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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2020 ·Vol. 413 ·期 1 ·193-203 · IF 3.637

Ultrasensitive photoelectrochemical aptasensor for diclofenac sodium based on surface-modified TiO2-FeVO4 composite

Yang Liwei,Li Lele,Li Fen,Zheng Hejie,Li Tongtong,Liu Xiaoqiang,Zhu Jichun,Zhou Yanmei,Alwarappan Subbiah

Herein, a photoelectrochemical (PEC) aptasensing platform was designed by integrating surface oxygen vacancy (OV) defects, Ti 3+ self-doping, the heterojunction, and resonance energy transfer (RET) effect into one platform for the detection of diclofenac sodium (DCF). Briefly, OV defects were introduced on TiO 2 nanospheres with simultaneous Ti 3+ self-doping, followed by a well-separated deposition of FeVO 4 nanoparticles on TiO 2 to obtain a Ti 3+ -O-TiO 2 /FeVO 4 heterojunction. The surface modification of OVs, Ti 3+ doping, and deposition of FeVO 4 were confirmed by SEM, XPS, EPR, DRS, and PEC measurements. The surface OVs and doping of Ti 3+ species created a new donor (defect) energy level under the conduction band of TiO 2 , which minimized the bandgap and thereby improved the visible light absorption of TiO 2 . Moreover, the capture of photo-excited electrons by surface OVs could hinder the electron-hole recombination. Due to the intimate surface contact and perfect energy matching between TiO 2 and FeVO 4 , the formation of heterojunction decreased the bandgap and facilitated the electron-hole separation of TiO 2 . All these above events contributed to the enhancement of the PEC signals, which were then quenched by the RET effect between Ti 3+ -O-TiO 2 /FeVO 4 and Au nanoparticle (AuNP)–labeled cDNA that had been attached to its complementary DCF aptamer on Ti 3+ -O-TiO 2 /FeVO 4 |ITO. The addition of target-DCF detached AuNP-labeled cDNA from the electrode to recover the photocurrent, resulting in a “signal-on” PEC aptasensor that exhibited a 0.1–500-nM linear range and a detection limit of 0.069 nM for DCF, attributed to the excellent amplification of the proposed aptasensing platform.

研究领域: 分析化学 · 环境科学 · 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Nitrogen doping mediated oxygen vacancy and Ti valence regulation to enhance photocatalytic H2 generation

Lei Dai,Peng Fu,Jieming Chen,Fazhe Sun

The band gap width has always been the main reason for the low photocatalytic performance of TiO 2 semiconductors. “Band gap engineering” is often used to change the band gap width of TiO 2 . On this basis, the impurity band gap was induced below the TiO 2 conduction band by regulating N element. What's interesting was that N element adjusted the valence state of adjacent Ti element and caused the generation of oxygen vacancy . This is due to the extraction of neutral oxygen atoms, resulting in electron transfer to the Ti cation band structure . The 300-N-T catalyst exhibited the best photocatalytic hydrogen production performance under visible light, which was 307.65 μmol/(g·h) and was 61.53 times higher than that of anatase. And the concentration of Ti 3+ defects and oxygen vacancy reduced with decreasing of N content in TiO 2 . According to Kubelke Munk formula, the band gap of 300-N-T photocatalyst was narrowed to 2.73 eV, which indicated that there are impurity energy levels near the CB and VB of TiO 2 material. The Ti 3+ ions as the active site of the photocatalytic reaction was confirmed by instantaneous photocurrent response and EIS characteristic. This study revealed the structure-activity relationship between the content of N element, Ti 3+ ions and oxygen vacancy in TiO 2 materials, as well as the decisive process of defect induced visible light catalysis.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 催化 · 光催化 · 能源材料
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APPLIED CATALYSIS A-GENERAL · 2020 · IF 5.006

Silica/titania composite-supported NiCo catalysts with combined catalytic effects for phenol hydrogenation under fast and mild conditions

Yucheng Li,Jing Liu,Jing He,Luying Wang,Jiandu Lei

The effect of titanium as a promoter for the nickel-cobalt/silica-titania (NiCo/Si-Ti) catalyst in the hydrogenation of phenol was comparatively studied. In the phenol hydrogenation under mild reaction conditions (1 MPa H 2 pressure and 100 °C), the Ti-promoter induces the formation of the Co δ− −O V −Ti 3+ active sites and enhances the hydrogenation activity of the NiCo/Si catalyst to convert phenol to cyclohexanol. The catalytic hydrogenation with the optimal composition of the NiCo/Si-1.0Ti (Si:Ti ratio of 8.5:1) catalyst was completed within 1 h (conversion 98.2 % and selectivity >99 %), which was more efficiently than that with other Ti-doped catalysts and NiCo/Si as baseline, indicating a strong positive synergistic effect between the metal (Ni-Co) and support (Ti-Si) components of the catalyst in this reaction. Additionally, the kinetics, pathway and catalytic mechanism of the hydrogenation of phenol are also examined. Furthermore, the NiCo/Si-1.0Ti catalysts also showed a good performance at reducing the unstable oxygenated compounds in the bio-oil.

