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Narrowband blue emitter based on fused nitrogen/carbonyl combination with external quantum efficiency approaching 30%

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Science China Chemistry 2024年第1期67卷 351-359页

作者： Long Chen Jia-Heng Cai You-Jun Yu Yang-Kun Qu Sheng-Yi Yang Sheng-Nan Zou Rui-Hong Liu Dong-Ying Zhou Liang-Sheng Liao Zuo-Quan Jiang Institute of Functional nano&Soft materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of materials Science and Engineering Macao University of Science and TechnologyMacao 999078China

Multi-resonance thermally activated delayed fluorescence(MR-TADF)emitters can enable narrowband emission with high color purity and electroluminescence efficiency.Nitrogen/carbonyl(N/C=O)system is receiving increasing attention while the nitrogen/boron(N/B)system has been widely studied.Donor decoration is an effective approach for N/B type MR-TADF system but always leads to broadening and red-shifting of the emission band in N/C=O MR-TADF system.We attribute these unfavorable phenomena to the formation of intramolecular charge transfer between the MR-core and peripheral donors.To address this issue,we have developed a new strategy by decorating DMQAO(a fused N/C=O MR-core)with a triazine acceptor and a neutral terphenyl group to construct MTDMQAO and MBDMQAO,respectively.The introduction of the triazine acceptor not only realizes efficient narrowband emission in MTDMQAO,but also accelerates the reverse intersystem crossing process through enhanced spin-orbital coupling.As a result,MTDMQAO exhibits a significantly higher external quantum efficiency of 29.4%compared to the referent emitters,validating the rationality of our derivation strategy.This study highlights the potential of the N/C=O system for MR-TADF emitters and provides important insights for understanding the difference between N/B and N/C=O systems.

关键词： carbonyl group narrowband acceptor decoration thermally activated delayed fluorescence OLEDs

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Hydrodynamic analysis of carbon nanotube clusters in distributor-less conical fluidized beds with step-by-step scaling

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Chinese Journal of Chemical Engineering 2024年第3期67卷 117-125页

作者： Tianle Zhang Wenjuan Bai Qianpeng Dong Dianming Chu Lianlian Wang Yan He Shandong Engineering Laboratory for Preparation and Application of High-performance carbon-materials College of Electromechanical EngineeringQingdao University of Science and TechnologyQingdao 266061China Shandong Dazhan nano materials Co. Ltd.Binzhou 256220China

As a high-performance material with great application potential,the application of carbon nanotubes has been limited by their production volume.A distributor-less conical fluidized bed is the main equipment used in the industrial production of carbon nanotubes.To improve the production volume and product quality of carbon nanotubes,the study of fluidized-bed-diameter scaling is important.Three different diameters of distributor-less conical fluidized beds were established,and then the particle behavior and bubble characteristics of carbon nanotube clusters at these bed diameters were investigated.Time-series and wavelet analysis methods were used to analyze the pressure-fluctuation signals inside the fluidized beds.Results showed that the distributor-less design caused the airflow to break through the middle of the bed,which did not change with the change in bed diameter.The powder-bridging phenomenon of carbon nanotube clusters in a 100-mm-diameter fluidized bed was related to the special microstructure of carbon nanotube clusters.The frequency of pressure fluctuations in the bed decreased nonlinearly with increasing bed diameter.This study can guide the design and scale-up of distributor-less conical fluidized beds,especially for the scale-up of carbon nanotube production equipment,which can contribute to the improvement of carbon nanotubes’capacity and quality in industrial production.

关键词： carbon nanotubes Fluidized bed Multiphase flow Scale-up Multiscale

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Room-temperature synthesis of full-component APbX_(3)perovskite nanocrystal inks for optoelectronic applications

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Journal of Energy Chemistry 2024年第5期92卷 87-94页

作者： Xinyu Zhao Du Li Xuliang Zhang Hehe Huang Chenyu Zhao Wanli Ma Jianyu Yuan Institute of Functional nano&Soft materials(FUNSOM) Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory for carbon-Based Functional materials&Devices Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory of Advanced Negative carbon Technologies Soochow UniversitySuzhou 215123JiangsuChin

