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graphene quantum dots as sulfiphilic and lithiophilic mediator toward high stability and durable life lithium-sulfur batteries

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Journal of Energy Chemistry 2023年第10期85卷 254-266,I0008页

作者： Chaojiang Fan Rong Yang Yong Huang Lei Mao Yuanyuan Yang Le Gong Xin Dong Yinglin Yan Yiming Zou Lisheng Zhong Yunhua Xu International Research Center for Composite and Intelligent Manufacturing Technology Institute of Chemical Power SourcesXi'an University of TechnologyXi'an 710048ShaanxiChina School of Materials Science and Engineering Xi'an University of TechnologyXi'an 710048ShaanxiChina School of Chemistry&Chemical Engineering Yulin UniversityYulin 719000ShaanxiChina

The development of lithium-sulfur(Li-S) battery as one of the most attractive energy storage systems among lithium metal batteries is seriously hindered by low sulfur utilization, poor cycle stability and uneven redeposition of Li anode. It is necessary to propose strategies to address the problems as well as improve the electrochemical performance. One of the effective solutions is to improve the sulfiphilicity of sulfur cathode and the lithiophilicity of the Li anode. Herein, we reported that a synergistic functional separator(graphene quantum dots(GQDs)-polyacrylonitrile(PAN) @polypropylene(PP) separator)improved the electrochemical activity of sulfur cathode as well as the stability of Li anode. GQDs induced uniform Li^(+)nucleation and deposition, which slowed down the passivation of Li anode and avoided shortcircuit. Further, three-dimensional network constructed by electrospinning nanofibers and the polar functional groups of GQDs could both effectively inhibit the shuttle of LiPSs and improve the sulfur utilization. The stability of Li-S battery was improved by the synergistic effect. In addition, GQDs and electrospinning nanofibers protector increased lifetime of separators. Benefiting from the unique design strategy, Li//Li symmetric battery with GQDs-PAN@PP separators exhibited stably cycling for over 600 h. More importantly, the Li-S full batteries based GQDs-PAN@PP separators enabled high stability and desirable sulfur electrochemistry, including high reversibility of 558.09 mA h g^(-1)for 200 cycles and durable life with a low fading rate of 0.075% per cycle after 500 cycles at 0.5 C. Moreover, an impressive areal capacity of 3.23 mA h cm^(-2)was maintained under high sulfur loading of 5.10 mg cm^(-2). This work provides a new insight for modification separator to improve the electrochemical performance of Li-S/Li metal batteries.

关键词： Lithium-sulfur batteries Separator graphene quantum dots Cycle stability Durable life

graphene quantum dots: From efficient preparation to safe renal excretion

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Nano Research 2021年第3期14卷 674-683页

作者： Caroline Hadad JoséMiguel González-Domínguez Silvia Armelloni Deborah Mattinzoli Masami Ikehata Akcan Istif Adrian Ostric Francesco Cellesi Carlo Maria Alfieri Piergiorgio Messa Belén Ballesteros Tatiana Da Ros Centre of Excellence for Nanostructured Materials(CENMAT) INSTMDepartment of Chemical and Pharmaceutical SciencesUniversity of TriesteVia L.Giorgieri 134127TriesteItaly Laboratoire LG2A-CNRS UMR 7378 Universitéde Picardie Jules Verne33 rue Saint Leu-UFR des Sciences80039AmiensFrance Instituto de Carboquímica(CSIC) C/Miguel Luesma Castán 4E-50018ZaragozaSpain Renal Research Laboratory-Fondazione IRCCS Ca’Granda Ospedale Maggiore Policlinico via Pace 920122MilanItaly Dipartimento di Chimica Materiali ed Ingegneria Chimica“G.Natta”Politecnico di MilanoVia Mancinelli 720131MilanItaly Unit of Nephrology Dialysis and Renal Transplant Fondazione IRCCS Ca’Granda Ospedale Maggiore Policlinicovia della commenda 420122MilanItaly Department of Clinical Sciences and Community Health University of Milan20122MilanItaly Catalan Institute of Nanoscience and Nanotechnology(ICN2) CSIC and the Barcelona Institute of Science and TechnologyCampus UABBellaterra08193BarcelonaSpain

