ChemPlusChem
·
2016
·Vol. 81
·期 11
·1166-1173
·
IF 2.836
Xiaozhao Wang,Kui Cheng,Wenjian Weng,Huiming Wang,Jun Lin
Graphical Break away : Carbon quantum dots (CQDs) have been incorporated as a sensitizer into TiO 2 films to regulate the light-induced cell-detachment performance. This incorporation inhibits charge recombination of the TiO 2 system under UV illumination, which increases the negative surface potential and changes the secondary structure of adsorbed extracellular protein molecules, and consequently results in a faster release of cells (see figure). Carbon quantum dots (CQDs) have been incorporated as a sensitizer into TiO 2 films to regulate the light-induced cell-detachment performance. Depending on the amount of CQDs incorporated, nanodots or porous films are obtained. It was found that the right amount of CQDs incorporation significantly improves the cell-sheet detachment efficiency, and an intact cell sheet could be obtained after merely five minutes of UV illumination (365 nm, UV365), which is much faster than that from CQDs-free TiO 2 film. Furthermore, cell sheets on CQDs-sensitized TiO 2 films show improved viability, and alkaline phosphatase and collagen I activity either before or after light-induced detachment. The improved cell-detachment performance is ascribed to the effective inhibition of charge recombination of the TiO 2 film and the microstructure variations, which increase the negative surface potential and change the secondary structure of the adsorbed extracellular protein molecules; this results in a faster release of cells. It is suggested that the faster release reduces the possible detrimental impact on cell functions during detachment and helps in maintaining the excellent cellular activity. This study demonstrates that CQDs sensitization is an effective approach for optimizing the performance of light-induced cell-sheet harvest.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 19
·5383-5393
·
IF 5.726
Qingquan Tang,Jiang Gong,Qiang Zhao
Organic photocatalysts have recently drawn intense attention to wastewater treatment through the efficient utilization of solar energy. Rational design and synthesis of organic photocatalysts with facilitated charge-carrier transfer are crucial for achieving high-performance photodegradation of pollutants. In this work, functional polymers of intrinsic microporosity (PIMs) were synthesized by a quaternization reaction, and the zwitterionic and D–π–A structured polymers show visible-light-driven catalytic activity for the degradation of organic pollutants. The formation of D–π–A structures in PIMs is demonstrated to extend visible-light absorption and promote charge-transfer transition. Besides, the zwitterionic structures improve hydrophilicity and induce the aggregation of polymer chains, facilitating charge-carrier diffusion at the polymer–water and polymer–polymer interfaces. The combination of these favorable features endows the resulting PIMs with high catalytic degradation ability toward organic dyes under visible-light irradiation, which prevails over state-of-the-art organic photocatalysts.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Juanjuan Jin,Changjun Yang,Bingguang Zhang,Kejian Deng
A highly efficient oxidation of amines including primary and secondary amines into imines using O 2 as the oxidant was realized by cobalt tetra(2-hydroxymethyl-1,4-dithiin)porphyrazine (CoPz(hmdtn) 4 ) under irradiation of visible light ( λ ≥ 420 nm). Particularly, the photocatalytic selective oxidation of benzylamine into N -benzylidenebenzylamine was thoroughly studied in order to get more insight into the reaction kinetics and mechanism for the oxidation of amine. The photocatalytic oxidation of benzylamine was observed to follow pseudo-first-order reaction kinetics. Moreover, a reasonable linear relationship between the log( k X / k H ) values and the Brown-Okamoto constant ( σ + ) parameters was obtained for oxidation of para - and meta -substituted benzylamines. Besides imine, the presence of other intermediate products such as NH-imine and H 2 O 2 was further evidenced in this photocatalytic system. Additionally, the reactive oxygen species (ROSs) generated in this photocatalytic process were confirmed by electron spin resonance (ESR) technique. The possible photocatalytic transformation pathway of amine into imine was also proposed, involving the dehydrogenation of amine to form NH-imine and the nucleophilic addition of NH-imine by free amine to afford the final imine.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Huilei Wang,Yilin Le,Jianzhong Sun
Widespread application of synthetic dyes could generate colored wastewaters causing a range of serious environmental problems. Due to the complex nature of effluents from textile industries , it is difficult to obtain satisfactory treatment of dyes-contaminated wastewater using one single method. Biohybrids coupling of photocatalysts and biocatalysts have great potential in environmental purification. However, how to select suitable organisms and enhance the hybrid’s catalytic activities remain challenging. Here, a novel biohybrid system ( Clostridium thermocellum -CdS), created for light-driven biodecolorization under thermophilic treatment by using non-photosynthetic microorganism C. thermocellum self-photosensitized with CdS nanoparticles was established. The biohybrids exhibited remarkable decolorization effects on triphenylmethane dyes. The highest decolorization rate was 0.206 min −1 . More importantly, enhanced catalytic activities of cadmium sulfide (CdS)-based biohybrids by controlling the particle sizes of semiconductors were demonstrated. Biohybrids systems ( Clostridium thermocellum -CdS) through the self-precipitation of CdS with different particle sizes not only showed dramatic changes in the optical properties but also exhibited a very different decolorization rate. This work can not only further broaden targeted applications of CdS-based biohybrids but also demonstrate a promising route for improving biohybrids corresponding photocatalytic capabilities through in situ precipitation CdS with different particle sizes.
