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Achieving highly efficient long-wavelength phosphorescence emission of large singlet-triplet energy gap materials by host-guest doping

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Science China Chemistry 2024年第6期67卷 1922-1928页

作者： Shasha Zhang Wei Yao Anqi Lv Kun Liu Yusheng Zhang Chifeng Zhou Huili Ma Huifang Shi Zhongfu An key laboratory of flexible electronics(KLOFE)&Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing211816China

High-efficiency long-wavelength phosphorescence emissions of large singlet-triplet energy gap(ΔE_(ST))materials are essential for applications in biology and display.However,few long-wavelength phosphorescence emissions of largeΔE_(ST)materials have been reported due to the weak spin-orbit coupling(SOC)and strong non-radiative transitions.Herein,we develop a strategy to achieve highly efficient long-wavelength room temperature phosphorescence(RTP)emission of largeΔE_(ST)materials,which display bright red RTP emission with above 400μs lifetime and 6.5%phosphorescent quantum efficiency.Our experiments and theoretical calculations reveal that the fishbone-like packing and the zig-zag interactions provide favorable conditions for suppressing the non-radiative transitions of triplet state excitons,and heavy atoms effectively promote the intersystem crossing(ISC)process for highly efficient long-wavelength phosphorescence emission.The universality of the method for highly efficient long-wavelength RTP emission of largeΔE_(ST)materials was further investigated in various guests.Moreover,these materials with largeΔE_(ST)manifest the advantages of large color contrast on the display and utilization potentiality in information encryption.This strategy paves the way for the high contrast display and development of information encryption with RTP emission.

关键词： room temperature phosphorescence singlet-triplet energy gap host-guest doping heavy atom effect red phosphorescence

Incorporating metal nanoparticles in porous materials via selective heating effect using microwave

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Nano Research 2024年第4期17卷 3175-3179页

作者： Yingyu Zhou Jiacheng Liu Fuyuan Sun Junchen Ouyang Ruifa Su Fanchen Meng Yongqi Luo Cheng Xu Weina Zhang Suoying Zhang Fengwei Huo key laboratory of flexible electronics(KLOFE)&Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816China

Metal nanoparticle@porous material composites have attracted increasing attention due to their excellent synergistic catalytic performance.However,it is a challenge to introduce metal nanoparticles into cavities of porous materials without agglomeration on the exterior.Despite the progress achieved,a universal approach that can integrate different kinds of metal nanoparticles and porous materials is still highly desirable.Here we report a facile and general approach to fabricating metal nanoparticle@porous materials by microwave-triggered selective heating.The microwave can pass through the non-polar solvent and act on the polar solvent in the porous materials,causing the polar solvent to be heated,vaporized,and away from the pores of porous materials.The local void produced by the escape of polar solvent facilitates non-polar solvent containing metallic precursor to be dragged into the narrow pores,followed by further reduction,resulting in the complete encapsulation of nanoparticles.A series of metal nanoparticles@porous materials,ranging from metal-organic frameworks(MOFs)to zeolites,are successfully prepared by this method and show excellent size selectivity in catalytic reactions.

关键词： porous material nanoparticle encapsulation microwave synthesis selective heating effect selective catalysis

Tailored multifunctional hydrazine derivatives for efficient printable hole-conductive-free mesoscopic perovskite solar cells via enhancing defect passivation

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Journal of Energy Chemistry 2024年第8期95卷 357-363页

作者： Minghao Xia Ziwei Zheng Yanjie Cheng Chaoyang Wang Zhaozhen Cui Guodong Zhang Jinwei Gonga Anyi Mei Hongwei Han Michael Gr?tzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for Optoelectronics Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and Technology key laboratory of flexible electronics(KLoFE) & Institute of Advanced Materials(IAM) School of Flexible Electronics(Future Technologies) Nanjing Tech University (NanjingTech)

The low-cost and easy large-scale fabrication advantages of printable mesoscopic perovskite solar cells(p-MPSCs) are overshadowed by their limited photovoltaic conversion efficiency(PCE). Here, we introduce the hydrazide derivative of 4-Hydroxybenzoylhydrazine(4-HBH) to improve the PCE of p-MPSCs by inducing enhanced defect passivation. Both carbonyl and hydrazine groups in hydrazide groups present strong interaction with perovskite. The hydroxyl group, as an electron donor group, increases the electron cloud density of the hydrazide group in 4-HBH under the conjugation of the benzene ring,and thus enhances its interaction with perovskite. Additionally, the hydroxy group itself interacts with perovskite and passivates defects synergistically. The hydrazine agents can also reduce I2and suppress the loss of iodine in perovskite films, which inhibits the formation of iodine-related defects.Consequently, p-MPSCs with 4-HBH achieve a high PCE of 19.21%, and present well improved stability.

