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AgInS_(2)量子点调控及其在WLED应用上的研究进展
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作者 刘汉语 谢志翔 +5 位作者 陈婷 董延茂 周兴 袁妍 吴海涛 陈勇号 《功能材料》 CAS CSCD 北大核心 2024年第2期2041-2051,2104,共12页
AgInS_(2)量子点是一种有趣的材料,其近红外带隙范围从1.87到1.98 eV,作为直接带隙半导体,它能通过调节Ag/In比例来调节带隙,它还具有较宽的PL峰和较大的Stokes位移,同时低毒环保的特性也使它成为有望替代含Cd、Hg和Pb等重金属元素的二... AgInS_(2)量子点是一种有趣的材料,其近红外带隙范围从1.87到1.98 eV,作为直接带隙半导体,它能通过调节Ag/In比例来调节带隙,它还具有较宽的PL峰和较大的Stokes位移,同时低毒环保的特性也使它成为有望替代含Cd、Hg和Pb等重金属元素的二元量子点的理想材料,在光电器件领域尤其在发光二极管中有着广泛的应用前景。本文详细阐述了AgInS_(2)量子点晶体结构和发光机制,总结了其合成方法的特点并综述了通过壳体工程和掺杂的方法对AgInS_(2)量子点进行调控的策略,最后介绍了该类量子点在发光二极管方面的应用进展。 展开更多
关键词 agins_(2) 量子点 合成 优化 WLED
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N-doped graphene quantum dot-decorated N-TiO2/P-doped porous hollow g-C_(3)N_(4) nanotube composite photocatalysts for antibiotic photodegradation and H2 production 被引量:1
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作者 Jingshu Yuan Yao Zhang +2 位作者 Xiaoyan Zhang Junjie Zhang Shen’gen Zhang 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CSCD 2024年第1期165-178,共14页
Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r... Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion. 展开更多
关键词 N-doped TiO_(2) N-doped graphene quantum dots P-doped g-C_(3)N_(4) porous hollow nanotube heterojunction photocatalysis
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Highly enhanced UV absorption and light emission of monolayer WS_(2)through hybridization with Ti_(2)N MXene quantum dots and g-C_(3)N_(4)quantum dots
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作者 Anir S.Sharbirin Rebekah E.Kong +5 位作者 Wendy B.Mato Trang Thu Tran Eunji Lee Jolene W.P.Khor Afrizal L.Fadli Jeongyong Kim 《Opto-Electronic Advances》 SCIE EI CAS CSCD 2024年第6期31-39,共9页
Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and t... Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD. 展开更多
关键词 monolayer TMD WS_(2) 2D-derived quantum dots UV absorption energy transfer
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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction
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作者 Kangwang Wang Zhuofeng Hu +8 位作者 Peifeng Yu Alina M.Balu Kuan Li Longfu Li Lingyong Zeng Chao Zhang Rafael Luque Kai Yan Huixia Luo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期68-84,共17页
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in... We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR. 展开更多
关键词 quantum efficiency Electronic structure Steric interaction Bridging sites CO_(2)reduction
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Small but mighty:Empowering sodium/potassium-ion battery performance with S-doped SnO_(2) quantum dots embedded in N,S codoped carbon fiber network
