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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University state key laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

High-speed flexible near-infrared organic photodiode for optical communication

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National Science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin Chen Ruiman Han Hao Qin Zhaoyang Yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng Chen The Centre of Nanoscale Science and Technology and key laboratory of Functional Polymer materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University state key laboratory of Elemento-Organic chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

Near-infrared non-fused electron acceptors for efficient organic photovoltaics

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Chinese Chemical Letters 2024年第4期35卷 436-441页

作者： Wenxiang Ma Xinyu He Tianyi Chen De-Li Ma Hongzheng Chen Chang-Zhi Li state key laboratory of silicon and Advanced Semiconductor materials Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of organic photovoltaics(OPVs). Herein, two near-infrared non-fused ring acceptors(NIR NFRAs), PTBFTT-F and PTBFTT-Cl have been developed with A-π_A-π_D-D-π_D-π_A-A non-fused structures. It is revealed that the introduction of electron deficient π-bridge(π_A) and multiple intramolecular noncovalent interactions effectively retained the structural planarity and intramolecular charge transfer of NFRAs, extending strong NIR photon absorption up to 950 nm. Further, the chlorinated acceptor, with the enlarged π-surface compared to the fluorinated counterpart, promoted not only molecular stacking in solid, but also the desirable photochemical stability in ambient, which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs. Overall, this work provides valuable insights into the design of NIR organic semiconductors.

关键词： Organic photovoltaic Near-infrared Non-fused electron acceptor Noncovalent interaction Stability

Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National Science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing key Lab of Microstructure and Property of Advanced materials College of Materials Science &Engineering Beijing University of Technology department of materials Science and Engineering City University of Hong Kong key laboratory of Partial Acceleration Physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences department of materials Science &Engineering Southern University of Science and Technology department of Physics City University of Hong Kong state key laboratory of silicon materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

Electrolyte Design for Low‑Temperature Li‑Metal Batteries:Challenges and Prospects

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Nano-Micro Letters 2024年第2期16卷 365-382页

作者： Siyu Sun Kehan Wang Zhanglian Hong Mingjia Zhi Kai Zhang Jijian Xu department of chemistry City University of Hong KongHong Kong 999077People’s Republic of China state key laboratory of silicon materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China state key laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Haihe Laboratory of Sustainable Chemical TransformationsCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)College of ChemistryNankai UniversityTianjin 300071People’s Republic of China department of Chemical and Biomolecular Engineering University of Maryland College ParkCollege ParkMD 20742USA

Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases.Herein,this review critically outlines electrolytes’limiting factors,including reduced ionic conductivity,large de-solvation energy,sluggish charge transfer,and slow Li-ion transportation across the electrolyte/electrode interphases,which affect the low-temperature performance of Li-metal batteries.Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding.Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared.Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature Li-metal batteries.

关键词： Solid electrolyte interphase Li metal Low temperature Electrolyte design Batteries

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

Recent advances in the synthesis and application of N-heterocyclic carbene-based molecular cages

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Science China chemistry 2024年第5期67卷 1510-1523页

作者： Qiongjie Chai Lixin Duan Yanzhe Ma Tianheng Hou Tao Tu Shanghai key laboratory of Molecular Catalysis and Innovative materials Department of ChemistryFudan UniversityShanghai 200438China state key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

N-Heterocyclic carbene(NHC)-based cages have emerged as a prominent and dynamic research area within the research field of chemistry. Leveraging the distinctive electronic and steric properties of NHC ligands, the design, synthesis, and application of these corresponding cages have garnered substantial scholarly interest. In recent years, we have witnessed the successful fabrication of diverse NHC-based cages through a range of synthetic methodologies, which hold significant potential for applications in molecular recognition and catalysis. In this review, we delve into the foundational synthetic strategies that underlie the creation of NHC-based cages, employing approaches encompassing metal–NHC chelation, coordination assembly,and covalent bonding. Additionally, we compile the diverse applications of these cages within catalytic processes and molecular recognition. Lastly, we shed light on the current limitations of synthesis and outline future trends in the development of NHCbased cages.