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高影响因子
Journal of Water Chemistry and Technology
·
2022
·Vol. 44
·期 6
·482-487
·
IF 0.484
Ruijia Lan,Su Wenbin,Jia Yanan,Li Jitai
Abstract With the increasingly extensive application of persulfate for water treatment, the development of persulfate detection technology has gradually become a research hotspot. Ferrous ions can catalyze peroxydisulphate (PDS) to produce \({\text{SO}}_{4}^{ - }• \) and \(• {\text{OH}}\) , which oxidize excessive KI to form \({\text{I}}_{3}^{ - }\) . Then \({\text{I}}_{3}^{ - }\) and cationic dye (Basic Blue 54) form ion association complex through electrostatic interaction. These complexes aggregate to form particles with the average size of 362 nm. Formation of ion association particles leads to sharp enhancement of resonance scattering intensity of the system. Based on this principle, a new method for the resonance light scattering determination of peroxydisulphate has been developed, and the optimum reaction conditions, influential factors and applications were investigated. Initial solution pH of 4.5, initial Fe 2+ concentration of 3.0 × 10 –6 mol L –1 , KI concentration of 1.0 × 10 –3 mol L –1 , BB54 concentration of 2.0 × 10 –5 mol L –1 , these conditions were selected as the optimized initial concentration for the detection of PDS. Under the optimal reaction conditions, peroxydisulphate concentrations of 2.5 × 10 –7 –1.8 × 10 –5 mol × L –1 were linearly correlated with the reduction of the resonance light scattering intensity with a correlation coefficient of 0.99 and a detection limit of 7.8 × 10 –8 mol L –1 . This method of measuring PDS shows a higher sensitivity than other methods. The interferences of coexisting substances were also investigated. It has been applied to the analysis of peroxydisulphate in water samples. The recovery rates of the spiked samples were in the range between 91.1–106.2% which showed that the method had high accuracy for the analysis of peroxydisulphate.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2019
·Vol. 43
·期 6
·2162-2171
·
IF 3.343
Wei Li,Shu-ao He,Xiao Wang,Qiong Ma,Chen-hui Zhao
Summary β-iron oxide hydroxide (β-FeOOH) had been proven to be an effective co-catalyst during H 2 evolution reaction (HER) process. In this research, a BiOCl/β-FeOOH heterojunction was successfully synthesized by a solid-state doping method. Then, the structure, composition, and photo-electrochemical properties of the prepared photocatalysts were studied. For the superior HER photocatalytic activity of ultrasmall β-FeOOH nanoparticles (NPs) and the formation of the BiOCl/β-FeOOH heterojunction, this heterojunction photocatalyst exhibited very superior photocatalytic performance in the HER process. Especially, when the amount of incorporated β-FeOOH NPs was appropriate, the BFOH-2 possessed the highest photocatalytic activity in HER process, and the HER rate was about 16.64 mmol·g −1 ·h −1 during illuminated time of 6 hours under visible light. When appropriate, ultrasmall β-FeOOH NPs were implanted into the structure of BiOCl, the BiOCl/β-FeOOH heterojunction interfaces would form for the existence of interfacial interactions. Therefore, this BiOCl/β-FeOOH heterojunction exhibited superior visible-light response, fast photo-carrier migration, and high-efficient separation of photo-carriers, so that the BFOH-2 heterojunction possessed high-efficient hydrogen evolution reaction (HER) photocatalytic activity.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2020
·
IF 1.943
Qingxu Bu,Guan-E Wang,Gang Xu,Xiaojing Long,Yanzhi Xia
Various luminescent organic-inorganic metal halide hybrid materials focus on fluorescence modulation. The commonly method to tunes the luminescence is usually via either modifying the structure of the inorganic anionic or the cation moiety. We here show the first time to modulate the fluorescent emission by inserting neutral organic molecules. The synthesis, crystal structure and optical properties of three organic-inorganic hybrids, [HEV][BiCl 5 ] (1), [MV] 3 [Bi 4 Cl 18 ]·[C 16 H 10 ] (2) and [MV] 3 [Bi 4 Cl 18 ]·[C 20 H 12 ] (3) ([HEV] 2+ = N-proton-N′-ethyl-4,4′-bipyridinium, [MV] 2+ = N,N′-dimethyl-4,4′-bipyridinium) were demonstrated. The compounds contain MV 2+ cations, bismuth (III)-chloro anions and pyrene or perylene molecules achieve fluorescence modulation upon the insertion of neutral molecules.
