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Metal-organic polyhedra as dynamic cross-linker for recyclable mixed matrix membranes with promising dimension stability

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Science China Chemistry 2024年

作者： Linjie Lan Mingxin Zhang Haiyan Xiao Liufu Wei Yuyan Lai Jiadong Chen Jiafu Yin Panchao Yin State Key Laboratory of Luminescent Materials and Devices&South China Advanced Institute for soft matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer MaterialsSouth China University of Technology State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan University

Mixed matrix membranes （MMMs） are designed by incorporating microporous inorganic fillers into polymer matrix for the integration of inorganics’excellent gas separation performance with polymers’promising ***,due to the complex interphase interaction,the prevention of long-term aging is still challenging and the poor processability/recyclability of MMMs hinders their extensive ***,a coordination assembly protocol is developed for the fabrication of MMMs with both excellent processability/recyclability upon thermal annealing and promising dimension stability even under high gas *** bearing isophthalic acid （IPA） as side chains are applied to coordinate with Cu2+and the assembled 2.5 nm microporous metal-organic polyhedra （MOP）,{Cu24IPA24},serves as multi-functional cross-linkers for the polymer network *** MOPs’well-defined microporosity grants MMMs the capability for O2/N2separation while their activated dynamics at high temperatures （>120°C） endows polymer networks with excellent *** contrast to conventional supramolecular units,the MOPs possess unique logarithmic ligand-exchange kinetics and they show nearly frozen bonding dynamics at room temperature,ensuring promising dimensional stability to overcome the long-term aging and high gas pressure *** work not only provides fundamental understanding of the unique relaxation dynamics of complex systems with intertwined dynamics of supramolecular bonds and polymer chains,but also paves new avenues for the fabrication of robust and recyclable MMMs and elastomers.

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Near-infrared double-cable conjugated polymers based on alkyl linkers with tunable length for single-component organic solar cells

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Chinese Chemical Letters 2024年第4期35卷 452-456页

作者： Yikun Wang Qiaomei Chen Shijie Liang Dongdong Xia Chaowei Zhao Christopher R.McNeill Weiwei Li Beijing Advanced Innovation Center for soft matter Science and Engineering&State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Institute of Applied Chemistry Jiangxi Academy of SciencesNanchang 330096China Department of Materials Science and Engineering Monash UniversityWellington RoadClaytonVictoria 3800Australia

The photovoltaic properties of double-cable conjugated polymers are significantly influenced by the length of the alkyl linkers that connect donor backbones and acceptor side units. In this study, a series of 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile(IC)-based double-cable polymers with alkyl linkers ranging from C_8H_(16)to C_(16)H_(32)(Px, x = 8, 10, 12, 14, 16) were synthesized for single-component organic solar cells(SCOSCs). Among these, the linker length x = 12(P12) is found to optimize the power conversion efficiencies(PCEs) in SCOSCs. Specifically, PCEs increase from P8 to P12 and then decline from P12to P16. Detailed investigations of optical absorption, charge transport, and morphology provide insights into the underlying factors contributing to these PCE variations. The findings indicate that the exceptional photovoltaic properties observed in P12 can be attributed to three key factors: A delicate balance between enhanced charge separation facilitated by the increased spacer length and reduced crystallinity resulting from longer spacers, higher charge mobilities, and well-balanced hole/electron transport characteristics. This study highlights the critical role of linker length in determining the photovoltaic properties of double-cable conjugated polymer-based SCOSCs and offers valuable guidance for the design of novel double-cable conjugated polymers.

关键词： Single-component organic solar cells Double-cable conjugated polymers Photovoltaic properties Alkyl linkers

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Magnetic proximity effect in the two-dimensional ε-Fe_(2)O_(3)/NbSe_(2)heterojunction

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Chinese Physics B 2024年第2期33卷 492-497页

作者：车冰玉胡国静朱超郭辉吕森浩刘轩冶吴康赵振潘禄禄祝轲齐琦韩烨超林晓李子安申承民鲍丽宏刘政周家东杨海涛高鸿钧 Beijing National Center for Condensed matter Physics and Institute of Physics Chinese Academy of SciencesBeijing 100190China school of Physical Sciences University of Chinese Academy of SciencesBeijing 100190China school of Materials Science and Engineering Nanyang Technological UniversitySingapore school of Physical Science and Technology Guangxi UniversityGuangxi 530004China school of Physics Beijing Institute of TechnologyBeijing 100081China

