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CHEMOSPHERE · 2024 · IF 8.1

E-peroxone with a novel GDE decorated with hydrophobic membrane for the degradation of pyridine: Stability, byproducts and toxicity

Qiqi Zhang,Leping Chu,Qin Yang,Wenqing Wo,Anlin Xu,Yide He,Yongjun Zhang

E-peroxone process is an emerging electrochemical oxidation process , based on ozone and the in-situ cathodic generation of H 2 O 2 , but the stability of cathode is one of the key restraining factors. In this study, we designed a multilayer gas diffusion electrode (GDE) decorated with a commercial hydrophobic membrane for the degradation of pyridine. It was found that a proper control of membrane pore sizes and hot-pressing temperature can significantly promote the GDE stability. Subsequently, key operational parameters of the constructed E-peroxone system were investigated, including the ozone concentration, current density, pH value, electrolyte type and initial concentration of pyridine. The degradation pathways were proposed according to six identified transformation products. The toxicity variation along the degradation progress was evaluated with microbial respiration tests and Toxicity Estimation Software Tool (T.E.S.T.) calculation and an efficient detoxification capacity of E-peroxone was observed. This research provides a theoretical basis and technical support for the development of highly efficient and stable E-peroxone system for the elimination of toxic organic contaminants.

研究领域: 环境科学 · 电化学工程
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2024 · IF 4.1

Enhancing H2O2 production with a self-breathing gas diffusion electrode fabricated via ultrasonic impregnation and vacuum filtration

Zilong Zhang,Xia Qin,Cuicui Xu,Fanbin Zhang,Xinrui Liu,Yumei Yang

In this study, an electro-Fenton gas diffusion electrode featuring air self-respiration was fabricated by incorporating carbon nanotubes, carbon nitride, and polytetrafluoroethylene onto graphite felt. The fabrication process involved a synergistic approach of ultrasonic impregnation and vacuum filtration, establishing a gas–liquid-solid tri-phase interface both on the surface and within the electrode. This preparation method facilitates autonomous air intake, diffusing it to the tri-phase reaction interface, thereby eliminating the necessity for aeration and reducing operational costs. The optimal electrode preparation conditions were determined through Box-Behnken Design response surface experiments, leading to the enhancement of H 2 O 2 production conditions. Under the optimized conditions, H 2 O 2 accumulation reached 45.83 mg L −1 cm −2 h −1 , surpassing the performance achieved with conventional ultrasonic impregnation and vacuum filtration methods. Furthermore, the performance of self-breathing and the impact factors are explored. Finally, the electrode’s efficacy was demonstrated through the degradation of phenol and bisphenol A with concentrations of 100 mg L −1 exhibiting degradation rates of 92 % and 95 %, respectively, within 60 min.

研究领域: 环境科学 · 材料科学 · 化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Two-dimensional ZrCo nanosheets as highly effective catalyst for hydrogen storage in MgH2

Liuting Zhang,Zeliang Cai,Xinqiao Zhu,Zhendong Yao,Ze Sun,Liang Ji,Nianhua Yan,Beibei Xiao,Lixin Chen

Magnesium, a cheap and abundant metal, holds tremendous promise for on-board hydrogen storage over the past several decades. However, the practical application of MgH 2 is still hampered by various challenges, including a high efficient catalyst. Zirconium and Zr-based alloys show great potential to serve as hydrogen transfer center due to their high activity in hydrogen dissociation and diffusion. In this paper, ZrCo nanosheets were successfully prepared via a facile wet-chemical technique and then introduced to improve the hydrogen storage properties of MgH 2 . With the addition of 10 wt% ZrCo nanosheets, the modified MgH 2 composite could desorb approximately 6.3 wt% H 2 within 5 min at 300 °C and absorb 4.4 wt% H 2 under 3 Mpa hydrogen pressure in 10 min even at 120 °C. The de/hydrogenation activation energy were calculated to be 90.4 ± 1.6 kJ/mol and 57.6 ± 1.0 kJ/mol for the MgH 2 +10 wt% ZrCo composite, which reasonably explain the remarkably improved de/hydrogenation performance. X-Ray Diffraction (XRD) and Transmission electron microscope (TEM) results revealed that hydrogen could be diffused between the composite more easily with the presence of well dispersed ZrCo, which acted as “hydrogen pump” for hydrogen boundaries/interface diffusion along the Mg/MgH 2 interfaces. Theoretical calculations revealed that the Mg–H bonds were extracted and weakened when adsorbed on the surface of ZrCo. Furthermore, the MgH 2 +10 wt% ZrCo composite showed superior cycling performance with the aid of graphene, indicative of potential application in the nearest future in the area of hydrogen storage.

