ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Xiaoya Fan,Yanying Wang,Li Deng,Lin Li,Xinfeng Zhang,Peng Wu
Singlet oxygen, generated from type-II photosensitization, has become increasingly popular in bioassay development in recent years. However, the transient nature of singlet oxygen in water (lifetime shorter than 4 μs) as well as its high activity make it easily inactivated by solvent molecules and other coexisting species, thus deteriorating use in the analytical sensitivity. Here, we proposed the use of a simple redox mediator for storing the energy of the transient singlet oxygen. To demonstrate such an idea, singlet oxygen generated from photosensitization of the double strand DNA–SYBR Green I (dsDNA-SG) complex was explored as a redox donor that can be modulated through formation and deformation of the dsDNA structure. After screening of a series of redox mediators with luminol chemiluminescence (CL) as the probe, ferrocyanide (K4Fe(CN)6) was found to be the most efficient, resulting in ∼30-fold intensified luminol CL. By storing the oxidative capacity of singlet oxygen in ferrocyanide, the dsDNA-SG complex was evolved into a photosensitization-mediated chemiluminescence (PMCL) biosensing platform for DNA detection. Such a PMCL sensing platform allows label- and amplification-free detection of picomolar-scale DNA with a limit of detection (LOD) of 1.5 pM (0.45 fmol in absolute). The excellent sensitivity of PMCL sensing confirmed that such a facile storage approach to oxidative capacity would be appealing for singlet-oxygen-involved biosensing.
研究领域:
分析化学
·
生物医学工程
·
光化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 30
·期 1
·647-657
·
IF 2.324
Xiao Tai,Huang Zu-Sheng,Wang Lingyun,Cao Derong
Three novel dithieno[3,2- f :2′,3′- h ]quinoxaline-based organic dyes ( IQ-C, IQ-D and IQ-F ) with three π-spacers were synthesized and developed for dye sensitized solar cells, where dithieno[3,2- f :2′,3′- h ]quinoxaline was used as electron-withdrawing π-spacers, and 2,3-diphenylquinoxaline or dibenzo[ a,c ]phenazine as auxiliary electron-withdrawing π-spacers. The dye IQ-D with 2,3-diphenylquinoxaline as auxiliary electron-withdrawing π-spacer exhibited higher photocurrent ( J sc ) and photovoltage ( V oc ) than that of the dye IQ-C with 2,3-bis(4-(octyloxy)phenyl)quinoxaline as the additional electron-withdrawing π-spacer, due to the larger adsorption amount of IQ-D . The dye IQ-F with a rigid conjugated dibenzo[ a,c ]phenazine as additional electron-withdrawing π-spacer showed the highest efficiency of 6.54% under AM 1.5 G irradiation. It was demonstrated that the π-spacers influence the photovoltaic performance of the dithieno[3,2- f :2′,3′- h ]quinoxaline-based organic dyes significantly. The results indicated that the dyes with three π-spacers are promising candidates for efficient dye-sensitized solar cells.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
Nano Energy
·
2012
·
IF 0
Chenbo Wang,Zifei Jiang,Lin Wei,Yanxue Chen,Jun Jiao,Micah Eastman,Hong Liu
We combine CdS semiconductor quantum dots and single-crystalline rutile TiO 2 nanorod arrays to produce a practical quantum dot sensitized solar cell . A facile wet-chemical approach was implemented for growth of this CdS@TiO 2 architecture. Rutile TiO 2 nanorod arrays with lengths of 1–2 μm and diameters of 40–60 nm were synthesized on fluorine-doped tin oxide glass by a hydrothermal process in a titanium tetrachloride precursor solution . CdS quantum dots with a size of 5–10 nm were deposited onto a TiO 2 nanorod surface using an ultrasonic-assisted chemical bath deposition method . The resulting CdS quantum dots and TiO 2 nanorods formed a type-II heterojunction and showed increased absorption over visible light range. Incident photon-to-current conversion efficiencies (IPCE) as high as 85% and power conversion efficiencies of 2.54% were obtained using a polysulfide electrolyte.
