Journal of Materials Chemistry B
·
2018
·Vol. 6
·期 45
·7503-7510
·
IF 4.776
Huan Liu,Luping Feng,Yuanyuan Cai,Yue Hua,Min Liu,Mengyuan Yin,Shuai Li,Xiaoxia Lv,Jiangwei Wen,Hua Wang
An ultrasensitive and high-throughput visualized colorimetric method has been initially developed with a wettable microwells array for probing guanine base-containing anthrax DNAs in blood based on silver deposition amplified by the synergic TiO2 photocatalysis and guanine photoreduction under visible light. Hydrophilic microwells were first created on the hydrophobic slides to yield the wettable microwells array, on which photocatalytic titanium dioxide (TiO2) nanoparticles were deposited with dopamine (DA) to yield TiO2@DA for anchoring single strand DNA (ssDNA) capture probes without guanine bases. After the hybridization of the targeted anthrax DNAs, exonuclease I (Exo I) was introduced into the microwells to selectively digest the unhybridized ssDNA probes. The silver deposition was further conducted by the synergic photocatalysis of TiO2@DA and photoreduction of guanine bases of anthrax DNAs, thus achieving the amplified silver signals for the visualized colorimetric assays. Moreover, benefitting from the wettability feature of the hydrophilic–hydrophobic interfaces of the microwells array so fabricated, DNA analytes could be accumulated from the sample droplets through the condensing enrichment process to realize the ultrasensitive detection, in addition to circumventing any crossover contaminants between the sample droplets. The developed visualized colorimetric method with the microwells array was subsequently applied for probing anthrax DNAs in blood with levels down to 1.0 fM. DNAs with single-base and double-base mutations could also be identified accurately. Importantly, such a biosensing design route of a wettable microwells array, in combination with the photocatalytic silver deposition and specific Exo I-catalytic probe digestion, may promise extensive applications for the high-throughput, ultrasensitive, and selective detection of guanine-containing DNA targets with ultra-trace levels in complicated samples like blood.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Zihan Tian,Yumei Xu,Qingyu Liu,Xiao Wu,Shuhao Qin,Jing Zhang,Hong Wang,Jianxin Li,Zhenyu Cui
The ridge-like PVDF/CQDs-TiO 2 @CQDs hybrid piezo-photocatalytic film was fabricated via an " in situ hydrothermal-vapor induction" method, in which the S-scheme TiO 2 @CQDs heterostructures were grown in situ and uniformly immobilization onto the polyvinylidene fluoride (PVDF) film surface through Ti-F coordination bonds. The effects of hybrid film morphology, carbon quantum dots (CQDs) doping, and flow rate on piezo-photocatalytic degradation performance were investigated. The ridge-like microstructure increased the exposure of adsorption and catalytic active sites. The film reactor driven by the flow of dye solution and light illumination promoted the adsorption of pollutants while establishing a dual built-in electric field (IEF) between the piezoelectric PVDF and catalysts, TiO 2 and CQDs, which accelerated photogenerated charge transfer and separation. Finally, a dynamic piezo-photocatalytic process was realized for the efficient and synergistic degradation of RhB. The reaction rate constant ( ks ) of the dynamic piezo-photocatalytic degradation was about 2.3 times that of the static photocatalytic process. Structural optimization and density functional theory (DFT) calculations of Rhodamine B (RhB) molecules were performed using Gaussian software. The degradation products, degradation pathways, and degradation mechanisms of RhB were thoroughly studied by combining the results of total organic carbon (TOC), DFT and liquid chromatography mass spectrometry (LC-MS).