Two-dimensional(2D)magnet/superconductor heterostructures can promote the design of artificial materials for exploring 2D physics and device applications by exotic proximity ***,plagued by the low Curie temperature and instability in air,it is hard to realize practical applications for the reported layered magnetic materials at *** this paper,we developed a space-confined chemical vapor deposition method to synthesize ultrathin air-stable ε-Fe_(2)O_(3) nanosheets with Curie temperature above 350 *** ε-Fe_(2)O_(3)/NbSe_(2) heterojunction was constructed to study the magnetic proximity effect on the superconductivity of the NbSe_(2) *** electrical transport results show that the subtle proximity effect can modulate the interfacial spin–orbit interaction while undegrading the superconducting critical *** work paves the way to construct 2D heterojunctions with ultrathin nonlayered materials and layered van der Waals(vdW)materials for exploring new physical phenomena.

关键词： two-dimensional heterojunctions magnetic proximity effect non-layered magnetic nanosheet spin-orbit interaction

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Matrix-Mediated Color-Tunable Ultralong Organic Room Temperature Phosphorescence of 7H-Benzo[c]carbazole Derivatives

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CCS Chemistry 2024年第3期6卷 798-811页

作者： Chen Qian Xue Zhang Zhimin Ma Xiaohua Fu Zewei Li Huiwen Jin Mingxing Chen Hong Jiang Zhiyong Ma Beijing Advanced Innovation Center for soft matter Science and Engineering State Key Laboratory of Organic–Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029 Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Building on the recent systematic research on 1Hbenzo[f]indole(Bd),an important advancement in constructing ultralong organic room temperature(UORTP)materials with a universal strategy via a readily obtained unit(7H-Benzo[c]carbazole,BCz)is proposed in this *** powders of BCz and its derivatives merely exhibit blue fluorescence at ambient ***,when BCz and its derivatives are dispersed into polymer or powder matrixes,strong photo-activated green UORTP can be observed from their doped systems at room ***,the UORTP color can be tuned between green and yellow depending on the *** ultralong phosphorescence originates from the generation of charge-separated states via *** matrixes play a key role in both stabilizing charge-separated states and controlling UORTP *** interestingly,when using polymethyl methacrylate as matrix,the doped films achieve stronger photo-activated ultralong phosphorescence underwater than in air at room *** Bd,BCz achieves better performance not only in ultralong phosphorescence properties but also in practical *** work gains a deeper insight into the mechanism of UORTP and paves a new approach to applying organic phosphorescent materials to underwater coating and imaging.

关键词： 7H-Benzo[c]carbazole ultralong organic room temperature phosphorescence ion radical matrix-mediated color tunning underwater application

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Unveiling size-fluorescence correlation of organic nanoparticles and its use in nanoparticle size determination

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Aggregate 2024年第1期5卷 331-336页

作者： Wu-Jie Guo Shixiang Ma Hui Wang Lu Qiao Lei Chen Chenyu Hong Bin Liu Xiaoyan Zheng Hui-Qing Peng State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijingChina Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electro-photonic Conversion MaterialsKey Laboratory of Medicinal Molecule Science and Pharmaceutics Engineering of Ministry of Industry and Information TechnologySchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijingChina

Quantitatively establishing the correlation between nanoparticle size and fluorescence is essential for understanding the behavior and functionality of fluorescent nanoparticles(FNPs).However,such exploration focusing on organic FNPs has not been achieved to ***,we employ the use of supramolecular polymeric FNPs prepared from tetraphenylethylene-based bis-ureidopyrimidinone monomers(bis-UPys)to relate the size to the fluorescence of organic *** an equal concentration of bis-UPys,a logarithmic relationship between them is built with a correlation coefficient higher than *** calculations indicate that variations in fluorescence intensity among FNPs of different sizes are attributed to the distinct molecular packing environments at the surface and within the interior of the *** leads to different nonradiative decay rates of the embedded and exposed bis-UPys and thereby changes the overall fluorescence quantum yield of nanoparticles due to their different specific surface *** established fluorescence intensity-size correlation possesses fine universality and reliability,and it is successfully utilized to estimate the sizes of other nanoparticles,including those in highly diluted dispersions of *** work paves a new way for the simple and real-time determination of nanoparticle sizes and offers an attractive paradigm to optimize nanoparticle functionalities by the size effect.

