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Ultrahigh zT from strong electron-phonon interactions and a low-dimensional Fermi surface

Energy and Environmental science 2024年第5期17卷 1904-1915页

作者： Ranganayakulu, V.K. Wang, Te-Hsien Chen, Cheng-Lung Huang, Angus Ma, Ma-Hsuan Wu, Chun-Min Tsai, Wei-Han Hung, Tsu-Lien Ou, Min-Nan Jeng, Horng-Tay Lee, Chih-Hao Chen, Kuei-Hsien Li, Wen-Hsien Brod, Madison K. Snyder, G. Jeffrey Chen, Yang-Yuan Institute of Physics Academia Sinica Taipei11529 Taiwan Department of Engineering and System Science National Tsing Hua University Hsinchu30013 Taiwan Taiwan International Graduate Program Taipei11529 Taiwan Department of Physics National Chung Hsing University Taichung City40227 Taiwan Graduate School of Materials Science National Yunlin University of Science and Technology Yunlin64002 Taiwan Bachelor Program in Semiconductor Materials and Fabrication Ming Chi University of Technology New Taipei City243303 Taiwan Department of Physics National Tsing Hua University Hsinchu30013 Taiwan Center for Theory and Computation National Tsing Hua University Hsinchu30013 Taiwan Physics Division National Center for Theoretical Sciences Taipei10617 Taiwan Department of Physics National Central University Jhongli32001 Taiwan National Synchrotron Radiation Research Center Hsinchu Science Park Hsinchu30076 Taiwan Institute of Atomic and Molecular Sciences Academia Sinica Taipei10617 Taiwan Department of Materials Science and Engineering Northwestern University EvanstonIL60208 United States Graduate Institute of Applied Physics National Chengchi University Taipei11605 Taiwan

The outstanding thermoelectric performance of GeTe has attracted significant attention in the research community in recent years. However, many of the underlying physical mechanisms that contribute to GeTe's exceptionally high figure of merit (zT) remain not fully understood. In this study, an Sb-Bi codoped GeTe single crystal (Ge0.86Sb0.08Bi0.06)Te with an ultrahigh zT of 2.7 at 700 K and a record high device zT of 1.41 in the temperature range of 300-773 K was synthesized and investigated. The ultrahigh zT is attributed to the extremely low lattice thermal conductivity induced by strong electron-phonon (EP) interactions as revealed by the experimentally observed Kohn anomaly, through inelastic neutron scattering (INS) measurements. First-principles calculations further demonstrate that the remarkable EP interaction arises from the Fermi surface nesting featured in a one-dimensional (double-walled) topology. Our finding unravels the ultrahigh-zT mechanism in GeTe-based materials, serving as an inspiring guide toward high thermoelectric performance. © 2024 The Royal Society of Chemistry.

关键词： Neutron scattering

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揭示氧化铜在电催化生物质转化中存在的电势依赖的结构演变规律

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science Bulletin 2023年第23期68卷 2982-2992,M0005页

作者：王烨徐明王茜葛瑞翔朱玉荃李岸臻周华陈凤恩郑黎荣段昊泓 Department of Chemistry Tsinghua UniversityBeijing 100084China State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Department of Chemical Engineering Tsinghua UniversityBeijing 100084China Center of Basic Molecular Science(CBMS) Department of ChemistryTsinghua UniversityBeijing 100084China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Engineering Research Center of Advanced Rare Earth Materials(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China

通过电催化氧化葡萄糖等可再生生物质生产高附加值化学品为实现碳中和目标提供了一条有效途径.目前用于电催化生物质氧化反应的电催化剂主要分为贵金属基催化剂和非贵金属基催化剂.对于贵金属基电催化剂,文献报道了铂基催化剂的氧化态... 详细信息

通过电催化氧化葡萄糖等可再生生物质生产高附加值化学品为实现碳中和目标提供了一条有效途径.目前用于电催化生物质氧化反应的电催化剂主要分为贵金属基催化剂和非贵金属基催化剂.对于贵金属基电催化剂,文献报道了铂基催化剂的氧化态随电势变化,进而调控电催化葡萄糖氧化的活性和选择性.对于非贵金属基催化剂,钴基和镍基氧化物和氢氧化物被广泛应用于电催化生物质氧化反应,但铜基催化剂直到最近才引起关注.最近,金属铜、氧化亚铜和氢氧化铜在内的铜基材料被证实是一类有应用前景的电催化生物质氧化催化剂,但在电化学条件下的真实活性位结构仍难以鉴定.本文针对电催化葡萄糖等生物质平台分子的氧化反应,证明了氧化铜的催化活性相随电压升高从氢氧化铜演变为羟基氧化铜,阐明了结构和反应活性及选择性的构效关系,该工作加深了对铜基催化剂活性位动态重构的理解,有助于电催化生物质转化的催化剂理性设计,促进可再生资源利用和碳中和目标的实现.