关键词： N-heterocyclic carbene molecular cages supramolecular chemistry synthetic strategies applications

Efficient and bright broadband electroluminescence based on environmentfriendly metal halide nanoclusters

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Light(Science & Applications) 2024年第4期13卷 727-737页

作者： Dingshuo Zhang Meiyi Zhu Yifan He Qingli Cao Yun Gao Hongjin Li Guochao Lu Qiaopeng Cui Yongmiao Shen Haiping He Xingliang Dai Zhizhen Ye School of materials Science and Engineering State Key Laboratory of Silicon and Advanced Semiconductor MaterialsZhejiang University310027 HangzhouChina. Wenzhou key laboratory of Novel Optoelectronic and Nano materials and Engineering Research Centre of Zhejiang Province Institute of WenzhouZhejiang University325006 WenzhouChina. Wenzhou XINXINTAIJING Tech.Co.Ltd. 325006 WenzhouChina. department of chemistry Zhejiang Sci-Tech University310018 HangzhouChina

Broadband electroluminescence based on environment-friendly emitters is promising for healthy lighting yet remains an unprecedented challenge to progress.The copper halide-based emitters are competitive candidates for broadband emission,but their high-performance electroluminescence shows inadequate broad emission bandwidth of less than 90 nm.Here,we demonstrate efficient ultra-broadband electroluminescence from a copper halide(CuI)nanocluster single emitter prepared by a one-step solution synthesis-deposition process,through dedicated design of ligands and subtle selection of solvents.The CuI nanocluster exhibits high rigidity in the excitation state as well as dual-emissive modes of phosphorescence and temperature-activated delayed fluorescence,enabling the uniform cluster-composed film to show excellent stability and high photoluminescent efficiency.In consequence,ultra-broadband light-emitting diodes(LEDs)present nearly identical performance in an inert or air atmosphere without encapsulation and outstanding high-temperature operation performance,reaching an emission full width at half maximum(FWHM)of~120 nm,a peak external quantum efficiency of 13%,a record maximum luminance of~50,000 cd m^(−2),and an operating half-lifetime of 137 h at 100 cd m^(−2).The results highlight the potential of copper halide nanoclusters for next-generation healthy lighting.

关键词： halide cluster rigidity

A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su key laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China state key laboratory of Supramolecular Structure and materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction ratio.Here we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton conduction.Remarkably,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting materials.This result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

A novel Tb^(3+) and Eu^(3+) co-doped dual-emitting phosphate K_(3)SrBi(P_(2)O_(7))_(2) phosphor for application in FIR thermometers

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Journal of Rare Earths 2024年第3期42卷 455-463,I0001页

作者： Baochen Wang Shifeng Sun Zeqi Li Zongwang Li Weiwei Lin Chao Zeng Yan-gai Liu Ruiyu Mi School of Chemical and Environmental Engineering Anhui Polytechnic UniversityWuhu241000China state-Province Joint Engineering laboratory of Zeolite Membrane materials Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationInstitute of Advanced MaterialsCollege of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China Beijing key laboratory of materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing100083China

Rare earth co-doped phosphor for fluorescence intensity ratio(FIR) thermometer has gained increasing attention in recent years. Herein, the novel Tb^(3+)and Eu^(3+)co-doped K_(3)SrBi(P_(2)O_(7))_(2)(KSBP) phosphate phosphors were reported. The crystal structure of the title phosphor was determined using Rietveld refinement and proved to have a three-dimensional structure. The time-resolved spectroscopy reveals that there is almost no energy transfer between Tb^(3+)and Eu^(3+). More importantly, Tb^(3+)and Eu^(3+)emissions show different thermal quenching behaviors, which claims the potential of this material for application in optical thermometer. The FIR of the typical KSBP:0.02Tb^(3+),0.04Eu^(3+)sample demonstrates a polynomial relationship as a function of temperature and the absolute and relative sensitivity are0.025 K^(-1) and 0.59%/K, respectively. In general, our study reports a novel and potential KSBP:Tb^(3+),Eu^(3+)phosphate phosphor that is promising for use in high-sensitive FIR thermometers.

关键词： Phosphor Thermometer Fluorescence intensity ratio Thermal stability Rare earths