关键词： aggregation-induced emission fluorescence detection fluorescent nanoparticle nanoparticle size supramolecular polymer

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Inhibition of Heterogeneous Nucleation in Water by Hydrogel Coating

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research 2024年第2期2023卷 139-147页

作者： Siyang Li Panpan Zhu Yaoting Xue Lei Wangg Tuck-Whye Wong Xuxu Yang Haoei Zhou Tiefeng Li We Yang Department of Engineering Mechanics Zhejiang UniversityHangzhou 310027China Key Laboratory of soft Machines and Smart Devices of Zhejiang Province Zhejiang UniversityHangzhou 310027China Center for X-Mechanics Department of Engineering MechanicsZhejiang UniversityHangzhou 310027China school of Biomedical Engineering and Health Sciences and Advanced Membrane Technology research Centre Universiti Teknologi MalaysiaSkudai 81310Malaysia

Heterogeneous nucleation plays a critical role in the phase transition of water,which can cause damage in various ***,we report that heterogeneous nucleation can be inhibited by utilizing hydrogel coatings to isolate solid surfaces and ***,which contain over 90%water when fully swelled,exhibit a high degree of similarity to *** to this similarity,there is a great energy barrier for heterogeneous nucleation along the water-hydrogel ***,hydrogel coatings,which possess polymer networks,exhibit higher fracture energy and more robust adhesion to solid surfaces compared to *** high fracture and adhesion energy acts as a deterrent for fracture nucleation within the hydrogel or along the hydrogel-solid *** a hydrogel layer approximately 100μm thick,the boiling temperature of water under atmospheric pressure can be raised from 100 to 108℃.Notably,hydrogel coatings also result in remarkable reductions in cavitation pressure on multiple solid *** have demonstrated the efficacy of hydrogel coatings in preventing damages resulting from acceleration-induced *** coatings have the potential to alter the energy landscape of heterogeneous nucleation on the water-solid interface,making them an exciting avenue for innovation in heat transfer and fluidic systems.

关键词： fracture cavitation similarity

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Impact of Polymer Matrix on Polymer Mechanochromism from Excited State Intramolecular Proton Transfer

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Chinese Journal of Chemistry 2024年第6期42卷 611-616页

作者： Yu Wu Xin Cheng Huan Hu Shui Hu Zhimin Ma Zhiyong Ma Beijing Advanced Innovation Center for soft matter Science and Engineering Beijing State Key Laboratory of Organic-Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing100029 China Center of Advanced Elastomer Materials College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing100029 China College of Engineering Peking UniversityBeijing100871 China

Mechanochromic polymers based on non-covalent changes have attracted much attention ***,we report the impact of inter/intramolecular hydrogen bonds on polymer mechanochromism from the excited state intramolecular proton transfer (ESIPT) ***-NH2-OH and PhMz=2A are designed and obtained by simple and high-yield synthesis,and are connected into polyurethane and poly(methyl acrylate-co-2-ethylhexyl acrylate),*** the initial state,the PhMz-NH2-OH@PU sample shows blue fluorescence from the excited enol form (E*) excitons,owing to intermolecular hydrogen bonds that interrupt the ESIPT reactions but the PhMz=2A@PMA-2-EA sample expresses cyan fluorescence belonging to the excited keto form (K*) emission,implying that the intramolecular hydrogen bonds ***,under stretching,external force can tune the emission of the PhMz=2A@PMA-2-EA sample from K* to E* *** external force can putatively still promote a bond rotation,ESIPT reactions remain equivalently interrupted in both the relaxed and stressed states in a hydrogen-bond donating *** calculation confirms the force-induced increase in dihedral angle for the transition of ESIPT-on/***,PhMz-NH2-OH@PU and PhMz=2A@PMA-2-EA showed disparate initial ESIPT states and further different responses/sensitivity to *** study reports a novel and efficient strategy for enriching mechanochromic investigation and extending the applications of ESIPT reactions.

