APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Dexu Zhang,Xiaoying Peng,Jie Zhang,Shixuan Zhu,Zhihong Xue,Shubin Xiong,Shuai Xiong,Bo Sheng,Yiqiang He,Guiming Peng,Jiadong Zhang
Graphitic carbon nitride (g-C 3 N 4 ) has become a favored universal photocatalyst. Despite its numerous advantages, the photocatalytic efficiency of g-C 3 N 4 is hindered by the substantial recombination of photoexcited charge carriers and holes. In this work, we demonstrate that Zn-doped tubular carbon nitride photocatalyst (Zn-tCN) can serve as highly efficient catalysts for H 2 O 2 photosynthesis. Mechanism studies confirm that the presence of Zn in g-C 3 N 4 prolongs the lifetimes of photogenerated carriers and inhibits their recombination, which triggers the reduction of O 2 to reaction intermediates ( O 2 − ), as supported by in situ electron paramagnetic resonance (EPR) spectroscopy. More importantly, sacrificial agent experiments coupled with in situ EPR results confirmed that the reaction mechanism involves a concerted two-electron transfer process. The optimal catalyst displays a H 2 O 2 productivity of 162.4μmol g –1 h −1 under visible-light irradiation without a sacrificial agent, which is 11.7 times higher than that of pristine g-C 3 N 4 (13.8μmol g –1 h −1 ). This work proposes a synthetic strategy for the preparation of high-performance Zn-doped g-C 3 N 4 , which offers insights and perspectives for developing highly active photocatalysts and deepening the understanding of photocatalytic mechanisms.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Lu Zhang,Jianhao Qiu,Zongpeng Zou,Shengwei Tang,Wenxiang Tang
This work demonstrates the rational design of a Z-scheme CdS/Fe-MOF heterojunction for photo-Fenton processes utilizing in situ generated H2O2 under visible light. The photocatalysts were synthesized by depositing CdS nanoparticles onto MIL-53(Fe), optimizing interfacial charge transfer and light absorption, and ensuring effective spatial segregation of photogenerated carriers, thereby maintaining robust redox potentials. The modified CdS/Fe-MOF exhibited exceptional catalytic performance, achieving 92% degradation of 40 mg·L–1 tetracycline within 15 min, surpassing pure CdS (43%) and MIL-53(Fe) (30%) by factors of 2.3 and 3.3, respectively. Mechanistic studies identified on-site H2O2 generation through two-step oxygen reduction (236 μmol·L–1) and its subsequent activation by Fe3+/Fe2+ cycling to produce ·OH as key pathways, with h+, ·O2–, 1O2, and ·OH collectively driving pollutant degradation. The prepared photocatalysts demonstrated remarkable stability (>90% efficiency after five cycles) and structural integrity, attributed to the robust heterojunction interface. This study provides deep insight into designing Z-scheme photo-Fenton catalysts and advancing sustainable wastewater treatment.
研究领域:
环境催化
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材料化学
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光化学
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环境污染治理
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纳米材料
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可持续水处理
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Shiqi Chen,Xinyu Wang,Can Liu,Jiapeng Yue,Zhiwei Yang,Qian Ye,Hao Xu,Yujian Zhang,Xinyi Xing,Jing Zhang
Rational design and controllable synthesis of oxygen functional groups on carbon/metal catalysts surface as the effective means to enhance catalytic performance, however, still remains a great challenge. Herein, to obtain the relationship between oxygen functional groups and catalytic performance, taking MoO 2 -C as an object, the correlation between the C=O, C-O, Mo O bonds and strengthened iron reduction is quantitatively assessed, with electrochemical experiments validating that this relationship arises from its influence on the electron transport process, specifically concerning the roles of electron donors and mediators. The metal–oxygen and C-O bonds synergistically enhance electron transport, whereas the C=O and C-O bonds exhibit an antagonistic effect on electron-mediated processes. The influence of the metal–oxygen bonds was found to stem from their role as an electron donor, while the carbon–oxygen bonds primarily modulate the material’s catalytic properties by altering its electron transfer characteristics. In this study, the C-O, C=O bonds, and metal–oxygen bonds, as the typical surface oxygen functional groups, were identified the mechanism by changing the electron supply and mediation to enhance the Fe 3+ reduction reaction in the Fenton system, which provided theoretical support and design ideas for the design of catalyst with excellent catalytic properties.