CAS / MDL: 142-82-5
研究领域: 催化 · 化学工程 · 材料科学
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Small · 2023 ·Vol. 19 ·期 38 ·2302831 · IF 13.3

Introducing Hybrid Defects of Silicon Doping and Oxygen Vacancies into MOF-Derived TiO2–X@Carbon Nanotablets Toward High-Performance Sodium-Ion Storage

Tianhao Yao,Hongkang Wang,Xin Ji,Deyu Wang,Qingmiao Zhang,Lingjie Meng,Jian-Wen Shi,Xiaogang Han,Yonghong Cheng

Titanium dioxide (TiO 2 ) is a promising anode material for sodium–ion batteries (SIBs), which suffer from the intrinsic sluggish ion transferability and poor conductivity. To overcome these drawbacks, a facile strategy is developed to synergistically engineer the lattice defects (i.e., heteroatom doping and oxygen vacancy generation) and the fine microstructure (i.e., carbon hybridization and porous structure) of TiO 2 -based anode, which efficiently enhances the sodium storage performance. Herein, it is successfully realized that the Si-doping into the MIL-125 metal-organic framework structure, which can be easily converted to SiO 2 /TiO 2–x @C nanotablets by annealing under inert atmosphere. After NaOH etching SiO 2 /TiO 2–x @C which contains unbonded SiO 2 and chemically bonded Si  O  Ti, thus the lattice Si-doped TiO 2–x @C (Si-TiO 2–x @C) nanotablets with rich Ti 3+ /oxygen vacancies and abundant inner pores are developed. When examined as an anode for SIB, the Si-TiO 2–x @C exhibits a high sodium storage capacity (285 mAh g −1 at 0.2 A g −1 ), excellent long-term cycling, and high-rate performances (190 mAh g −1 at 2 A g −1 after 2500 cycles with 95.1% capacity retention). Theoretical calculations indicate that the rich Ti 3+ /oxygen vacancies and Si-doping synergistically contribute to a narrowed bandgap and lower sodiation barrier, which thus lead to fast electron/ion transfer coefficients and the predominant pseudocapacitive sodium storage behavior.

研究领域: 材料科学 · 能量存储 · 纳米技术 · 电池技术
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OPTICAL MATERIALS · 2022 · IF 3.754

Pd nanoparticle-modified TiO2-x composites as efficient visible-light active photocatalysts for tetracycline degradation and microbial disinfection

Jingtao Zhang,Mengwan Zhai,Xueying Wang,Shurui Liu,Lijuan Zhang,Xing Liu,Yao Geng,Xiaodong Sun,Bingkun Liu

In the present work, Ti 3+ -self-doped TiO 2 heterostructure photocatalysts were prepared by coupling with different additions of palladium quantum dots by means of deposition-reduction methodology. The electron paramagnetic resonance (EPR) analysis indicated the existence of Ti 3+ in synthesized samples. The transmission electron microscopy (TEM) images presented the modification of TiO 2-x nanoparticles by coupling with nano palladium. Photoluminescence (PL) results demonstrated the lowest charge carrier recombination rate in 5% Pd/TiO 2-x composites. Photocatalytic performances of photocatalysts were evaluated by degrading Tetracycline (TC) and inactivating Escherichia coli ( E. coli ) and Fusarium oxysporum f. sp. Vasinfectum ( Fov ) with the presence of visible light , in which an enhanced photocatalytic degradation and inactivation activity was found in all Pd coupled composites with the highest efficiency in 5% Pd/TiO 2-x . The improved photocatalytic activity of Pd/TiO 2-x was associated to the generation of more hydroxyl radicals (•OH) and superoxide anions radicals (•O 2- ) during photocatalytic process which were demonstrated by the electron spin-resonance spectroscopy (ESR) technique. Moreover, 5% Pd/TiO 2-x composites were found to remain high photocatalytic properties in a circulating photo-disinfection system.

研究领域: 材料科学 · 环境科学 · 纳米技术 · 光催化 · 水处理
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