Carbon nanomaterials offer excellent prospects as therapeutic agents,and among them,graphene quantum dots(GQDs)have gained considerable interest thanks to their aqueous solubility and intrinsic fluorescence,which enable their possible use in theranostic approaches,if their biocompatibility and favorable pharmacokinetic are *** prepared ultra-small GQDs using an alternative,reproducible,top-down synthesis starting from graphene oxide with a nearly 100%*** materials were tested to assess their safety,demonstrating good biocompatibility and ability in passing the ultrafiltration barrier using an in vitro *** leads to renal excretion without affecting the ***,we studied the GQDs in vivo biodistribution confirming their efficient renal clearance,and we demonstrated that the internalization mechanism into podocytes is ***,considering the reported characteristics,it appears possible to vehiculate compounds to kidneys by means of GQDs,overcoming problems related to lysosomal degradation.

关键词： graphene quantum dots podocytes biodistribution uptake pathway renal clearance nanocarrier

graphene quantum dots derived from hollow carbon nano-onions

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Nano Research 2018年第1期11卷 174-184页

作者： Chenguang Zhang Jiajun LI Xianshun Zeng Zhihao Yuan Naiqin Zhao [1School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China [2School of Materials Science and Engineering Tianin University Tianin 300072 China [3Tianjin Key Lab for Photoelectric Materials & Devices Tianjin 300384 China [4Collaborative Innovation Center of Chemical Science and Engineering Tianjin University Tianjin 300072 China

Herein, carbon nano-onions （CNOs） with different structures have been investigated as precursors for the synthesis of graphene quantum dots （GQDs）. It was found that hollow CNOs yield GQDs with a uniform size distribution, whereas metal encapsulation in the CNO structure is disadvantageous for the same. Furthermore, the hollow CNOs are also advantageous for the synthesis of GQDs with a yellow-green hybrid luminescence and long-ranged excitation wavelength （λex）-independent photoluminescent （PL） behavior, in which the λex upper limit was 480 nm. These features enable safe sensing and cell tracking applications with a longer excitation wavelength in the visible light region. The potential applications of the synthesized GQDs as fluorescent sensing probes for detecting Cu（II） ions and non-toxic cell imaging under visible light excitation have been demonstrated. This means that sensing and bioimaging can be accomplished in the natural environment with no need for UV excitation. This work provides a reference to researchers in tailoring CNO structures in terms of their inner space to synthesize GQDs with the desired luminescence behavior.

关键词： graphene quantum dots carbon nano-onions fluorescent quenching bioimaging

graphene quantum dots for tumor optical diagnosis and treatment

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沈阳药科大学学报 2017年第9期34卷 805-816页

作者： ZHANG You-ying LI Quan WANG Wen-cheng ZHANG Qi-hao HUANG Ya-dong SU Zhi-jian XIANG Qi College of Pharmacy Jinan University College of Life Science and Technology Jinan University Institute of Biomedicine and Guangdong Provincial Key Laboratory of Bioengineering Medicine Jinan University

graphene quantum dots(GQDs)are two-dimensional carbon nano-material with excellent physicochemical properties,including biocompatibility,high photoluminescence,water-solubility,hypotoxicity and so *** to bigπ-conjugated structure and oxygen-containing functional groups,GQDs have the ability to absorb various chemical drugs viaπ-πstacking and electrostatic *** the other hand,owning to photoluminescence,GQDs also have potential to serve as fluorescence probe for bioimaging,especially for optical *** addition,GQDs have the ability to generate reactive oxygen species(ROS)including singlet oxygen upon ***,GQDs are likely to be used for photodynamic *** article aims to review the frontier researches about GQDs in the field of fluorescence probe,photodynamic therapy and anti-tumor drug delivery system.

