NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 43
·17104-17115
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IF 3.069
Lisha You,Minghuan Gao,Tiesheng Li,Linna Guo,Penglei Chen,Minghua Liu
Semiconductor-based photocatalysis attracts wide attention owing to its ability to directly utilize solar energy for the production of solar fuels. In particular, the construction of Z-scheme heterojunctions is demonstrated to benefit the photocatalytic performance because of the separation and transfer of the photogenerated charge carriers and well-preserved strong redox ability. In this work, a series of Z-scheme Ag3PO4/WO3 p–n junction photocatalysts were prepared employing a facile impregnation method. The photocatalysts (Ag3PO4/WO3 p–n junction) presented enhanced photo-degradation efficiency; for example, with AW-45, 99.9% degradation could be obtained for RhB (30 ppm) on irradiation (λ > 420 nm, 350 W xenon lamp) for 7 min, which is a great improvement compared with the individual constituents. The degradation rate for AW-45 was 27 times higher than that of a commercial powder (P25). The apparent kinetic rate of catalytic degradation was obtained according to the results from the degradation process. The mechanism for electron transfer between Ag3PO4 and WO3 was also investigated. The reduction and oxidation processes concentrated on the CB (conducting band) of Ag3PO4 and the VB (valence band) of WO3, resulting in promoting the mechanism for photocatalytic degradation in the Z-scheme Ag3PO4/WO3 p–n junction photocatalysts.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yang Zhou,Zhu Zeng,Junhao Fu,Yuan Gao,Jinxing Ma,Zhong Zhang,Daoyuan Zu,Bin Han,Xixin Lu,Jun Ma,Jin Jiang
Humic acid (HA) ubiquitously existing in aquatic environments has been reported to significantly impact permanganate (KMnO4) decontamination processes. However, the underlying mechanism of the KMnO4/HA system remained elusive. In this study, an enhancing effect of HA on the KMnO4 oxidation of diclofenac (DCF) was observed over a wide solution pH range of 5–9. Surprisingly, the mechanism of HA-induced enhancement varied with solution pH. Quenching and chemical probing experiments revealed that manganese intermediates (Mn(III)-HA and MnO2) were responsible for the enhancement under acidic conditions but not under neutral and alkaline conditions. By combining KMnO4 decomposition, galvanic oxidation process experiments, electrochemical tests, and FTIR and XPS analysis, it was interestingly found that HA could effectively mediate the electron transfer from DCF to KMnO4 in neutral and alkaline solutions, which was reported for the first time. The formation of an organic–catalyst complex (i.e., HA-DCF) with lower reduction potential than the parent DCF was proposed to be responsible for the accelerated electron transfer from DCF to KMnO4. This electron transfer likely occurred within the complex molecule formed through the interaction between HA-DCF and KMnO4 (i.e., HA-DCF-KMnO4). These results will help us gain a more comprehensive understanding of the role of HA in the KMnO4 oxidation processes.
研究领域:
环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
NEW CARBON MATERIALS
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2016
·
IF 0.993
Yue Wang,Wen-ting Wu,Ming-bo Wu,Hong-di Sun,Hui Xie,Chao Hu,Xue-yan Wu,Jie-shan Qiu
Yellow-visual fluorescent carbon quantum dots (CQDs) were prepared from petroleum coke by ultrasonic-assisted chemical oxidation and were used as label-free probes for Cu 2+ detection in water. The detection of Cu 2+ by CQD probes is related to a quenching of fluorescence by a photoinduced electron transfer mechanism. The quenched fluorescence of the CQDs by Cu 2+ can be recovered by adding ethylene diamine tetraacetic acid. The yellow-visual fluorescent CQD probes have a linear detection range from 0.25 to 10 μM, a detection limit of 0.0295 μM, a response time of 3 s, and a superior sensitivity and selectivity for Cu 2+ detection compared to other fluorescent probes. The CQDs are easy to prepare, economical, reusable, fast to respond and can be used in on-line detection.
研究领域:
化学
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环境科学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 101
·98899-98907
·
IF 3.289
Xiaoling Xu,Shiyao Ma,Xincai Xiao,Yan Hu,Dan Zhao
This paper reports the synthesis of water-soluble fluorescence silicon quantum dots (Si QDs) through a hydrothermal route with urea propyl triethoxysilane (UPTES) as the source of silicon and sodium citrate as the deoxidizer. The UPTES was for the first time reported as the source of silicon. The preparation process is simple and green, and the prepared Si QDs exhibit high quantum yields, which would be ideal as a low-toxic material in biochemical applications. In addition, the prepared QDs emit excellent and stable fluorescence in a wide range of pH values (2–14), and show strong tolerance to salt and several common organic reagents, overcoming the weak anti-interference ability of traditional QDs and thus ensuring them as satisfactory candidates for biochemical detection. Using the prepared QDs as fluorescence probes, formaldehyde has been successfully detected in aqueous phase and acetonitrile through an electron transfer mechanism. The detection method is simple, sensitive and strongly anti-interfering, providing a new way for detecting formaldehyde in different solvents and expanding the potential applications of water-soluble low-toxic QDs in biochemical detection.
