ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2025
·Vol. 64
·期 27
·e202425601
·
IF 16.9
Yuemei Li,Shi-Yu Guo,Hongfei Gu,Bingyu Wang,Peiwu Su,Xiuming Zhang,Haoqing Zhang,Shuping Zhang,Fanzhi Yang,Jia Liu,Qing-An Chen,Jiatao Zhang
Visible light photoredox catalysis has become a rapidly emerging area owing to its potential of using sunlight to tame previously hard-to-harness radicals for organic synthesis. At present, such a blueprint faces a significant challenge, namely how to accomplish thermodynamically demanding reactions with sunlight encompassing a wide range of low-energy photons. Here, we report a new reaction framework to overcome this bottleneck through decoupling the thermodynamic limits of photoreduction from photoexcitation. This is fulfilled based on the construction of a heterogeneous photocatalyst Cu@CdS possessing in situ-formed surficial polysulfide species (including S 3 •− and S 4 2− ), which can efficiently harvest solar energy via plasmonic absorption of Cu while manifest sufficient redox potential for activating inert aryl bromides/chlorides enacted by excited polysulfides. We demonstrate that this designed material composes a potent photoredox catalyst for efficient aryl cross-coupling, borylation, hydrogenation, as well as Birch-type dearomatization reactions, with good recyclability and stability. In particular, when exclusively using natural sunlight as an energy source, the product yield can still reach up to 90%. Our findings introduce a straightforward yet viable way to progress toward the century-long dream of leveraging natural sunlight to produce structurally complex organic molecules, just like plants on Earth. Graphical Chemists have long aspired to construct complex organic compounds the way that plants do by harnessing natural sunlight as an energy source. This study presents an advancement toward this goal via synergistic exploitation of the plasmonic absorption of Cu and the unique redox potentials of excited polysulfide species (S 3 •− and S 4 2− ) on semiconductor surfaces to decouple the thermodynamic limits of photoreduction from photoexcitation.
研究领域:
光催化
·
有机合成
·
材料化学
·
可再生能源
·
物理化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Fengqing Wang,Changjiang Hu,Chong Chen,Shuiyan Cao,Qiuhao Li,Yunlong Wang,Jun Ma
The work presents an ambient, facile, and controllable radiation-induced method to synthesize nickel-doped CdS (CdS-xNi) nanocomposites. We found that the optimized CdS-2Ni exhibited enhanced photocatalytic hydrogen (H 2 ) evolution activity (∼3.86 mmol/g/h), which was three times that of pristine CdS-γ, and far superior to that of CdS-H (0.04 mmol/g/h) prepared by the conventional hydrothermal method. The analysis of transient photocurrent response, EIS, Mott-Schottky plot, PL, UV–vis, and TEM data, attributed the significant enhancement of photocatalytic activity to the sulfur vacancies and Ni active sites. We showed the ionizing radiation synthesis routine could alter the conduction band (CB) to be more negative and enable a stronger reduction capacity of electron-hole pairs. Furthermore, the doping of Ni induced the increase of sulfur vacancy and lattice distortion, which acted as the electron capture center of proton reduction and suppressed the electron transport, thereby efficiently separating the carriers and prolonging their lifetime. The radiation synthesis technology developed in this study provides a new path for the mild and controllable synthesis of high-performance photocatalysts.
研究领域:
材料科学
·
化学工程
·
环境科学
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DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2018
·Vol. 410
·期 29
·7645-7653
·
IF 3.307
Zhang Dong-Ping,Wang Ling-E,Liu Xiao-Ying,Luo Zhi-Hua,Zheng Lei,He Yun,Zhang Bo
A facile and feasible photoelectrochemical (PEC) immunoassay based on plasmon-enhanced energy transfer between gold nanoparticles (AuNPs) and CdS quantum dots (QDs)/g-C 3 N 4 nanosheets was developed for the ultrasensitive detection of lipoprotein-associated phospholipase A 2 (Lp-PLA 2 ). To construct such a sensing platform, the immunosensor was prepared by immobilizing Lp-PLA 2 on a CdS QDs/g-C 3 N 4 -modified electrode. A competitive-type immunoreaction was utilized for Lp-PLA 2 detection, with AuNP-labeled anti-Lp-PLA 2 antibody used as the competitor. Introducing AuNPs with the specific antibody for the antigen target Lp-PLA 2 led to heavy quenching of the photocurrent of CdS QDs/g-C 3 N 4 due to the plasmon-enhanced energy transfer between AuNPs and CdS QDs. The quenching efficiency decreased with increasing target Lp-PLA 2 concentration. Under optimal conditions, the PEC immunosensor presented a good photocurrent response to the target Lp-PLA 2 in the dynamic linear range of 0.01–300 ng mL −1 , with a low detection limit of 5.3 pg mL −1 . Other biomarkers and natural enzymes did not interfere with response of this system. The reproducibility and accuracy of this method for the analysis of human serum specimens were evaluated, and the results given by the method developed here were found to closely correspond to the results obtained with commercial Lp-PLA 2 ELISA kits. Importantly, this protocol offers promise for the development of exciton–plasmon interaction-based PEC detection systems.