关键词： graphene quantum dots drug delivery system tumor photodynamic therapy

Minimising non-selective defects in ultrathin reduced graphene oxide membranes with graphene quantum dots for enhanced water and NaCl separation

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Chinese Journal of Chemical Engineering 2022年第1期35卷 278-285页

作者： Shi Yuan Yang Li Ruosang Qiu Yun Xia Cordelia Selomulya Xiwang Zhang Department of Chemical Engineering Monash UniversityClaytonVictoria 3800Australia School of Chemical Engineering University of New South WalesNew South Wales 2052Australia

Reduced graphene oxide(rGO)membranes have been intensively evaluated for desalination and ionic sieving applications,benefiting from their stable and well-confined interlayer ***,rGO membranes generally suffer from low permeability due to the high transport resistance resulting from the narrowed two-dimensional(2D)*** high permeability can be realized by reducing membrane thickness,membrane selectivity normally declines because of the formation of nonselective defects,in particular *** this study,we demonstrate that the non-selective defects in ultrathin rGO membranes can be effectively minimised by a facile posttreatment via surfacedeposition of graphene quantum dots(GQDs).The resultant GQDs/rGO membranes obtained a good trade-off between water permeance(14 L·m^(-2)·h^(-1).MPa^(-1))and NaCl rejection(91%).This work provides new insights into the design of high quality ultrathin 2D laminar membranes for desalination,molecular/ionic sieving and other separation applications.

关键词： rGO membranes graphene quantum dots Non-selective defects Water permeance NaCl rejection

Recent Advances on graphene quantum dots for Electrochemical Energy Storage Devices

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Energy & Environmental Materials 2022年第1期5卷 201-214页

作者： Noura Zahir Pierre Magri Wen Luo Jean Jacques Gaumet Philippe Pierrat CNRS L2CM UMR 7053 Universit e de Lorraine LCP-A2MC EA4632 Institut Jean Barriol Universit e de Lorraine State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technologywuhan 430070china

graphene quantum dots(GQDs)which are nanofragments of graphene with an average size between 2 and 50 nm have attracted much attention due to their outstanding properties such as high conductivity,high surface area,and good solubility in various *** combine the quantum confinement and edges effects and the properties of ***,GQDs offers a broad range of applications in various fields(medicine,energy conversion,and energy storage devices).This review will present the recent research based on the introduction of GQDs in batteries,supercapacitors,and microsupercapacitors as electrodes materials or mixed with an active material as an auxiliary ***,discussed on selected examples,summarize the electrochemical performances and finally,challenges and perspectives are recalled for the subsequent optimization strategy of electrode *** review is expected to appeal a broad interest on functional GQDs materials and promote the further development of high-performance energy storage device.

关键词： energy storage graphene quantum dots lithium ion batteries sodium ion batteries supercapacitor

Optimization of electrical performance and stability of fully solution-driven α-InGaZnO thin-film transistors by graphene quantum dots

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Journal of Materials Science & Technology 2023年第10期141卷 100-109页

作者： Xiaofen Xu Gang He Leini Wang Wenhao Wang Shanshan Jiang Zebo Fang School of Materials Science and Engineering Anhui UniversityHefei 230601China School of Integration Circuits Anhui UniversityHefei 230601China School of Mathematical Information Shaoxing UniversityShaoxing 312000China

This work presents solution-processed high-performance graphene quantum dots(GQDs)decorated amor-phous InGaZnO(α-IGZO)thin-film transistors(TFTs)based on ZrO x as gate *** with pure IGZO TFTs,GQDs-modifiedα-IGZO TFTs devices with optimized doping content have demonstrated better performances,including a larger field-effect mobility(μFE)of 35.91 cm 2 V^(-1)s^(-1),a higher on/offcurrent ratio(I ON/I OFF)of 5.04×10^(8),a smaller subthreshold swing(SS)of 0.11 V dec^(-1)and a smaller interfacial trap states(D it,1.57×10^(12)cm^(−2)).Moreover,the GQDs-doped IGZO TFTs with a doping concentration of 0.5 mg ml^(-1)have shown excellent stability under bias stress and illumination stress *** demonstrate the potential applications ofα-IGZO TFTs in logic circuits,a resistor-loaded unipolar inverter based on GQDs-IGZO/ZrO x has been integrated,demonstrating good dynamic behavior and a high gain of ***-frequency noise(LFN)characteristics of GQDs-IGZO/ZrO x TFTs have suggested that the fluctua-tions in mobility are the noise *** on all the experimental findings,it can be concluded that solution-processed GQDs-IGZO/ZrO x TFT may envision promising applications in optoelectronics.

