PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2022
·Vol. 24
·期 22
·13661-13670
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IF 3.945
Si-Yuan Yu,Ying Liu,Hai-Tao Ren,Zhao-Yu Liu,Xu Han
Photooxidation of As(III) by TiO2 is a complicated process in which the oxidation mechanisms are always controversial. In this study, the enhanced photooxidation rates of As(III) with increasing pH values from 8.0 to 11.0 indicate the high photocatalytic reactivity of TiO2 under alkaline conditions. Moreover, As(III) improves the production of H2O2, indicating H-abstraction from As(III) (soluble or adsorbed) for H2O2 production. Although O2˙−, h+, ˙OH and –OOH are always regarded as the reactive oxygen species in the UV-TiO2 system, the superoxo and peroxo species formed on the surface of TiO2 also contribute to As(III) oxidation. The As(III)–O–Ti(IV) surface complexes formed on TiO2, as well as the decreased bandgaps of TiO2 with increasing concentrations of As(III) indicate that the ligand-to-metal charge transfer (LMCT) pathway also contributes to the oxidation of As(III) under alkaline conditions. Electrochemical analyses further reveal that As(III) enhances the electron density on the surface of TiO2, thereby improving the catalytic reactivity of TiO2. We therefore suggest that H-abstraction from As(III) or H2O to the formed superoxo and peroxo species results in the formation of H2O2, accompanied by the oxidation of As(III). This enriches our knowledge on the oxidation of As(III), as well as other contaminants rich in –OH groups during the photocatalytic oxidation processes.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
Nanomaterials
·
2024
·Vol. 14
·期 23
·1930
·
IF 4.4
Sha Ni,Wenjing Wu,Zichao Yang,Min Zhang,Jianjun Yang
The Cu cocatalyst supported on the surface of TiO2photocatalysts has demonstrated unique activity and selectivity in photocatalytic CO2reduction. The valence state of copper significantly influences the catalytic process; however, due to the inherent instability of copper’s valence states, the precise role of different valence states in CO2reduction remains inadequately understood. In this study, CuOx/TiO2catalysts were synthesized using an in situ growth reduction method, and we investigated the impact of various valence copper species on CO2photocatalytic reduction. Our results indicate that Cu+and Cu0serve as primary active sites, with the selectivity for CH4and CO products during CO2photoreduction being closely related to their respective ratios on the catalyst surface. The adsorption and activation mechanisms of CO on both Cu+and Cu0surfaces are identified as critical factors determining product selectivity in photocatalytic processes. Furthermore, it is confirmed that Cu+primarily facilitates CH4production while Cu0is responsible for generating CO. This study provides valuable insights into developing highly selective photocatalysts.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaodi Jiang,Yaoning Bai,Xu Wang,Weiyao Wang,Yuxian Duan,Yingnan Liu,Xinru Li,Zichen Wang,Jinming Cai,Xiaoming Cai,Honglin Tan
Bimetallic nanostructures are currently a hot pot material among many hydrogen generation co-catalysts. In this study, CuCo bimetallic nanostructures were formed by introducing Co into Cu as the co-catalyst for TiO 2 . Characterization results from XRD , XPS , and TEM indicated the successful preparation of the high-crystallinity, impurity-free CuCo/TiO 2 photocatalyst , with CuCo bimetallic nanoparticles uniformly dispersed on TiO 2 . After the addition of Co, density functional theory (DFT) calculations showed that the free energy of H adsorption on the Cu site was optimized from 0.27 eV to −0.56 eV, which was beneficial for hydrogen production from TiO 2 . Electrochemical characterization, photoluminescence (PL) spectroscopy, infrared (IR) thermography, and finite difference in time domain (FDTD) results showed that the bimetallic CuCo acted as the co-catalyst, which increased the temperature of the reaction system, facilitated the separation of light-generated electron-hole pairs, and accelerated the charge transfer, thus promoting the photocatalytic hydrogen generation. The findings of the photocatalytic performance demonstrate that the photocatalyst exhibits the H 2 generation rate of 1933.8 μmol/g/h, which is approximately 9 times greater than that of pure TiO 2 (213.4 μmol/g/h), when the bimetallic CuCo is loaded in the molar ratio of 5:5 and at the loading amount of 2 wt%. Additionally, the photocatalyst demonstrated excellent catalytic stability, reaching 87.1% of the initial after 16 h of cycling tests. It is foreseen that further study and optimization of various metal couplings may enable the larger widespread application of bimetals as co-catalysts for hydrogen generation.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
