炭-/石墨烯量子点在超级电容器中的应用

炭-/石墨烯量子点作为新兴的炭纳米材料,因具有独特的小尺寸效应和丰富的边缘活性位点而在高性能超级电容器电极材料的研发方面展现出巨大潜力。针对目前炭-/石墨烯量子点在超级电容器电极材料方面的应用优势和存在的关键问题,本文以炭-/石墨烯量子点、量子点/导电炭复合材料、量子点/金属氧化物复合材料、量子点/导电聚合物复合材料以及量子点衍生炭这些电极材料为脉络,梳理了近年来该领域的发展状况,尝试阐释炭-/石墨烯量子点在电极材料、复合材料和衍生炭电极材料中所起到的关键作用,最后对炭-/石墨烯量子点电极材料的发展进行了展望。本综述以期为炭-/石墨烯量子点基电极材料的研究提供一定参考和依据。     

基于碳量子点过氧化物模拟酶的肌氨酸比色测定

以果皮为原料制备了水溶性碳量子点(CQDs), 透射电子显微镜分析表明其平均粒径为2.4 nm; 红外光谱分析证实CQDs表面富含含氧官能团. 所得CQDs可催化H₂O₂氧化3,3',5,5'-四甲基联苯胺(TMB)生成蓝色氧化产物(ox-TMB). 基于上述反应, 建立了测定H₂O₂的分析方法, 在pH=3.5, 温度40 ℃, TMB浓度为1.0 mmol/L及孵育时间15 min的条件下, 当H₂O₂浓度在5.0~100 μmol/L范围时, ox-TMB的吸光度随H₂O₂浓度的升高而线 性增强, 方法的检出限为3.0 μmol/L. 鉴于H₂O₂是肌氨酸氧化酶催化肌氨酸氧化的产物之一, 建立了CQDs催化H₂O₂氧化TMB间接测定肌氨酸的分析方法. 结果表明, 当肌氨酸浓度在0.5~350 μmol/L范围内时, 吸光度 与其浓度呈良好的线性关系, 方法的检出限为0.3 μmol/L; 将该方法应用于人体尿样的测定, 回收率为94%~99%.     

基于碳量子点的绿色合成及生物成像研究进展EI北大核心CSCD

碳量子点(CQDs)作为碳纳米材料家族成员之一,因其原材料广、成本低廉、较高的光致发光性能和良好的生物相容性,在研究和应用领域都受到了广泛的关注,是应用于生物成像的理想材料。CQDs的绿色合成是指采用环保型或无毒型原料,通过绿色合成方法,如炭化法、微波法、水热法等,合成具有荧光性能的无毒碳量子点,与传统的化学氧化、激光烧蚀、热解处理等方法相比,更加绿色环保、经济,其应用已成为研究热点。本文对碳量子点材料特性、绿色合成过程机理、绿色合成原料来源、合成方法,及其在癌细胞、微生物细胞等细胞成像方面的应用进行了综述,探讨了绿色合成CQDs的利弊问题,并提出了今后该研究领域面临的机遇与挑战。     

量子点敏化太阳能电池研究进展

量子点敏化太阳能电池(QDSCs)因其制备成本低、工艺简单及量子点(QDs)本身的优异性能(如尺寸效应、多激子效应)等优点,近年来受到广泛关注。在此类电池中,无机半导体量子点敏化剂作为吸光材料,其自身的光电性质、制备方法、表面缺陷、化学稳定性及其在TiO₂光阳极上的敏化方法等是影响电池性能的关键。本文综述了无机半导体量子点敏化剂(包括窄带隙二元量子点、多元合金量子点及Type-Ⅱ核壳量子点)的最新研究进展,重点介绍了胶体量子点的制备方法;分类阐释了量子点在TiO₂光阳极表面的沉积与敏化方法,特别是双官能团辅助自组装吸附法;总结了针对提高电子注入效率和减少复合的量子点表面修饰方法;最后简要介绍了QDSCs的电解质和对电极的研究进展。     