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Hongxu Liu,Junhao Xie,Jingxuan Zhao,Ruijia Wang,Yuchao Qi,Ziwei Lv,Yang Yu,Shulin Sun
The industrial wastewater filtered by water treatment membranes is very complex in practical applications, therefore, it is a challenge to prepare a membrane with large pore size and high flux that can efficiently separate various wastewater containing pollutants of different scales. To solve this problem, an SA-TiO 2 hydrogel-coated PVDF-g-IL composite fibre membrane with super hydrophilicity, anti-pollution, and pH-responsive self-cleaning properties has been designed and prepared by electrostatic spinning and layer-by-layer coating techniques in the present work. The super hydrophilic gel layer on the surface gives the composite membrane efficient separation capability while maintaining rapid passage of the aqueous phase; the underlying PVDF-g-IL fibre membrane is positively charged and removes not only anionic/cationic pollutants by electrostatic repulsion or attraction but also creates an ionic bond with oppositely assigned SA so that the gel layer tightly bond to the base membrane. The PVDF-g-IL@SA-TiO 2 membrane achieves stable and efficient separation of oil-water emulsions and dye wastewaters with a high filtration flux while retaining a retention rate higher than ∼95%. After multiple self-cleaning cycles, the ultra-thin gel layer still offers satisfactory durability with ≈100% flux recovery. This study provides a promising new strategy for designing efficient multiple contaminant separation and simpler self-cleaning membranes.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
·
IF 8.2
Xin Jiang,Kaiwei Li,Yimin Tang,Xiuwen Wang,Wei Kan,Libin Yang,Bing Zhao
High-performance flexible semiconductor material can be used as an excellent multifunctional matrix for in-situ ultrasensitive surface-enhanced Raman scattering (SERS) detection and synchronous photocatalytic degradation of antibiotic residues in aquatic ecosystem. Here, a calcium-doped TiO 2 flexible matrix with double defects (surface oxygen vacancy defect and Ti 3+ energy level defect) was developed by its “in-situ one-step” hydrothermal synthesis on cotton fabric for the above purposes. Due to the joint contribution of double defects, a multi-channel charge transfer mode and a high-efficiency carrier separation are achieved, which endows flexible cotton fabric/Ca-doped TiO 2 (Cot/Ca-TiO 2 ) substrate with the greatly boosted SERS effect for in-situ detection of antibiotic residues on fish body surface and in fishpond water by a simple wiping or dipping sampling method, even for simultaneous identification of multi-component residues. The detection limits of three antibiotic residues (enrofloxacin, ciprofloxacin and enoxacin) are as low as 10 −9 M, which are far lower than the EU standard. More meaningfully, the flexible Cot/Ca-TiO 2 can be used as a multifunctional filter-membrane type photocatalyst for efficient on-site degradation of antibiotic residues in flowing fishpond water by a multi-grade photocatalysis means. Moreover, the flexible matrix exhibits good recyclability in both actual detection and photocatalysis.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Yong Shi,Xin Lan Ma,Jin Suo Gao,Feng Yun Yu,Chun Yan Li,Wei Xiong,Li Ping Huang
The catalytic activity, adsorption and synergistic effect over bimetallic MOF derivatives with different dopant metal were systemically compared. A series of Me-Cu/TiO 2 (Me=Fe, Co, Ni) derived from bimetallic Me/Cu-BTC MOFs were fabricated via a sacrificing template method and applied for CO-SCR. Among the bimetallic catalysts, Fe-Cu/TiO 2 presented the best low-temperature of nearly 100% NO conversion from 150 °C to 350 °C with good NO selectivity. For Me-Cu/TiO 2 (Me=Fe, Co, Ni), the productions of crucial Cu + intermediate were determined to be 51.17%, 50.45%,49.4% by XPS, which were consistent with their catalytic activity results. The superior redox behavior of Fe-Cu/TiO 2 can be attributed to its higher Oβ / (Oα +Oβ) ratio of 32.90% and the higher Me 2+ / Me 3+ ratio of 1.79. In situ infrared analysis revealed that the Fe doping not only improved the formation and stability of nitrate species, but also enhanced the quantity of Lewis acid sites by forming Cu + -CO. Furthermore, a possible low-temperature Langmuir-Hinshelwood (L-H) mechanism over Me-Cu /TiO 2 (Me=Fe, Co, Ni) was proposed.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3856
·
IF 4.2
Xiaoxue Liu,Lanfen Zhang,Jian Hu,Wei Zhang,Xiaorong Xiang,Huiqing Cheng,Li Qin,Hao Li