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作者 Shengnan He Hui Wu +4 位作者 Shuang Li Ke Liu Yaxiong Yang Hongge Pan Xuebin Yu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第5期186-200,共15页
SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish ... SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices. 展开更多
关键词 carbon fiber network heteroatom doping potassium-ion battery sodium-ion battery S-SnO_(2)quantum dot
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Platinum quantum dots-decorated MXene-derived titanium dioxide nanowire/Ti_(3)C_(2) heterostructure for use in solar-driven gas-phase carbon dioxide reduction to yield value-added fuels 被引量:1
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作者 Kamakshaiah Charyulu Devarayapalli S.V.Prabhakar Vattikuti +4 位作者 Dong Jin Kim Youngsu Lim Bolam Kim Gyuhyeon Kim Dae Sung Lee 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第7期627-637,I0013,共12页
Solar-driven photocatalytic CO_(2) reduction to produce valuable chemicals and fuels offers an attractive strategy in alleviating the energy crisis.Pt quantum dots(PtQDs)with TiO_(2) nanowire(TiO_(2)NW)/Ti_(3)C_(2) MX... Solar-driven photocatalytic CO_(2) reduction to produce valuable chemicals and fuels offers an attractive strategy in alleviating the energy crisis.Pt quantum dots(PtQDs)with TiO_(2) nanowire(TiO_(2)NW)/Ti_(3)C_(2) MXene heterostructures(Pt-TiO_(2)NW/Ti_(3)C_(2)) with tight interfacial contacts between the various components were prepared at room temperature via oxidation reactions.The incorporated PtQDs played crucial roles as electron conduction bridges supported by the cocatalyst effect,effectively enhancing the separation efficiencies of photoinduced electron/hole pairs and improving CO_(2) reduction under simulated solar light irradiation.The Pt-TiO_(2)NW/Ti_(3)C_(2) heterostructures exhibited remarkable carbon monoxide(CO)and methane(CH_(4)) production at respective rates of 38.14 and 36.15μmol g^(-1)after 10 h of simulated solar light irradiation,an apparent quantum yield of 1.68%,and 79.2%selectivity for CH4.The photocatalytic activities of the Pt-TiO_(2) NW/Ti_(3)C_(2) heterostructures for CO_(2) reduction were significantly enhanced compared to those of TiO_(2)NW/Ti_(3)C_(2) and the single-component photocatalysts,and they exhibited remarkable stabilities even after five cycles.In addition,the densities of states and electronic characteristics of Ti_(3)C_(2) MXene and Pt-TiO_(2)NW/Ti_(3)C_(2) were studied using density functional theory,and a synergistic mechanism of the improvement in CO_(2) photoreduction is proposed. 展开更多
关键词 MXene CO_(2)reduction Density functional theory quantum dot PHOTOCATALYST