Non-precious metal-based integrated electrodes for overall alkaline water splitting

A bifunctional electrocatalyst interface requires a superior charge transfer and good electric conductivity to produce an efficient and stable water splitting reaction. In the context of controlling the electrochemical activity of bifunctional catalytic materials, we demonstrate a novel approach to bridge conductive C-Qd-Mn interfaces with precise control. The excellent performance for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) can be dominantly attributed to the unique structure of C-Qds-Mn, which provides abundant active sites and facilitates electron transfer between electrode and electrolyte. Eco-friendly C-Qds were synthesized using a large-scale thermal assisted technique and utilized as electrocatalysts with Mn₃O₄ in alkaline splitting ToF (Turn over Frequency) calculation to make an effective combination. Due to their increased ECSA, conductivity, and electron-hole transfer, the prepared C-Qds-Mn delivered excellent HER/OER (0.494 V/1.6671V) activity, lower Standard deviation 0.006 V and 0.009V, surpassing the 10 mA limit comparable to commercially.     

Amiloride-modulated phosphorescence turn-off/on method for the detection of abasic site-containing dsRNA based on uridine triphosphate-capped Mn-doped ZnS quantum dots

RNA plays a crucial role in biochemical processes. RNAs with abasic sites (AP-RNA), as one of RNA lesions, will cause serious negative consequences. Efficient and sensitive detection of AP-RNA deserves but does not receive enough attention. Water-soluble uridine triphosphate (UTP)-capped Mn-doped ZnS quantum dots (QDs), which have excellent room-temperature phosphorescence (RTP) properties, were prepared by wet-chemical method. The UTP on the surface of QDs could form a precipitation complex with amiloride (AMI) to quench the RTP. Meanwhile, abasic double-stranded RNA (AP-dsRNA) with a high affinity to AMI could dissociate AMI from the surface of UTP-QDs, resulting in RTP recovery. In this process, a highly sensitive and selective RTP-detection system for AP-dsRNA was constructed with AMI as the modulation factor and UTP-QDs as the luminescence matrix. RTP was turned off and on for the determination of AP-dsRNA, and the interference of background fluorescence and scattered light was effectively avoided during complex formation and aggregation. Steric hindrance of the conformation of AP-dsRNA provided efficient selectivity. The detection limit for AP-dsRNA was 0.86 nM, the relative standard deviation was 2.1%, and the recovery of biological samples with AP-dsRNA addition ranged from 95% to 103% at optimal conditions. The system is expected to provide new methods for environmental monitoring, early disease screening, and evaluation of gene editing efficiency.     

Synthesis of Carbon Quantum Dots Nanoparticles by Cyclic Voltammetry and Its Application as Methanol Tolerant Oxygen Reduction Reaction Electrocatalyst

Carbon quantum dot (CQD) nanoparticles are synthesized by one‐step electrochemical method, cyclic voltammetry (CV), at different potentials using graphite rods and NaOH/EtOH as electrolyte. The electro‐chemically manufactured CQD is characterized by Transmission electron microscopy, Ultra violet absorption, X‐ray diffraction and Fourier transform infrared spectrometry. The morphology and microstructure methods confirm the formation of high quality CQD. Finally, we design a new gas diffusion electrode (GDE) based on CQD pasted on carbon paper for the oxygen reduction reaction at cathode side as methanol tolerance in direct methanol fuel cell and compared it with standard Pt‐C catalysts using cyclic voltammetry and linear sweep voltammetry. The ORR results in presence of methanol indicate that the GDE prepared from CQD exhibits methanol tolerance compared to the GDE prepared from Pt/C (Electrochem).     