In recent years, TiO2-based catalysts have received extensive attention from researchers for their excellent oxidative desulfurization (ODS) performances. In this paper, a series of mesoporous TiO2/SiO2catalysts with different TiO2loadings are prepared, using an incipient wetness impregnation method with agricultural waste rice husk as both the silicon source and mesoporous template and tetrabutyl titanate as the titanium source. The effect of different TiO2loadings on the ODS performance of the samples is investigated, and the appropriate TiO2loading is 2.5%. Compared with pure TiO2, the 2.5%TiO2/SiO2sample exhibits high catalytic activity for oxidative desulfurization. This is, on the one hand, due to the high specific surface area and mesopore volume of the 2.5%TiO2/SiO2sample. On the other hand, it is due to the uniform dispersion of TiO2grains with an average diameter of 6.1 nm on the surface of the mesoporous SiO2carrier, which greatly increases the active sites of the 2.5%TiO2/SiO2sample, thus improving the catalytic activity of the sample. The recycling performances of the 2.5%TiO2/SiO2sample are further investigated. The results show that, after fifteen cycles, the 2.5%TiO2/SiO2sample still maintains high conversions of dibenzothiophene (99.8%) and 4,6-dimethyldibenzothiophene (99.7%) without deactivation. In addition, the 2.5%TiO2/SiO2sample treated with TBHP aqueous solution is characterized by the technique of UV-Vis, and the Ti-peroxo (Ti-OOtBu) species, the active intermediate for the ODS of bulky organic sulfides, is successfully captured. Finally, a possible reaction mechanism for the ODS process over the 2.5%TiO2/SiO2sample is proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhilei Guo,Guohua Jing,Sara A. Tolba,Chung-shin Yuan,Yu-Hua Li,Xiaowei Zhang,Zhiwei Huang,Huawang Zhao,Xiaomin Wu,Huazhen Shen,Wenjie Xia
Transition metal oxide (TMO)-decorated TiO 2 catalysts excel at low-temperature Hg 0 oxidation. However, TMOs are typically found in large nanoparticles (NPs), resulting in a lower atom utilization efficiency. The current paper presents the design of an Au single atom (SA)-doped Ti 4+ defected TiO 2 (Au SAC-Ti 1-x O 2 ) and investigations concerning the influence of an O-Au-O coordination environment on Hg 0 oxidation. Au SAC-Ti 1-x O 2 was designed using an O-Au-O coordination environment and the O-Au-O orbital interaction was elucidated using density functional theory (DFT). The enhanced oxidative capability of lattice oxygen atoms and the interaction between Hg 0 and oxygen atoms were investigated. The O-Au-O coordination environment containing Au SAC Ti 1-x O 2 was then synthesized and characterized using X-ray absorption fine structure (XAFS), X-ray photoelectron spectroscopy (XPS), etc. Finally, Hg 0 oxidation catalytic activity was determined. Due to the increasing population of Au-O antibonding orbital interactions in the valence band, the bond order of O-Au-O in Au SAC Ti 1-x O 2 decreased significantly, thereby enhancing the oxidation ability of its adjacent oxygen atoms. Au SA and ultra-small Au clusters coexisted on a Ti 1-x O 2 catalyst, and the Hg 0 -oxidation efficiency at 150–200 °C was 14 times and 1.5 times greater than those of TiO 2 and 0.1 % Au/TiO 2 , respectively. Furthermore, Au SAC Ti 1-x O 2 was more resistant to the inhibition of SO 2 and NO. It provides an efficient method for developing highly active SA catalysts for Hg 0 oxidation.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Qin Cheng,Azhu Wang,Zhimin Song,Jun Bao,Jiawei Xue,Yuxue Wei,Shikuo Li,Lingling Lv,Jianjun Ding,Mengdie Cai,Jingshuai Chen,Qi Wang,Chen Gao,Song Sun
Hydroxyl groups on the photocatalyst surface provide adsorption sites and starting species to form hydroxyl radicals , and are thus considered as the most important species for the photocatalytic degradation of toluene. However, the complete mineralization of toluene over TiO 2 photocatalysts is still challenging because of insufficient and unstable hydroxyl groups. Here, a hydrogenated TiO 2 nanotube array mesh (H-TiO 2 ) was fabricated. H-TiO 2 capable of trapping light and serving high surface areas for active sites exhibited a toluene mineralization conversion of 100%. It was found that surface distortion and oxygen vacancies ensured the chemical dissociative adsorption of water to generate sufficient isolated hydroxyls on the surface and subsurface and benefited the regeneration in long-term operations. This study may provide an efficient TiO 2 -based photocatalyst for the removal of volatile organic compounds for air purification and give comprehensive understandings of the photocatalyst surface modification and theoretical guidance for designing hydroxyl-demanding photocatalysts.
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WATER RESEARCH
·
2025
·
IF 12.4
Delong Yu,Guoquan Zhang,Xiaoli Lv,Xiaochen Xu,Fenglin Yang
Achieving efficient NH 4 + -N degradation into harmless N 2 and simultaneous harvesting hydrogen energy is of great significance for protecting aquatic ecosystems and alleviating energy shortages. Herein, a photoelectrochemical-chlorine (PEC-Cl) system was developed aiming to selective converting ammonia to N 2 with simultaneous H 2 evolution in a wide pH range of 3–13. The Pt decorated black TiO 2 nanotube arrays (Pt/BTNAs) with sufficient oxygen vacancies defects and the enhanced PEC properties were synthesized as the bifunctional electrode. The parameters optimization illustrated high N 2 selectivity (88 %) and H 2 yield rate (67.5 μmol cm -2 h -1 ) at pH 9. The ClO • derived from the cross reactions between active chlorine and HO • plays a predominant role in oxidizing ammonia. More importantly, the Gibbs free energy calculation indicated that Pt decorating can also significantly promote the direct electrochemical ammonia oxidation reaction (AOR) on Pt/BTNAs anode. Under alkaline conditions (pH 9–13), the efficient removal and conversion of ammonia into N 2 in the PEC-Cl system was achieved primarily through the direct anodic AOR, with N 2 selectivity (89 %-93 %) and H 2 yield rate (60.9–68.6 μmol cm -2 h -1 ) comparable to those of the ClO • -mediated indirect AOR. This study presents a flexible method for treating high and medium-concentration NH 4 + -N and simultaneously producing H 2 through the synergistic PEC-Cl and direct electrochemical AOR processes, across a wide pH range.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·