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研究领域:
分析化学
·
生物化学
·
纳米技术
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DOI
PubMed
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2022
·
IF 0.847
Ruiqi Gao,Huan He,Junxian Bai,Lei Hao,Rongchen Shen,Peng Zhang,Youji Li,Xin Li
ABSTRACT Nowadays, conjugated polymers have garnered numerous attention as a new class of organic photocatalysts due to their tunable electronic properties, low cost, excellent stability and sufficient light-absorption performance. In particular, pyrene-benzothiadiazole-based conjugated polymer (PBBP) has been considered to be a new type of conjugated polymers for photocatalytic H 2 evolution. However, the poor charge separation seriously limits its practical application in H 2 evolution. In this work, a PBBP-based polymer/CdS 2D/2D organic/inorganic S-scheme heterojunction photocatalyst with a strong internal electric field is, for the first time, prepared for efficient photocatalytic hydrogen evolution. The pyrene-benzothiadiazole-based conjugated polymers (PBBP) are synthesized by the Suzuki-Miyaura reactions. Then, the hybrid heterojunction photocatalysts are fabricated by coupling CdS with it through the ultrasonic mixing method. As a result, the highest H 2 -production rate of 15.83 mmol h −1 g −1 is achieved on 20% PBBP/CdS composite under visible-light irradiation, nearly 2.7 times higher than that of pure CdS. The apparent quantum efficiency (AQE) of 20% PBBP/CdS composite could reach 8.66% at λ = 420 nm. The enhanced activity could be attributed to the construction of S-scheme heterojunction, which accelerates the recombination of carriers with weaker redox ability and maintains the strong reducibility of electrons in CdS. This work provides a protocol for pyrene-benzothiadiazole-based conjugated polymers to prepare S-scheme heterojunction photocatalysts based on organic/inorganic coupling.
研究领域:
材料科学
·
化学工程
·
光化学
·
催化
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Wenjing Shen,Dandan Xiang,Junnan Yang,Yanting Tang,Changhui Xin,Quanhui Guo,Xin Yu
In this work, beta zeolite supported Ti 3+ -TiO 2 /CdS heterojunction was prepared for photodegradation of tetracycline under visible-light irradiation, and zeolite served as a support for the high dispersions of the Ti 3+ -TiO 2 nanoparticles . The obtained zeolite/Ti 3+ -TiO 2 /CdS heterojunction showed a relatively high surface areas of approximately 63.2 m 2 g −1 , much higher than those of the prepared Ti 3+ -TiO 2 /CdS (27.1 m 2 g −1 ), Ti 3+ -TiO 2 (36.5 m 2 g −1 ), and CdS (31.1 m 2 g −1 ), strongly demonstrating the significant of zeolite for high dispersion of the Ti 3+ -TiO 2 /CdS composite. Besides, the experimental results also showed that the photocatalytic degradation efficiency could reach 78 % in 3 min for the zeolite/Ti 3+ -TiO 2 /CdS heterojunction, and the corresponding rate constant was as high as 0.788 min −1 , which was 26.90 times that of pristine Ti 3+ -TiO 2 , 2.24 times of pristine CdS , and 2.04 times of the Ti 3+ -TiO 2 /CdS composite, mainly because of the supporting effects of zeolite and the formation of Ti 3+ -TiO 2 /CdS heterostructure for highly enhanced charge separation. In addition, the trapping experiment revealed that the main reactive species involved in tetracycline degradation were attributed to the photo-generated holes and ⸱O 2 - species.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2013
·
IF 3.535
Yizhong Shen,Shaopu Liu,Ling Kong,Dan Li,Youqiu He
Thioglycolic acid-capped (TGA-capped) CdTe/CdS quantum dots (QDs) were prepared in the water phase. The interaction of TGA-CdTe/CdS QDs with polymyxin B sulfate (POBS) was investigated by ultraviolet–visible (UV–vis) absorption, fluorescence (FL), resonance Rayleigh scattering (RRS) spectroscopy and the measurement of fluorescence lifetime . Under optimum conditions, not only the UV–vis absorption and fluorescence spectra were changed, but also the RRS intensity was greatly enhanced. These phenomena offered useful techniques for the determination of POBS with fluorescence quenching and RRS methods . The linear ranges and detection limits of POBS were 0.09–5.25 μg mL −1 and 27.5 ng mL −1 for the fluorescence quenching technique, 0.02–6.0 μg mL −1 and 6.36 ng mL −1 for the RRS technique. Among them, the RRS approach obtained the higher sensitivity. Accordingly, a novel rapid, convenient, and highly sensitive RRS method for the determination of POBS was proposed and applied to detect POBS in pharmaceutical preparations with satisfactory results. Furthermore, the suitable reaction conditions, affecting factors as well as the influence of coexisting substances were studied. Some possible reaction mechanisms were also discussed.