关键词： Conjugation redox activity Cooperative coordination Multifunctional hydrazine derivatives Printable mesoscopic perovskite solar cells

Lactonization of dyes promoted by a coordination cage facilitates cavity-induced chromism as ion mobile detector

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Science China Chemistry 2024年第5期67卷 1554-1560页

作者： Liangliang Zhang Yu Liang Zhifeng Xiao Yuxuan Meng Jinyi Huang Xi Lin Ji Li Hong-Cai Zhou Yu Fang Strait Institute of flexible electronics(SIFE Future Technologies)Fujian Normal University and Strait Laboratory of Flexible Electronics(SLoFE)Fuzhou 350017China State key laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Chemistry Texas A&M UniversityCollege StationTexas 77842-3012USA State key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Frontiers Science Center for flexible electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KLoFE)Northwestern Polytechnical UniversityXi’an 710072China

Dye molecules often change colors(so-called “chromism”) according to the environment variation. However, they are rarely induced by a catalytic amount of cavity. Through encapsulation in the cavity of a porous coordination cage(PCC-2), Rhodamine B(1) is transformed from red quinonoid form(1q) into colorless lactone form(1l) in aprotic polar solutions. The μ4-OH groups in the cavity of PCC-2 are shown to stabilize the uncommon zwitterion intermediate(1z), followed by converting to 1l, thus accelerating the equilibrium. The chromism is catalyzed by 0.25 mol% of PCC-2, and the reaction rate is improved by 80,400times. 1@PCC-2 can be further fabricated to a sol-gel that exhibits ion recognition properties. The resulting encapsulation and stabilization of an unconventional intermediate by a catalytic amount of the coordination cage provides fundamental insights into molecular isomerization and has potential use in chemical sensing.

关键词： porous coordination cage Zwitterion intermediate cavity Rhodamine B chromism

Efficient micrometer-scale thick-film perovskite solar cells with superior stability

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Rare Metals 2024年第4期43卷 1647-1657页

作者： Jian-Fei Hu Gang Chen Shun-Zhang Yu Yue-Xin Lin Kai-Yu Wang Zong-Wei Li Guo-Dong Zhang Teng-Fei Pan Ya-Jing Li Ming-Jie Li Ying-Dong Xia Yi-Fan Lv Yong-Hua Chen key laboratory of flexible electronics (KLoFE) and Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies)Nanjing Tech University (NanjingTech) Department of Applied Physics The Hong Kong Polytechnic University Shenzhen Research Institute The Hong Kong Polytechnic University Optics Valley laboratory

It is essential to enhance the thickness of the absorber layer for perovskite solar cells(PSCs) to improve device performance and reduce industry refinement.However,thick perovskite films(> 1 μm) are difficult to be fabricated by employing traditional solvents,such as N,N-dimethylformamide(DMF),dimethyl sulfoxide(DMSO).Besides,it is a challenge to fabricate thick-film perovskite owing to the deteriorated surface morphology and serious defect density.Herein,a simple method was reported to deposit uniform pinhole-free perovskite films with a thickness of more than 2 μm utilizing the methylamine acetate(MAAc) ionic liquid as the solvent.Combined with methylammonium chloride(MACl) as an additive,thick-film perovskite with～ 2μm in grain size and few grain boundaries(GBs) was prepared,which dramatically improved the perovskite crystal quality and enhanced carrier transport performance.The final PSCs exhibited a power conversion efficiency(PCE) of 20.16%.The device showed improved stability with 95% of its initial efficiency in a nitrogen environment over 5000 h.This work provides an alternative strategy to produce extremely efficient and stable thick-film PSCs.It can be believed that this device has great potential in the application of large areas and laminated PSCs.

关键词： Perovskite solar cells Thick-film Stability Ionic liquid

Asymmetric Electrolytes Design for Aqueous Multivalent Metal Ion Batteries

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Nano-Micro Letters 2024年第3期16卷 227-253页

作者： Xiaochen Yang Xinyu Wang Yue Xiang Longtao Ma Wei Huang Frontiers Science Center for flexible electronics Institute of Flexible ElectronicsNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510641People’s Republic of China