研究领域:
材料科学
·
纳米技术
·
光伏技术
✓ 已验证
DOI
Science China-Chemistry
·
2024
·
IF 10.4
Yang Ning,Gong Chu,Zhang Dongmei,Gao Xufeng,Han Lifeng,Fu Pingqing,Zhang Xinxing
Humic-like substances (HULIS), a class of macromolecular photosensitizers, are major components of light-absorbing aerosols in the atmosphere. Due to the amphiphilic nature of HULIS, they tend to appear at the air-water interface of atmospheric water. However, there have been limited studies on the photosensitized chemistry of HULIS at the air-water interface owing to the lack of methods with high interface selectivity. Here, a unique field-induced droplet ionization mass spectrometry (FIDI-MS) technique was used to investigate the photosensitized chemistry of several samples at the air-water interface. These samples include commercially available humic acid and the PM 2.5 sample collected during Beijing’s severe winter haze in December 2016. Ultrahigh-resolution Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) was also applied to analyze the atomic compositions, the degree of unsaturation and the aromaticity of these samples. Both Type I and Type II photosensitized oxidation pathways were observed, which were postulated to be dictated by the packing density of the molecules at the air-water interface. These findings reveal that the photosensitization of HULIS at the air-water interface contributes greatly to the formation of atmospheric aerosols, further advancing our understanding of the important roles played by photosensitized chemistry in the atmosphere.
研究领域:
大气科学
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2013
·Vol. 3
·期 48
·26367-26375
·
IF 2.562
Lining Sun,Yannan Qiu,Tao Liu,Hongshang Peng,Wei Deng,Zhijuan Wang,Liyi Shi
The homogeneously transparent hybrid gels (Ln–N–P-gel, Ln = Sm, Yb, Nd, Er, Pr, Ho, Tm) containing lanthanide complexes (by using dinaphthoylmethane (dnm) as the primary ligand and 1,10-phenanthroline (phen) as the synergic ligand) via the in situ approach have been prepared. The dnm ligand was synthesized and adopted with the aim to sensitize the lanthanide ions with visible light. The properties of Ln–N–P-gels were investigated by Fourier-transform infrared (FT-IR), diffuse reflectance (DR), scanning electron micrographs (SEM), fluorescence spectra and thermogravimetric analyses. The results reveal that the lanthanide complexes are successfully in situ synthesized in the corresponding Ln–N–P-gels. Under the excitation of visible-light, the Ln–N–P-gels showed the respective visible (Sm3+) and near-infrared (Sm3+, Yb3+, Nd3+, Er3+, Pr3+, Ho3+, Tm3+) luminescence. The near-infrared (NIR) luminescence of Sm3+, Pr3+, Ho3+, and Tm3+ complexes sensitized by visible-light had been rarely reported previously, which is highly desired for biomedical and photonics applications. Based on the relevant energy levels, a model was proposed to explain the visible-NIR luminescence of the Ln–N–P-gels based on the visible-light excitation.
研究领域:
材料科学
·
光学
·
生物医学工程
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 5
·959-967
·
IF 7.779
Chao Wang,Shoujuan Wang,Fangong Kong,Ning Chen
Sensitized Ti-oxo clusters have attracted growing attention as analogous molecular model compounds of dye-sensitized titanium dioxide solar cells. However, reports on the introduction of metal complexes as photosensitizers into Ti-oxo clusters are still very rare. Herein, with the use of an organometallic complex ferrocene as a sensitizer, two novel ferrocene-sensitized Ti-oxo clusters, namely, [Ti8(μ3-O)4(Dipa)2(Fcdc)4(OiPr)10]·2HOiPr (H2Fcdc = 1,1-ferrocene dicarboxylic acid, Dipa = diisopropanolamine, and HOiPr = isopropanol, Ti8Fcdc4) and [Ti10(μ4-O)2(μ3-O)4(Fcdc)2(μ2-OEt)8(OEt)10]·2HOEt (Ti10Fcdc2) have been successfully synthesized. Their molecular structures, light absorption, charge transfer, and photoelectrochemical properties were systematically investigated. It is demonstrated that the incorporation of Fcdc ligands shows a significant influence on the light absorption of the resulting clusters, and their absorption band edge is extended to about 580 nm. Furthermore, experimental measurements and theoretical calculations showed that the intense intramolecular charge transfer occurs from the Fcdc ligands to the Ti-oxo core. Based on these advantages, clusters Ti8Fcdc4 and Ti10Fcdc2 were used as photoelectrode precursors to carry out photoelectrochemical experiments, and both exhibited clear photocurrent responses. The molecular structure, light absorption, and effective charge transfer of materials have a direct bearing on their photoelectrochemical performances. This work not only provides novel structural models for sensitized Ti-oxo clusters towards the modulation of photoelectric properties but also provides new insights into further understanding the structure–property relationships of sensitized clusters.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2019