JOURNAL OF CLUSTER SCIENCE
·
2018
·Vol. 29
·期 6
·981-988
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IF 1.715
Liu ZhangSheng,Li LinNa
Coal cinder-supported TiO 2 photocatalysts were synthesized via a novel coal combustion method. As-obtained samples were characterized by XRD, SEM, EDS mapping, Raman spectra, FTIR and DRS, and their photocatalytic performances were evaluated by degradation of methylene blue (MB) and methyl orange (MO) under UV–Vis light illumination. The results revealed that mixed-phases TiO 2 with adjustable anatase–rutile ratio could be obtained by adjusting the amount of precursor tetrabutyl titanate, which was uniformly covered on the coal cinder. These coal cinder-supported TiO 2 photocatalysts exhibited commendable photocatalytic activity. Among them, the indexed CCT-7.5 sample presented the maximum of activity, which can be attributed to the optimal phase composition of TiO 2 . The present work provided a novel synthetic route to fabricate immobilized photocatalysts, which might be extended to the preparation of other functional materials.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 5
·1942-1952
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IF 3.288
Qiong Sun,Kaijing Li,Songhao Wu,Bing Han,Lina Sui,Lifeng Dong
A simple hydrothermal post-treatment has been developed to construct a TiO2 photocatalyst with a desirable anatase phase, porous structure, large surface area, small particle size and hydrophilic surface. When aggregated nanoparticles are treated under a high temperature and pressure, the crystal structure of TiO2 is first deeply destroyed and then reconstructed. The dispersity can then be greatly improved and a typical mesoporous structure is simultaneously produced, accompanied with an increase in the specific surface area, average pore size, total pore volume and the production of oxygen vacancies. The structural changes have positive effects on the photocatalytic degradation of dye molecules. For example, the kinetic constant (0.085 min−1) can be increased by 10 times as compared with that for the untreated ones (0.0085 min−1). Other parameters including temperature, time, solvent, calcination treatment and type of TiO2 are also explored to optimize the treatment. In addition, electrochemical tests prove that the hydrothermal post-treatment for TiO2 results in an accelerated O2 reduction reaction and improved photo-induced charge transfer process. From radical quenching experiments, superoxide radicals (O2−˙) are proven to be the major oxidative species for both post-treated and untreated TiO2, but the production of hydroxyl radicals (˙OH) is dramatically promoted by the post-treatment, which is a key factor for the acceleration of the photocatalytic reaction.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Bo Sun,Yu Tian,Menglin Feng,Sihan Zhang,Hong Yang,Junmei Qin,Wenlong Bi,Xingxing Qiao,Fenwu Liu,Qingjie Hou
Flocculation is often used for the preliminary treatment of wastewater. However, pollutants especially some emerging contaminants, cannot be completely removed in this process. Meanwhile, the flocculated sludge may cause secondary pollution to the environment. This study investigates producing functional sludge biochar (FBC) from flocculated sludge obtained in the initial wastewater treatment phase, then introducing functional elements (Fe 3+ , Cu 2+ , Zn 2+ , and N) derived from flocculated sludge to modified waxberry-shaped TiO 2 photocatalyst. The next step involved using FBC/TiO 2 with functional elements for the deep degradation of swine wastewater. Under simulated sunlight, FBC/TiO 2 demonstrated a COD removal efficiency is 51.35 %, which is 2.65 times greater than that of pure TiO 2 . Furthermore, FBC/TiO 2 showed enhanced removal of dissolved organic matter (fulvic-like acids and soluble microbial products) and biotoxic substances from wastewater under both sunlight and visible light, particularly exhibiting significant efficacy in the removal of hard-degradation humic-like acids. In the photocatalytic process, water molecules oxidation by h + generates •OH, the primary reactive oxygen species responsible for organic matter degradation in wastewater. Applying this process to prepare FBC 15 /TiO 2 can lower sludge treatment costs for wastewater treatment plants while generating a profit of 52.28 $·kg −1 . This research offers a win–win solution for treating swine wastewater, promoting sludge reuse, and reducing the cost of TiO 2 deployment, thus presenting a new approach for efficient, cost-effective treatment of livestock and poultry wastewater.
