ACS ES&T Engineering
·
2025
·
IF 6.7
Ao Zhong,Kehan Li,Zeyu Duan,Haiqiang Wang,Zhongbiao Wu
Trimethylamine (TMA) is a common malodorous compound that poses serious environmental and health risks. Four different structures of cerium oxide (CeO2), namely, cubes, hollow spheres, octahedrons, and spindles, were successfully synthesized via a hydrothermal method and then used for TMA degradation in a vacuum ultraviolet photocatalytic oxidation system. All the synthesized catalysts exhibited enhanced activity compared with commercial CeO2. The hollow-sphere CeO2 demonstrated high catalytic performance, achieving 75.9% mineralization of TMA within 90 min and substantially reduced ozone generation (stable 0 ppm in outlet). Additionally, the total outlet concentration of secondary nitrogenous pollutants (NOx and NH3) remained below 2.5 ppm. In situ infrared spectroscopy was employed to elucidate the degradation pathway of TMA under vacuum ultraviolet irradiation, comparing sphere CeO2 with commercial CeO2. The superior TMA degradation performance of the hollow-sphere CeO2 was attributed to its higher Ce3+ ratio as well as increased oxygen, increased charge separation efficiency, and radical generation. This study provides new insights into the optimization of CeO2-based photocatalysts to efficiently degrade TMA and offers promising solutions for odor control and environmental protection.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Min Li,Chenglong Qiu,Tulai Sun,Xiaosa Wang,Liwei Xia,Xinying Yang,Wei Zhao,Huaijie Shi,Lei Ding,Xing Zhong,Yihan Zhu,Jianguo Wang
A major challenge that limits the applications of nanostructured electrocatalysts is precise surface structure regulation. The critical performance-impeding factors for the important electrochemical ozone production (EOP) lie in the leaching-induced poor stability as well as the competing oxygen evolution and ozone production reactions over the most promising platinum-based electrocatalysts. Although composition diversification by alloying appears to be a prevailing strategy to optimize platinum-based electrocatalysts, a practical restriction turns out to be the inevitable surface segregation and termination of platinum-enriched structures due to their lower surface energies. In this work, we introduce the nanoconfinement of intermetallic platinum–nickel nanostructures encapsulated by boron carbide, which effectively frustrates the surface segregation of alloy nanostructures and well maintains the pristine termination of the alloy. Precise atomic-level structural elucidation and model construction of the encapsulated alloy nanostructures are achieved by quantitative electron microscopy. The composite nanoalloy with a unique surface termination evokes synergetic catalytic effects that promote the charge transfer between the surface and adsorbed oxygen intermediates, which entails outstanding EOP performance with a high Faraday efficiency of 14.8% in neutral media and long-term stability of up to 120 h as a qualified electrocatalyst for the EOP electrolyzer devices. More importantly, the current work paves a new route to overwhelm the thermodynamically limited surface structures of bare nanoalloy catalysts through diverse nanoconfinement strategies.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Yan Shao,Ming Qiao,Jintao Wu,Yifan Yan,Huanhao Chen,Xueying Zhang
This study presents an innovative and eco-friendly method for wastewater treatment, emphasizing the degradation of tetracycline hydrochloride (TCH) through the use of monolithic materials in a trickle-bed dielectric-barrier-discharge (DBD)-based plasma reactor. Modifications to monolithic surface coatings can be utilized to investigate their impact their effects on plasma degradation and energy efficiency. Loading graphitic carbon nitride (g-C 3 N 4 , CN) onto the surface of a monolithic material allows for the modulation of functional groups on the material's surface and the homogeneity of liquid film flow, thereby influencing the generation of active substances and mass transfer at the gas-liquid interface. This study employed hydrothermal techniques to synthesize hydroxyl-grafted and fluorine-grafted g-C 3 N 4 coatings on the surface of open-cell ceramic foam (CN-OH@CF and CN-F@CF, respectively). The CN-OH-6@CF/plasma system exhibits the highest degradation efficiency at 91.1 % and an energy efficiency of 0.5 g/kWh. Active substances generated by plasma, such as ozone (O 3 ), hydroxyl radicals ( OH), and hydrogen peroxide (H 2 O 2 ), were quantified in a liquid falling film DBD-based plasma system. In the CN-OH-6@CF/plasma system, the concentration of OH was 4.55 mg/L at 60 min, the yield H 2 O 2 exceeded 4.04 mg/L and the concentration of O 3 reached 1.17 mmol/L at 60 min. These values were significantly higher than those observed in the CN@CF/plasma or CN-F@CF/plasma systems. The incorporation of – OH groups in CN coatings significantly enhances the production of the direct plasma product O 3 and optimizes O 3 mass transfer at the gas-liquid interface, achieving up to 85 % O 3 contribution in the CN-OH-6@CF/plasma system. The electron transfer number of 2.7 and the H 2 O 2 selectivity of 64.5 % for grafting − F on CN coatings support the selective generation of H 2 O 2 via a two-electron reaction process, as evidenced by rotating ring-disk electrode tests. The selective generation of H 2 O 2 is not conducive to energy efficiency and promotes accelerated degradation. O 3 , in conjunction with H 2 O 2 , promotes the acceleration of its decomposition and the production of OH.