研究领域: 材料科学 · 能源存储
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FOOD RESEARCH INTERNATIONAL · 2023 · IF 8.1

Influence of interfacial properties/structure on oxygen diffusion in oil-in-water emulsions

Yanlei Li,Fangfang Chen,Zhiming Gao,Wei Xiang,Yuehan Wu,Bing Hu,Xuewen Ni,Katsuyoshi Nishinari,Yapeng Fang

Oxygen diffusion played an important role in the lipid oxidation of food emulsions . In this study, a simple method was developed to quantitatively observe the oxygen diffusion in the oil–water biphasic system, and it was further applied to investigate the relationship between the oxygen diffusion and lipid oxidation in O/W emulsions. Various factors that related to the emulsion oxidation were considered, from their influence on the oxygen diffusion and lipid oxidation in the emulsions. Results showed that there was obvious correlation between the oxygen diffusion and lipid oxidation in O/W emulsions, which reveals the inhibition of oxygen diffusion could apparently slow down the lipid oxidation. Moreover, the changes of oil phase, water phase and interfacial layer of the emulsions, which were related to the oxygen diffusion, could improve the oxidative stability of the emulsions effectively. Our findings are helpful for deep understanding the mechanisms of the lipid oxidation in food emulsions.

CAS / MDL: 57-11-4
研究领域: 食品科学 · 生物化学
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Water · 2024 ·Vol. 16 ·期 12 ·1658 · IF 3

Efficient H2O2 Production and Activation by Air Diffusion Cathode Combined with Ultraviolet for Lake Water Treatment: A Long-Term Evaluation

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.

CAS / MDL: 13825-74-6
研究领域: 环境科学 · 水处理工程
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Aiming the water transport issues of anion exchange membrane fuel cells by introducing hydrophobic carbon nanotube diffusion layer

Zijie Zhang,Cailin Xiao,Haodong Huang,Mahmood ul Haq,Zheng Li,Lin Zeng

The gas diffusion layer (GDL) enhances the transport efficiency of reaction gases and facilitates the removal of accumulated liquid water, thereby improving water management in anion exchange membrane fuel cells (AEMFCs). Carbon nanotubes (CNTs) are recognized as one of the promising materials to optimize mass transport within GDLs. In this study, we successfully synthesized an abundance of CNTs on the surface of commercial gas diffusion media. The as-prepared CNT layer exhibits exceptionally high hydrophobic properties and forms a hierarchically hydrophobic structure combined with the gas diffusion media, effectively enhancing the mass transfer of the membrane electrode assembly (MEA) and reducing ohmic impedance. Under supersaturation conditions, the power density of the MEA containing CNTs reaches 1031.7 mW/cm 2 , significantly higher than the 760.64 mW/cm 2 observed for the commercial GDL. Further testing demonstrates that the MEA containing CNTs exhibits a limiting current density of 2507.4 mA/cm 2 , which is much superior to the benchmark MEA with the commercial GDL (1591 mA/cm 2 ). Electrochemical impedance spectroscopy analysis reveals that the mass transfer resistance of MEAs with CNTs is lower than that of MEAs with the commercial GDL. More importantly, the phase-field modeling is performed to simulate the transport of the liquid water in the hierarchical GDL.

CAS / MDL: 7697-37-2 7664-93-9
研究领域: 材料科学 · 能源科学 · 电化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Promoting Photodegradation Efficiency via a Heterojunction Photocatalyst Combining with Oxygen Direct and Fast Diffusion from the Gas Phase to Active Catalytic Sites

Fengying Shao,Li Mi,Zhaoyan Tian,Cheng Zheng,Yuanjian Zhang,Quan Li,Songqin Liu

The low solubility of oxygen in solution is the main obstacle for the biodegradation of organic pollutants in wastewater. To address this problem, inspired by the degradation mechanism of aerobic bacteria toward organic pollutants, a novel photodegradation system was presented and operated by a heterojunction photocatalyst combining with a hydrophobic triphase interface, allowing oxygen to directly diffuse from the gas phase to active catalytic sites submersed in polluted solutions. Especially, the heterojunction photocatalyst was fabricated by graphitic carbon nitride nanosheets (C3N4 NS) sensitized with 5,10,15,20-tetrakis(4-carboxylphenyl)porphyrin (TCPP). The resulting photocatalyst was coated on a certain part of the commercial superhydrophobic carbon paper (CP) and submersed in the polluted wastewater, while the other part of hydrophobic CP (without coating with C3N4-TCPP nanocomposite) was exposed to air to form a gas–liquid–solid tri-phase photodegradation system. With this system, the photodegradation rate was 10-fold higher than that of a conventional liquid/solid diphase system in oxygen-saturated solutions. This was, on one hand, due to the abundant oxygen on the surface of a photocatalyst coming from the fast and direct diffusion from the gas phase through the superhydrophobic nanoporous part of CP. On the other hand, the hybrid C3N4-TCPP nanocomposite enhanced the light absorption efficiency under simulated sunlight irradiation and restrained the recombination of photogenerated electron–hole. Moreover, the triphase photodegradation system was stable in aqueous solutions for a long time and can be reused almost without attenuation for five cycles, which provided a great potential to be utilized for practical wastewater treatment.