研究领域:
催化
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表面化学
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电化学
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环境科学
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材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xinyu Han,Qiyuan Huang,Zhaolian Zhu,Muyao Li,Yuping Dai,Xuefei Gao,Yan Gao
Hydrogen peroxide (H 2 O 2 ) in situ production via 2-electron oxygen reduction reaction (ORR) exhibits several advantageous characteristics, including safety, convenience, environmental friendliness, and the potential to replace the traditional anthraquinone process. Nevertheless, ORR occurs at the gas–liquid-solid interface, where O 2 diffusion to the electrode and H 2 O 2 transfer from the electrode to the solution are easily limited by the pore structure of the electrode, thus reducing the efficiency of H 2 O 2 electrosynthesis. Herein, the graphite/PTFE electrodes with different pore structures were prepared using a salt template to improve the gas permeability and promote mass diffusion. A series of characterization methods, including SEM, CV, and LSV were used to investigate the effect of inorganic pore-forming agents on the electrode pore structures and their oxygen reduction activity. The pore size distribution and gas permeability of the electrode were determined by bubble point characterization. Furthermore, the impact of inorganic salt addition, current density, pH, and aeration on H 2 O 2 electrosynthesis was examined. The results demonstrate that the graphite/PTFE electrode with 0.15 g NH 4 Cl as a pore-forming agent (0.15 g-Ele) shows an obvious micron-sized honeycomb pore structure and has the highest gas permeability, contributing to the mass transfer and 2-electron ORR to produce H 2 O 2 . At a current density of 30 mA·cm −2 , pH = 3.0, and O 2 aeration rate of 400 mL·min −1 , the H 2 O 2 production of 0.15 g-Ele is found to be 425.4 mg·L -1 ·g catalyst -1 ·h −1 , with a current efficiency of 62.9 % at 60 min. The continuous and repeated use results also indicate that maintaining an abundant micron-sized honeycomb pore of the electrode is crucial for improving the H 2 O 2 production and current efficiency in electrosynthesis.
研究领域:
电化学
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材料科学
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环境工程
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化学合成
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Zimou Liu,Kuiling Li,Lie Liu,Hang Song,Yong Zhang,Mike Tebyetekerwa,Xiwang Zhang,Ke Wang,Lili Xu,Jun Wang
Electrosynthesis of hydrogen peroxide (H 2 O 2 ) presents a sustainable alternative to the anthraquinone process, while the transition to applying this process at industrial-relevant currents remains a significant challenge. Most studies tried to solve it by catalysts modulations, whereas we found that the accessibility to the gaseous O 2 , might be the crux of this matter. Herein, we developed a series of membrane-based gas diffusion electrodes (Mem-GDEs) with varied O 2 accessibility. Their endurable currents were found to be well correlated with the O 2 mass transferability. By constructing high O 2 -accessible triphasic interfaces, Mem-GDE achieved a recorded current density , 1.4 A cm −2 , with the current efficiency higher than 80.6 %. It was also verified for the first time that the insufficient O 2 triggered a severe flooding problem and thus further deteriorate the O 2 mass transfer. This study highlights the importance of O 2 accessibility and provides new insights into triphasic interfaces construction for realizing industrial-used H 2 O 2 -generated electrodes.
研究领域:
化学工程
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电化学
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材料科学
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DOI
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Nano-Micro Letters
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2025
·Vol. 17
·期 1
·1-12
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IF 36.3
Hu Zhen-Yu,Liu Tian,Yang Yu-Ru,An Alicia Kyoungjin,Liew Kim Meow,Li Wen-Wei
Polyvinylidene fluoride nanofibers were treated by dimethylformamide to create micropores on membrane surface.
Photocatalysts were firmly bounded by nanofibers during stretching and shrinking.
Particulate catalysts were fixed yet high exposed on the membrane surface.