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基于N掺杂Ti_(3)C_(2)MXene量子点的荧光探针用于Hg2+和S2-的传感检测
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作者 张慧莲 杨新杰 +6 位作者 李军 李泉 张福娟 张艳丽 王红斌 杨文荣 庞鹏飞 《高等学校化学学报》 SCIE EI CAS CSCD 北大核心 2024年第5期38-45,共8页
基于N掺杂Ti_(3)C_(2) MXene量子点(N-Ti_(3)C_(2) MQDs)荧光探针和配位相互作用,构建了一种检测Hg^(2+)和S^(2-)的“开-关-开”型荧光传感新方法.研究发现,制备的N-Ti_(3)C_(2) MQDs发射蓝色荧光(λem=440 nm),荧光量子产率为15.7%.Hg^... 基于N掺杂Ti_(3)C_(2) MXene量子点(N-Ti_(3)C_(2) MQDs)荧光探针和配位相互作用,构建了一种检测Hg^(2+)和S^(2-)的“开-关-开”型荧光传感新方法.研究发现,制备的N-Ti_(3)C_(2) MQDs发射蓝色荧光(λem=440 nm),荧光量子产率为15.7%.Hg^(2+)与N-Ti_(3)C_(2) MQDs表面的—NH2,—COOH,—OH等官能团产生选择性配位作用,导致N-Ti_(3)C_(2) MQDs体系荧光猝灭.当加入S^(2-)后,由于S^(2-)与Hg^(2+)之间强的结合力,形成HgS沉淀,从而使N-Ti_(3)C_(2) MQDs体系荧光恢复.基于该原理,构建了一种“开-关-开”型荧光传感方法,实现了对Hg^(2+)和S^(2-)的定量检测.N-Ti_(3)C_(2) MQDs探针的荧光强度与Hg^(2+)浓度在0.02~200μmol/L范围内呈良好线性关系,检出限为10 nmol/L(S/N=3);与S^(2-)浓度在0.07~150μmol/L范围内呈良好线性关系,检出限为30 nmol/L(S/N=3).该方法具有成本低、操作简单、灵敏度高和选择性好等特点,并可用于水样中Hg^(2+)和S^(2-)的检测. 展开更多
关键词 汞离子 硫离子 N掺杂Ti_(3)C_(2)MXene 量子点 荧光探针
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Pb^(2+)对掺杂硼硅酸盐玻璃中CsPbBr_(3)钙钛矿量子点发光性能的影响
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作者 岳仔豪 杨小兔 +3 位作者 张正亮 邓瑞翔 张涛 宋力昕 《无机材料学报》 SCIE EI CAS CSCD 北大核心 2024年第4期449-456,共8页
硼硅酸盐玻璃包覆钙钛矿CsPbBr_(3)量子点(PQDs@glass)能够大幅提高PQDs的稳定性,使其在LED照明和显示技术中拥有广泛的应用空间。然而,玻璃包覆的同时也导致了PQDs发光强度与量子产率降低。本工作为提高其发光强度探讨了热诱导温度及Pb... 硼硅酸盐玻璃包覆钙钛矿CsPbBr_(3)量子点(PQDs@glass)能够大幅提高PQDs的稳定性,使其在LED照明和显示技术中拥有广泛的应用空间。然而,玻璃包覆的同时也导致了PQDs发光强度与量子产率降低。本工作为提高其发光强度探讨了热诱导温度及Pb^(2+)的含量对PQDs@glass结构的影响,当热诱导温度为460℃,Pb^(2+)浓度为6 mol时,其发光强度最高。研究发现,Pb^(2+)浓度的增加会导致玻璃网状结构的致密化,改变玻璃组分的扩散行为,影响PQDs的析晶过程,导致PQDs@glass发光强度的变化。本工作得到量子产率高达95.6%的PQDs@glass,并实现了硼硅酸盐玻璃基质内PQDs的尺寸可控制备。结果表明,PQDs尺寸分布在10 nm左右,超过86%的颗粒尺寸在6~14 nm内,且具有优越的稳定性,经历10次室温至200℃热循环后,发光强度仍能保持初始强度的98.9%。最后,为了验证其在LED照明及显示领域的应用,将制备的量子点微晶玻璃粉料与二甲基硅氧烷(PDMS)混合,得到的LED器件性能优异,色域范围覆盖110%sRGB。本研究为PQDs@glass的大规模制备及其在LED器件领域的应用奠定了基础。 展开更多
关键词 CsPbBr_(3) Pb^(2+) LED 量子点 硼硅酸盐玻璃
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Na_(2)CO_(3)-K_(2)CO_(3)-NaVO_(3)熔盐结构的拉曼光谱和理论计算
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作者 张一帆 胡宪伟 +1 位作者 于江玉 王兆文 《东北大学学报(自然科学版)》 EI CAS CSCD 北大核心 2024年第3期331-336,共6页
NaVO_(3)在Na_(2)CO_(3)-K_(2)CO_(3)熔盐体系中可原位催化电还原CO_(2)制备高附加值碳材料,对Na_(2)CO_(3)-K_(2)CO_(3)-NaVO_(3)体系熔盐结构进行研究有助于明晰电极过程机理和优化反应条件.本文采用拉曼光谱学和量子化学计算(基于Gau... NaVO_(3)在Na_(2)CO_(3)-K_(2)CO_(3)熔盐体系中可原位催化电还原CO_(2)制备高附加值碳材料,对Na_(2)CO_(3)-K_(2)CO_(3)-NaVO_(3)体系熔盐结构进行研究有助于明晰电极过程机理和优化反应条件.本文采用拉曼光谱学和量子化学计算(基于Gaussian和Molclus程序)相结合的方法探究了1073 K下Na_(2)CO_(3)-K_(2)CO_(3)-NaVO_(3)熔盐体系的离子结构.结果表明,在该熔盐体系中,除了存在CO_(3)^(2-)以外,还存在由CO_(3)^(2-)和VO_(3)^(-)发生反应生成的VO_(4)^(3-),而不存在VO_(3)^(-);VO_(4)^(3-)所属C1空间点群,其中V-O键的对称伸缩振动模对应的拉曼特征峰位于802 cm^(-1)处;随着体系中NaVO_(3)质量分数由5%增加至15%,熔盐中VO_(4)^(3-)的相对含量急剧增加,而CO_(3)^(2-)的相对含量相应地减少. 展开更多