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SOLAR ENERGY
·
2020
·
IF 4.608
Yi Wei,Huailong Chu,Baoquan Chen,Yuyang Tian,Xichuan Yang,Bin Cai,Yongfei Zhang,Jijun Zhao
Two-dimensional Ruddlesden-Popper perovskites (2D-RPPs) have attracted attention due to their superior moisture stability. In this study, we prepared and characterized a new group of 2D perovskites with cyclohexane methylamine (CMA + ) as a spacer cation. The compounds (CMA) 2 (MA) n−1 Pb n I 3n+1 ( n = 1, 2, 3, and 4) showed high self-assembly (where MA is CH 3 NH 3 ), which allowed for high-quality films to be deposited through the one-step spin-coating method in ambient air. Hot-casting technique, additives, and glove box were not required in the fabrication process. The bandgaps of this group of compounds can be varied from 2.36 eV for (CMA) 2 PbI 4 ( n = 1) to 1.52 eV for MAPbI3 ( n = ∞) with increasing n value. Moreover, we found that the thin films of (CMA) 2 (MA) n−1 Pb n I 3n+1 showed considerable stability in moisture and thermal tests. We successfully inserted these new 2D-RPPs in solar cells, and obtained the best power conversion efficiency of 10.66%, with an open-circuit voltage ( V oc ) of 1.00 V, and a short-circuit current density ( J sc ) of 16.99 mA/cm 2 for our first-generation device containing (CMA) 2 (MA) 3 Pb 4 I 13 ( n = 4). The CMA-based devices exhibited superior long-term stability, the unencapsulated (CMA) 2 (MA) 3 Pb 4 I 13 solar cell retained nearly 95% of its initial efficiency when exposed to ambient conditions with a 60% relative humidity for 1500 h.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jielin Huang,Jing Liu,Lina Tian,Xiangli Li,Xinqi Ma,Xin Yu,Quanhui Guo,Junwei Zhao
Broadband solar light absorption and visible light photocatalysis of surface modified ultrawide bandgap semiconductors are receiving wide attentions because of their more negative conduction band potential and positive valence band potential for refractory organics degradation. Here, we reported a novel modified solvothermal strategy by the introduction of distilled water into small molecular alcohols to synthesize crystallized carbon-coated Zr 3+ -ZrO 2 composites for enhanced visible light absorption and visible light photocatalytic tetracycline degradation, in which the distilled water favored for the crystallization of Zr 3+ -ZrO 2 and the formed ultrathin carbon layers derived from the polymerization of small molecular alcohols were contributing to the generation of Zr 3+ species and well dispersion of Zr 3+ self-doped ZrO 2 nanoparticles. The experimental results also showed that carbon-coated Zr 3+ -ZrO 2 composites exhibited enhanced visible light absorption, long-lived charges, efficient visible light photocatalytic performance and good recyclable stability. Besides, possible photocatalytic mechanism and antibiotic degradation pathways over carbon-coated Zr 3+ -ZrO 2 composites under visible light irradiation were also proposed in detail.