研究领域:
环境科学
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污水处理
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材料科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Liu Yang,Yingxue Wu,Hongyi Shu,Chuang Wang,Changetong Song,Xianhong Zhang,Dong Chen,Yuhong Ma,Wantai Yang
Polymer-supported catalysts have attracted intensive research attentions due to easy handling, facile separation and outstanding recycling performance. Herein, a simple, efficient and universal strategy was developed to fabricate isocyanate-functionalized polymer microspheres bearing highly reactive surface isocyanate groups, which could serve as a versatile support for the immobilization of photocatalyst. Firstly, self-stabilized precipitation polymerization of maleimide, maleic anhydride and styrene was performed in the presence of divinyl benzene (crosslinker) to prepare imide-functionalized poly(styrene- co -maleimide- co -maleic anhydride) (PSMM) microspheres. By simply adjusting the solvent composition and monomer feed ratio, monodisperse PSMM particles with diameter in the range of 0.52–1.01 μm were successfully obtained, which were further modified with hexamethylene diisocyanate (HDI). As a proof-of-concept, TiO 2 nanoparticles were readily and covalently bound to the surface of HDI-functionalized PSMM (PSMM-HDI) particles through reaction with isocyanate groups, leading to the formation of PSMM-HDI supported TiO 2 (PSMM-HDI@TiO 2 ). Furthermore, anhydride groups on the surface of PSMM was hydrolyzed to endow PSMM-HDI@TiO 2 with better dispersibility and adsorption performance. The degradation of methylene blue under UV-light was performed to evaluate the photocatalytic performance of the resultant PSMM-HDI@TiO 2 . Compared with pristine TiO 2 , the PSMM-HDI@TiO 2 exhibited not only higher degradation efficiency, but also facile separation and better reusability.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2013
·
IF 3.473
Ziyang Lu,Weichao Zhou,Pengwei Huo,Yingying Luo,Ming He,Jianming Pan,Chunxiang Li,Yongsheng Yan
Fly-ash cenospheres were obtained from coal fly ash, while coal fly ash, as a kind of by-product produced during the combustion of coal, was a typical solid waste. In order to achieve the purpose of treating wastewater by solid waste and increasing the reuse rate of photocatalyst, the novel TiO 2 photocatalyst was achieved based on a magnetic composite as the carrier via a mild sol–gel method. This magnetic composite was prepared by coating a special layer of macromolecule onto the surface of the floating carboxyl-functionalized fly-ash cenospheres via microemulsion process, and magnetic Fe 3 O 4 nanoparticles were introduced into the special layer of macromolecule. The as-prepared photocatalyst was extensively characterized by scanning electron microscope (SEM), UV–vis diffused reflectance spectra (UV–vis), Fourier-transformed infrared spectra (FT-IR), thermogravimetric analyzer (TGA) and vibrating sample magnetometer (VSM). The results indicated that the as-prepared TiO 2 photocatalyst possessed hollow spherical structure and magnetic properties (Ms = 0.74 emu/g), floated in aqueous solution and had the average diameter between 100 μm and 150 μm. Moreover, this photocatalyst was proved to exhibit high catalytic efficiency and excellent photochemical stability, and the removal efficiency could reach nearly 75.32% for degradation of enrofloxacin hydrochloride residues in 60 min under visible light irradiation. In addition, the influence of calcination temperatures and inorganic salts on photocatalytic activity was also investigated. The results showed that different calcination temperatures and the presence of inorganic salts both had a great impact on the photodegradation of enrofloxacin hydrochloride.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2017
·
IF 2.764
Chao Li,Weiyi Yang,Qi Li
To develop TiO 2 -based photocatalysts with visible light activity for better solar energy utilization, a simple flash oxidation method was developed by calcining commercial TiN nanoparticle to prepare N-doped TiO 2 photocatalyst and TiN/TiO 2 composite photocatalysts through the modulation of the calcination time and temperature. It was found that more energy and processing time were needed to prepare N-doped TiO 2 photocatalyst than that of TiN/TiO 2 composite photocatalyst during this process, while TiN/TiO 2 composite photocatalyst had a better visible light absorption/photocatalytic performance than that of N-doped TiO 2 photocatalyst prepared from the oxidation of the same TiN precursor. Thus, the preparation of TiN/TiO 2 composite photocatalyst from TiN precursor should be a more preferred approach than the preparation of N-doped TiO 2 photocatalyst for visible-light-activated photocatalysis for its cost-effectiveness.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Jialin Jia,Stefanos Giannakis,Dong Li,Boyin Yan,Tao Lin
