Water
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2024
·Vol. 16
·期 12
·1658
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IF 3
Hui Hong,Shiwei Xie,Aoxue Qiu,Yuming Yao,Wenzhe Jiang,Jilei Li,Zihao Wan,Shengjie Xiang,Chenyi Xi,Jingxian Xiao,Na Zhang
This study utilizes a natural air diffusion cathode (ADC) and an ultraviolet lamp to construct a UV/H2O2reactor for the in situ synthesis and activation of H2O2and evaluates its potential application in practical lake water treatment. The results indicate that the reactor exhibits stable treatment performance during a continuous flow experiment of 80 h. The air diffusion cathode maintains an H2O2concentration of above 350 mg·L−1in sodium sulfate electrolyte and shows no decreasing trend. Under the condition of approximately 59% H2O2utilization, the removal rates of COD and TOC are 37.6% and 40.0%, respectively; the rate of reduction of A254is 64.3%; while the total bacterial count removal rate reaches 100%. Large organic molecules in surface water are degraded to small organic molecules and mineralized to inorganic minor molecules. It effectively ameliorates the problem of organic pollution of surface water and effectively kills bacteria and improves the microbiological safety of the water body. Therefore, the UV/H2O2system developed in this study, based on electrochemically produced H2O2, is an effective method for treating micro-polluted surface water.
研究领域:
环境科学
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水处理工程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Binrong Li,Na Li,Zhiwei Guo,Chen Wang,Xuedong Wang,Zhi Zhu,Xu Tang,Pengwei Huo
Polymeric carbon nitride (PCN) is an environmentally friendly photocatalyst for solar-driven H 2 O 2 production, but the activity of original PCN is still not satisfactory. The main limitation is the sluggish exciton dissociation leading to slow generation and conversion of superoxide radical (•O 2 − ) intermediate. Herein, the PCN with dual defect sites and compact interlayer is rationally designed for H 2 O 2 photosynthesis with an ultrahigh rate of 3930.9 μmol g −1 h −1 and rapid •O 2 − yield rate of 1.92 min −1 . The enhanced activity is attributed to effective exciton dissociation during interlayer and intralayer process. Moreover, nitrogen vacancies change the oxygen adsorption configuration (formation of C − O − O − C bridge mode), thus promoting O 2 adsorption and activation. A well-matched linear relationship was established between the concentration of nitrogen vacancies and •O 2 − /H 2 O 2 production. This work not only provides in-depth insights for the photocatalytic H 2 O 2 generation mechanism, but also offers a new paradigm for designing efficient PCN-based photocatalysts for energy conversion.
研究领域:
材料科学
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光催化
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能源转换
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Chuan Wang,Hongchao Li,Fanglin Shen,Shijian Ge,Xuan Zhang,Jun Ma,Kan Zhang,Jieshu Qian,Bingcai Pan
Proton-coupled electron transfer (PCET) is a key factor in determining the H 2 O 2 production efficiency from oxygen reduction reaction (ORR) or direct H 2 /O 2 reaction, which usually requires the aid of proton donors including alcohols. Here, we report a strong metal-support interaction (SMSI) strategy to facilitate the PCET process of a typical Pd/TiO 2 photocatalyst for photocatalytic ORR into H 2 O 2 production in pure water. Compared to conventional Pd/TiO 2 photocatalysts, the Pd/TiO 2 photocatalyst with SMSI between Pd and TiO 2 (Pd/TiO 2 -850H) promotes photocatalytic H 2 O 2 production in pure water by 4.21-fold, which can be ascribed to that the SMSI simultaneously promotes the H 2 O dissociation and the photogenerated charge transfer from TiO 2 to Pd catalyst, enabling highly efficient proton transfer to be participated into converting •O 2 - to H 2 O 2 . Moreover, the formation of TiO 2-x overlayer caused by SMSI suppresses the H 2 O 2 decomposition and stabilizes Pd NPs, finally achieving an H 2 O 2 production rate of 4.10 mmol g −1 h −1 , which surpasses most metal/TiO 2 photocatalytic system.