研究领域:
分析化学
·
生物医学工程
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DOI
高影响因子
Journal of Materials Chemistry B
·
2019
·Vol. 8
·期 5
·919-927
·
IF 5.047
Minghui Zan,Cong Li,Daoming Zhu,Lang Rao,Qian-Fang Meng,Bei Chen,Wei Xie,Xingwang Qie,Li Li,Xiaojiao Zeng,Yirong Li,Wen-fei Dong,Wei Liu
Copper ions (Cu2+) and L-cysteine (L-Cys) in the human body always play critical roles in various physiological processes, while abnormal Cu2+ and L-Cys concentrations in the biological system lead to many diseases. In this manuscript, Si-doped carbon dots (Si-CDs) with near-infrared fluorescence were designed for the detection of Cu2+ and L-Cys through the fluorescence “on–off–on” mode. The carbon dots exhibited not only excellent optical merits including good stability against photobleaching and high chemical stability, but also superior biological compatibility. Interestingly, due to the abundant amino groups distributed on the surface of Si-CDs, they could bind to copper ions to form cupric amine complexes and then quench the fluorescence of Si-CDs due to an electron transfer process. In addition, upon the addition of L-Cys, the FL intensity of Si-CDs could be effectively recovered accompanied with complexation between Cu2+ and the functional groups in L-Cys, due to which Cu2+ was removed from the surface of Si-CDs. Notably, as far as we know, these are the first red-emitting carbon dots for copper ion and L-Cys assays in water samples and human plasma samples. Furthermore, this strategy was successfully applied to the determination of Cu2+ and L-Cys in living systems, demonstrating great practicability in biomedical applications.
研究领域:
分析化学
·
生物医学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
·
2017
·
IF 4.164
Manqing Yan,Mingchen Zhou,Jing Chen,Tianlei Zhao,Longxiang Tang,Hong Bi
In this paper, the environment-friendly, water-soluble carbon dots (CDs) with stable photoluminescence (PL) have been prepared via the one-step pyrolysis of lotus leaf. Then the as-prepared CDs containing abundant hydroxylic and carboxylic groups were employed as cocatalyst with tartaric acid (TA) in ring-opening polymerization (ROP) of ε-caprolactone (ε-CL). The low-toxic organic acid TA, as main catalyst, was used to catalyze the ROP of ε-CL efficiently. The fluorescent CDs@PCL hybrids were obviously hydrophobic and they exhibited an excellent biocompatibility, and biodegradability due to the existence of PCL. Therefore the hydrophobic, biodegradable and multi-color fluorescent CDs@PCL hybrids may have potential applications in biomedicine, photocatalyst, bioimaging, and environmental analysis. Furthermore the application of CDs in catalyzing and initiating polymerization reaction will exemplify the versatility of CDs in the most unexpected fields.
