-free Bismuth-based X-ray detection Sensitivity

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