研究领域:
化学
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材料科学
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环境科学
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高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Jing Li,Suxia Ma,Nuo Xu
Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), offers significant potential for valorization through the high-value synthesis of zeolites, exemplifying the waste-to-wealth approach. We determined the optimal synthesis conditions for FA-β zeolite using the alkali fusion hydrothermal synthesis method, with fly ash as the primary raw material. The conditions included a NaOH/FA ratio of 1.2, a SiO2/Al2O3 ratio of 30, an H2O/Al2O3 ratio of 1200, a TEAOH/Al2O3 ratio of 14, a β-seed addition of 7.5%, and hydrothermal conditions of 140 °C for 72 h. XRD and FTIR analyses confirmed that the diffraction peaks of the synthesized fly ash-based zeolite align well with the standard pattern of commercial β zeolite. Removal experiments indicated that the efficiency of nitrogen oxides removal hinges on the adequate oxidation of NO. Under optimized conditions, the FA-β zeolite demonstrated a removal efficiency of 83%. ESR analysis revealed that the removal mechanism involves the oxidative elimination of NO, catalyzed by FA-β zeolite through the decomposition of H2O2 to OH radicals. This novel synthesis method, which utilizes fly ash as the raw material to prepare β zeolite, offers advantages in terms of cost-effectiveness and environmental protection. It holds significant potential for applications in environmental conservation.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xiaobo Han,Wei Chen,Mao Xu,Tieliang Bai,Benxia Li
Photocatalytic synthesis of H 2 O 2 from O 2 reduction coupled with selective oxidation of organics into value-added chemicals is highly appealing; however, the troubling separation process presents a technical difficulty when both H 2 O 2 and organic products are obtained in a homogeneous solution. Herein, an amphiphilic Bi 2 WO 6 catalyst was synthesized through a facile solvothermal method based on the synergetic modification with both hydrophobic and hydrophilic groups, which enables the construction of Pickering emulsion interfacial photocatalysis systems in various organic/water mixtures to facilitate synchronous production and spontaneous separation of H 2 O 2 and value-added organics. The amphiphilic Bi 2 WO 6 catalyst exhibited significantly enhanced photocatalytic performance compared to its oleophilic and hydrophilic counterparts, resulting in remarkable generation rates of H 2 O 2 and benzaldehyde reaching up to 121.53 and 99.25 mmol g −1 h −1 , respectively, in a benzyl-alcohol/water biphasic system under simulated sunlight. The excellent photocatalytic performance could be maintained in a long-term reaction process. The photocatalytic mechanism was investigated through various control experiments and detailed characterizations. The interfacial photocatalysis played a crucial role in accelerating the redox reactions, showcasing its favorable applicability in various organic/water biphasic systems. This study provides guidelines for the realization of interfacial photocatalysis assisted by amphiphilic semiconductors, opening up a novel strategy to the simultaneous production of solar fuels and organic chemicals.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
FOOD CHEMISTRY
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2024
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IF 8.5
Yaxin Li,Shiwen Wu,Hongzhi Lu,Shoufang Xu
Organicphosphorus is a ubiquitous pesticide that has potential hazards to human health and environmental well-being. Therefore, the precise identification of residues of organophosphorus pesticides (OPs) emerges as an urgent necessity. A ratiometric fluorescent sensor for the detection of OPs by leveraging the catalytic activities of Ce 3+ and Ce 4+ on the two fluorescent substrates 4-Methylumbelliferyl phosphate (4-MUP) and o -phenylenediamine (OPD) correspondingly was designed. Ce 3+ can not only dephosphorylate 4-MUP to generate 4-methylumbelliferone (4-MU) with blue fluorescence, but it can also react with H₂O₂ to produce Ce 4+ and hydroxyl radicals (·OH), both of which exhibit peroxidase-like activity. These two species can oxidize the colorless substrate OPD into the yellow fluorescent product 2,3-diaminophenazine (DAP). Owing to the inner filter effect, the produced DAP diminishes the blue luminescence of 4-MU. So, with the increase of H 2 O 2 concentration, the blue fluorescence of 4-MU decreased while the yellow fluorescence of DAP increased. A ratiometric fluorescent sensor based on Ce 3+ -4-MUP-OPD triple system was established for H 2 O 2 detection with the fluorescence color of the solution changes from blue to yellow. OPs inhibit the activity of acetylcholinesterase (AChE) and prevent AChE and choline oxidase (ChOx) from acetylthiocholine chloride (ATChCl) to produce H 2 O 2 , thereby OPs can diminish DAP generation and reinstating the blue luminescence of 4-MU. The detection limits of H₂O₂ and OPs using fluorescence spectroscopy are 0.03 μM and 0.59 ng/mL, respectively. However, when coupled with a smartphone color recognition application, the visual detection limits for H₂O₂ and OPs are 9.7 μM and 19.6 ng/mL, respectively. The materials used in this ratiometric sensor are cost-effective and readily available, eliminating the need for material synthesis and simplifying the detection process. Additionally, the sensor integrates with a smartphone color recognition application, further streamlining the detection workflow and enabling real-time data analysis and result feedback. This combination provides a straightforward, efficient and economical solution for monitoring OPs in agricultural products.