研究领域:
环境科学
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材料科学
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等离子体技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Qiuyang Yu,Ziyi Jiang,Jinlong Yin,Shengli Chen,Xiaohong Hu
Because of its metal-like conductivity, excellent catalytic activity, and acid resistance, lead dioxide (PbO2) is the most used electrocatalyst for the practical electrochemical ozone production (EOP) technique. Introducing fluorine (F) into PbO2 electrodes or electrolytes can significantly improve EOP activity. However, there is still lack of valid evidence on understanding the role of doping F in the PbO2 electrode. In this work, we report a comprehensive study on the effect of F on EOP activity on electrochemically prepared PbO2 electrodes. F doping suppresses the side reaction of dioxygen (O2) evolution by inhibiting the formation of an α phase impurity of PbO2 electrodes. The more hydrophobic surfaces by doping F promote O2 adsorption as evidenced by low-temperature O2-temperature-programmed desorption experiments and thus are more favorable for ozone (O3) generation. The in situ isotope labeling oxygen (18O2) experiment proves that at room temperature, O2 can adsorb and dissociate on the operando PbO2 electrode surface and participate in the formation of O3 molecules. This work provides a comprehensive understanding of doping F for enhanced EOP.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2022
·Vol. 9
·期 22
·e202200919
·
IF 4.782
Qiuyang Yu,Xiaohong Hu
Graphical O 3 generation : By adjusting the concentration of sodium hydroxide during hydrothermal preparation process, the phase and size-controlled synthesis of PbO 2 was achieved. Later, a phase/size effect in electrochemical ozone generation reaction was found and an optimal PbO 2 microsphere catalyst was successfully screened out. This achieved a 61 % higher O 3 current efficiency at 2 A cm −2 than electrochemically prepared PbO 2 -based catalyst. Traditional electrochemically prepared lead dioxide (e-PbO 2 ) is one of the most used electrode materials for electrochemical ozone production (EOP), because of its high catalytic activity, excellent electrical conductivity, relative stability and low cost. But the electrochemically prepared conditions are complicated and harsh. Bulk PbO 2 electrodes have the very limited surface area and are inconvenient to process into the fine film electrodes for a PEM electrolyser. In contrast, chemical synthesis is easy to prepare uniform PbO 2 catalysts with high surface area and catalytic activity. Here, a facile one-pot approach to prepare a highly active PbO 2 microsphere catalyst was established and used for the EOP reaction in a PEM ozone generator. Sodium hydroxide could be used to regulate the relative content of α/β allotropic phase and crystallite size of PbO 2 microspheres. Experiment results revealed that high β phase content and large β-PbO 2 crystallite size were beneficial to the high EOP activity. By optimizing the composition and crystal structure, chemically prepared PbO 2 could have much better EOP performance than e-PbO 2 .
