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CdTe 量子点增强的过氧单碳酸盐分解产生的化学发光。

Chemiluminescence arising from the decomposition of peroxymonocarbonate and enhanced by CdTe quantum dots.

机构信息

Department of Chemistry, Tsinghua University, Beijing 100084, China.

出版信息

J Phys Chem A. 2010 Sep 23;114(37):10049-58. doi: 10.1021/jp104060x.

Abstract

CdTe quantum dots (QDs) capped with mercaptoacetic acid were applied to the hydrogen peroxide-sodium hydrogen carbonate chemiluminescence (CL) system. The CL emission intensity was significantly enhanced by different sizes of CdTe QDs. Peroxymonocarbonate (HCO(4)(-)) was formed in the reaction of hydrogen peroxide and sodium hydrogen carbonate, which was a reactive oxygen species. Decomposition of HCO(4)(-) generated superoxide ion radical (·O(2)(-)) and hydroxide radical (·OH). The enhanced CL was induced by the excited CdTe QDs, which could be produced from the combination of hole (oxidized QDs (h(+))) and electron (reduced QDs (e(-))) injected QDs. Radical scavengers and organic reagents such as nitro blue tetrazolium chloride (NBT), cytochrome c, sodium azide, ascorbic acid, thiourea, tert-butanol, and dimethyl sulphoxide were used to study the emitting species. The intermediate hydroxide radical and superoxide ion were key species for producing hole and electron-injected QDs. Four emitters such as (1)O(2), (O(2))(2), (CO(2))(2) and CdTe* were detected in the CL system. The mechanism was discussed based on the CL emission spectra, electron spin resonance spectra, fluorescence spectra, and UV-vis absorption spectra. The CL properties of CdTe QDs will be helpful to study semiconductor nanocrystals and will open new avenues for the application of QDs in many fields, such as chemistry, biology, microbiology, and biochemistry.

摘要

巯基乙酸修饰的 CdTe 量子点(QDs)被应用于过氧一碳酸盐-碳酸氢盐化学发光(CL)体系。不同尺寸的 CdTe QDs 显著增强了 CL 发射强度。过氧一碳酸盐(HCO(4)(-))是在过氧一氢和碳酸氢钠的反应中形成的,它是一种活性氧物质。HCO(4)(-)的分解生成超氧离子自由基(·O(2)(-))和氢氧根自由基(·OH)。增强的 CL 是由激发态 CdTe QDs 诱导的,这些 QDs 可以通过注入 QDs 的空穴(氧化 QDs(h(+)))和电子(还原 QDs(e(-)))的结合产生。自由基清除剂和有机试剂,如氯化硝基四氮唑蓝(NBT)、细胞色素 c、叠氮化钠、抗坏血酸、硫脲、叔丁醇和二甲亚砜,被用于研究发光物种。中间的氢氧根自由基和超氧离子自由基是产生空穴和电子注入 QDs 的关键物种。在 CL 体系中检测到四种发射体,如(1)O(2)、(O(2))(2)*、(CO(2))(2)和 CdTe。基于 CL 发射光谱、电子顺磁共振光谱、荧光光谱和紫外-可见吸收光谱,讨论了该机制。CdTe QDs 的 CL 性质将有助于研究半导体纳米晶体,并为 QDs 在化学、生物学、微生物学和生物化学等许多领域的应用开辟新的途径。

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