Small
·
2021
·Vol. 18
·期 6
·2103528
·
IF 13.281
Bijiang Geng,Shuang Xu,Ping Li,Xiaokai Li,Fuling Fang,Dengyu Pan,Longxiang Shen
Sonodynamic therapy as a promising noninvasive modality is being developed for tumor therapy, but there is a lack of next-generation sonosensitizers that can generate full ROS at high yields and simultaneously deplete elevated levels of glutathione (GSH) in tumor cells. Semiconductor p-n junctions are engineered as high-efficacy sonosensitizers for sonodynamic tumor eradication using pyridine N-doped carbon dots (N-CDs) as a p -type semiconductor and oxygen-deficient TiO 2− x nanosheets as a n -type semiconductor. The rate constants of 1 O 2 and •OH generation by ultrasound-excited N-CD@TiO 2− x p-n junctions are 4.3 and 4.5 times higher than those of TiO 2 , respectively. A Z-scheme carrier migration mechanism in the p-n junction achieving the rapid spatial separation of the ultrasound-generated electron–hole pairs for enhanced full ROS production is proposed. GSH-cleavable, Pt-crosslinked, N-doped CD fluorescent probes to detect the presence of intracellular GSH are also constructed. A GSH-responsive, p-n junction platform (Pt/N-CD@TiO 2− x ) with integrated GSH detection, GSH depletion, and enhanced sonodynamic performance is then assembled. Malignant tumors are completely eradicated without relapse via intravenous administration of low-dose Pt/N-CD@TiO 2− x under ultrasound irradiation. This work substantiates the great potential of biocompatible, GSH-responsive p-n junctions as next-generation sonosensitizers via p-n junction-enhanced ROS generation and metal ion oxidation of intracellular GSH.
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Advanced Science
·
2023
·Vol. 11
·期 5
·2305439
·
IF 15.1
Fucheng Zhang,Huanhuan Dong,Yi Li,Dengjiang Fu,Lu Yang,Yupeng Shang,Qiuyang Li,Yuwen Shao,Wu Gang,Tao Ding,Tao Chen,Wenkun Zhu
Photo-assisted uranium reduction from uranium mine wastewater is expected to overcome the competition between impurity ions and U(VI) in the traditional process. Here, B-TiO 2 @Co 2 P-X S-scheme heterojunction with metal-oxygen-hydrogen (M-O-H) is developed insitu modification for photo-assisted U(VI) (hexavalent uranium) reduction. Relying on the DFT calculation and Hard-Soft-Acid-Base (HSAB) theory, the introduction of metal-oxygen-hydrogen (M-O-H, hard base) metallic bonds in the B-TiO 2 @Co 2 P-X is found to enhance the hydrophilicity and the capture capability for uranyl ion (hard acid). Accordingly, B-TiO 2 @Co 2 P-500 hybrid nanosheets exhibit excellent U(VI) reduction ability (>98%) in the presence of competing ions. By self-consistent energy band calculations and in-situ KPFM spectral analysis, the formation of the internal electric field between B-TiO 2 and Co 2 P at the heterojunction is proven, offering a strong driving force and atomic transportation highway for accelerating the S-scheme charge carriers directed migration and promoting the photocatalytic reduction of uranium. This work provides a valuable route to explore the functionally modified photocatalyst with high-efficiency photoelectron separation for U(VI) reduction.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2023
·
IF 4.1
Tingting Du,Congzhi Hu,Yuye Li,Youyong Pang,Ming Li,Botian Liu,Ling Li,Yongping Liu,Huidan Lu,Bin Huang
This paper discusses the photocatalytic properties of Ag/Ag 3 PO 4 /Ti 3+ -TiO 2 composites. The nanostructured composites were synthesized by gas-phase hydrolysis, precipitation, and photoreduction methods. The photocatalytic performance of the photocatalysts was evaluated by degrading RhB and TC under visible light. The degradation efficiency of AT4 for RhB and TC reached 99.9 % and 78.2 % under visible light irradiation for 20 min and 2.5 min, respectively. The superior performance of AT4 is facilitated by the combined influence of the heterojunction and the SPR . The free radical capture test proved that h + and •O 2 − were the major reactive groups, and in conjunction with UV–vis DRS curves and Mott-Schottky curves, a probable reaction mechanism was proposed.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Deqing Zhang,Yingfei Xiong,Junye Cheng,Hassan Raza,Chuanxu Hou,Tingting Liu,Xuewei Ba,Ping Zhang,Maosheng Cao