Lead halide perovskite nanocrystals(PNCs)have received great research interests due to their excellent optoelectronic properties.However,high temperature,inert gas protection and insulating long-chain ligands are used during the conventional hot-injection synthesis of PNCs,which limits their practical applications.In this work,we first develop a simple and scalable polar-solvent-free method for the preparation of full-component APbX_(3)(A=Cs,methylammonium(MA),formamidinium(FA),X=Cl,Br,I)PNCs under ambient condition.Through an exothermic reaction between butylamine(BA)and propionic acid(PA)short ligands,the PbX_(2) precursors could be well dissolved without use of any polar solvent.Meanwhile,the relatively lower growth rate of PNCs in our room-temperature reaction enables us to modulate the synthetic procedure to enhance the scalability(40-fold)and achieve large-scale synthesis.The resultant short ligands passivated PNC inks are compatible with varying solution depositing technique like spray coating for large-area film.Finally,we showcase that adopting the as-prepared MAPbI_(3) PNC inks,a self-powered photodetector is fabricated and shows a high photoresponsivity.These results demonstrate that our ambient-condition synthetic approach can accelerate the preparation of tunable and ready-to-use PNCs towards commercial optoelectronic applications.

关键词： Room-temperaturesynthesis Perovskite nanocrystals Short-chainligands Large-scale Photodetector

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Magnetic-biased chiral molecules enabling highly oriented photovoltaic perovskites

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National Science Review 2024年第2期11卷 221-230页

作者： Jing Chen Caner Deger Zhen-Huang Su Kai-Li Wang Guang-Peng Zhu Jun-Jie Wu Bing-Chen He Chun-Hao Chen Tao Wang Xing-Yu Gao Ilhan Yavuz Yan-Hui Lou Zhao-Kui Wang Liang-Sheng Liao Institute of Functional nano&Soft materials(FUNSOM) Laboratory of Advanced Negative Carbon TechnologiesSoochow University Department of Physics Marmara University Shanghai Synchrotron Radiation Facility(SSRF) Shanghai Advanced Research InstituteChinese Academy of Sciences College of Energy Soochow Institute for Energy and Materials Innovations Soochow University Macao Institute of materials Science and Engineering Macau University of Science and Technology

The interaction between sites A, B and X with passivation molecules is restricted when the conventional passivation strategy is applied in perovskite（ABX3） photovoltaics. Fortunately, the revolving A-site presents an opportunity to strengthen this interaction by utilizing an external field. Herein, we propose a novel approach to achieving an ordered magnetic dipole moment, which is regulated by a magnetic field via the coupling effect between the chiral passivation molecule and the A-site（formamidine ion） in perovskites.This strategy can increase the molecular interaction energy by approximately four times and ensure a well-ordered molecular arrangement. The quality of the deposited perovskite film is significantly optimized with inhibited nonradiative recombination. It manages to reduce the open-circuit voltage loss of photovoltaic devices to 360 mV and increase the power conversion efficiency to 25.22%. This finding provides a new insight into the exploration of A-sites in perovskites and offers a novel route to improving the device performance of perovskite photovoltaics.

关键词： perovskite photovoltaics magnetic moment A-site regulation chiral molecules

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Self-fueling ferroptosis-inducing microreactors based on p H-responsive Lipiodol Pickering emulsions enable transarterial ferro-embolization therapy

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National Science Review 2024年第1期11卷 74-85页

作者： Chunjie Wang Lei Zhang Zhijuan Yang Dongxu Zhao Zheng Deng Jialu Xu Yumin Wu Yu Hao Ziliang Dong Liangzhu Feng Zhuang Liu Institute of Functional nano & Soft materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Center of Interventional Radiology & Vascular Surgery Department of Radiology Zhongda Hospital Medical School Southeast University Department of Interventional Radiology The First Afflliated Hospital of Soochow University

Lipiodol chemotherapeutic emulsions remain one of the main choices for the treatment of unresectable hepatocellular carcinoma(HCC) via transarterial chemoembolization(TACE). However, the limited stability of Lipiodol chemotherapeutic emulsions would lead to rapid drug diffusion, which would reduce the therapeutic benefit and cause systemic toxicity of administrated chemotherapeutics. Therefore, the development of enhanced Lipiodol-based formulations is of great significance to enable effective and safe TACE treatment. Herein, a stable water-in-oil Lipiodol Pickering emulsion(LPE) stabilized by pH-dissociable calcium carbonate nanoparticles and hemin is prepared and utilized for efficient encapsulation of lipoxygenase(LOX). The obtained LOX-loaded CaCO3&hemin-stabilized LPE(LHCa-LPE) showing greatly improved emulsion stability could work as a pH-responsive and self-fueling microreactor to convert polyunsaturated fatty acids(PUFAs), a main component of Lipiodol, to cytotoxic lipid radicals through the cascading catalytic reaction driven by LOX and hemin, thus inducing ferroptosis of cancer cells. As a result, such LHCa-LPE upon transcatheter embolization can effectively suppress the progression of orthotopic N1S1 HCC in rats. This study highlights a concise strategy to prepare pH-responsive and stable LPE-based self-fueling microreactors, which could serve as bifunctional embolic and ferroptosis-inducing agents to enable proof-of-concept transarterial ferro-embolization therapy of HCC.