研究领域:
分析化学
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环境科学
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食品科学
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DOI
PubMed
高影响因子
Analytical Methods
·
2024
·Vol. 16
·期 44
·7460-7467
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IF 2.7
Zhaolu He,Haiyang Xian,Liang Xu,Jianxi Zhu,Mang Lin,Xiaoliang Liang,Hongping He
Accurately quantifying hydrogen peroxide (H2O2) is essential for elucidating its role across diverse environments. Spectrophotometry is widely employed in laboratories for this purpose due to its convenience, cost-effectiveness, and low detection limits for micromolar H2O2 concentrations. However, accurate measurement of H2O2 in iron-containing solutions presents challenges due to the interference of iron ions. In this study, we propose a modified spectrophotometric method for H2O2 determination in iron-containing solutions by adding two types of iron ion chelators and selecting leuco crystal violet (LCV) as a chromogenic reagent due to its stability. By sequentially adding 1,10-phenanthroline and EDTA, and using a phosphate buffer at pH 4.2 to provide the optimal chromogenic pH condition, this modified method effectively mitigates the interference of iron ions in the LCV chromogenic reaction. The applicability of this method under aerobic and anaerobic conditions was confirmed by comparing the experimental results with theoretical simulations. Under optimal chromogenic conditions, this method achieves a detection limit of 300 nM. This improved method allows better detection of H2O2 in iron-containing systems and investigation of its significance in various environmental processes.
研究领域:
分析化学
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环境科学
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化学工程
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DOI
PubMed
高影响因子
Catalysts
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2024
·Vol. 14
·期 6
·364
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IF 3.8
Qiaoting Cheng,Hu Ding,Lang Chen,Jiatong Dong,Hao Yu,Shen Yan,Hua Wang
The two-electron oxygen reduction reaction (2e−ORR) has emerged as an attractive alternative for H2O2production. Developing efficient earth-abundant transition metal electrocatalysts and reaction mechanism exploration for H2O2production are important but remain challenging. Herein, a nitrogen-doped carbon-coated NiSe2(NiSe2@NC) electrocatalyst was prepared by successive annealing treatment. Benefiting from the synergistic effect between the NiSe2nanoparticles and NC, the 2e−ORR activity, selectivity, and stability of NiSe2@NC in 0.1 M HClO4was greatly enhanced, with the yield of H2O2being 4.4 times that of the bare NiSe2nanoparticles. The in situ Raman spectra and density functional theory (DFT) calculation revealed that the presence of NC was beneficial for regulating the electronic state of NiSe2and optimizing the adsorption free energy of *OOH, which could enhance the adsorption of O2, stabilize the O-O bond, and boost the production of H2O2. This work provides an effective strategy to improve the performance of the transition metal chalcogenide for 2e−ORR to H2O2.
研究领域:
材料科学
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电化学
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催化反应
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DOI
高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Qiang Wang,Haiqing Hao,Zhengyang Wu,Meng Wang,Zongyu Feng,Yongqi Zhang,Xiangxin Xue,Xiaowei Huang
The MgCl 2 wastewater generated from rare earth extraction and separation process was treated by spray pyrolysis with H 2 O 2 as an additive for the first time, and achieving full recycling of MgCl 2 wastewater. The effect of H 2 O 2 on the spray pyrolysis process, the kinetic of the spray pyrolysis process, and the mechanism of the effect on the activity of MgO powder were investigated. The results showed that H 2 O 2 and the O 2 produced by its decomposition had strong oxidizing property, which contributed to the removal of Cl roots. The kinetic results indicated that the rate determining step of MgCl 2 spray pyrolysis was transformed from chemical reaction to diffusion process after the temperature exceeded 1023 K. The activity study indicated that the doping of Cl led to severe distortion of the MgO grains, and polycrystalline basic magnesium chloride had more defect sites too. Thus, the powder showed high activity. Moreover, the thermal decomposition rate of MgCl 2 reached 99.83 %, the alkalinity of the powder reached 0.044 mol/g, and the iodine absorption value reached 131.81 mg I 2 /g MgO at temperature of 1073 K and amount of H 2 O 2 addition of 1 %. Meanwhile, the high purity hydrochloric acid with concentration of 6.54 mol/L was obtained.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
International Journal of Environmental Science and Technology
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2024
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IF 3
Cui Y. P.,Huang Q.,Cao J. G.,Dong W.,Cui X. X.,Lu Y.,Li Y. J.,Huang Z. Q.