With the rapid development of portable electronics and electric road vehicles,high-energy-density batteries have been becoming front-burner issues.Traditionally,homogeneous electrolyte cannot simultaneously meet diametrically opposed demands of high-potential cathode and low-potential anode,which are essential for high-voltage batteries.Meanwhile,homogeneous electrolyte is difficult to achieve bi-or multi-functions to meet different requirements of electrodes.In comparison,the asymmetric electrolyte with bi-or multi-layer disparate components can satisfy distinct requirements by playing different roles of each electrolyte layer and meanwhile compensates weakness of individual electrolyte.Consequently,the asymmetric electrolyte can not only suppress by-product sedimentation and continuous electrolyte decomposition at the anode while preserving active substances at the cathode for high-voltage batteries with long cyclic lifespan.In this review,we comprehensively divide asymmetric electrolytes into three categories:decoupled liquid-state electrolytes,bi-phase solid/liquid electrolytes and decoupled asymmetric solid-state electrolytes.The design principles,reaction mechanism and mutual compatibility are also studied,respectively.Finally,we provide a comprehensive vision for the simplification of structure to reduce costs and increase device energy density,and the optimization of solvation structure at anolyte/catholyte interface to realize fast ion transport kinetics.

关键词： Asymmetric electrolyte Aqueous multivalent metal ion batteries Electrochemical stability windows Electrolyte interface

Coupling Au with BO_(x) matrix induced by Closo-boron cluster for electrochemical synthesis of ammonia

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Journal of Energy Chemistry 2024年第6期93卷 471-477,I0012页

作者： Wenjing Liu Nan Yang Yuao Wei Yingjie Yu Jie Chen Mo Wei Yuting Huang Xiaohan Li Linghai Zhang Faisal Saleem Weina Zhang Haibo Zhang Fengwei Huo key laboratory of flexible electronics(KLOFE)&Institute of Advanced Materials(IAM) School of Flexible Electronics(Future Technologies)Nanjing Tech UniversityNanjing 211816JiangsuChina College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072HubeiChina

Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.

关键词： Boron clusters Nitrogen reduction reaction Au–B coupling

Hetero-phase zirconia encapsulated with Au nanoparticles for boosting electrocatalytic nitrogen reduction

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Chinese Chemical Letters 2024年第5期35卷 509-513页

作者： Xue Xin Qiming Qu Islam E.Khalil Yuting Huang Mo Wei Jie Chen Weina Zhang Fengwei Huo Wenjing Liu key laboratory of flexible electronics(KLOFE)&Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as an attractive approach for ammonia synthesis under mild conditions.A bottleneck of NRR is the exploration of efficient catalysts for accelerating reaction kinetics,among which heterogeneous structures possessing distinct atomic arrangement could modify electronic structure,and therefore altering their NRR activity.Here,we report a facile strategy for fabricating hetero-phase metal oxides derived from metal organic framework that are further integrated with Au nanoparticles as NRR catalysts.The phase composition of zirconia can be easily adjusted by simply changing the reaction temperature,where the monoclinic and tetragonal phases with the roughly close proportions have a distinct interface,leading to a strong interaction between Au and ZrO_(2).The enhanced interaction renders Au to be more electropositive and facilitates stronger binding to N_(2).As a result,a remarkable ammonia yield of 22.32μg h^(-1)mg_(cat.)^(-1) and a Faradaic efficiency of 31.92%can be achieved at low overpotential.This work is expected to pave the way for the design of heterogeneous structures and the exploration of hetero-phase nanostructures in boosting the electrocatalytic NRR.

关键词： Hetero-phase Metal-organic framework derivatives Zirconia Nitrogen reduction reaction Electrochemistry

Boosting MA-based two-dimensional Ruddlesden-Popper perovskite solar cells by incorporating a binary spacer

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Journal of Energy Chemistry 2024年第8期95卷 348-356页

作者： Xue Dong Yinhao Tang Yiqun Li Xin Li Yuzhen Zhao Wenqi Song Fangmin Wang Shudong Xu Yipeng Zhou Chenxin Ran Zongcheng Miao Lin Song Zhongbin Wu Xi'an key laboratory of Advanced Photo-electronics Materials and Energy Conversion Device Technological Institute of Materials & Energy Science (TIMES) Xijing University Frontiers Science Center for flexible electronics Xi'an Institute of Flexible Electronics (IFE) Northwestern Polytechnical University School of Artificial Intelligence Optics and electronics (iOPEN) Northwestern Polytechnical University

Two-dimensional Ruddlesden-Popper（2DRP） perovskite exhibits excellent stability in perovskite solar cells（PSCs） due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid（GPA） and 4-fluorophenethylamine（FPEA） are realized.These films(GPA0.85FPEA0.15)2MA4Pb5I16show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37% with a VOCof1.15 V,a JSCof 20.13 mA cm-2,and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP（n ≤ 5） PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.

关键词： Binary spacers Perovskite solar cells Stability Two-dimensional Ruddlesden-Popper perovskite