关键词： CaCO3 nanoparticles Pickering emulsion ferroptosis lipid peroxidation transarterial ferro-embolization

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Organic near-infrared optoelectronic materials and devices:an overview

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Advanced Photonics 2024年第1期6卷 17-42页

作者： Zong-Lu Che Chang-Cun Yan Xue-Dong Wang Liang-Sheng Liao Soochow University Institute of Functional Nano and Soft Materials(FUNSOM)Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSuzhouChina Soochow University College of ChemistryChemical Engineering and Materials ScienceJiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhouChina Macao University of Science and Technology Macao Institute of Materials Science and EngineeringMacaoChina

Near-infrared(NIR)light has shown great potential for military and civilian applications owing to its advantages in the composition of sunlight,invisibility to human eyes,deeper penetration into biological tissues,and low optical loss in optical fibers.Therefore,organic optoelectronic materials that can absorb or emit NIR light have aroused great scientific interest in basic science and practical applications.Based on these NIR organic optoelectronic materials,NIR optoelectronic devices have been greatly improved in performance and application.In this review,the representative NIR organic optoelectronic materials used in organic solar cells,organic photodetectors,organic light-emitting diodes,organic lasers,and organic optical waveguide devices are briefly introduced,and the potential applications of each kind of device are briefly summarized.Finally,we summarize and take up the development of NIR organic optoelectronic materials and devices.

关键词： near-infrared organic optoelectronic materials organic solar cells organic light-emitting devices organic optical waveguides

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Surface iodine and pyrenyl-graphdiyne co-modified Bi catalysts for highly efficient CO_(2) electroreduction in acidic electrolyte

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nano Research 2024年第4期17卷 2381-2387页

作者： Min Zhang Juan Wang Xin Rong Xiu-Li Lu Tong-Bu Lu MOE International Joint Laboratory of materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

CO_(2) electroreduction to formic acid/formate would contribute to alleviating the energy and climate crisis.This work reports a Bi-based catalyst derived from the in-situ electroreduction of Bi_(2)O_(2)CO_(3) modified with iodine and pyrenyl-graphdiyne(PGDY)on the surface for efficient electroreduction of CO_(2) in acidic electrolyte,with a high partial current density of 98.71 mA·cm^(-2) and high Faradaic efficiency(FE)>90%over the potential range from^(-1).2 to-1.5 V vs.reversible hydrogen electrode(RHE),as well as the long-term operational stability over 240 h without degradation in H-type cell.Experimental results and density function theory calculations show that the synergistic effect of surface iodine and PGDY is responsible for this active and extremely stable process of CO_(2) electroreduction via lowering the energy barriers for formation of*OCHO intermediate,suppressing the competitive HER by enhancing the concentration of both K+and CO_(2) at reaction interface,as well as preventing the dissolution and re-deposition of active Bi atoms on surface during catalytic reaction.This work provides new insight into designing highly active and stable electrocatalysts for CO_(2) reduction.

关键词： CO_(2) reduction electrocatalysis Bi-based catalysts acidic electrolyte

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nanoscale Precise Editing of Multiple Immune Stimulating Ligands on DNA Origami for T Cell Activation and Cell-Based Cancer Immunotherapy

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CCS Chemistry 2024年第3期6卷 719-732页

作者： Lele Sun Fengyun Shen Zijian Xiong Yu Chao Chunhai Fan Zhuang Liu Institute of Functional nano&Soft materials(FUNSOM) Jiangsu Key Lab Carbon Based Functional Materials and DevicesSoochow UniversitySuzhou 215123Jiangsu School of Life Sciences Shanghai UniversityShanghai 200444 School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 201240

The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a great challenge.Here,with DNA origami,we precisely organized the CD3ɛantibodies simulating T cell receptor(TCR)ligands and CD28 antibodies simulating co-stimulatory ligands to interrogate the independent role of TCR-ligand spacing and local copy numbers as well as the spacing between TCR ligands and co-stimulatory ligands on T cell activation.We found that T cell activation benefited fromlocally concentrated TCR ligands with a shorter spacing and was maximized by an∼38 nm spacing between TCR ligands and co-stimulatory ligands.The T cell expander constructed based on our findings could efficiently expand CD8+T cells for tumor immunotherapy.Thus,the DNA nanostructurebased ligands’precise arrangement can be a unique tool in studying immune cell activations and cellbased immunotherapies.