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CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Ziyan Wu,Qiqi Zhang,Binghan Li,Zhifang Shi,Kaimin Xu,Yi Chen,Zhijun Ning,Qixi Mi
All-inorganic metal halide perovskites are noted for their excellent optoelectronic properties and good chemical stability but also a propensity to transform into nonperovskite phases. A case in point is lead-free CsSnCl3, whose perovskite Phase I is metastable at room temperature and could not be stabilized by partial substitution of Cs+ or Cl–. Judging from the radii of the constituent ions of CsSnCl3, we paid attention to octahedral cations smaller than Sn2+ and selected Mn2+ and In3+ for substitution at the B-site. A quantitative structural indicator, volume per formula unit (V/Z), guided the syntheses of CsSn0.9Mn0.1Cl3 (CTMC) and CsSn0.9In0.067Cl3 (CTIC), which are shown by single-crystal X-ray diffraction and differential scanning calorimetry to be homogeneous, stable perovskite phases at room temperature. CTMC turns into a disordered perovskite structure at 193 K, lower than the corresponding transition temperature of CsSnCl3 by nearly 100 K. Vacancies in CTIC result in a more flexible crystal structure than CTMC and CsSnCl3. CTMC and CTIC appear bright yellow with a steep absorption edge at ∼450 nm, and their photoluminescence peaks are located at 645 and 484 nm, respectively, with intensities significantly enhanced from CsSnCl3. Energy transfer processes are proposed to account for the Stokes shifts in the photoluminescence of CTMC and CTIC. Thin films of CTMC glow red under ultraviolet excitation and hold promise for electroluminescence devices. This study gives insights into the structural and electronic effects of ionic substitution in CsSnCl3 and can be extended to other metastable perovskite phases.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Hong Zhang,Xiaoxiang Xu
More than 1.6 eV band gap reductions have been realized on Mg 5 Ta 4 O 15 by nitrogen doping with its pseudobrookite structure maintained. The nitrogen doped Mg 5 Ta 4 O 15 , i.e. Mg 5 Ta 4 O 15-x N y , shows broad absorption in the visible light region and promising photocatalytic activity for both water reduction and oxidation reactions under visible light illumination (λ ≥ 400 nm). Apparent quantum efficiency as high as ~0.90% has been achieved at 420 ± 20 nm on Mg 5 Ta 4 O 15-x N y which is comparable to a number of active metal oxynitrides photocatalysts . Apart from visible light absorption, Nitrogen doping on Mg 5 Ta 4 O 15 is also accompanied by improved surface hydrophilicity and a negative shift of flat band potential. This simple strategy for band gap engineering can be extended to other metal oxides which may open new playgrounds in the design and development of efficient visible light active photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Lei Wang,Jafar Ali,Zhibin Wang,N.A. Oladoja,Rong Cheng,Changbo Zhang,Gilles Mailhot,Gang Pan
Nanobubbles have gained much attention due to their unusual properties such as large specific surface area, surface energy and internal energy, thereby, increase the surface reaction and improve the mass transfer efficiency. The long term stability of nanobubbles and generation of reactive oxygen species enables them to address various environmental issues for water purification without secondary pollution. However, there are few studies concerning the application of oxygen nanobubbles in the advanced oxidation processes (AOPs). In this study, first time, oxygen nanobubbles were introduced into the photoreaction system under visible light irradiation for enhanced photodegradation of oxytetracycline (OTC). Results indicated that oxygen nanobubbles significantly improved the photodegradation of OTC through high mass transfer and generation of reactive radicals during the nanobubble collapse. The oxygen nanobubble stability was confirmed to be pH dependent. The nanobubbles concentration increased from 0.76 to 3.78 × 10 8 particles/mL, while the mean size decreased from 205 nm to 138 nm as the pH value increased (3.2–11.0). The photodegradation efficiency of OTC was improved from 45% to 98% with the increase of pH (4.0–11.0). Oxygen nanobubbles hold promise to improve the AOPs , such as reducing catalysts and chemicals usage and costs. Quenching experiments demonstrated that OH was the predominant active species induced the photodegradation of OTC. With the development of nanobubbles technology, it is anticipated to realize totally chemicals free green technology. This study provides a novel nanobubble/AOPs technology, which will be more efficient and environmental friendly and will have broad application in waste water treatment and drinking water purification.
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