Surface self-bounded photocatalytic membrane exhibited tenfold higher decontamination activity than embedded catalyst.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Shengkai Sun,Yuan Li,Yusen Chen,Dehong Chen,Yu Yang,Meng Liu,Shaoxiang Li,Binjie Li,Xuan Sun,Sadritdin Turabdjanov,Sardor Donaev,Lei Wang,Bin Li
Volatile organic compounds (VOCs) in the atmosphere pose a critical global challenge due to their detrimental health effects. The ultraviolet (UV)/Fenton-like system has shown promise for VOC degradation. However, maintaining long-term catalytic efficiency by minimizing intermediate byproduct accumulation remains key challenges. In this study, a novel core–shell catalyst is developed which composed of anatase-phase titanium dioxide (TiO 2 ) nanoparticles deposited on titanium silicalite-1 (TS-1) via a Stöber method in an ethanol/ammonia mixture. The TS-1@TiO 2 structure promotes efficient spatial separation of photogenerated electrons and holes under UV irradiation, enhancing the activation of H 2 O 2 to yield highly reactive free radicals ( OH, OOH and O 2 − ) for effective xylene degradation. In a UV/H 2 O 2 bubble reactor, the TS-1@TiO 2 catalyst demonstrates stable xylene degradation efficiency (75 % over 200 min), surpassing the performance of standalone TS-1 (53.2 %) and TiO 2 (62.1 %). This design addresses critical challenges in sustained radical generation and intermediate suppression, offering a robust strategy to improve the longevity and efficiency of UV/H 2 O 2 systems for environmental remediation.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Qing Cheng,Yuqi Zhang,Yingying Cao,Peihao Dou,Long Liu,Yanqiang Zhang
Ionic liquid-H2O2 is a green hypergolic propellant system, and the poor self-ignition hinders its application. Herein, the stable zero-valent catalyst Cu nano-particle with twin boundaries (T-Cu) was synthesized. As the twin boundary regulates the electron micro-environment of the T-Cu surface, the electron transfer from the d electrons of Cu atom to the σ* anti-bonding orbital of H2O2 is intensified to create ·OH and ·OOH. The resulted free radicals possess strong oxidizing ability, and react violently with [BMIM]N(CN)2 to achieve a rapid ignition with the delay time as low as 25 ms. This work provides an effective way to get excellent ignition performance, and promotes the application of Ionic liquid-H2O2 green hypergolic propellants.
研究领域:
材料科学
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推进剂工程
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催化化学
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DOI
高影响因子
Journal of Water Process Engineering
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2026
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IF 6.7
Tariq Ali,Yiwei Li,Yuxian Wu,Yuke Zhang,Bingjie Fang,Saleem Raza,Ruidi Chen,Yeyuan Xiao
Photocatalytic technology offers a promising solution for degrading organic pollutants in wastewater. However, catalysts often suffer from limited light absorption and rapid electron-hole recombination. To address the challenges, we developed a heterogeneous TiO 2 /CoAl-LDH catalyst for photocatalytic degradation of dyes such as Acid fuchsin (AF) and methyl orange (MO) and real wastewater under UV light irradiation. The aligned band structures of TiO 2 and LDH enhanced UV light energy absorption and electron-hole separation, resulting in superior photocatalytic activity. In treating real dyeing wastewater, TiO 2 /CoAl-LDH + H 2 O 2 + UV achieved higher decolorization than UV/H 2 O 2 or catalyst/H 2 O 2 alone under the same operating conditions. The process within the early stage (0–45 min) followed pseudo-first-order kinetics (kₐₚₚ ≈ 1.50 × 10 −2 min −1 ), with a clear H 2 O 2 optimum at 40.8 mM. Excitation–emission matrix (EEM) fluorescence showed rapid quenching of protein-like (B/T) and humic/fulvic-like (A/M/C) peaks with blue-shifts under the TiO 2 /CoAl-LDH + H 2 O 2 + UV condition corroborating deeper oxidation and mirroring the ADMI decolorization trend (fast loss of B/T within 15 min, followed by progressive depletion of humic-like emission). This study presents a simple and cost-effective method for developing efficient hierarchical semiconductor materials potentially applicable as photocatalysts for wastewater treatment.
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ChemistrySelect
·
2024
·Vol. 9
·期 36
·e202401875
·
IF 1.9
Haonan Li,Chenping Gao,Qingjie Liu,Yanchun Guo,Yufen Zhao
Graphical We report here a new I 2 /H 2 O 2 co-catalyzed oxidative [4+1] cyclization of benzaldehyde with 2-(aminomethyl)pyridine or o -phenylenediamine/2-aminothiophenol to provide various substituted imidazo[1,5- a ]pyridines and benzimidazoles/thiazole via C(acyl)−N bond construction. Some of heterocyclic products exhibit blue luminescence properties, as well as large Stokes shifts, eminent fluorescence quantum yields (64 %) and long fluorescence lifetimes. An efficient I 2 (10 mmol %)/H 2 O 2 mediated oxidative formal [4+1] cyclization of 2-pyridinemethylamine or o -phenylenediamine (2-aminobenzenethiol) with benzaldehyde via C−N bond formation has been developed. This strategy provides a straightforward approach to imidazo[1,5- a ]pyridines, iodo-substituted imidazo[1,5- a ]pyridines and benzimidazole (benzothiazole) derivatives in yields ranging from 60 % to 98 %, respectively. Several heterocyclic products exhibit promising blue luminous performance with satisfactory fluorescence quantum yields of up to 64 %, large Stokes shifts, and a longer lifetime (7.35 ns). The band gap energies obtained from DFT are also consistent with the absorption spectra.