·Vol. 4
·期 2
·911-920
·
IF 4.912
Junjian Xie,Xiangwen Zhang,Chengxiang Shi,Lun Pan,Fang Hou,Genkuo Nie,Jiawei Xie,Qing Liu,Ji-Jun Zou
Hydrocarbons with a highly strained four-membered ring are synthesized via self-photosensitized [2 + 2] cycloaddition and hydrodeoxygenation using cyclohexene and isophorone as feedstocks, which show high density and high heat values. Photoreaction can take place selectively with isophorone as a self-sensitizer and a reactant. Isophorone/cyclohexene co-cycloaddition has a much faster reaction rate than self-cycloaddition of isophorone, and both DFT calculations and photochemical kinetics show that the energy barrier for the former is much lower than that for the latter. Under optimal conditions, the selectivity of co-cycloaddition and self-cycloaddition can reach 93.3% and 94.9%, with isophorone conversion of 95.4% and 68.8%, respectively. In addition, a series of olefins can undergo self-photosensitized [2 + 2] cycloaddition with isophorone smoothly in high selectivity. After hydrodeoxygenation, hydrocarbons derived from isophorone/cyclohexene mixture and pure isophorone (with an overall yield of 82.1% and 61.3%) have high densities of 0.903 g mL−1 and 0.892 g mL−1, respectively, along with good cryogenic properties. Especially, the hydrocarbons synthesized through photosensitized cycloaddition show considerably higher density and heat values compared with those derived from a common C–C coupling route, which is attributed to the constructed strained cyclic structures. This work provides a new way for photosynthesis of high-energy-density hydrocarbons.
研究领域:
化学合成
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2018
·
IF 2.524
Zhijuan Wang,Song Dang,Shu'na Zhao,Lining Sun
Recently, much attention has been paid to the lanthanide luminescent materials based on the visible-light sensitization for their potential applications in the fields of bio-imaging and optical devices. In this work, the lanthanide complexes have been covalently bonded to the ordered mesoporous titania (OMT) matrix, and the resulting titania-based hybrid ordered mesoporous materials (named as LnDB-OMT, Ln = Eu, Sm, Yb, Nd) were characterized by using Fourier-transform infrared (FT-IR) spectroscopy, small-angle X-ray powder diffraction (SAXD), N 2 adsorption–desorption isotherms, transmission electron microscopy (TEM), fluorescence spectroscopy , and thermogravimetric analysis . Generally, exciting with visible light is advantageous over UV excitation. Of importance here is that, under excitation with visible light, the LnDB-OMT all show characteristic visible (Eu 3+ , Sm 3+ ) as well as near-infrared (Sm 3+ , Yb 3+ , Nd 3+ ) luminescence of the corresponding Ln 3+ ions (multicolor emission covered from 500 to 1400 nm spectral region), which is attributed to the energy transfer from the ligands to the Ln 3+ ions via an antenna effect.
研究领域:
材料科学
·
光学
·
生物成像
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 26
·5776-5782
·
IF 5.344
Yueling Xu,Lehui Xiao
The deposition of amyloid plaques resulting from the aggregation of amyloid-β (Aβ) peptides is closely related to Alzheimer's disease (AD). With the development of various therapeutic methods, the oxidative modification of Aβ has emerged as a fascinating noninvasive photo-therapeutic intervention for treating AD by altering the Aβ aggregation tendency. Herein, we report the photo-triggered inhibition of Aβ aggregation and cytotoxicity by utilizing polymer nanodots (Pdots) modified with rose bengal (RB), methylene blue (MB), and riboflavin (RF). Experimental results demonstrate that these functionalized Pdots manifest a superior suppression effect on Aβ aggregation under irradiation. This can be attributed to the formation of reactive oxygen species (ROS) (i.e., singlet oxygen (1O2)), resulting in the oxygenation of Aβ and the change of Aβ aggregation tendency. Especially, RB-Pdots manifest better biocompatibility and higher 1O2 productivity. In a word, this hybridized nanostructure will provide a promising platform for the noninvasive photo-therapeutic treatment of AD in the future.