Fe 0 -based heterogeneous Fenton process has been increasingly developed for organic pollutants removal. However, the reaction activity of Fe 0 catalyst is easily weakened due to the formation of dense oxide layer or the precipitation of iron hydroxides on the surface. Herein, the effect and mechanism of magnetic field (MF), visible light (Vis), nitrilotriacetic acid (NTA) and inorganic salt ions on the Fe dissolution and dimethyl phthalate (DMP) degradation in the Fe 0 /H 2 O 2 system were investigated. The results showed that the magnetic field (100 mT), NTA and inorganic salt ions effectively enhanced the dissolution of Fe from the surface of iron filings, and visible light significantly accelerated the Fe 3+ /Fe 2+ cycle in the aqueous phase, which promoted the decomposition of H 2 O 2 by Fe 2+ to generate •OH and further enhanced the degradation of DMP. DMP was nearly completely degraded within 60 min in the pH range of 3.0–9.0, indicating the MF/Vis/NTA/Fe 0 /H 2 O 2 system effectively broadened the pH range of Fenton-like system. The iron sand column tests proved that the MF/solar/NTA/Fe 0 /H 2 O 2 system was effective for the treatment of waste leachate reverse osmosis concentrate as a typical actual high-salt wastewater, in which the removal rates of chemical oxygen demand and humic acid reached 84.5 and 90.6%, and the chromaticity was almost completely removed. Generally, the activation mechanism of Fe 0 -based heterogeneous photo-Fenton system was set up and an effective method for organic pollutant removal and high-salt wastewater treatment was provided.
研究领域:
环境科学
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化学工程
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高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 14
·8420-8428
·
IF 10.7
Xinyue Li,Qiuang Zheng,Xiaoran Wang,Qiuyu Zheng,Yi Zhang,Yanqing Cong,Shi-Wen Lv
Photocatalytic two electron oxygen reduction reaction is considered to be a promising approach for green H2O2 production. Herein, for the first time, an intramolecular donor–acceptor (D–A) conjugated polymer was constructed in resorcinol-formaldehyde (RF) resin by embedding benzothiadiazole. As a typical electron deficient group, the introduction of benzothiadiazole can increase the specific surface area of RF and expose more active sites, and the hydrophobicity was also improved, thereby enhancing the affinity of RF to O2. Owing to the potential difference between the electron donor and acceptor, the formation of a D–A conjugated polymer can provide a driving force to separate photoinduced charge, prolonging the lifetime of photogenerated charge and restraining the recombination of photogenerated electrons and holes. Furthermore, the light absorption ability of RF was enhanced after the introduction of benzothiadiazole. As expected, the catalyst (namely RF-BZ) exhibited excellent performance in photocatalytic H2O2 evolution, and the highest yield of H2O2 over RF-BZ can reach 2553.2 μmol g−1. More importantly, the thermodynamic analysis based on DFT calculations revealed that the introduction of benzothiadiazole can reduce the adsorption energy of O2 over RF, and the Gibbs free energy of the rate-determining step for the two-electron oxygen reduction reaction was also reduced to 0.28 eV from 2.05 eV. In short, the current study provides a valuable reference for future research on photocatalytic H2O2 production.
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
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Tianshuang Song,Huilin Huang,Aiping Zhang
While copper-based Fenton-like systems can effectively degrade organic matter in the effluent from membrane bioreactor (MBR), the performance is hindered by sluggish Cu 2+ /Cu + cycling and oxidant inefficiency. In this study, a UV-synergized CuS-activated H 2 O 2 system was constructed, and the removal efficiency and synergistic mechanism for organic matter in MBR effluent were investigated. Under optimized conditions (UV=14 W, CuS=0.06 g/L, [H 2 O 2 ]=50 mM, pH=3.0, t=60 min), the UV/CuS/H 2 O 2 system achieved removal efficiencies of 62.49%, 89.81%, and 38.48% for UV 254 , color number (CN), and total organic carbon (TOC) respectively. This performance is attributed to the disruption of aromatic structures and a reduction in molecular weight, condensation degree, and humification degree. Reactive oxygen species characterization confirmed the presence of hydroxyl radicals ( • OH), singlet oxygen ( 1 O 2 ) and superoxide radical anions (O 2 •− ) in the system, with O 2 •− identified as the dominant reactive species driving the process. Through analysis of the material morphology, distribution of copper compounds, and changes in oxidation states, the reaction mechanism of the UV/CuS/H 2 O 2 system can be summarized as homogeneous and heterogeneous Fenton-like reactions coupled with CuS adsorption, all of which are jointly promoted by the photochemical effects of ultraviolet radiation. Additionally, benzoic acid removal remained above 96% over six cycles with minimal Cu 2+ leaching, confirming the reusability and environmental compatibility of CuS. This study provides a theoretical basis for using the UV/CuS/H 2 O 2 system to remove organic matter from landfill leachate.
研究领域:
环境工程
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高级氧化技术
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水和废水处理
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化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）