关键词： Biomass upcycling Copper oxide Electrocatalysis Glucose electrooxidation Potential dependency

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An angle-insensitive electromagnetic absorber enabling a wideband absorption

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Journal of materials science & Technology 2022年第18期113卷 33-39页

作者： Zhichao Lou Qiuyi Wang Xiaodi Zhou Ufuoma I.Kara Rajdeep S.Mamtani Hualiang Lv Meng Zhang Zhihong Yang Yanjun Li Chenxuan Wang Solomon Adera Xiaoguang Wang Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources Nanjing Forestry UniversityNanjing 210037China Willian G.Lowrie Department of Chemical and Biomolecular Engineering The Ohio State UniversityColumbusOH43210United States of America Institute of Materials Research and Engineering Agency for SciencesTechnology and ResearchSingapore State Key Laboratory of Medical Molecular Biology Institute of Basic Medical Sciences Chinese Academy of Medical SciencesSchool of Basic Medicine Peking Union Medical CollegeBeijing 100005China Department of Mechanical Engineering University of MichiganAnn ArborMI48109United States of America Sustainability Institute The Ohio State UniversityColumbusOH43210United States of America School of Materials Science and Engineering Henan University of Science and TechnologyLuoyang 471023China

Electromagnetic(EM)wave absorbers with wideband absorption capability are proposed as a strategy to mitigate environmental pollution by EM ***,designing an EM absorber with its performance capacity independent of the EM wave incident angle remains elusive to *** this challenge requires development of EM absorbers whose EM absorption performance is insensitive to the EM wave incident ***,we synthesized EM absorbers with a variety of structures with different symme-tries(including micro-/nanospheres,nanoflakes and nanotubes)to study the effect of the EM absorbers’structure and the EM wave incident angle on the EM absorption *** analysis reveals that non-magnetic EM absorbers with spatially symmetric nanostructures exhibit excellent EM wave incident ***,we demonstrate that a class of non-magnetic EM absorbers made from bam-boo derived-carbon nanospheres exhibit EM incident angle-insensitivity and wideband EM absorption performance with an effective absorption band up to 3.5 GHz when the thickness is 1.4 mm,a signif-icant improvement from prior studies which used thicknesses as high as 3-4 mm for comparable EM absorption performance.

关键词： Nanostructure Angle-insensitive EM absorption Biomass derived carbon Wideband

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Study on the Flow, Foaming Characteristics and Structural Strength of Polypropylene Structural Foam Injection Molding by Innovative Nitrogen and Molten Plastic Mixing Mechanism

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Polymers 2023年第9期15卷 2116-2116页

作者： Huang, Po-Wei Peng, Hsin-Shu Hwang, Sheng-Jye Huang, Chao-Tsai Program of Mechanical and Aeronautical Engineering Feng Chia University of Engineering and Science Taichung407102 Taiwan Department of Mechanical and Computer Aided Engineering Feng Chia University of Engineering and Science Taichung407102 Taiwan Department of Mechanical Engineering National Cheng Kung University of Engineering Tainan70101 Taiwan Department of Chemical and Materials Engineering Tamkang University of Engineering New Taipei City251301 Taiwan