研究领域:
材料科学
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生物医学工程
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分析化学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Jiaxing Yu,Qi Fu,Huangsheng Yang,Junhui Wang,Gangfeng Ouyang,Zhengping Hao
Highly resistant organic pollutants and heavy metals (such as hexavalent chromium (Cr(VI)) usually coexist in industrial wastewater. However, efficient synergistic removal of them is still challenging in practical applications, due to low efficiency and high energy input required for this process. In this study, the metal-free multiwalled carbon nanotubes (MWCNTs) are demonstrated to simultaneously remove bisphenol A (BPA) and Cr(VI) without any external energy or chemical input. In this novel synergistic removal system, the catalytic performance is even higher than those of most of the reported metal-based catalysts in photo/electrocatalytic systems. The catalytic performances are negligibly affected by ions and humid acid, indicating applicability of the catalyst in actual wastewater. In addition, the MWCNT catalyst exhibits good recyclability after thermal treatment under inert atmosphere. Furthermore, the catalytic mechanism of this system has also been comprehensively investigated. This MWCNT-activated synergistic organic pollutants–Cr(VI) elimination system provides a novel and cost-effective strategy of “waste control by waste” for removing multiple industrial contaminants.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Qiang Li,Lijie Wang,Jupu Song,Linshen Zhang,Chunfeng Shao,Hong Li,Hemin Zhang
Construction of heterojunction photocatalysts is a valid tactics to boost the photocatalytic property of catalyst. Herein, a novel S-scheme heterojunction of zero/three dimensional (0D/3D) In 2 S 3 /Bi 2 WO 6 hybrid catalyst was obtained by assembling In 2 S 3 nanoparticles on floriated shaped Bi 2 WO 6 microsphere through a simple precipitation route for the first time. The morphology, structures, composition, chemical and optical properties of the resulting materials were carefully researched through various instruments. The degradation experiments revealed that In 2 S 3 /Bi 2 WO 6 composites exhibited superior photocatalytic behavior for dyes decomposition. The optimized In 2 S 3 /Bi 2 WO 6 composite showed remarkable photocatalytic decomposition Rhodamine B (RhB) and Methylene blue (MB), 16.0 (2.68)-fold and 70.3 (1.66)-fold larger than that of pristine Bi 2 WO 6 (In 2 S 3 ), and it also possessed good stability and reusability. The largely improved photoactivity may derive from the formed S-scheme heterojunction between Bi 2 WO 6 and In 2 S 3 , which accelerated photocarriers disassociation and retained strong redox power. Liquid chromatography-mass spectrometry (LC-MS) was applied to reveal the RhB decomposition pathway. Besides, the S-scheme charge transfer mechanism was well elucidated based on in-situ X-ray photoelectron spectroscopy analysis, density functional theory calculation (DFT), and trapping experiment along with electron paramagnetic resonance (EPR) tests.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
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2024
·
IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Bo Ju,Yi Wang,Yu-Mo Zhang,Ting Zhang,Zhihe Liu,Minjie Li,Sean Xiao-An Zhang
Advances in the development of fluorescent carbon dots (CDs) for detecting nitro-explosives have attracted great interest. However, developing long-wavelength luminescence CDs for highly selective determination of 2,4,6-trinitrophenol (TNP) and getting insight into the detection mechanism remain further to be investigated. Here, excitation-independent yellow-green emission CDs with good photostability and low biotoxicity were introduced for detecting TNP selectively. Then, two types of electron transfer (ET) processes including hydrogen-bond interaction-assisted ET and proton transfer-assisted ET are suggested to be responsible for their photophysical behavior. Finally, the visual detection of TNP has been successfully developed by a CD-based indicator paper. The facile, highly sensitive, and selective detection for TNP in both of a solution and a solid phase makes CDs potentially useful in environmental sensor applications.
研究领域:
分析化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RUSSIAN JOURNAL OF GENERAL CHEMISTRY
·
2025
·Vol. 95
·期 7
·1670-1685
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IF 0.8
Liu X.,Yue Q.-x.,Wang Y.-h.,Lei M.-d.,Zhang Y.-l.,Zhang Y.-w.,Ji A.-l.,Zhang Y.-c.,Zhang X.-q.,Ding R.,Liu J.