As a novel 2D transition metal sulfide material, WS 2 has been proven to possess potential electromagnetic wave absorption (EMWA) property due to its peculiar electronic structure. However, the intrinsic weak impedance match and single dielectric loss domination of this material only produce high-frequency electromagnetic absorption (EMA), which is seemingly futile for the prevalent low-band 4G and 5G EMW. In this study, efforts have been made to effectively texture rod-like TiO 2 semiconductor with different mass ratios on the a few layers of WS 2 nanosheets via a simple step-by-step hydrothermal method. It is found that the WS 2 /TiO 2 hybrids loaded with 10% TiO 2 at a sample thickness of 5.30 mm, the minimum RL is −43.90 dB at 5.12 GHz. When the thickness of the sample is 2.00 mm, the bandwidth with RL value less than −10 dB can reach 4.70 GHz, and the effective EMA band could be adjusted in a range of 13.84 GHz (4.16–18 GHz) by increasing the thickness from 1.0 mm to 5.5 mm. It was found that the introduction of TiO 2 nanosheets with high dielectric loss into the dielectric WS 2 nanosheets can produce a synergistic effect. The benefits of such synergestic effect include, optimization of the EMA strength and bandwidth, and a reduction of the effective EMA frequency band from high frequency to low frequency. This study paves a new avenue for the future design of low-frequency EMA materials with high efficiency.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Chencheng Dong,Yan Bao,Tian Sheng,Qiuying Yi,Qiaohong Zhu,Bin Shen,Mingyang Xing,Irene M.C. Lo,Jinlong Zhang
Sulfate-radical (SO 4 − ) based Advanced Oxidation Process (SR-AOP), which is mainly generated from peroxymonosulfate (PMS) activation, is an excellent route for water treatment. Bimetallic nanoparticles have been widely applied in electronic, chemical, biological, and mechanical fields, etc.; however, few researchers have attempted to adopt bimetallic nanoparticles in environmental remediation. Further, in recent years, element molybdenum (Mo) has addressed much more environmental field attention than ever. Although singlet oxygen ( 1 O 2 ) generated commonly in SR-AOPs, its generation mechanism remains controversial. Hence, in this work, bimetallic MoFe/TiO 2 nanospheres were rationally constructed via a facile two-step methodology. Undoubtedly, it exhibited superior performance for the degradation of organic pollutants (e.g., rhodamine, phenol, 4-chlorophenol and sulfadiazine) irradiated by simulated solar light. Both photo-generated electrons and transition metallic redox couples (i.e., Mo 6+ /Mo 4+ , Fe 3+ /Fe 2+ and Mo 4+ /Fe 3+ ) play vital roles in the PMS activation. Distinct from conventional SR-AOPs, sulfate radicals (SO 4 − ), hydroxyl radicals ( OH) and peroxymonosulfate radicals (SO 5 − ) indeed participate in the transformation and generation of singlet oxygen ( 1 O 2 ). With the combination of DFT calculation, the Mo sites on the bimetallic MoFe (110) facet are more favorable to adsorb PMS molecules, then followed by the dissociation of PMS progressing on the Mo sites. Electrons transferring from the Mo atoms to the Fe atoms facilitated the adsorption of the negatively charged HSO 5 - anions, resulting in enhanced PMS activation efficiency. Considering its novelty and generation mechanism, this work highlights the mechanism of 1 O 2 generation from PMS reduction and oxidation simultaneously and furnishes theoretical support for further relevant studies.