关键词 NaVO_(3) Na_(2)CO_(3)-K_(2)CO_(3)熔盐 拉曼光谱 量子化学计算 VO_(4)^(3-)
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Pressure induced insulator to metal transition in quantum spin liquid candidate NaYbS_(2)
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作者 贾雅婷 龚春生 +6 位作者 李芷文 刘以轩 赵建发 王哲 雷和畅 于润泽 靳常青 《Chinese Physics B》 SCIE EI CAS CSCD 2023年第9期369-372,共4页
Pressure induced insulator to metal transition followed by the appearance of superconductivity has been observed recently in inorganic quantum spin liquid candidate NaYbSe_(2).In this paper,we study the properties of ... Pressure induced insulator to metal transition followed by the appearance of superconductivity has been observed recently in inorganic quantum spin liquid candidate NaYbSe_(2).In this paper,we study the properties of isostructural compound NaYbS_(2)under pressure.It is found that the resistance of Na YbS_(2)single crystal exhibits an insulating state below 82.9 GPa,but with a drop of more than six orders of magnitude at room temperature.Then a minimum of resistance is observed at about 100.1 GPa and it moves to lower temperature with further compression.Finally,a metallic state in the whole temperature range is observed at about 130.3 GPa accompanied by a non-Fermi liquid behavior below 100 K.The insulator to metal transition,non-monotonic resistance feature and non-Fermi liquid behavior of NaYbS_(2)under pressure are similar to those of NaYbSe_(2),suggesting that these phenomena might be the universal properties in NaLnCh_(2)(Ln=rare earth,Ch=O,S,Se)system. 展开更多
关键词 high pressure quantum spin liquid insulator to metal transition NaYbS_(2)
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Activated dissociation of H_(2) on the Cu(001)surface:The role of quantum tunneling
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作者 于小凡 童洋武 杨勇 《Chinese Physics B》 SCIE EI CAS CSCD 2023年第10期151-162,共12页
The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determi... The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determined to be~0.59 eV in height.It is found that the electron transfer from the copper substrate to H_(2) plays a key role in the activation and breaking of the H–H bond,and the formation of the Cu–H bonds.Two stationary states are identified at around the critical height of bond breaking,corresponding to the molecular and the dissociative states,respectively.Using the transfer matrix method,we also investigate the role of quantum tunneling in the dissociation process along the minimum energy pathway(MEP),which is found to be significant at or below room temperature.At a given temperature,the tunneling contributions due to the translational and the vibrational motions of H_(2) are quantified for