关键词： DNA origami T cell activation T cell receptor immune cancer immunotherapy

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3D printed silicon-based micro-lattices with ultrahigh areal/gravimetric capacities and robust structural stability for lithium-ion batteries

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nano Research 2024年第4期17卷 2693-2703页

作者： Jie Fu Dong Wang Yan Li Xianzheng Liu Rui Zhang Zhiyuan Liu Pengdong Liu Lijuan Zhang Xuefei Li Guangwu Wen School of materials Science and Engineering Shandong University of TechnologyZibo 255000China Shandong Si-nano materials Technology Co. Ltd.Zibo 255000China

nanostructured silicon anodes have shown extraordinary lithium storage properties for lithium-ion batteries(LIBs)but are usually achieved at low areal loadings(<1.5 mg·cm^(-2))with low areal capacity.Sustaining sound... 详细信息

nanostructured silicon anodes have shown extraordinary lithium storage properties for lithium-ion batteries(LIBs)but are usually achieved at low areal loadings(carbon nanotube(3D-Si/G/C)electrode for simultaneously achieving ultrahigh areal/gravimetric capacities at high mass loading.The periodically arranged vertical channels and hierarchically porous filaments facilitate sufficient electrolyte infiltration and rapid ion diffusion,and the carbonaceous network provides excellent electron transport properties and mechanical integrity,thus endowing the printed 3D-Si/G/C electrode with fast electrochemical reaction kinetics and reversibility at high mass loading.Consequently,the 3D-Si/G/C with high areal mass loading of 12.9 mg·cm^(-2) exhibits excellent areal capacity of 12.8 mAh·cm^(-2) and specific capacity of 1007 mAh·g^(-1),respectively.In-situ optical microscope and ex-situ scanning electron microscope(SEM)confirm that the hierarchically porous filaments with interconnected carbon skeletons effectively suppress the volume change of silicon and maintain stable micro-lattice architecture.A 3D printed 3D-Si/G/C-1||3D-LiFePO_(4)/G full cell holds excellent cyclic stability(capacity retention rate of 78%after 50 cycles)with an initial Coulombic efficiency(ICE)of 96%.This work validates the feasibility of 3D printing on constructing high mass loading silicon anode for practical high energy-density LIBs.

关键词： silicon anode areal capacity three-dimensional(3D)printing lithium-ion batteries

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Guanine-derived F,N co-doped carbon-shell encapsulated iron carbide nanoparticles for enhanced CO_(2)electroreduction activity

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nano Research 2024年第6期17卷 4744-4752页

作者： Shuo Chen Lishun Pei Ying Peng Xuefei Zhang Zailai Xie Key Laboratory of Advanced carbon-Based Functional materials(Fujian Province University) Fuzhou UniversityFuzhou 350016China

The development of highly selective,cost-effective,and energy-efficient electrocatalysts is critical for carbon dioxide reduction reaction(CO_(2)RR)to produce high-value products.Herein,we propose a facile strategy to obtain F,N co-doped carbon-coated iron carbide(Fe3C)nanoparticles by using biomolecule guanine and hexadecafluorophthalocyanine iron as raw materials.Remarkably,this method involves only one-step pyrolysis and does not require any guiding agent or sacrificial template.Benefiting from the advantageous surface microenvironment adjustments achieved through graphitic N(GN)and F co-doping,Fe3C@NF-G-1000 demonstrates exceptional efficacy in the electroreduction of CO_(2)to carbon monoxide(CO)with an impressive Faradic efficiency(FEco)up to 98%at the potential of−0.55 V(vs.reversible hydrogen electrode(RHE)).Furthermore,it delivers a remarkable current density of up to−43 mA·cm^(−2)and exhibits virtually no current attenuation over a span of 20 h within the flow cell.Insights from density functional theory(DFT)calculations reveal that the composite structure of GN and F co-doped graphitic layer and Fe3C exhibits different electron density distributions from that of iron carbide nanoparticles.This is attributed to the synergistic effect of the composite structure leading to the enrichment of electrons in the graphite layer on the surface,which contributes to the stability of the key reaction intermediate*COOH,thus,resulting in an enhanced catalytic activity and efficiency.Overall,this work introduces a new and promising approach to the design of green and low-cost carbon-coated metal materials for CO_(2)reduction reactions.

关键词： guanine F,N co-doped carbon dioxide reduction reaction(CO_(2)RR) Fe-based catalyst

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