Plastic foam molding methods include thermoforming, extrusion and injection molding. Injection foam molding is a one-time molding method with high production efficiency and good product quality. It is suitable for foamed plastic products with complex shapes and strict size requirements. It is also the main method for producing structural bubbles. In this investigation, we developed a structural foam injection molding technology using the gas supply equipment connected to the unique plasticizing mechanism of the injection machine and studied its influence on the specimens’ melt rheology quality and foam structures. In the experiment, the forming material was polypropylene (PP), and the gas for mixing/forming foaming characteristics was nitrogen (N2). Additionally, in order to observe the rheological properties of N2/melt mixing, a melt flow specimen mold cavity was designed and the change in the melt viscosity index was observed using a melt pressure sensing element installed at the nozzle position. With the nitrogen supply equipment connected to a unique plasticizing mechanism, the mixing of gas and molten plastic can be achieved at the screw plasticizing stage, where the foaming effect is realized during the melt-filling process due to the thermodynamic instability of the gas. It was also found that an increase in N2 fill content increased melt fluidity, and the trend of melt pressure and melt viscosity index showed that the higher the gas content, the lower the trend. The foaming characteristic depends on the gas thermodynamic instability and the pressure release, so it can be seen from the melt fill path that, the greater the pressure near the gate, the lower the foaming amount and the internal structure (SEM) after molding;the farther from the gate, the greater the relative increase in the foaming growth/amount. This phenomenon will be more obvious when the N2 fill content is increased. © 2023 by the authors.

关键词： Gases

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Deep Ultraviolet Phototransistor Based on Thiophene-Fluorobenzene Oligomer with High Mobility and Performance

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Chinese Journal of Chemistry 2023年第13期41卷 1539-1544页

作者： Yongxu Hu Zhongwu Wang Yinan Huang Rui Shi Shuguang Wang Xiaosong Chen Jinshun Bi Yundong Xuan Yong Lei Liqiang Li Chuluo Yang Wenping Hu Shenzhen Key Laboratory of New Information Display and Storage Materials College of Materials Science and EngineeringShenzhen UniversityShenzhenGuangdong518060 China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhenGuangdong518060 China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistryInstitute of Molecular Aggregation ScienceTianjin UniversityTianjin300072 China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhouFujian350207 China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192 China Institute of Microelectronics Chinese Academy of SciencesBeijing100029 China University of Chinese Academy of Sciences Beijing101408 China Fachgebiet Angewandte Nanophysik Institut für Physik&IMN MacroNanoTechnische Universität Ilmenau98693 IlmenauGermany

Deep ultraviolet(UV)photodetectors have important applications in the industrial and military ***,little research has been reported on organic phototransistors(OPTs)in the deep ultraviolet ***,a novel organic semiconductor containing a small torsion angle and lowπ-conjugation 2,2':5',2"-terthiophene groups,oF-PTTTP,is designed and synthesized,which exhibits high carrier mobility and unique deep ultraviolet ***,an OPT based on oF-PTTTP single crystal shows high responsivity to deep-UV *** photodetectors achieve high photoresponsivity(R)of 857 A/W and detectivity(D*)of 3.2×10^(15)Jones under 280 nm light illumination(only 95 nW·cm^(–2)).To the best of our knowledge,280 nm is the deepest detection wavelength reported for organic phototransistors and this work presents a new molecule design concept for organic phototransistors with deep-UV detection.

关键词： Deep-UV phototransistors Organic semiconductors molecular devices Single crystals OFETs

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Asymmetric Hydrogenation of Tetrasubstituted α,β-Unsaturated Ketones:Access to Chiral 2-Substituted Cyclopentyl Aryl Ketones

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Precision Chemistry 2023年第3期1卷 146-152页

作者： Zhengdong Ding Feng Gao Yining Lu Qianjia Yuan Wei-Ping Deng Wanbin Zhang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Shanghai Key Laboratory of New Drug Design School of PharmacyEast China University of Science and TechnologyShanghai 200237China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Department of ChemistryZhejiang Normal UniversityJinhua 321004China

Asymmetric hydrogenation of tetrasubstituted alkenes is an important but challenging research ***,we report an efficient iridium-catalyzed asymmetric hydrogenation of tetrasubstituted α,β-unsaturated ketones for the synthesis of chiral 2-substituted cyclopentyl aryl ketones,an important chiral structural motif for the preparation of chiral pharmaceuticals and bioactive *** reaction proceeded very well with good functional group compatibility and delivered the hydrogenated products in high yields and stereoselectivities(up to 99% yield,>20:1 dr and 99%ee).In addition,the reaction could be carried out on a gram-scale,and all four stereoisomers of the hydrogenated products bearing two contiguous stereocenters were ***,the hydrogenated product can be transformed into the ERβ agonist Erteberel,and the reaction pathway was also studied via deuterium-labelling experiments.

