JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2024
·Vol. 171
·期 8
·085501
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IF 3.1
Yinghong Zhu,Minling Zhou,Zhanbang Ge,Yufeng Jiao,Menghui Wang,Wujin Peng
An efficient and transition-metal-free synthesis strategy of aromatic nitriles from corresponding aldehydes with H2SO4(NH2OH)2 as the nitrogen source and Cl−/ClO− as the redox mediator was developed. The redox Cl−/ClO− showed electrochemical reversibility in acidic condition. The possible mechanism involving the transformation of Cl−, the generation and electrochemical reduction of nitrile oxides based on the results of cyclic voltammetry and constant current electrolysis was proposed.
研究领域:
有机化学
·
电化学
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DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Lixian Zhong,Peidi Luo,Yaoyao Wu,Kai Yang,Can Zhang,Ruihao Peng,Chuanhao Li,Xianping Luo
Thallium (Tl), an unconventional and highly toxic metal, is increasingly recognized as a significant contaminant in wastewater. One promising strategy to enhance Tl removal is the electrocatalytic oxidation of Tl(I), yet the contribution of chloride ions—prevalent in wastewater from metallurgical and smelting industries—has often been overlooked in such processes. Herein, this study introduces a novel chlorine-mediated electrochemical oxidation system, coupled with a coagulation process, designed to efficiently treat thallium-contaminated saline wastewater. The dimensionally stable anode (Ti/TiO 2 -RuO 2 -IrO 2 , DSA) demonstrates exceptional electrocatalytic chlorine evolution and efficient oxidation of Tl(I), with a kinetic rate constant of 0.131 min −1 , which is 21.8 times faster than that of a carbon cloth anode (0.006 min −1 ) in the presence of Cl − ions. Under optimized conditions of 5 mM Cl − ions at pH 3.0, over 98.3 % of Tl(I) was removed within 30 min. After coagulation treatment, the total Tl removal efficiency reached 98.5 %, in stark contrast to the mere 18.0 % achieved without the pre-electro-oxidation step. Mechanistic analysis revealed that the reactive chlorine species (Cl•) plays a more significant role in the oxidation of thallium (Tl) compared to the hydroxyl radicals. Notably, the system exhibits excellent recyclability (up to 35 cycles) and stable performance in the presence of various competing ions and actual wastewater, even under unsteady-state continuous-flow conditions. These findings offer valuable insights into chlorine-mediated electrocatalytic oxidation coupling with coagulation processes for thallium removal, providing guidance for practical applications in purifying thallium-contaminated industrial wastewater.
研究领域:
环境科学
·
化学工程
·
水处理技术
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 26
·69473-69485
·
IF 5.8
Liu Shanshan,Xu Longqian,Lin Xiaoqing,Zhang Jiaming,Wu Deli
Removing ammonia from black water is one of the most urgent issues before it can be recycled as flushing water. In this study, an electrochemical oxidation (EO) process with commercial Ti/IrO 2 -RuO 2 anodes to treat black water could remove 100% of different concentrations of ammonia by adjusting the dosage of chloride. Through the relationship between ammonia, chloride, and corresponding the pseudo-first-order degradation rate constant ( K obs ), we could determine the chloride dosage and predict the kinetics of ammonia oxidation based on initial ammonia concentration in black water. The optimal N/Cl molar ratio was 1:1.8. The difference between black water and the model solution in terms of ammonia removal efficiency and oxidation products was explored. A higher chloride dosage was beneficial for removing ammonia and shortening the treatment cycle, but it also led to the generation of toxic by-products. Especially HClO and ClO 3 − generated in black water were 1.2 and 1.5 times more than the synthesized model solution under 40 mA cm −2 . Through SEM characterization of electrodes and repeated experiments, the electrodes always maintained a high treatment efficiency. These results demonstrated the potential of the electrochemical process as a treatment method for black water.
研究领域:
环境科学
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污水处理
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Jiaqi Sun,Lifen Liu,Fenglin Yang
Electrochemical technology has unique superiorities in chlorine-mediated pollutant oxidation, but has limited application in saline wastewater treatment due to inadequate efficiency and high energy consumption. To promote electrochemical oxidation capacity, a novel but low-cost electrode containing TiO 2 /Co-WO 3 /SiC was prepared and optimized, achieving highly efficient chlorine-mediated ammonium nitrogen oxidation (98.3 ± 2.2% in 120 min, with initial NH 4 + -N of 10.2 ± 0.5 mg L −1 ) in a simple electrochemical system with supplied current density only at 1.00 mA cm −2 . Comparing with unmodified carbon fiber cloth, the catalytic anode achieved 96.0% nitrogen selectivity , enhanced the system current efficiency by 20.6% and reduced the energy consumption by 54.4%, making the treatment of simulated mariculture wastewater both energy-saving (36.5 ± 2.8 kWh kg −1 NH 4 + -N) and cost-effective (1.45 US$ m −3 ), comparing with previously reported electrochemical processes (54–622 kWh kg −1 NH 4 + -N). The nitrogen content (<1 mg L −1 ) in the treated wastewater, containing only 0.18 mg L −1 NH 4 + -N, meets the discharge standard of mariculture wastewater. The promoted electrochemical oxidation should be attributed to the chloride derived species (HOCl and ClO − ) and related active species (Cl , ClO , OH, etc.). This easily prepared and reusable catalytic electrode is a promising alternative to conventional anode materials in sustainable electrochemical treatment of saline wastewater.
研究领域:
环境科学
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电化学工程
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yucheng Liu,Jing Hou,Haoran Sun,Hailiang Tang,Yufan Chen,Lizhang Wang
Chlorine-Mediate Electrochemical Advanced Oxidation (Cl-EAO) technology emerges as a highly promising method for ammonia removal. However, the electron transfer mechanism behind the Cl-EAO process in three-dimension (3D) electrode systems remains unclear. This study revealed a two-stage linear degradation trend for ammonia under low chlorine-nitrogen mass ratio (Cl/N) conditions. This segmented degradation was attributed to changes in the electron transfer process. Ammonia and intermediates serve as electron donors on the granular activated carbon (GAC) surface before and after the “inflection point”, respectively. It has been observed that Cl/N demonstrates a volcanic relationship with the number of electron transfers, leading to the development of a universal volcanic model. Using this model, the optimal electron transfer moment (Cl/N = 10) and electron transfer occupancies for ammonia oxidation reaction (0.94), oxygen evolution reaction (0.02) and chlorine evolution reaction (0.04) in the 3D electrode system were obtained. Additionally, quenching experiments showed that the chlorine radicals (70 %) and active chlorine (56 %) were the main contributors to 2D and 3D electrode systems, respectively. Based on the important results found in this work, we elucidated the electron transfer mechanism behind the ammonia oxidation on anode and GAC: chlorine radical-mediated three-electron transfer and single-electron transfer breakpoint chlorination mechanism, respectively.
研究领域:
环境科学
·
电化学工程
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产品关联
DOI
高影响因子
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