CulnS2量子点敏化太阳能电池中尺寸依赖的电子注入和光电性质

研究了CulnS2(CIS)量子点敏化太阳能电池(QDSSCs)的电子注入和器件性能与粒子尺寸之间的依赖关系.首先合成了不同尺寸的CulnS2量子点(QDs),制备了CulnS2量子点敏化的TiO2薄膜,并组装了量子点敏化太阳能电池.通过循环伏安法确定了CulnS2量子点的能级位置.采用时间分辨荧光光谱分析测量了CulnS2量子点到TiO2薄膜的电子转移速率和效率.结果发现,随着粒子尺寸从4.0 nm减小到2.5nm,电子注入速率略微增加而电子注入效率减小,同时量子点敏化太阳能电池的开路电压基本不变,而光电转换效率、短路电流和填充因子(FF)均减小.上述研究结果表明量子点敏化太阳能电池性能的优化可以通过改变量子点的尺寸来实现.     

制备条件对PEI功能化石墨烯量子点荧光性能的影响

石墨烯量子点凭借其良好的水溶性、低生物毒性等特点,被不断尝试应用于生物成像领域,但其有限的荧光性能限制了其进一步应用。为改善石墨烯量子点的荧光性能以及进一步揭示石墨烯量子点的制备机理,本文对聚乙烯亚胺(PEI)功能化石墨烯量子点的制备条件进行了探索,讨论了不同反应时间、制备温度以及混悬液pH值对其荧光性能的影响。测试结果显示,当混悬液pH值为12时,在反应釜中经过200 ℃高温反应20 h,所制备的功能化石墨烯量子点能取得良好的紫外吸收峰和荧光性能,同时达到较高的量子产量。     

通过S2-中间态将CdSe量子点有机配体转化为ZnS保护层及其器件光伏特性

通过S2-中间态将有机配体三辛基氧膦(TOPO)转化为ZnS保护层,显著改善了CdSe量子点(QDs)器件的转换效率.配体交换后的傅里叶变换红外(FTIR)光谱结果表明,有机配体已被S2-离子配体取代;离子反应后的X射线光电子能谱(XPS)结果表明S2-离子配体反应生成了ZnS,紫外-可见(UV-Vis)吸收光谱结果表明量子点溶液吸收峰位没有发生明显改变,透射电子显微镜(TEM)结果表明配体交换后量子点粒径减小.电化学阻抗谱(EIS)结果表明光照条件下有机配体转化为ZnS保护层后TiO2/QDs/电解质界面电阻减少,证明该条件下正向电子传输增强;强度调制光电压谱(IMVS)和强度调制光电流谱(IMPS)结果表明电子寿命和扩散速度增加.相比于有机配体,形成ZnS保护层后的量子点敏化太阳能电池(QDSC)效率由0.98%提高到1.75%,相对提高了1.78倍.     

CuInS_2量子点敏化太阳能电池中尺寸依赖的电子注入和光电性质

研究了CuInS2(CIS)量子点敏化太阳能电池(QDSSCs)的电子注入和器件性能与粒子尺寸之间的依赖关系.首先合成了不同尺寸的CuInS2量子点(QDs),制备了CuInS2量子点敏化的TiO2薄膜,并组装了量子点敏化太阳能电池.通过循环伏安法确定了CuInS2量子点的能级位置.采用时间分辨荧光光谱分析测量了CuInS2量子点到TiO2薄膜的电子转移速率和效率.结果发现,随着粒子尺寸从4.0 nm减小到2.5 nm,电子注入速率略微增加而电子注入效率减小,同时量子点敏化太阳能电池的开路电压基本不变,而光电转换效率、短路电流和填充因子(FF)均减小.上述研究结果表明量子点敏化太阳能电池性能的优化可以通过改变量子点的尺寸来实现.     

A convenient synthesis of cadmium chalcogenide quantum dots from cadmium acetate and bis(diphenylphosphino)methane monosulfide and –selenide or 1,4-bis(diphenylphosphino)butane monoselenide

The synthesis of both cadmium selenide and cadmium sulfide quantum dots has been effected using a synthetic protocol that avoids the use of volatile, toxic organocadmium reagents and alkyl phosphines.     