关键词： asymmetric hydrogenation tetrasubstituted alkenes iridium chiral cyclopentane 2-substituted cyclopentyl aryl ketones

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Supramolecular systems for bioapplications:recent research progress in China

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science China Chemistry 2024年第5期67卷 1397-1441页

作者： Yue-Yang Liu Xiao-Yong Yu Yu-Chen Pan Hang Yin Shuang Chao Yujie Li He Ma Minzan Zuo Kun-Xu Teng Jun-Li Hou Yong Chen Dong-Sheng Guo Ruibing Wang Yuxin Pei Zhichao Pei Jiang-Fei Xu Xiao-Yu Hu Chunju Li Qing-Zheng Yang Leyong Wang Yu Liu Zhan-Ting Li State Key Laboratory of Organometallic Chemistry Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional MoleculesShanghai Institute of Organic ChemistryChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai 200032China Department of Chemistry Fudan UniversityShanghai 200438China College of Chemistry State Key Laboratory of Elemento-Organic ChemistryCollaborative Innovation Center of Chemical Science and EngineeringNankai UniversityTianjin 300071China State Key Laboratory of Quality Research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao 999078China College of Chemistry&Pharmacy Northwest A&F UniversityYangling 712100China Key Lab of Organic Optoelectronics&Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China College of Materials Science and Technology Nanjing University of Aeronautics and AstronauticsNanjing 211106China Key Laboratory of Radiopharmaceuticals Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China State Key Laboratory of Analytical Chemistry for Life Science Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Supramolecular systems feature dynamic,reversible and stimuli-responsive characteristics,which are not easily achieved by molecular *** last decade has witnessed tremendous advances in the investigations of supramolecular systems for various bioapplications,which include drug delivery,anticancer therapy,antibacterial therapy,photodynamic therapy,photothermal therapy,combination therapy,antidotes for residual drugs or toxins,and bioimaging and ***-guest chemistry has played a key role in the development of such bioactive supramolecular systems,and natural macrocycles(such as cyclodextrins),synthetic macrocycles(such as calixarenes,cucurbit[n]urils,and pillararenes),and porous framework polymers(such as supramolecular organic frameworks and flexible organic frameworks)have been most successfully used as hosts to build different kinds of host-guest systems for attaining designed *** self-assembly of rationally designed amphiphilic molecules,macromolecules and polymers represent another important approach for the construction of supramolecular architectures with advanced *** this review,we summarize the important contributions made by Chinese researchers in this field,with emphasis on those reported in the past five years.

关键词： host-guest chemistry drug delivery anticancer and antibacterial photodynamic therapy photothermal therapy antidote transmembrane channel bioimaging and biosensing

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pH/GSH dual responsive nanosystem for nitric oxide generation enhanced type I photodynamic therapy

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Bioactive materials 2024年第4期34卷 414-421页

作者： Jianhua Zou Zheng Li Yang Zhu Yucen Tao Qing You Fangfang Cao Qinghe Wu Min Wu Junjie Cheng Jianwei Zhu Xiaoyuan Chen Departments of Diagnostic Radiology SurgeryChemical and Biomolecular Engineeringand Biomedical EngineeringYong Loo Lin School of Medicine and College of Design and EngineeringNational University of SingaporeSingapore119074Singapore Nanomedicine Translational Research Program NUS Center for NanomedicineYong Loo Lin School of MedicineNational University of SingaporeSingapore117597Singapore Clinical Imaging Research Centre Centre for Translational MedicineYong Loo Lin School of MedicineNational University of SingaporeSingapore117599Singapore Institute of Molecular and Cell Biology Agency for ScienceTechnologyand Research(A*STAR)61 Biopolis DriveProteosSingapore138673Singapore Department of Plastic and Reconstructive Surgery Shanghai Ninth People’s HospitalShanghai Jiaotong UniversityShanghai200011PR China Department of Chemistry Center for Bioanalytical Chemistry University of Science and Technology of ChinaHefei230026PR China College of Life Science Nanjing Normal University1 Wenyuan RoadNanjing210023PR China

Tumor hypoxia diminishes the effectiveness of traditional type II photodynamic therapy(PDT)due to oxygen *** I PDT,which can operate independently of oxygen,is a viable option for treating hypoxic *** this study,we have designed and synthesized JSK@PEG-IR820 NPs that are responsive to the tumor microenvironment(TME)to enhance type I PDT through glutathione(GSH)*** approach aims to expand the sources of therapeutic benefits by promoting the generation of superoxide radicals(O_(2)^(-).)while minimizing their *** diisopropyl group within PEG-IR820 serves a dual purpose:it functions as a pH sensor for the disassembly of the NPs to release JSK and enhances intermolecular electron transfer to IR820,facilitating efficient O_(2)^(-).***,the release of JSK leads to GSH depletion,resulting in the generation of nitric oxide(NO).This,in turn,contributes to the formation of highly cytotoxic peroxynitrite(ONOO^(-).),thereby enhancing the therapeutic efficacy of these ***-II fluorescence imaging guided therapy has achieved successful tumor eradication with the assistance of laser therapy.