研究领域: 环境科学 · 材料科学 · 化学工程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2015 ·Vol. 22 ·期 20 ·15812-15820 · IF 2.828

Enhanced hydroxyl radical generation in the combined ozonation and electrolysis process using carbon nanotubes containing gas diffusion cathode

Wu Donghai,Lu Guanghua,Zhang Ran,Lin Qiuhong,Yan Zhenhua,Liu Jianchao,Li Yi

Combination of ozone together with electrolysis (ozone-electrolysis) is a promising wastewater treatment technology. This work investigated the potential use of carbon nanotube (CNT)-based gas diffusion cathode (GDC) for ozone-electrolysis process employing hydroxyl radicals (·OH) production as an indicator. Compared with conventional active carbon (AC)-polytetrafluoroethylene (PTFE) and carbon black (CB)-PTFE cathodes, the production of ·OH in the coupled process was improved using CNTs-PTFE GDC. Appropriate addition of acetylene black (AB) and pore-forming agent Na 2 SO 4 could enhance the efficiency of CNTs-PTFE GDC. The optimum GDC composition was obtained by response surface methodology (RSM) analysis and was determined as CNTs 31.2 wt%, PTFE 60.6 wt%, AB 3.5 wt%, and Na 2 SO 4 4.7 wt%. Moreover, the optimized CNT-based GDC exhibited much more effective than traditional Ti and graphite cathodes in Acid Orange 7 (AO7) mineralization and possessed the desirable stability without performance decay after ten times reaction. The comparison tests revealed that peroxone reaction was the main pathway of ·OH production in the present system, and cathodic reduction of ozone could significantly promote ·OH generation. These results suggested that application of CNT-based GDC offers considerable advantages in ozone-electrolysis of organic wastewater.

研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2023 · IF 8.8

Activated carbon filled in a microporous titanium-foam air diffusion electrode for boosting H2O2 accumulation

Fengxia Deng,Shilin Yang,Baojian Jing,Shan Qiu

In the electro-Fenton process, there still suffers concern of low H 2 O 2 generation caused by inadequate mass transfer of oxygen and low selectivity of oxygen reduction reaction (ORR). To solve it, in this study, various particle sizes (850 μm, 150 μm, and 75 μm) of granular activated carbon filled in a microporous titanium-foam substate was used to develop a gas diffusion electrode (AC@Ti–F GDE). This facile-prepared cathode has seen a 176.15% improvement in H 2 O 2 formation compared to the conventional one. Aside from a much higher oxygen mass transfer by creating gas-liquid-solid three-phase interfaces coupled with much high dissolved oxygen, the filled AC played a significant role in H 2 O 2 accumulation. Among these particle sizes of AC, the one in 850 μm has observed the highest H 2 O 2 accumulation, reaching 1487 μM in 2 h electrolysis. Because there is a balance between chemical nature for H 2 O 2 formation and micropore-dominant porous structure for H 2 O 2 decomposition, resulting in an electron transfer of 2.12 and H 2 O 2 selectivity of 96.79% during ORR. In a word, the facial AC@Ti–F GDE configuration is promising for H 2 O 2 accumulation.

研究领域: 环境科学 · 电化学工程
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Pocket-shaped air-breathing electrodes used for in-situ synthesis of hydrogen peroxide and application

Shunxi Zhang,Hengyuan Tong,Yongkang Mou,Yiyang Zhou,Xinyi Huang,Yun He,Wenjuan Shen,Jianfen Li