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OPTICAL MATERIALS
·
2021
·
IF 3.08
Kun Jiang,Jin Zhang,Yingfei Wan,Zengjian Liu,Jinwei Chen
In order to obtain the advanced photocatalyst with high performance for removing the gaseous formaldehyde, a new strategy with amination of titanium dioxide (TiO 2 ) and combination with reduced graphene oxide (rGO) is proposed in this work. TiO 2 was first aminated into amino-TiO 2 and then combined with rGO by an electrostatic self-assembly process to form the amino-TiO 2 /rGO photocatalysts. The structure and morphology were characterized by XRD , FTIR, and SEM, respectively. Physicochemical properties were measured by EIS, XPS , ESR , PL , and photocurrent measurements. The mechanism of the photocatalytic reaction was studied. Optimal amino-TiO 2 /rGO catalyst exhibits high catalytic activity and recyclability. The reaction rate constant of HCHO over this catalyst is approximately 9.8 × 10 −3 L mol −1 ·min −1 , which is 10.5 times higher than that of the commercial Degussa P25 TiO 2 . The analysis results from XPS and ESR indicates that the high catalytic activity could be mainly attributed to the imine formed by chemisorption of amino and HCHO. The reaction speed of formaldehyde photolysis increases as the concentration of HCHO on the photocatalyst surface increased. In addition, the introduction of graphene enhances carrier separation efficiency so that leads to more reactive radicals such as hydroxyl radicals (·OH) and superoxide radicals (·O 2 − ), leading to improved performance on formaldehyde photolysis. This could provide a useful method for highly efficient formaldehyde photocatalysis .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yi Yu,Fanfan Li,Xinghao Han,Shanghai Long,Shishuai Shi,Li Xu,Guoji Liu
2-Naphthaldehyde is industrially produced from 2-naphthalene nitrile and 2-naphthoyl chloride in acid. Greener gas-solid catalytic oxidation of 2-methylnaphthalene to 2-naphthaldehyde has rarely been investigated. In this study, the preparation of 2-naphthaldehyde over V/TiO2 catalysts doped with 13 metal promoters was explored and the V-Cu(1)/TiO2 catalyst showed excellent performance with 63.37% 2-methylnaphthalene conversion and 70.09% 2-naphthaldehyde selectivity at 400 °C, gas hourly space velocity (GHSV) of 10 000 h–1, and feed flow rate of 3.87 × 10–4 mol·h–1, giving the highest turnover frequency (TOF) value of 17.05 × 10–6 s–1. We have consequently studied the effect of Cu doping on the physicochemical properties of the V/TiO2 catalyst and found that structural changes are not the main reason to improve the catalytic performance. Increased vacancies and oxygen mobility accelerate the formation of nucleophilic oxygen from electrophilic oxygen, which are the key factors to improve 2-NA selectivity. The synergy between V, Cu, and O through the V–O–Cu bridging bond also improves the weak acid ratio, redox ability, and the reactivity of active sites (bridging and terminal oxygen). X-ray photoelectron spectroscopy (XPS), in situ diffuse-reflectance infrared Fourier transform (DRIFT) spectroscopy, and density-functional theory (DFT) calculations have proved that this reaction obeys the Mars–van Krevelen mechanism and involves a reduction process of V5+ and Cu2+ during oxidation.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Nuo Duan,Qian Li,Xiangyi Meng,Zhouping Wang,Shijia Wu
A nano-composite film was prepared from k-carrageenan (KC), konjac glucomannan (KGM) and TiO 2 nanoparticles (NPs) by solvent casting method. The morphology and structure of the KC/KGM based nano-composite films prepared from different weight ratio of TiO 2 NPs were characterized by SEM, XRD and FT-IR techniques. The addition of TiO 2 NPs to KC/KGM films improved the mechanical, thermal, structural, and barrier properties of nano-composite films. In particular, the film containing 7 wt% of TiO 2 NPs exhibited effective photocatalytic anti-fungal activity (79%) for Penicillium viridicatum after irradiating 6 h through generating reactive oxygen species thus destroying the fungi. Benefitting from the improved characteristics investigated above, the nano-composite films showed a favorable effect on strawberry storage. Overall, the fabricated KC/KGM/TiO 2 nano-composite films have a broad application in the field of food preservation and packaging applications.
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高影响因子
Catalysts
·
2021
·Vol. 11
·期 5
·533
·
IF 4.146
Jing Chen,Yingchun Guo,Tengteng Kang,Xingchi Liu,Xiaomei Wang,Xu Zhang
It is wise to mimic a bioinspired system to design a nanoreactor as a catalyst containing multiple components for a cascade reaction. Here, we report the uniform growth of well-dispersed nano-scale ZIF-8 crystals on the pore walls of 3DOM TiO2via the TEA-assisted crystallization process. The UV-vis spectra indicate that the ZIF-8 photosensitizer can extend the visible-light absorption of 3DOM TiO2. The obtained nanoreactor can efficiently catalyze the one-pot aromatic alcohol oxidization and Knoevenagel condensation cascade reaction for larger molecules. This work offers an important strategy for preparing semiconductor–MOF multifunctional composites with a spatially separated compartmentation for the cascade reaction.Keywords:crystal growth;cascade reaction;nanoreactor;semiconductor–MOF composite
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 28
·期 10
·12459-12473
·
IF 3.056
Guo Tongtong,Yang Shuang,Chen Yunning,Yang Lu,Sun Yingnan,Shang Qingkun
In this paper, the kinetic characteristics and cycle stability of Fe-complex/TiO 2 in the process of degradation of phenolic pollutants and reduction of heavy metal Cr(VI) were studied systematically. First, the structural characteristics and photocatalytic activities of Fe(III)-(8-hydroxyquinoline-5-carboxylic acid)-TiO 2 (Fe-HQC-TiO 2 ) nanoparticle to degrade phenolic pollutants and reduce Cr(VI) simultaneously had been investigated. Compared with the single degradation, the efficiency of synergistic degradation/reduction had been improved and the degradation/reduction rate had been obviously accelerated. In particular, the cyclic stability of Fe-HQC-TiO 2 photocatalyst decreased obviously when it was used to reduce Cr(VI) alone, but it could still keep above 90% after three cycles when it was used for reduction of Cr(VI) and degradation of phenol synergistically. Second, to Fe-HQS/TiO 2 nanoparticle or Fe-HQS/TiO 2 nanotube (HQS (8-hydroxyquinoline-5-sulfonic acid)), the synergistic degradation/reduction (2,4-dichlorophenol/Cr(VI)) efficiencies were always greater than those of a single degradation/reduction and the time was greatly reduced. All the results indicated that there were interactions between Cr(VI) and phenol or 2,4-dichlorophenol in the photocatalytic process. The possible mechanism of synergistic accelerated degradation of phenolic compounds and reduction of Cr(VI) was proposed by analyzing and testing the surface characteristics of photocatalyst and the properties of photocatalytic system during the synergistic degradation/reduction.