the dissociation process.Within a wide range of temperature,the effects of quantum tunneling on the effective barriers of dissociation and the rate constants are observed.The deduced energetic parameters associated with the thermal equilibrium and non-equilibrium(molecular beam)conditions are comparable to experimental data.In the low-temperature region,the crossover from classical to quantum regime is identified. 展开更多
关键词 H_(2) CU(001) DISSOCIATION quantum tunneling density functional theory(DFT) transfer matrix method
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Bi_(2)O_(2)Se纳米线的生长及其超导量子干涉器件
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作者 刘怀远 肖建飞 +2 位作者 吕昭征 吕力 屈凡明 《物理学报》 SCIE EI CAS CSCD 北大核心 2024年第4期285-290,共6页
Bi_(2)O_(2)Se是一种新型半导体材料,具有载流子迁移率高、空气中稳定和自旋轨道耦合强等优点,并且其合成方法多种多样,应用范围十分广泛.但已有研究大多集中在其二维薄膜,本文介绍一种使用三温区管式炉通过化学气相沉积生长Bi_(2)O_(2... Bi_(2)O_(2)Se是一种新型半导体材料,具有载流子迁移率高、空气中稳定和自旋轨道耦合强等优点,并且其合成方法多种多样,应用范围十分广泛.但已有研究大多集中在其二维薄膜,本文介绍一种使用三温区管式炉通过化学气相沉积生长Bi_(2)O_(2)Se一维纳米线的方法,研究了云母衬底处于水平方向不同位置以及竖直方向不同高度对Bi_(2)O_(2)Se纳米线生长的影响,并归纳出适于其生长的优化条件.之后,基于生长的Bi_(2)O_(2)Se纳米线构建了超导量子干涉器件,并观测到随磁场的超导量子干涉,为拓宽Bi_(2)O_(2)Se纳米线的应用提供了思路. 展开更多
关键词 Bi_(2)O_(2)Se纳米线 化学气相沉积 超导量子干涉器
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电荷迁移方向调控的BiVO_(4)量子点/苝四羧酸Z型异质结与纳米金修饰在人工光合成H_(2)O_(2)中的协同作用
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作者 梁腾 李雨彤 +5 位作者 徐帅 姚宇欣 许荣萍 边辑 张紫晴 井立强 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第7期277-286,共10页
利用太阳能驱动的半导体光催化技术将H_(2)O和O_(2)转化为H_(2)O_(2),是传统蒽醌工艺的可持续替代方案之一.在光催化O_(2)还原生产H_(2)O_(2)的过程中,主要涉及到O_(2)的还原和H_(2)O的氧化两个半反应.然而,单一的窄带隙半导体往往难以... 利用太阳能驱动的半导体光催化技术将H_(2)O和O_(2)转化为H_(2)O_(2),是传统蒽醌工艺的可持续替代方案之一.在光催化O_(2)还原生产H_(2)O_(2)的过程中,主要涉及到O_(2)的还原和H_(2)O的氧化两个半反应.然而,单一的窄带隙半导体往往难以满足整体反应的热力学电位要求.为了克服这一挑战,研究人员借鉴自然光合作用的原理,提出了构建Z型异质结体系的策略.这种体系不仅能有效促进电荷的分离,从而增强光催化效率,而且能保留光生电荷较强的氧化还原能力,这对于H_(2)O_(2)的光合成至关重要.此外,O_(2)的活化对于H_(2)O_(2)光合成同样重要.然而,目前在构建Z型异质结时,对于Z型异质结的两组分自身电荷传输方向的匹配性鲜有关注.因此,构建具有电荷定向传输的Z型异质结,并精准负载O_(2)活化位点,对于提高H_(2)O_(2)的光合成效率和稳定性具有重要意义.本文以苝-3,4,9,10-四羧酸二酐(PTCDA)为前驱体,在水解的过程中,引入预制备的钒酸铋量子点(BQD),原位构建BQD/PTA Z型异质结.然后,通过低温辅助光还原策略将纳米Au精确修饰在苝四甲酸(PTA)上,制得具有定向电荷传输的BQD/PTA-Au Z型异质结.形貌表征结果表明,PTA的形态为平均厚度为3.5 nm的不规则纳米片,其表面均匀负载了直径约为7 nm的BQD纳米颗粒,而超小的Au纳米粒子(直径约为5 nm)则负载在PTA纳米片的边缘.优化后的BQD/PTA-Au异质结光催化H_(2)O_(2)产率为218.6μmol g^(-1)h^(-1),约为PTA纳米片的6.4倍;此外,在405 nm波长下,该异质结的表观量子产率为PTA的4.8倍.在模拟太阳光条件下,BQD/PTA-Au异质结的太阳能到化学能转换效率(SCC)为0.47%;且在连续5次的循环实验中表现出良好的稳定性.光物理和光化学测试结果表明,BQD/PTA Z型异质结的构建显著促进了PTA的电荷分离,Au修饰后复合体的电荷分离进一步增强.扫描开尔文探针(SKP)测试结果表明,BQD和PTA的能带结构满足Z型电荷传输路径,电子顺磁共振和原位X射线光电子能谱分析结果表明,所构建的Z型异质结由于电荷传输方向匹配,显著促进·O_(2)-自由基的形成;而后续的Au修饰则能够定向接受来自PTA的光生电子.旋转圆盘电极测试结果表明,BQD/PTA-Au的平均电子转移数最接近2,说明其遵循两电子氧还原反应(ORR)路径.结合物种捕获实验推测,·O_(2)-自由基是BQD/PTA-Au异质结光合成H_(2)O_(2)的主要活性物种.原位漫反射红外光谱测试证实,纳米Au修饰可进一步提高O_(2)在催化剂表面吸附,并加速两电子的O_(2)还原反应.综上,本文围绕着具有各向异性电荷迁移的PTA,设计构建了电荷定向迁移的Z型异质结体系,实现了高效的H_(2)O_(2)光合成,为高效Z型异质结体系设计构建提供了新思路. 展开更多