A novel pocket-shaped air-breathing electrode (PSABE) is prepared using carbon material (CM), polytetrafluorethylene (PTFE), pulp and filler. Additionally, an in-situ electro-synthesis of H 2 O 2 is constructed using the PSABE and the carbon felt. The results show that under current density of 50 mA/cm 2 and solution pH of 3, compared with classical gas diffusion electrode and micropore-adjusted gas diffusion electrode, the PSABE's H 2 O 2 yield is the highest and 110.1 mg/(L.cm 2 ) in 90 min, and its oxygen diffusion coefficient is also the highest and 1.68 × 10 −5 m 2 /s. When the optimal mass ratio of PTFE:filler in the electrode wall:filler in the electrode pocket:CM is 1.5:3:3:1, the PSABE's H 2 O 2 yield further climbs to 112.0 mg/(L.cm 2 ). A series of detections show that when filler in the electrode wall increases, the PSABE's pore structure is more abundant, active sites are more and oxygen diffusion capability becomes better. Similarly, when filler in the electrode pocket increases, air mobility inside and outside the cavity goes easier and the PSABE oxygen diffusion capability improves, too. Additionally, when current density varies from 20 to 70 mA/cm 2 , H 2 O 2 yield for 70 mA/cm 2 can attain to 143.4 mg/(L.cm 2 ) while current efficiency and energy consumption for 20 mA/cm 2 is 84.9% and 8.4 KWh/kg, respectively. Moreover, results of H 2 O 2 yield, disinfection and wastewater treatment show that the prepared PSABE is effective and feasible.

CAS / MDL: 9002-84-0
研究领域: 环境科学 · 电化学工程 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

A triple-cathode electron-Fenton system for efficient Fe2+ regeneration and in-situ H2O2 electro-activation

Dongliang Wang,Yuxiao Li,Shaogang Hu,Jingping Hu,Huijie Hou,Bingchuan Liu,Han Zheng,Xi Luo,Haixiao Li

Electro-Fenton (EF) has shown great advantages in the effecient degradation of recalcitrant organic pollutants through in situ generation of •OH, and the main limitations on system performance are the efficiencies of H 2 O 2 activation and Fe 2+ regeneration. In this research, a triple-cathode EF system with a microbial fuel cell (MFC) cathode for the acceleration of Fe 2+ regeneration, a gas diffusion electrode for H 2 O 2 production and a stainless steel mesh (SSM) for electro-activation of H 2 O 2 was designed for efficient degradation of organic pollutants. The triple-cathode EF exhibited improved removal rate for recalcitrant organic pollutants with an average electricity consumption of 18.2 kWh Kg −1 TOC for Rhodamine B degradation, and the dosage of Fe 2+ could be reduced to 0.1 mM due to better utilization of H 2 O 2 and inhibition of parasitic reactions. Electrochemical characterization and theoretical calculation revealed that both one-electron reduction and H*-mediated activation contributed to the electro-activation of H 2 O 2 on SSM. This work demonstrates a novel construction and feasible approach for efficient EF with low cost.

CAS / MDL: 7782-42-5
研究领域: 环境科学 · 电化学工程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 30 ·期 7 ·17854-17864 · IF 5.19

Singlet oxygen generation for selective oxidation of emerging pollutants in a flow-by electrochemical system based on natural air diffusion cathode

Li Yi,Xie Shiwei,Yao Jiaxiong

The decay of free radicals involved in side reactions is one of the challenges faced by electrochemical degradation of organic pollutants. To this end, a non-radical oxidation system was constructed by a natural air diffusion cathode (ADC) and a Ti-based dimensional stable anode coated by RuO 2 (RuO 2 -Ti anode) for cathodic hydrogen peroxide activation by anodic chlorine evolution. The ADC fabricated by the carbon black of BP2000 produced a stable concentration of hydrogen peroxide of 339.94 mg L −1 (current efficiency of 73.4%) without aeration, which was superior to the cathode made by the XC72 carbon black. The flow-by ADC-RuO 2 system consisted of an ADC and a RuO 2 -Ti anode showed high selectivity to aniline (AN) compared to benzoate (BA) in a NaCl electrolyte, whose degradation efficiencies were 97.72% and 1.3%, respectively. Rapid degradations of a mixture of emerging pollutants and AN were also observed in the ADC-RuO 2 system, with pseudo-first-order kinetic constants of 0.51, 1.29, 0.89, and 0.99 min −1 for Bisphenol A (BPA), tetracycline (TC), sulfamethoxazole (SMX) and AN, respectively. Quenching experiments revealed the main reactive oxygen species for the pollutant degradation was singlet oxygen ( 1 O 2 ), which was also identified by the electron spin resonance (ESR) analysis. Finally, the steady-stable content of 1 O 2 was quantitatively determined to be 6.25 × 10 −11  M by the method of furfuryl alcohol (FFA) probe. Our findings provide a fast, low energy consumption and well controlled electrochemical oxidation method for selective degradation of organic pollutants. Graphical abstract H 2 O 2 generated on an air diffusion cathode by naturally diffused O 2 , reacts with ClO − produced from chloride oxidation on the RuO 2 -Ti anode to form singlet oxygen ( 1 O 2 ). The electrochemical system shows an efficient oxidation to electron-rich emerging pollutants including bisphenol A, tetracycline, sulfamethoxazole and aniline, but a poor performance on the electron-deficient compounds (e.g., benzoate).

研究领域: 环境科学 · 电化学工程
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