Enhanced visible-light-driven photocatalytic activities of 0D/1D heterojunction carbon quantum dot modified CdS nanowires

Zero-dimensional carbon dots (0D C-dots) and one-dimensional sulfide cadmium nanowires (1D CdS NWs) were prepared by microwave and solvothermal methods, respectively. A series of heterogeneous photocatalysts that consisted of 1D CdS NWs that were modified with 0D C-dots (C-dots/CdS NWs) were synthesized using chemical deposition methods. The mass fraction of C-dots to CdS NWs in these photocatalysts was varied. The photocatalysts were characterized using X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and ultraviolet-visible spectroscopy. Their photocatalytic performance for the spitting of water and the degradation of rhodamine B (RhB) under visible light irradiation were investigated. The photocatalytic performance of the C-dots/CdS NWs was enhanced when compared with that of the pure CdS NWs, with the 0.4% C-dots/CdS NWs exhibiting the highest photocatalytic activity for the splitting of water and the degradation of RhB. The enhanced photocatalytic activity was attributed to a higher carrier density because of the heterojunction between the C-dots and CdS NWs. This heterojunction improved the electronic transmission capacity and promoted efficient separation of photogenerated electrons and holes.     

Detection of proteins cross-linked within galactoside polyacrylate-based hydrogels by means of a quantum dot fluororeagent

Protein toxins have been immobilized in a galactoside polyacrylate hydrogel in a microarray format. The large pore size and solution-like environment of these novel hydrogels allow for easy penetration of large proteins and detection reagents. Confocal microscopy provided three-dimensional visualization of dye-labeled toxins cross-linked within the gel and of streptavidin-coated quantum dot (QD) fluorophores used to visualize the toxins after incubation with biotinylated anti-toxin antibodies. Fluorescence microscopy was utilized to visualize arrays of toxins detected by a biotinylated antibody and then exposure to streptavidin-conjugated QDs. The intensity of the QD fluorescence was quantified, and binding to two toxins on three types of hydrogels was examined.     

一种新型铜离子荧光探针——CdTe量子点

探讨了髙量子产率CdTe量子点作为铜离子探针的可能性,发现铜离子对碲化镉量子点的荧光有猝灭效应,且量子点溶液的荧光强度与铜离子浓度成良好的负相关线性关系.由于CdTe量子点比CdS具有更为优良的光学性质和稳定性,有望成为一种新型纳米离子探针.     

Zn_xCd_(1-x)S量子点组成与其光催化活性的关系（英文）

Aqueous colloidal dispersions containing Znx Cd1‐x S quantum dots (QDs) of different x compositions were prepared by precipitating zinc and cadmium acetates with sodium sulphide,in the presence of a cetyltrimethylammonium bromide stabilizer.Ultraviolet‐visible absorption spectroscopy was used to determine the transition energies of the QDs,which in turn were used to calculate their sizes,which depended on their composition.The QD size decreased with increasing Zn content.The photocatalytic activity of the Znx Cd1‐x S QDs was studied by the decomposition of methylene blue under ultraviolet irradiation,at a maximum intensity at 365 nm (3.4 e V).Three different photo‐catalytic activity regions were observed,which depended on the Zn content.The quantum levels of the QDs could be excited by incident irradiation,and influenced the resulting photocatalytic activity.Maximum photocatalytic activity was achieved at x = 0.6,where the QD transition energy was equal to the irradiation photon energy.The photocatalytic efficiency of the QDs depended on their surface area and arrangement of quantum levels,because of the quantum size effect.     

Dependence of photocatalytic activity of ZnxCd1-xS quantum dot composition

Aqueous colloidal dispersions containing ZnxCd1‐xS quantum dots (QDs) of different x compositions were prepared by precipitating zinc and cadmium acetates with sodium sulphide, in the presence of a cet...