A novel catalytic system for effective photocatalytic inactivation of Escherichia coli ( E. coli ) was constructed by anchoring Ag nanoparticles (AgNPs) on silane coupling agent (SCA) pretreated TiO 2 nano-tube arrays (Ag/SCA/TiO 2 NTAs). Morphology and structural analyses revealed that SCA could disperse AgNPs evenly on TiO 2 NTAs, thus inducing a superior surface plasmon resonance (SPR) effect. Ag/SCA/TiO 2 NTAs catalyst exhibited excellent inactivation performance when in the presence of peroxymonosulfate (PMS) and visible light (VL), with 6-log E. coli was completely inactivated within 60 min, which was 5.3, 12.5 and 13.2 times higher than that of Ag/SCA/TiO 2 NTAs/VL, PMS/VL and Ag/SCA/TiO 2 NTAs/PMS/dark systems, respectively. Additionally, the photocatalyst exhibited a highly reusable property, with the inactivation performance almost unchanged after ten cycles of uses with minimal Ag leaching. The inactivation mechanism analysis demonstrated that both radical (SO 4 •- , OH) and non-radical (h + , 1 O 2 ) pathways involved in E. coli inactivation, and SCA played a pivotal role in the production of reactive species. Chloride ions (Cl − ) greatly enhanced the inactivation efficiency, while bicarbonate (HCO 3 − ) and phosphate (H 2 PO 4 − ) showed an inhibitory effect. Humic acid (HA) displayed a dual effect on inactivation performance, where the low concentration of HA facilitated the bacteria inactivation, while the higher dose suppressed bacteria inactivation. Moreover, the system exhibited excellent inactivation performance in tap water . This work first used SCA as the binder to fix AgNPs on TiO 2 NTAs for VL photocatalytic inactivation of bacteria with the assistance of PMS, which was expected to provide some insights into the practical treatment of drinking water .
研究领域:
环境科学
·
微生物学
·
材料科学
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DOI
PubMed
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2023
·
IF 4.3
Xi Chen,Yu Huang,Xu Wang,Haibo Li,Lin Zhu,Xinyang Xu,Shaoyan Jiang
A novel, sample and economical method was used to prepare the new co-doped TiO 2 photocatalysts and evaluated for CO 2 photoconversion under visible-light irradiation. The La(NO 3 ) 3 -TiO 2 photocatalyst was obtained by the sol–gel method and then was heat treated with different concentrations of ammonia vapor. It was found that the synergistic modification of TiO 2 photocatalyst by La(NO 3 ) 3 and ammonia vapor could improve its photocatalytic performance under visible light. The photocatalytic assessment presented a significantly amelioration in CO 2 photoconversion, giving 3.078 μmol CH 4 production in 4 h. The structures and properties of the photocatalysts were characterized and analyzed by means of XRD, SEM-EDS, HRTEM, BET, XPS, FTIR, ICP-AES, UV–vis DRS and theoretical calculation. The performance of the photocatalyst could be correlated to contributions of various phenomena such as larger specific surface area and the co-exposed (1 0 1) and (0 0 1) facets of anatase TiO 2 . Finally, the most likely substituted structures were obtained. The results of DFT + U theoretical calculation showed that La and N could modify TiO 2 by replacing surface Ti atoms and internal O atoms, respectively.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 18
·4546
·
IF 3.1
Li Liu,Zhenghao Cui,Bo Feng,Mengjing Sui,Huaqin Huang,Zhaoyang Wu
In this study, novel Fe2O3/TiO2photocatalytic composites were synthesised by combining traditional oxidation roasting with the sol-gel method, using low-cost metallurgical waste (iron scales) as the raw material. The characterisation results revealed that the oxidised iron scales could be transformed into high-purity and porous Fe2O3particles through oxidation roasting, thereby providing additional sites for the adsorption process and thus serving as an effective carrier for TiO2-based photocatalytic materials. During the sol-gel process, TiO2was loaded onto the synthesised Fe2O3particles, generating core-shell heterostructure Fe2O3/TiO2photocatalytic composites. Under visible light irradiation for 90 min, the Fe2O3/TiO2photocatalytic composites achieved a remarkable methylene blue removal rate (97.71%). This reaction process followed the quasi-first-order kinetic model with a rate constant of 0.038 min−1. The results have demonstrated that this combination of various components in the Fe2O3/TiO2photocatalytic composites improved the adsorption, light utilisation, and charge separation effect of the photocatalysts. Moreover, the material exhibited favourable stability and recyclability, making it a decent candidate for the treatment of wastewater from the biochemical industry. Therefore, this study provides a new strategy for improving the photocatalytic activity of TiO2and expanding the high value-added utilisation of iron scales.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）