The catalytic performance and mechanism of the prepared iron meso-tetra (4-carboxyphenyl) porphyrin (FeTCPP) on oxygen reduction reaction in alkaline environments were studied. At high concentrations of FeTCPP, the oxygen reduction reaction followed an efficient direct 4-electron transfer mechanism instead of 2+2 electron transfer mechanism. The central iron ion in FeTCPP underwent redox reactions from Fe III to Fe II . O 2 molecules formed a superoxide anion coordination complex with Fe II TCCP, transferring an electron from the central iron ion. Protonation of the complex formed a superoxide hydrogen radical complex, which then acquired another electron, generating a hydroperoxide radical and completing the first 2-electron reduction. The peroxide formed a coordination complex with Fe II TCCP to produce a peroxide complex Fe III TCCP:O 2 – with intramolecular charge transfer. And then it acquired two electrons, completing the second 2-electron reduction and being reduced to OH – . When the concentration of Fe III TCCP was high, the complex Fe III TCCP:O 2 – could protonate without stepwise reactions, directly acquiring three electrons from the electrode surface and being reduced to OH – . The oxygen reduction reaction exhibited a 4-electron mechanism. Both the 2+2 and 4-electron pathways occurred simultaneously, with the 4-electron pathway becoming more prominent as the concentration of FeTCPP increased.
研究领域:
电化学
·
催化
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材料科学
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物理化学
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纳米技术
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yi Han,Mingjie Huang,Wei Xiang,Chen Wang,Yongjie Li,Xiaohui Wu,Juan Mao,Tao Zhou,Hong Li,Deming Wu
Fe-based metal–organic frameworks (MOFs) are popular in activating oxidants e.g·H 2 O 2 and persulfate (PS) for degrading recalcitrant organic substances, generally regarded with a simple interfacial efficient iron cycle. This study has revealed that a novel two-steps single-electron transfer mechanism would occur initially to activate the rapid degradation 4-chlorophenol (4-CP) in the MIL-88B(Fe)/H 2 O 2 system (88B/H 2 O 2 system). The degradation of 4-CP was acidic favorable (pH 0 ≤ 6.0) and could be divided into two reaction stages, i.e., initial lag phase (0–10 min) and following rapid decay phase (10–50 min). In the first stage, H 2 O 2 was slowly activated on the surface of 88B to form superoxide radical (O 2 •– ), which would lead to the accumulation of the key intermediate hydroquinone (HQ) through reducing 4-CP. Afterwards, HQ could reductively dissolve iron ions which would lead to the subsequent efficient homogeneous Fenton reaction for the rapid oxidation of 4-CP by hydroxyl radical (•OH) in the following rapid decay phase. It was interesting to note that specific aromatic compounds, which would form reductive benzenediols intermediates by O 2 •– , could be efficiently degraded in the 88B/H 2 O 2 system. The result of this study is expected to provide a new insight for understanding the catalytic oxidation process based on MOFs, and its application if possible.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Kaiyuan Luo,Yang Shi,Rongfu Huang,Xipeng Wei,Zelin Wu,Peng Zhou,Heng Zhang,Yin Wang,Zhaokun Xiong,Bo Lai
Periodate (PI) has recently been studied as an excellent oxidant in advanced oxidation processes , and its reported mechanism is mainly the formation of reactive oxygen species (ROS). This work presents an efficient approach using N-doped iron-based porous carbon (Fe@N-C) to activate periodate for the degradation of sulfisoxazole (SIZ). Characterization results indicated the catalyst has high catalytic activity , stable structure, and high electron transfer activity. In terms of degradation mechanism, it is pointed out that the non-radical pathway is the dominant mechanism. In order to prove this mechanism, we have carried out scavenging experiments, electron paramagnetic resonance (EPR) analysis, salt bridge experiments and electrochemical experiments, which demonstrate the occurrence of mediated electron transfer mechanism. Fe@N-C could mediate the electron transfer from organic contaminant molecules to PI, thus improving the efficiency of PI utilization, rather than simply inducing the activation of PI through Fe@N-C. The overall results of this study provided a new understanding into the application of Fe@N-C activated PI in wastewater treatment .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Chuhan Huang,Yu Ma,Qian Cheng,Xiaohan Liu,Hongman Sun,Fazle Subhan,Xinyuan Zhao,Youhe Wang,Zifeng Yan
The fundamental insights into the reaction mechanism, especially the electron transfer mechanism, are highly promising yet challenging for W 18 O 49 /g-C 3 N 4 heterojunction catalysts during photocatalytic nitrogen fixation. Herein, the 1D/2D nanostructured S-scheme heterojunctions were designed by in situ growth of 1D W 18 O 49 nanowires on 2D g-C 3 N 4 nanosheets through solvothermal method using methanol as solvent. In situ XPS analysis revealed that electrons in the conduction band of W 18 O 49 recombine with holes in the valence band of g-C 3 N 4 under the conduction effect of internal electric field, band bending, and Coulombic attraction in the W 18 O 49 /g-C 3 N 4 heterojunction. The photogenerated electrons are retained in g-C 3 N 4 , where the negative reduction potential of its conduction band enhances the activation of N 2 . As a result, the ammonia generation rate employing the optimal W 18 O 49 /g-C 3 N 4 heterojunction is 64.8 μmol g cat −1 h −1 , approximately double that of W 18 O 49 alone and 2.3 times higher than that of g-C 3 N 4 . The enhanced activity and facile methodology make the current material exceedingly appealing for implementation in photocatalytic nitrogen fixation for the synthesis of ammonia.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）