IF 6.7
Yaxiling Wang,Yaping Yu,Jing Lin,Chunyuan Zhu,Jing Qiu,Peiwen Hu,Nan Zhang
Critical to sensor performance in real agricultural matrices are high interference resistance and prevention of false-positive/negative signals. To address this, a Z-scheme BiOI nanoflakes (NFs)/Au NPs/TiO2 NPs heterojunction was designed with photocurrent-polarity-switching capability, an inherent feature that could minimize interference from oxidative and reductive species. Subsequently integrated Fe3O4 NPs with catalase-mimicking activity suppressed the photocurrent response to baseline levels, substantially reducing the background noise. In the presence of glyphosate (Gly), the quenching effect was inhibited, leading to a “signal on–off–on” photoelectrochemical (PEC) detection mode. In addition, the inherent magnetism of Fe3O4 NPs enhanced the specificity by facilitating the efficient removal of nonbound interferents and enabling “split-type” PEC detection processes. This approach achieved Gly quantification within a linear range of 0.05–5 mg·L–1, with practical applicability demonstrated in three agricultural matrices. By strategically integrating heterojunction engineering with magnetic nanozyme signaling, this work establishes a PEC sensing paradigm exhibiting exceptional anti-interference capability.
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Kané Rabé,Lifen Liu,Noor Ahmed Nahyoon,Yizhen Zhang,Ahmed Mahmoud Idris
Degradation of pollutants can be integrated with electricity generation in Photocatalytic fuel cell under light irradiation or self-powered fuel cell in the dark. In fuel cell driven by electrode reactions , the electrode reduction and oxidation transforms chemical energy in pollutants into electrical energy. In this work, Rhodamine B and coking wastewater were treated, using an efficient Z-scheme g-C 3 N 4 /Fe 0 (1%)/TiO 2 as an anodic catalyst and WO 3 as a cathodic catalyst. After 100 min of reaction in a single chamber fuel cell with 10 Ω of external resistance, in 0.05 M Na 2 SO 4 electrolyte, the paired stainless-steel electrodes loaded respectively with g-C 3 N 4 /Fe 0 (1%)/TiO 2 and WO 3 , degraded 98% Rhodamine B and generated 0.95 V cell voltage under 50 W visible-light irradiation, while removed 60% RhB and generated 0.5 V without light. To investigate the PFC performance of g-C 3 N 4 /Fe 0 (1%)/TiO 2 in treating real coking wastewater, at optimal pH 2, 91% chemical oxygen demand (COD) and 89% total organic carbon (TOC) were removed and generated 0.3 V cell voltage. The influence of pH on photocatalytic degradation performance and cell voltage are evaluated. The high cell voltage is attributed to the very low impedance of the g-C 3 N 4 /Fe 0 (1%)/TiO 2 loaded anode. The excellent electrochemical properties of paired electrodes help in generating higher current density , due to the increased photocatalyst activity of the tridimensional catalyst as proved by electron spinning resonance spectrum, photoluminescence , and Electric Impedance Spectrum analysis.
研究领域:
环境科学
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光催化
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能量转换
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废水处理
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电化学
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材料科学
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Materials
·
2023
·Vol. 16
·期 4
·1563
·
IF 3.4
Jing Zhang,Chen Wang,Xiaoguo Shi,Qing Feng,Tingting Shen,Siyuan Wang
The photocatalytic activity of titanium dioxide (TiO2) is largely hindered by its low photoresponse and quantum efficiency. TiO2modified by conjugated polymers (CPs) is considered a promising approach to enhance the visible light responsiveness of TiO2. In this work, in order to investigate the effect of CP structural changes on the photocatalytic performance of TiO2under visible light, trimesoyl chloride–melamine polymers (TMPs) with different structural characteristics were created by varying the parameters of the polymerisation process of tricarbonyl chloride (TMC) and melamine (M). The TMPs were subsequently composited with TiO2to form complex materials (TMP–TiO2) using an in situ hydrothermal technique. The photocatalytic activity of TMP–TiO2was evaluated by the degradation of rhodamine B (RhB). The results showed that the trend of the structure of the TMP with the reaction conditions was consistent with the visible light responsiveness of TMP–TiO2, and TMP (1:1)–TiO2had the best photocatalytic activity and could degrade 96.1% of the RhB. In conclusion, our study provided new insights into the influence of the structural changes of TMPs on the photocatalytic activity of TMP–TiO2under visible light, and it improves our understanding of how conjugated polymers affect the photocatalytic activity of TiO2under visible light.Keywords:conjugated polymer;structural regulation;TiO2;visible photocatalyst
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