关键词： TME responsive NO gas therapy NIR-II imaging Type I PDT

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Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

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CCS Chemistry 2023年第4期5卷 851-864页

作者： Gaofeng Chen Olga A.Syzgantseva Maria A.Syzgantseva Shuliang Yang Guihua Yan Li Peng Changyan Cao Wenxing Chen Zhiwei Wang Fengjuan Qin Tingzhou Lei Xianhai Zeng Lu Lin Weiguo Song Buxing Han College of Energy Xiamen UniversityXiamen 361102 Department of Chemistry Lomonosov Moscow State UniversityMoscow 119991 Fujian Engineering and Research Center of Clean and High-Valued Technologies for Biomass Xiamen Key Laboratory of Clean and High-Valued Utilization for BiomassXiamen 361102 College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005 Beijing National Laboratory for Molecular Science CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081 School of Environmental Engineering Henan University of TechnologyZhengzhou 450001 Institute of Urban and Rural Mining Changzhou UniversityChangzhou 213164

Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil ***,it is still challenging to construct high-performance HAS catalysts with satisfying selectivity,space–time yield(STY),and ***,we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix(Co/Cu–N–C).The Co/Cu–N–C is efficient for HAS and is among the best catalysts *** a COconversion of 81.7%,C2+OHselectivity could reach 58.5%with an outstanding C2+OH STY of 851.8 mg/g·*** found that the N4–Co1 and Cu1–N4 showed an excellent synergistic *** adsorption of CO occurred on the Co site,and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form ***,the Cu sites stabilized a CHOCu species to interact with CHxCo,facilitating a barrier-free formation of C2 species,which is responsible for the high selectivity of higher alcohols.

关键词： dual atomic catalyst synergistic effect heterogeneous catalysis carbonmaterial higher alcohol synthesis

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Metallophilicity-Induced Clusterization:Single-Component White-Light Clusteroluminescence with Stimulus Response

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CCS Chemistry 2022年第8期4卷 2570-2580页

作者： Xueqian Zhao Parvej Alam Jianyu Zhang Shiyun Lin Qian Peng Jun Zhang Guodong Liang Sijie Chen Jing Zhang Herman HYSung Jacky WYLam Ian DWilliams Xinggui Gu Zheng Zhao Ben Zhong Tang Department of Chemistry and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077 MOE Key Laboratory of Organic OptoElectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084 CAS Key Laboratory of Organic Solids Institute of ChemistryBeijing National Laboratory for Molecular SciencesChinese Academy of SciencesBeijing 100190 School of Materials and Chemical Engineering Anhui Jianzhu UniversityHefei 230601 PCFM and GDHPPC Labs School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275 Ming Wai Lau Centre for Reparative Medicine Karolinska InstitutetHong Kong 999077 Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and EngineeringState Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029 Shenzhen Institute of Molecular Aggregate Science and Engineering School of Science and EngineeringThe Chinese University of Hong KongShenzhenGuangdong 518172 Center for Aggregation-Induced Emission SCUT-HKUST Joint Research InstituteState Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhou 510640 AIE Institute Guangzhou Development DistrictHuangpuGuangzhou 510530

materials showing metallophilic interactions continue to attract considerable theoretical and experimental attention largely because of their unusual and unanticipated photophysical behavior as well as their unique stimuli-responsive behavior in an aggregate or solid *** interactions are mostly found between metals with either identical(d^(10)–d^(10))or different(s^(2)–d^(8),d^(8)–d^(10))*** various metallophilic interactions,aurophilic interactions(Au⋯Au)are well-known and widely *** this study,a new phosphorescent gold(I)complex,[(CF_(3)Ph)_(3)PAuC≡CPh](TPPGPA)was reported.

关键词： single-component white-light emission gold(I)complex aurophilic interactions stimuli-responsive materials metallophilicity-induced clusterization

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