关键词 Z型异质结 苝四甲酸 BiVO_(4)量子点 H_(2)O_(2)光合成 氧还原
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1,3-二甲基咪唑-2-羧酸盐辅助制备SnO_(2)量子点及其对乙醇的气敏性
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作者 刘松涛 郑贤军 +3 位作者 杨凯 孙仲明 方晨羽 侯海云 《西安工程大学学报》 CAS 2024年第4期56-64,共9页
为了制备气体灵敏度良好的SnO_(2)量子点,以聚乙二醇200(PEG200)为分散剂,采用咪唑基离子液体前驱体1,3-二甲基咪唑-2-羧酸盐辅助制备粒径约为4 nm、气敏性良好的SnO_(2)量子点。利用X射线衍射仪、高分辨率透射电镜对SnO_(2)量子点的物... 为了制备气体灵敏度良好的SnO_(2)量子点,以聚乙二醇200(PEG200)为分散剂,采用咪唑基离子液体前驱体1,3-二甲基咪唑-2-羧酸盐辅助制备粒径约为4 nm、气敏性良好的SnO_(2)量子点。利用X射线衍射仪、高分辨率透射电镜对SnO_(2)量子点的物相结构和微观形貌样品进行表征,通过傅里叶变换红外光谱仪、紫外-可见分光光度计和比表面积分析仪测试SnO_(2)量子点的纯度、光学性质和比表面积,并采用气敏测试系统检测SnO_(2)量子点对乙醇气体的灵敏度。结果显示:制备的SnO_(2)量子点颗粒大小均匀,比表面积为123.89 m^(2)/g,对可见光透过率达90%以上,乙醇气敏性能优良;在250℃,乙醇体积分数为300×10^(-6)时,SnO_(2)量子点的灵敏度可达195.34。 展开更多
关键词 SnO_(2)量子点 1 3-二甲基咪唑-2-羧酸盐 光学性质 气敏性能
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天冬氨酸和谷氨酸及其甘氨酸二肽调控Caco-2细胞钙离子吸收的研究
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作者 刘佳琛 李奕 +1 位作者 程永强 唐宁 《食品工业科技》 CAS 北大核心 2024年第14期97-105,共9页
为了探究天冬氨酸和谷氨酸及其甘氨酸二肽对钙离子吸收的影响机理,本文利用等温滴定量热技术、电化学、Caco-2细胞模型结合量子化学计算(密度泛函理论)对天冬氨酸和谷氨酸及其甘氨酸二肽与钙离子的相互作用进行了探究。结果表明,天冬氨... 为了探究天冬氨酸和谷氨酸及其甘氨酸二肽对钙离子吸收的影响机理,本文利用等温滴定量热技术、电化学、Caco-2细胞模型结合量子化学计算(密度泛函理论)对天冬氨酸和谷氨酸及其甘氨酸二肽与钙离子的相互作用进行了探究。结果表明,天冬氨酸和谷氨酸通过焓和熵驱动的放热反应与钙离子形成复合物,而其形成的二肽则是通过熵驱动的吸热反应与钙离子结合。此外,二肽比单独的氨基酸表现出更强的钙离子结合能力。量子化学计算表明,氨基酸/二肽中的羧基为钙离子的主要结合位点,在碱性条件下,会导致钙离子结合位点转移,氨基也可以参与钙离子结合。Caco-2细胞吸收实验表明,天冬氨酸和谷氨酸及其二肽均可促进钙的吸收,其中甘氨酸-谷氨酸二肽(Gly-Glu)的促进效果最好,促钙吸收率为1.33±0.115。此外,促钙吸收能力与钙离子结合能力之间没有明确的相关性,与其电子亲和力的关系更为密切。研究结果解释了天冬氨酸、谷氨酸及其甘氨酸二肽与钙之间的相互作用,为进一步开发钙补充剂提供科学依据。 展开更多
关键词 天冬氨酸 谷氨酸 甘氨酸 CACO-2 细胞模型 钙吸收 量子化学计算
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氮掺杂Ti_(3)C_(2)MXene量子点荧光探针用于α-葡萄糖苷酶活性检测
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作者 李军 杨新杰 +6 位作者 罗焰 李泉 宗玉红 张艳丽 王红斌 杨文荣 庞鹏飞 《分析测试学报》 CAS CSCD 北大核心 2024年第5期674-681,共8页
α-葡萄糖苷酶是生物体糖代谢途径中不可或缺的一类酶,发展简单、灵敏、准确的α-葡萄糖苷酶活性检测及抑制剂筛选方法对于糖尿病的治疗与预防具有重要意义。该文基于氮掺杂Ti_(3)C_(2)MXene量子点(NTi_(3)C_(2)MQDs)荧光探针和内滤效应... α-葡萄糖苷酶是生物体糖代谢途径中不可或缺的一类酶,发展简单、灵敏、准确的α-葡萄糖苷酶活性检测及抑制剂筛选方法对于糖尿病的治疗与预防具有重要意义。该文基于氮掺杂Ti_(3)C_(2)MXene量子点(NTi_(3)C_(2)MQDs)荧光探针和内滤效应(IFE),构建了一种“开-关-开”型荧光传感α-葡萄糖苷酶活性检测及抑制剂筛选的新方法。研究发现,N-Ti_(3)C_(2)MQDs发射蓝色荧光(λem=440 nm),荧光量子产率为15.7%。其检测机理为:α-葡萄糖苷酶水解底物对硝基苯基-α-D-吡喃葡萄糖苷,水解产物对硝基苯酚通过内滤效应导致NTi_(3)C_(2)MQDs荧光猝灭;而抑制剂阿卡波糖可使α-葡萄糖苷酶的活性受到抑制,水解产物减少,N-Ti_(3)C_(2)MQDs荧光恢复。结果显示,N-Ti3C2 MQDs探针荧光强度与α-葡萄糖苷酶浓度在5~300 U/L范围内呈良好线性关系,检出限为2.5 U/L(S/N=3),对阿卡波糖的半最大抑制浓度(IC_(50))为178.5μmol/L。该方法具有成本低、操作简单、灵敏度高、选择性好等特点,已成功用于人血清中α-葡萄糖苷酶活性的测定。 展开更多
关键词 Α-葡萄糖苷酶 氮掺杂Ti_(3)C_(2)MXene 量子点 荧光探针
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Experimental and computational study of annealed nickel sulfide quantum dots for catalytic and antibacterial activity