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
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 24
·24241-24252
·
IF 2.8
Zhu Jianqiang,Tsona Narcisse T.,Du Lin
Chloroalkenes are among the important anthropogenic organic compounds emitted in the atmosphere as a result of their wide use in synthetic processes in industry. Despite their well-known adverse effects on human health and air quality, the chemistry of these chloroalkenes remains poorly explored. In this work, reactions of 4-chloro-1-butene (CBE), a representative example of chloroalkenes, with O 3 , OH, NO 3 , and Cl are investigated in a 100-L Teflon reaction chamber equipped with gas chromatography-flame ionization detector (GC-FID). The absolute rate method was used for the reaction with O 3 while the relative rate method was used for reactions with OH, NO 3 , and Cl. The following rate constants were obtained at room temperature (298 ± 2) K and atmospheric pressure: (3.96 ± 0.43) × 10 −18 , (2.63 ± 0.96) × 10 −11 , (4.48 ± 1.23) × 10 −15 , and (2.35 ± 0.90) × 10 −10 cm 3 molecule −1 s −1 , for reactions with O 3 , OH, NO 3 , and Cl, respectively. Atmospheric lifetimes of CBE calculated from rate constants of the different reactions obtained in this work showed that reaction with OH is the main loss process for CBE, while in coastal areas and in the marine boundary layer, the CBE loss by Cl reaction becomes important. Estimation of the value of the photochemical ozone creation potential (POCP) indicated that CBE has a large ozone formation potential. The present work underlines the need for further studies on the atmospheric chemistry of chlorinated VOCs.
研究领域:
大气化学
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环境科学
·
有机化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 12
·123504
·
IF 4.316
Yuan Du,Liu Hao,Wang Zixuan,Wang Xi,Miao Guirong,Wu Xu
β-PbO2 is an important high oxygen overpotential anode coating material. Further study on nanoscale β-PbO2 with higher performance and lower cost is a critical issue in order to develop the electrochemical ozone generator. Herein, an improved β-PbO2 nanoparticles synthesizing strategy based on the traditional Pb(OAc)4 hydrolysis method is proposed in this work, which is more scalable for industrial-scale production compared with existed nano β-PbO2 synthesizing methods. The possible mechanism of synthesizing β-PbO2 nanoparticles via Pb(OAc)4 hydrolysis was discussed for the first time. Based on the proposed mechanism, the size and morphology of the β-PbO2 nanoparticles were effectively controlled, and alternative raw material that can significantly reduce costs was developed. SEM, TEM, XRD, and XPS results indicate that pure phase β-PbO2 nanoparticles range from 10–30 nm were obtained. In addition, the use of alternative raw materials reduces the cost by 90%–95% compared to the traditional Pb(OAc)4 hydrolysis method. The β-PbO2 nanoparticles showed good ozone generation performances. The energy consumption per unit ozone of the β-PbO2 nanoparticles is reduced by 51.9% at the optimized operation condition than the reference PbO2 particles used for comparison.
研究领域:
材料科学
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环境工程
✓ 已验证
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2023
·
IF 9.1
Yifen He,Chao Qu,Na Ren,Dawei Liang
ABSTRACT Recently, a novel 2-electron oxygen reduction reaction (ORR) based electro-oxidation (EO) system was developed, which utilizes a H 2 O 2 generation cathode instead of H 2 evolution cathode. A Ti-based Ni-Sb co-doped SnO 2 (Ti/NATO) anode was selected for efficient degradation of refractory organics and O 3 production. The synergistic reaction of O 3 /H 2 O 2 further accelerated the generation of hydroxyl radicals ( • OH) in the ORR-EO system. However, the catalytic activity and long-term effectiveness of the Ti/NATO anode limited the large-scale application of the ORR-EO process. In this study, a blue TiO 2 nanotube array (blue-TiO 2 -NTA) inter-layer was introduced into the fabrication process between the Ti substrate and NATO catalyst layer. Compared to the Ti/NATO anode, the Ti/blue-TiO 2 -NTA/NATO anode achieved higher efficiency of organic removal and O 3 generation. Additionally, the accelerated lifetime of the Ti/blue-TiO 2 -NTA/NATO anode was increased by 7 times compared to the Ti/NATO anode. When combined with CNTs-C/PTFE air cathode in ORR-EO system, all anodic oxidation and O 3 /H 2 O 2 processes achieved higher • OH production. Over 92% of TOC in leachate bio-effluent was effectively eliminated with a relatively low energy cost of 45 kWh/t.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xuan Yu,Xu Liu,Jinyan Zhao,Mingzhe Xue,Huaijie Shi,Chenghang Jiang,Jia Liu,Yufeng Xue,Fengying Gao,Xing Zhong,Zihao Yao,Jianguo Wang