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Chemosensors
·
2020
·Vol. 8
·期 3
·70
·
IF 3.108
Zirong Qin,Jinyan Zhang,Ying Liu,Jingtao Wu,Guangli Li,Jun Liu,Quanguo He
In this work, we report a simple but efficient voltammetric sensor for simultaneous detection of ponceau 4R and tartrazine based on TiO2/electro-reduced graphene oxide nanocomposites (TiO2/ErGO). TiO2/ErGO nanocomposites were prepared by ultrasonically dispersing TiO2nanoparticles (TiO2NPs) into graphene oxide (GO) solution followed by a green in-situ electrochemical reduction. TiO2NPs were uniformly supported on ErGO nanoflakes, which provides a favorable interface for the adsorption and subsequent oxidation of target analytes. TiO2/ErGO showed remarkable electrocatalytic capacity for the oxidation of ponceau 4R and tartrazine, with minimized oxidation overpotentials and boosted adsorptive striping differential pulse voltammetric (AdSDPV) response peak currents. Under the optimal experimental conditions, the anodic peak currents of ponceau 4R and tartrazine increase linearly with the respective natural logarithm of concentrations from 0.01 to 5.0 μM. The detection limits (LOD = 3σ/s) for ponceau 4R and tartrazine are 4.0 and 6.0 nM, respectively. The extraordinary analytical properties of TiO2/ErGO/GCE are primarily attributed to the synergistic enhancement effect from ErGO nanoflakes and TiO2NPs. Moreover, the proposed TiO2/ErGO/GCE achieves reliable determination of ponceau 4R and tartrazine in orange juice with excellent selectively, reproducibility and stability. Together with simplicity, rapidness, and low cost, the proposed sensor demonstrates great potential for on-site detection of azo colorants.Keywords:ponceau 4R;tartrazine;TiO2;electro-reduced graphene oxide;voltammetric sensor
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 36
·45605-45617
·
IF 3.056
Zhou Anran,Wang Yonglei,Sun Shaohua,Xin Xiaodong,Wang Mingquan,Zhao Qinghua,Zhu Huanhuan,Jia Ruibao
The addition of Fe 3+ to TiO 2 is one of the effective methods to inhibit the recombination of photogenerated electrons and holes and thus improve the photocatalytic activity of TiO 2 . The effect of PVDF-PVP-TiO 2 -FeCl 3 (PPTFe) membrane filtration-photocatalytic system on the removal of trace concentration of sulfadiazine (SD) in water was evaluated. A two-factor four-level experiment was established to optimize 16 self-made modified membranes. The optimal membrane was then characterized in seven tests (SEM, EDS, membrane pure water flux, contact angle, porosity, mean pore size, ATR-FTIR), resulting in the optimal ratio (PPTFe membrane with 1.2 wt%TiO 2 and 0.8 wt%FeCl 3 ). Compared with the original membrane, the pore number, pore size, permeability, and hydrophilicity of the PPTFe membrane were all enhanced. The removal efficiency (92.63%) of SD by PPTFe membrane filtration-photocatalysis system was investigated. The reaction rate (0.0214 min −1 ) of the removal SD of the system was determined according to the pseudo-first-order kinetic model. The removal performance of membrane type, pH, and water quality parameters (Cl − , SO 4 2− , NO 3 − , HA) on PPTFe membrane filtration-photocatalytic system were also made a deep inquiry. The results reflected that acidic conditions (pH = 3) were beneficial to SD removal, the presence of Cl − , SO 4 2− , and HA could inhibit SD removal, while the existence of NO 3 − was unaffected. Furthermore, the removal rate of SD in the actual water body was displayed well in this system. Finally, the possible photocatalytic degradation mechanism was proposed. Graphical abstract
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