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作者 Muhammad Ikram Sawaira Moeen +5 位作者 Ali Haider Anwar Ul-Hamid Haya Alhummiany Hamoud H.Somaily Souraya Goumri-Said Mohammed Benali Kanoun 《Nano Materials Science》 EI CAS CSCD 2024年第3期355-364,共10页
This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2) quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size ... This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2) quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size increased with longer annealing,reducing catalytic activity.UV–vis,XRD,TEM,and FTIR analyses probed optical structural,morphological,and vibrational features.XRD confirmed NiS2's anorthic structure,with crystallite size growing from 6.53 to 7.81 nm during extended annealing.UV–Vis exhibited a bathochromic shift,reflecting reduced band gap energy(Eg)in NiS_(2).TEM revealed NiS_(2)QD formation,with agglomerated QD average size increasing from 7.13 to 9.65 nm with prolonged annealing.Pure NiS_(2) showed significant MB decolorization(89.85%)in acidic conditions.Annealed NiS_(2) QDs demonstrated notable antibacterial activity,yielding a 6.15mm inhibition zone against Escherichia coli(E.coli)compared to Ciprofloxacin.First-principles computation supported a robust interaction between MB and NiS_(2),evidenced by obtained adsorption energies.This study highlights the nuanced relationship between annealing duration,structural changes,and functional properties in NiS_(2)QDs,emphasizing their potential applications in catalysis and antibacterial interventions. 展开更多
关键词 NiS_(2) ANTIBACTERIAL quantum dots DYE degradation DFT
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Investigating the charge transfer mechanism of ZnSe QD/COF S-scheme photocatalyst for H_(2)O_(2)production by using femtosecond transient absorption spectroscopy
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作者 Yanyan Zhao Chunyan Yang +4 位作者 Shumin Zhang Guotai Sun Bicheng Zhu Linxi Wang Jianjun Zhang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期258-269,共12页
Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like cov... Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h-1.This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production. 展开更多
关键词 ZnSe quantum dot Covalent organic framework S-scheme heterojunction Carrier migration and separation H_(2)O_(2)production
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二维半导体异质结MoS_(2)/MoSe_(2)中一维量子阱形成机制的电子显微学研究
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作者 庞靖博 时金安 +3 位作者 李昂 李林璇 朱俊桐 周武 《电子显微学报》 CAS CSCD 北大核心 2024年第1期29-37,共9页