Electrochemical ozone production (EOP) is a technology with great promise for ozone synthesis, where electrochemical anode and cathode reactions play key roles in electrolytic ozone generators. In this work, mesoporous three-dimensional Pt/TiN nanorods (NRs) have been designed and prepared for EOP and HER, exhibited impressive performance with the faraday efficiency of the anodic EOP was 13 %. The overpotential of cathodic HER was 38 mV at 10 mA·cm −2 with 0.5 M H 2 SO 4 . The porous structure of Pt/TiN NRs provides microenvironments favorable for enrichment of reaction intermediates, accelerating the kinetic processes of EOP and HER. Theoretical calculations have revealed that metal-support interactions (MSI) between Pt and TiN play an influential role in the adsorption of reactive intermediates. Furthermore, promising efficiencies in the electrochemical degradation of organic pollutants have been investigated, highlighting the potential application of the Pt/TiN NRs-1 || Pt/TiN NRs-2 in advanced electrochemical oxidation.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2023
·
IF 7.1
Xinying Yang,Wenwen Li,Shibin Wang,Huaijie Shi,Xiaosa Wang,Min Li,Lei Ding,Xing Zhong,Jianguo Wang
Diamond electrodes have been receiving increased attention because of their favorable properties for wastewater treatment. However, the surface properties of the diamond anode have not been fully determined. Herein, an extensive study was conducted to explore hybrid two-dimension nanodiamonds (2D NDs) with variable sp3/sp2 ratios as metal-free electrochemical ozone production (EOP) electrocatalysts. The 2D ND-1100 electrocatalyst with interface heterojunction of sp3/sp2 exhibited outstanding EOP performance compared with the normal ND@G with sp3@sp2 core–shell structure. Theoretical calculations further revealed that a high sp3/sp2 ratio could effectively prohibit the O2*/O3* intermediate dissociation. O3* with five-ring configurations exhibited lower adsorption energies than O2* under the high sp3/sp2 ratio condition, indicating the high O3 selectivity. The optimal sp3/sp2 ratio was predicted to be 4:5 to 8:1 for O3 selective formation. In addition, the 2D ND-1100 electrocatalyst demonstrated remarkable performance in electrodegrading organic pollutants, indicating its broad potential for efficient and advanced oxidation applications. This work provides an effective strategy for the removal of organic pollutants in wastewater based on high-performance hybrid two-dimension nanodiamonds with appropriate sp3/sp2 rations.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Yu Gu,Shibin Wang,Huaijie Shi,Jun Yang,Suiqin Li,Haiyang Zheng,Wenbin Jiang,Jia Liu,Xing Zhong,Jianguo Wang
Environment-friendly electrochemical ozone production (EOP) is a promising route for in situ sterilization and discoloration applications. Herein, a Pt-SAs/BNC catalyst with Pt single atoms embedded into B/N codoped nanotubes is rationally designed and prepared. The process provides a local environment rich in oxygen intermediates and hence improves the EOP performance in neutral media by influencing the EOP thermodynamics and kinetics. The Pt-SAs/BNC catalyst exhibits excellent EOP performance with a Faraday efficiency of 21% at the current density of 50 mA cm–2, which is almost twice as much as that of commercial β-PbO2. Density functional theory calculations further reveal the synergistic effect between the B sites and the Pt single atom of the EOP mechanism. In addition, the Pt-SAs/BNC catalyst presented a significant performance in electrodegradation of various pesticides and antibiotics, indicating the potential environmental application capabilities of Pt-SAs/BNC.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Rui Lei,Yuxiang Shi,Xingling Wang,Xinglin Tao,Hua Zhai,Xiangyu Chen
Ozone treatment is an excellent sterilization technology , but high voltage is essential for ozone generation. Here, for the first time, we report a multifunctional water purification system based on self-powered ozone generation. The TENG with “like charges repel” strategy (LCR-TENG), which can obtain a maximum short-circuit current of 22.15 uA, a peak power of 80 mW, and a maximum transient voltage over 30.7 kV, is designed as the power source of the system. Then, an air-breakdown-discharge is generated by this TENG to support the ozone generation, while the maximum concentration of generated ozone can be up to 30 mg/m 3 and it is enough for the application of water treatment. With continuous injection of ozone into solutions, Rhodamine B with 5 ppm concentration can be degraded by 97.6% in 20 min. The ozone generated by the system are effective for bio-sterilization in water, indicating the promising application for the treatment of organic matter and microorganisms in water. A variety of external loads, such as ultraviolet lamp and step-down circuit can be simultaneously integrated in the current loop and the function of the system can be further expanded without disturbing the ozone generation. Hence, this work broadens the high voltage applications of TENG for the multifunctional purification system.
研究领域:
环境工程
·
纳米能源
·
水处理技术
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生物医学工程
·
环境微生物学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）