研究领域:
材料科学
·
生物医学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Mingrui Liu,Guangmin Li,Shunsheng Wei,Hongfei Liu,Gaoling Yang
Chiral semiconductor nanocrystals (NCs) represent a promising class of materials for various applications, including biological sensing, photonics, and spin-polarized devices. However, the comprehension of the mechanisms underlying ligand-induced chiroptical effects in NCs has been limited by the constraints of current theoretical and experimental models, particularly those involving simple spherical NCs. In this study, we examined the relationship between optical activity and band structures in core–shell dot-in-rod NCs, specifically CdSe@CdS, ZnSe/CdS@CdS, and ZnSeTe/CdS@CdS dot-in-rod NCs, which were functionalized with chiral ligands. By manipulating the wave function distribution of electrons and holes within the dot-in-rod NCs, we demonstrated through circular dichroism (CD) measurements that a reduction in the number of holes within the synthesized dot-in-rod NCs correlates with a decrease in the g factor. This conclusion was corroborated by theoretical calculations. Furthermore, the fabrication of chiral CdS-Au heterojunctions and the application of electron quenchers revealed that the reduction of the g factor also suggests the significant role of electrons in the generation of chirality. Our findings not only enhance the understanding of the fundamental origins of induced chirality effects in semiconductor NCs but also provide a clear methodology for the design of optimal optically active chiral NCs, thereby paving the way for future applications utilizing chiroptical materials.
研究领域:
纳米材料
·
半导体物理
·
手性光学材料
·
量子点
·
光电子学
·
表面化学
·
理论凝聚态物理
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale Research Letters
·
2019
·Vol. 14
·期 1
·1-9
·
IF 3.159
Wang Liwei,Liu Zhe,Han Junhe,Li Ruoping,Huang Mingju
Fabrication of hybrid nanostructures with complex morphologies and high photocatalytic activity is a difficult challenge because these particles require extremely high preparation skills and are not always practical. Here, hierarchical flower-like Au@CdS-CdS nanoparticles (Au@CdS-CdS nanoflowers) have been synthesized using a stepwise method. The Au@CdS-CdS nanoflowers are consisted of Au core, CdS shell, and CdS nanorods. The UV-Vis absorption range of the Au@CdS-CdS nanoflowers reaches up to 850 nm which covers the whole visible range (400–760 nm). Photoinduced charge transfer property of Au@CdS-CdS nanoflowers was demonstrated using photoluminescence (PL) spectroscopy. Compared to CdS counterparts and Au@CdS counterparts, Au@CdS-CdS nanoflowers demonstrated the highest photocatalytic degradation rate under irradiation of λ = 400–780 nm and λ = 600–780 nm, respectively. Based on structure and morphology analyses, we have proposed a possible formation mechanism of the hybrid nanostructure which can be used to guide the design of other metal-semiconductor nanostructures with complex morphologies.
研究领域:
材料化学
·
纳米科学与技术
·
光催化
·
半导体异质结
·
功能纳米材料
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2014
·
IF 2.354
Yonghai Song,Mei Huang,Dan Luo,Dandan Zhong,Haoqing Hou,Fugang Xu
In this study, we investigated the interaction between EcoRI and CdS QDs modified with different functional groups as well as the conformational changes of EcoRI in the process. MUD capped (CdS–OH QDs) and UDT capped (CdS–CH 3 QDs) CdS QDs were separately prepared and used to react with EcoRI, respectively. The interaction was characterized by various spectroscopic techniques including UV–vis absorption, fluorescence and Fourier transform infrared (FTIR) spectroscopy, together with electrophoresis methods. The strength of interaction for EcoRI with CdS–OH QDs and CdS–CH 3 QDs was evaluated and analysed. Relevant thermodynamic parameters such as Δ H , Δ G and Δ S were calculated and a static quenching interaction process was proposed. The conformational change of EcoRI interacted with CdS–OH QDs or CdS–CH 3 QDs was also measured and compared. Finally agarose electrophoresis assay was performed and revealed that the enzyme activity of EcoRI was somewhat conserved after interaction with CdS QDs. This study contributed to a better understanding of protein-NPs interaction and created a framework for applications of nanomaterial-biomolecule conjugation in some fields such as nanobiology and nanomedicine.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Nanomaterials
·
2020
·
IF 1.98
Shibing Zou,Feng Li
Highly efficient all-inorganic perovskite solar cells require a fast charge transfer from CsPbBr3 to TiO2 to reduce the recombination from trap states. Herein, we insert a CdS/CdSe/CdS quantum dot (QD) layer between the TiO2 and CsPbBr3 layers to fabricate all-inorganic perovskite solar cells. By tuning the thicknesses of the CdSe layer of CdS/CdSe/CdS QDs, the conduction band (CB) levels can be adjusted to -3.72~-3.87 eV. After inserting the QD intermediate layer, the energy offset between the CB of TiO2 and CsPbBr3 is reduced, thus leading to a charge transfer rate boost from to . The power conversion efficiency (PCE) of the solar cell with QD intermediate layer achieves 8.64%, which is 20% higher than its counterpart without QDs.
✓ 已验证
产品关联
DOI
高影响因子
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