关键词： Thin-film transistor α-InGaZnO graphene quantum dots Stability

Edge-functionalized graphene quantum dots as a thickness-insensitive cathode interlayer for polymer solar cells

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Nano Research 2018年第8期11卷 4293-4301页

作者： Han Xu Lu Zhang Zicheng Ding Junli Hu Jun Liu Yichun Liu Key Laboratory of UV-Emitting Materials and Technology (Northeast Normal University) Ministry of Education Changchun 130024China State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied Chemistry Chinese Academy of SciencesChangchun 130022 China Han Xu and Lu Zhang contributed equally to this work.

A thickness-insensitive cathode interlayer （CIL） is necessary for large-area polymer solar cells （PSCs）, in which thickness variation is unavoidable. These C1L materials are typically based on n-type conjugated polymer/molecule backbones, which show strong light absorption in the visible/near-infrared （NIR） region. This interferes with the sunlight absorption by the active layer and deteriorates device efficiency. In this study, we developed graphene quantum dots functionalized with ammonium iodide （GQD-NI） at the edge as a thickness-insensitive CIL with high optical transparency. The peripheral ammonium iodide groups of GQD-NI formed the desired interfacial dipole with the cathode to decrease the work function. The graphene basal planes of GQD-NI with a lateral size of ca. 3 nm demonstrated a good conductivity of 3.56 ×10-6 ***-1 and high transparency in the visible/NIR region （λmax abs = 228 nm）. Moreover, GQD-NI was readily soluble in polar organic solvents, e.g., methanol, which enabled multilayer device fabrication with orthogonal solvent processing. As a result, the PSC device with GQD-NI as the CIL exhibited a power conversion efficiency （PCE） of 7.49%, which was much higher than that of the device without the CIL （PCE = 5.38%） or with calcium as the CIL （PCE = 6.72%）. Moreover, the PSC device performance of GQD-NI was insensitive to the GQD-NI layer thickness in the range of 2-22 nm. These results indicate that GQD-NI is a very promising material for application as a CIL in large-area printed PSCs.

关键词： graphene quantum dots ammonium edge-functionalization cathode interlayer polymer solar cells

Dual-mode emission of single-layered graphene quantum dots in confined nanospace： Anti-counterfeiting and sensor applications

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Nano Research 2018年第4期11卷 2034-2045页

作者： Liqian Bai Ning Xue Yufei Zhao Xinrui Wang Chao Lu Wenying Shi ing University of Chemical Technology 15 Beisanhuan East Road Beijing 100029 China Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 China Beijing Key Lab of Plant Resource Research and Development Beijing Technology and Business University Beijing 100048 China

Engineering of the luminescent properties for graphene quantum dots （GQDs） presents two enormous challenges： 1） The bandgap of GQDs is mainly determined by structural defects （size, shape, and the fraction of sp2 and sp3 domains）, which results in non-stoichiometric nature; 2） the preparation methods limit the achievement of an accurate chemical structure of GQDs, leading to many controversial explanations over the relationship between the structural defects and bandgaps. Here, single-layered GQDs with an exact structure are obtained by in-situ reaction of intercalated precursors in the confined nanospace of layered double hydroxides （LDHs）. Subsequently, the structure-property relationship is uncovered, demonstrating the enhanced fluorescence and activated room temperature phosphorescence of the as-pre- pared GQDs-LDHs, which originate from synergistic effects： 1） strong confine- ment provided by the nanospace of LDHs; 2） rich O-containing functional groups on the surface of GQDs resulting from LDH catalysis. Moreover, the colorless nature and dual-emission characteristics of GQDs-LDHs satisfy the preconditions as anti-counterfeiting markers for protecting valuable documents （bank notes, commercial invoices, etc.）. Particularly, owing to the low toxicity of GQDs and the edible property of LDHs, the GQDs-LDHs/gelatin capsules could be the new generation of potential green anti-counterfeiting material in the field of food and drugs.

关键词： graphene quantum dots dual-mode emission confinement sensors anti-counterfeiting