本文使用两步化学气相沉积法(chemical vapor deposition,CVD)成功合成了单层二维半导体MoS_(2)/MoSe_(2)面内异质结,通过扫描透射电子显微学(scanning transmission electron microscopy,STEM)对异质结中不同类型的量子阱进行了原子尺... 本文使用两步化学气相沉积法(chemical vapor deposition,CVD)成功合成了单层二维半导体MoS_(2)/MoSe_(2)面内异质结,通过扫描透射电子显微学(scanning transmission electron microscopy,STEM)对异质结中不同类型的量子阱进行了原子尺度结构和局域应力分析,探索了二维半导体材料中,不同结构特征处诱导形成一维量子阱结构的机理。主要包括:(1)晶格失配的二维半导体异质结界面处周期性位错阵列诱导形成的量子阱超晶格;(2)二维半导体晶格内非60°晶界所包含的周期性位错诱导形成周期可控的量子阱超晶格;(3)由连续4|8元环结构组成的60°晶界诱导形成的超长单一量子阱结构。 展开更多
关键词 MoS_(2)/MoSe_(2)异质结 位错 应力 量子阱 低电压STEM
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Mechanism of K/Ni Etching for Biochar-H_(2)O Gasification
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作者 Zhenyu Cheng Dongdong Feng +3 位作者 Qi Shang Yijun Zhao Wenda Zhang Shaozeng Sun 《Journal of Harbin Institute of Technology(New Series)》 CAS 2024年第3期1-18,共18页
Biomass-H_(2)O gasification is a complex thermochemical reaction,including three processes of volatile removal:homogeneous/heterogeneous reforming,biochar gasification and etching.The rate-determining step is biochar-... Biomass-H_(2)O gasification is a complex thermochemical reaction,including three processes of volatile removal:homogeneous/heterogeneous reforming,biochar gasification and etching.The rate-determining step is biochar-H_(2)O gasification and etching so the DFT is carried out to see the catalytic role of different metal elements(K/Ni)in the zigzag biochar model.The calculation results show that the gasification of biochar-H_(2)O needs to go through four processes:dissociative adsorption of water,hydrogen transfer(hydrogen desorption,hydrogen atom transfer),carbon dissolution and CO desorption.The energy barrier indicated that the most significant step in reducing the activation energy of K is reflected in the hydrogen transfer step,which is reduced from 374.14 kJ/mol to 152.41 kJ/mol;the catalytic effect of Ni is mainly reflected in the carbon dissolution step,which is reduced from 122.34 kJ/mol to 84.8 kJ/mol.The existence of K causes the edge to have a stronger attraction to H and does not destroy theπbonds of biochar molecules.The destruction ofπbonds is mainly due to the role of H free radicals,while the destruction ofπbonds will lead to easier C-C bond rupture.Ni shows a strong attraction to O in OH,which forms strong Ni-O chemical bonds.Ni can also destroy the aromatic structure directly,making the gasification easier to happen.This study explored the catalytic mechanism of K/Ni on the biochar-H_(2)O gasification at the molecular level and looked forward to the potential synergy of K/Ni,laying a foundation for experimental research and catalyst design. 展开更多
关键词 BIOCHAR Potassium-nickel catalysis H_(2)O gasification etching quantum chemistry Transition state theory
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