关键词： Polymer mechanochromism Excited state intramolecular proton transfer Hydrogen bonding Supramolecular chemistry Elastomers

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High-timing-precision detection of single X-ray photons by superconducting nanowires

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National Science Review 2024年第1期11卷 194-203页

作者： Shuya Guo Jingrou Tan Hengbin Zhang Jinguang Wang Tianhao Ji Labao Zhang Xiaolong Hu Jian Chen Jun Xie Kai Zou Yun Meng Xiaomin Bei Ling-An Wu Qi Chen Hao Wang Xuecou Tu Xiaoqing Jia Qing-Yuan Zhao Lin Kang Peiheng Wu research Institute of Superconductor Electronics Nanjing University Qian Xuesen Laboratory of Space Technology Beijing National Laboratory of Condensed matter Physics Institute of Physics Chinese Academy of Sciences Hefei National Laboratory school of Precision Instrument and Optoelectronic Engineering Tianjin University Key Laboratory of Optoelectronic Information Science and Technology Ministry of Education

Precisely acquiring the timing information of individual X-ray photons is important in both fundamental research and practical applications. The timing precision of commonly used X-ray single-photon detectors remains in the range of one hundred picoseconds to microseconds. In this work, we report on high-timing-precision detection of single X-ray photons through the fast transition to the normal state from the superconductive state of superconducting nanowires. We successfully demonstrate a free-running X-ray single-photon detector with a timing resolution of 20.1 ps made of 100-nm-thick niobium nitride film with an active area of 50 μm by 50 μm. By using a repeated differential timing measurement on two adjacent X-ray single-photon detectors, we demonstrate a precision of 0.87 ps in the arrival-time difference of X-ray photon measurements. Therefore, our work significantly enhances the timing precision in X-ray photon counting, opening a new niche for ultrafast X-ray photonics and many associated applications.

关键词： single-photon detection timing precision superconductor ultrafast phenomenon pulsar X-ray navigation

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Synthesis,structure,and luminescence properties of melilite Dy^(3+):Lu_(x)CaLa_(0.98-x)Ga_(3)O_(7) phosphors for use in yellow light-emitting devices

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Journal of Rare Earths 2024年第8期42卷 1489-1495,I0003页

作者： Yunyun Liu Chuanxin Huang Meng Wang Xihu Wang Yan Wang Ju Gao school of Opto-Electronic Engineering Zaozhuang UniversityZaozhuang277160China Key Laboratory of Functional Materials and Devices for Informatics of Anhui Educational Institutions Department of PhysicsFuyang Normal UniversityFuyang236037China Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002.China

Dy^(3+) and Lu^(3+) co-doped CaLaGa_(3)O_(7) phosphors were prepared via high-temperature solid-phase *** electronic structures of LuxCaLa_(0.98-x)Ga_(3)O_(7) were investigated by the first-principles *** influence of Lu^(3+) on yellow light emission was studied using X-ray diffraction(XRD)and photoluminescence(PL) *** XRD results indicate that compared to Dy^(3+):CaLaGa_(3)O_(7),the cell parameters of Dy^(3+):LuCaLaGa_(3)O_(7) tend to decrease,which is due to the smaller radius of Lu^(3+).When pumped by blue GaN laser diode(LD),the emission peaks of phosphors with different Lu^(3+)doping concentrations in the visible region are similar,with the strongest peak at 574 nm in the yellow light region,which is sensitive to human *** optimal doping concentration of Lu^(3+) is confirmed to be1 at%,when all emission spectra and measured fluorescence lifetimes are taken into ***,the optimal phosphor composition Dy^(3+):Lu_(x)CaLa_(0.98-x)Ga_(3)O_(7)(x=0.01) has an internal quantum efficiency(IQE) of 46.94% and an external quantum efficiency(EQE) of 15.19%.Most notably,the prepared phosphor demonstrates excellent thermal stability and a high activation energy(0.203 eV).In addition,the International Illumination Commission color coordinates of the Dy^(3+):LuxCaLa_(0.98-x)Ga_(3)O_(7) phosphors are in the yellow light *** above analysis indicates that the Dy^(3+):LuxCaLa_(0.98-x)Ga_(3)O_(7)(x=0.001)phosphor has promising application prospects in yellow light-emitting devices.

关键词： Dy^(3+):Lu_(x)CaLa_(0.98-x)Ga_(3)O_(7)phosphors Yellow emission Structure characteristics Luminescent properties Rare earths

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Introducing hydroxyl groups to tailor the d-band center of Ir atom through side anchoring for boosted ORR and HER

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Journal of Energy Chemistry 2024年第3期90卷 144-151,I0005页

作者： Qing Lv Meiping Li Xiaodong Li Xingru Yan Zhufeng Hou Changshui Huang Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100ShandongChina Institute of Chemistry Chinese Academy of ScienceBeijing 100191China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina

Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic ***,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination ***,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline *** from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical *** those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.

关键词： Oxygen reduction reaction D-band center Graphdiyne Hydroxyl group Electrocatalysis

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