研究领域:
有机化学
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光物理化学
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DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2026
·
IF 7.8
Mahmoud Radwan,Zhimin Qiang,Yu Lei,Huiyu Dong,Gholamreza Moussavi,Mengkai Li
Ultraviolet/chlorine (UV/Cl 2 ) process is promising for degrading persistent micropollutants, but suffers from toxic disinfection by-products (DBPs) formation. Here, we developed a new UV/Cl 2 /H 2 O 2 process by combining UV/Cl 2 with a low dosage of H 2 O 2 , which not only enhanced micropollutant degradation but also reduced DBP formation. Taking a recalcitrant taste and odor (T&O) compound, 2,4,6-tribromoanisole (TBA) as an example. UV/Cl 2 /H 2 O 2 increased 2,4,6-TBA degradation rate constants by 90 % and 60 % than those of UV/H 2 O 2 and UV/Cl 2 , respectively, primarily due to increased HO • production. The combined contribution of UV and HO • to the degradation was substantial, accounting for 82−96 % of the overall degradation. Regarding simultaneous DBP formation from 2,4,6-TBA, UV/Cl 2 /H 2 O 2 decreased trihalomethanes (THMs) levels by 79 % compared to UV/Cl 2 . Furthermore, during post-chlorination, UV/Cl 2 /H 2 O 2 reduced the DBP formation potential by 18 % compared to UV/Cl 2 . In UV/Cl 2 /H 2 O 2 , THMs formation was reduced by 52.5 %, haloacetamides (HAMs) formation by 48.5 %, and haloacetic acids (HAAs) formation by 16.7 % compared to UV/Cl 2 using real water samples. The reduced DBP formation may result from the competitive reaction of HO • with halogenation agents and the destruction of halogenated sites. This work establishes a practical AOP that simultaneously enhances micropollutant removal and suppresses DBP formation.
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SCIENCE PROGRESS
·
2025
·
IF 2.9
Jing Zhou,Guobo Du,Yi Li,Shiyao Liu,Xiaoyu Chen,Yue Peng,Xiaoming Wang
Objectives: To fabricate iron-doped WS2 (Fe-WS2) nanozymes with prominent peroxidase-like (POD-like) activity and explore their application in biomolecule detection. Methods: Fe-WS2 nanozymes were synthesized via a hydrothermal method, and their structural and chemical properties were characterized. The POD-like activity of the Fe-WS2 nanozymes was evaluated at different pH, temperatures, and substrate concentrations. Kinetic parameters were determined using the Michaelis–Menten equation. The detection capabilities of the Fe-WS2 nanozymes for H2O2 and glucose were assessed through colorimetric assays. Results: The synthesized Fe-WS2 nanozymes exhibited a uniform size distribution with an average diameter of approximately 300 nm. The successful loading of iron ions onto the WS2 nanosheets was confirmed by mapping and energy-dispersive X-ray spectroscopy analyses. The Fe-WS2 nanozymes demonstrated enhanced POD-like activity compared to unloaded WS2 nanozymes, as evidenced by the increased oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2. The optimal conditions for POD-like activity were found to be at pH 4 and 55 °C. Kinetic analysis revealed that the Fe-WS2 nanozymes had a high affinity for both H2O2 and TMB, with low Michaelis constants (Km). The Fe-WS2 nanozymes-based colorimetric assay exhibited a wide linear range (0.2 to 1 mM) for H2O2 detection, with a low detection limit of 7.27 × 10−7 M. For glucose detection, the assay showed good selectivity and sensitivity, attributed to the specificity of glucose oxidase in catalyzing glucose oxidation. Conclusions: This study successfully developed Fe-WS2 nanozymes with remarkable POD-like activity, which were utilized to construct a sensitive and specific colorimetric biosensing system for the detection of H2O2 and glucose. The results indicate that the Fe-WS2 nanozymes have great potential for applications in biomedical diagnostics due to their high catalytic efficiency, stability, and excellent biocompatibility. This work not only provides a novel inorganic nanozyme biosensor but also opens up new avenues for the application of other nanozyme biosensors in the biomedical field.
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高影响因子
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