研究领域:
生物化学
·
神经科学
·
药物开发
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yifu Fu,Yiqi Yan,Zongsu Wei,Richard Spinney,Dionysios D. Dionysiou,Davide Vione,Min Liu,Ruiyang Xiao
Photochemical transformation is an important process that involves trace organic contaminants (TrOCs) in sunlit surface waters. However, the environmental implications of their self-photosensitization pathway have been largely overlooked. Here, we selected 1-nitronaphthalene (1NN), a representative nitrated polycyclic aromatic hydrocarbon, to study the self-photosensitization process. We investigated the excited-state properties and relaxation kinetics of 1NN after sunlight absorption. The intrinsic decay rate constants of triplet (31NN*) and singlet (11NN*) excited states were estimated to be 1.5 × 106 and 2.5 × 108 s–1, respectively. Our results provided quantitative evidence for the environmental relevance of 31NN* in waters. Possible reactions of 31NN* with various water components were evaluated. With the reduction and oxidation potentials of −0.37 and 1.95 V, 31NN* can be either oxidized or reduced by dissolved organic matter isolates and surrogates. We also showed that hydroxyl (•OH) and sulfate (SO4•–) radicals can be generated via the 31NN*-induced oxidation of inorganic ions (OH– and SO42–, respectively). We further investigated the reaction kinetics of 31NN* and OH– forming •OH, an important photoinduced reactive intermediate, through complementary experimental and theoretical approaches. The rate constants for the reactions of 31NN* with OH– and 1NN with •OH were determined to be 4.22 × 107 and 3.95 ± 0.01 × 109 M–1 s–1, respectively. These findings yield new insights into self-photosensitization as a pathway for TrOC attenuation and provide more mechanistic details into their environmental fate.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 16
·5652-5659
·
IF 4.099
Yong-Jun Yuan,Gaoliang Fang,Daqin Chen,Yanwei Huang,Ling-Xia Yang,Da-Peng Cao,Jingjing Wang,Zhen-Tao Yu,Zhi-Gang Zou
Expanding the photoresponse range of TiO2-based photocatalysts is of great interest for photocatalytic H2 production. Herein, noble-metal-free CuInS2 quantum dots were employed as a novel inorganic dye to expand the visible light absorption of TiO2/MoS2 for solar H2 generation. The as-prepared CuInS2/TiO2/MoS2 photocatalysts exhibit broad absorption from the ultraviolet to near-infrared region. Under visible light irradiation (λ > 420 nm), the CuInS2/TiO2/MoS2 photocatalyst with 0.6 mmol g−1 CuInS2 and 0.5 wt% MoS2 showed the highest H2 evolution rate with a value of 1034 μmol h−1 g−1. Moreover, a considerable H2 evolution rate of 141 μmol h−1 g−1 was obtained under the irradiation of the optimized CuInS2/TiO2/MoS2 photocatalyst with >500 nm light. The reaction mechanism of the CuInS2/TiO2/MoS2 photocatalyst for photocatalytic H2 evolution was investigated in detail by photoluminescence decay study, and the results showed that the photoexcited electrons of CuInS2 can be transferred efficiently through TiO2 to MoS2 and then react with the absorbed protons to generate H2. The reported sensitization strategy tremendously improves the visible light absorption capacity and the photocatalytic performance of TiO2-based photocatalysts.
研究领域:
材料科学
·
光催化
·
能源化学
·
纳米材料
·
半导体物理
·
太阳能转化
✓ 已验证
DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 9
·5543-5553
·
IF 6.895
Shihong Wu,Ronghui Zhou,Hanjiao Chen,Jinyi Zhang,Peng Wu
Photosensitization is a promising avenue of oxygen activation, which can overcome the spin selection rule to transform the ground state oxygen (3O2) into a highly reactive singlet oxygen (1O2). Carbon dots (CDs) are a promising type of carbon-based photosensitizer, and nitrogen doping can further improve the oxygen photosensitization performance. Although the roles of nitrogen doping in tuning the optical properties (mainly absorption and fluorescence) of CDs have been well-studied, their association with oxygen photosensitization has not been reported. Herein, using the well-developed synthetic protocol of hydrothermal treatment of citric acid and ethylenediamine, we prepared nitrogen-doped CDs (N-CDs) of varied nitrogen contents. The oxygen photosensitization performances of the N-CDs were first confirmed by ROS investigation with TMB oxidation as the ROS probe and EPR. After XPS analysis of the surface nitrogen doping speciation, it was found that the changes of graphitic N and pyrrolic N correlated well with the oxygen photosensitization performances of N-CDs. Further theoretical calculations indicated that the two key factors for oxygen photosensitization, namely triplet activation and oxygen adsorption, are mainly associated with graphitic N and pyrrolic N, respectively. The results in this work help further understanding of the oxygen photosensitization mechanism of N-CDs, and are expected to be useful in the future design of carbon-based photosensitizers.
研究领域:
材料科学
·
光化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）