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International Journal of Electrochemical Science · 2023 ·Vol. 6 ·期 9 ·4341-4354 · IF 1.5

Preparation of a Praseodymium Modified Ti/SnO2-Sb/PbO2 Electrode and its Application in the Anodic Degradation of the Azo Dye Acid Black 194

Zhiqiao He,Chengxiang Huang,Qiong Wang,Zhe Jiang,Jianmeng Chen,Shuang Song

A series of praseodymium modified Ti/SnO 2 -Sb/PbO 2 (Ti/SnO 2 -Sb/PbO 2 -Pr) electrodes were synthesized by doping PbO 2 with praseodymium and the effect of Pr doping on the electrode catalytic activity toward the anodic oxidation of the model dye C.I. Acid Black 194 (AB-194) was examined in aqueous solution. The electrocatalytic activity of a Ti/SnO 2 -Sb/PbO 2 electrode can be greatly improved by adding an appropriate amount of Pr into the PbO 2 layer. Accelerated life tests indicate that Pr doping also dramatically improves the stability of the Ti/SnO 2 -Sb/PbO 2 anode. The introduction of Pr enhanced the formation of oxygen vacancies and surface hydroxyl groups, resulting in better activity and stability of the Ti/SnO 2 -Sb/PbO 2 -Pr electrode. A possible degradation pathway of AB-194 during the anodic oxidation process is proposed based on hydroxyl radical attack of the organic reactant.

研究领域: 电化学 · 环境工程 · 材料科学 · 水处理
✓ 已验证 DOI 高影响因子
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2020 · IF 7.864

Discovering the Importance of ClO• in a Coupled Electrochemical System for the Simultaneous Removal of Carbon and Nitrogen from Secondary Coking Wastewater Effluent

Wenxiao Zheng,Liuyi Zhu,Sheng Liang,Jinshao Ye,Xin Yang,Zhenchao Lei,Zhang Yan,Yongdong Li,Chaohai Wei,Chunhua Feng

Inorganic constituents in real wastewater, such as halides and carbonates/bicarbonates, may have negative effects on the performance of electrochemical systems because of their capability of quenching HO•. However, we discovered that the presence of Cl– and HCO3– in an electrochemical system is conducive to the formation of ClO•, which plays an important role in promoting the simultaneous elimination of biorefractory organics and nitrogen in secondary coking wastewater effluent. The 6-h operation of the coupled electrochemical system (an undivided electrolytic cell with a PbO2/Ti anode and a Cu/Zn cathode) at a current density of 37.5 mA cm–2 allowed the removal of 87.8% of chemical oxygen demand (COD) and 86.5% of total nitrogen. The electron paramagnetic resonance results suggested the formation of ClO• in the system, and the probe experiments confirmed the predominance of ClO•, whose steady-state concentrations (8.08 × 10–13 M) were 16.4, 26.5, and 1609.5 times those of Cl2•– (4.92 × 10–14 M), HO• (3.05 × 10–14 M), and Cl• (5.02 × 10–16 M), respectively. The rate constant of COD removal and the Faradaic efficiency of anodic oxidation obtained with Cl– and HCO3– was linearly proportional to the natural logarithm of the ClO• concentration, and the specific energy consumption was inversely correlated to it, demonstrating the crucial role of ClO• in pollutant removal.

研究领域: 环境工程 · 水处理 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

CNT/Nafion functionalized Ti/SnO2-Sb/β-PbO2-CNT/Nafion composite electrode toward highly active and robust degradation of octadecylamine and 4-dodecylmorpholine in real high-salinity system

Miao Lu,Siyuan Zhang,Liang Ma,Zhongmei Song,Xiushen Ye,Huifang Zhang,Haining Liu,Zhijian Wu

The efficient removal of recalcitrant organics in high-salinity systems, specifically brine, poses a significant challenge for electrochemically advanced oxidation processes in terms of both activity and stability. Herein, a composite electrode comprising of CNT/Nafion functionalized Ti/SnO 2 -Sb/β-PbO 2 -CNT/Nafion was developed for efficient and stable removal of octadecylamine (ODA) and 4-dodecylmorpholine (DMP) in a real high-salinity environment. The degradation efficiencies of ODA and DMP on the composite electrode can reach 100 % within 60 min, respectively. The total organic carbon (TOC) removal efficiency of ODA and DMP was significantly improved to 78 % and 66 % with remarkably low energy consumption (0.414 and 1.402 kWh/g TOC), respectively. The electrochemical characterizations demonstrate that the composite electrode exhibits improved electrochemical activity (oxygen evolution potentials = 1.791 V) and electrode surface area (ECSA = 20 cm 2 ), while maintaining reduced charge transfer resistance ( R ct  = 18.21 Ω/cm 2 ) and enhanced corrosion-resistant capacity (corrosion potential = 1.115 V). Based on recycling and accelerated lifespan testing, the composite electrode demonstrates exceptional stability and recyclability. Additionally revealed was the linked stability mechanism. The electrocatalytic degradation of ODA and DMP begins with the removal of amino and morpholine rings, and then the decomposition of the carbon chains. Gas chromatography-mass spectrometry (GC–MS) and theoretical calculations were used to identify intermediate products generated during the degradation of ODA and DMP, and possible degradation pathways were provided in high-salinity systems, respectively. This work offered a fresh perspective on electrocatalytic oxidation for a real high-salinity system that is more efficient and stable.

CAS / MDL: 124-30-1
研究领域: 环境科学 · 电化学工程
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CHEMOSPHERE · 2023 · IF 8.8

Insights into electrochemical oxidation of tris(2-butoxyethyl) phosphate (TBOEP) in aquatic media: Degradation performance, mechanisms and toxicity changes of intermediate products

Zhujun Luo,Wantang Huang,Wenyan Yu,Shaoyu Tang,Kun Wei,Yuanyuan Yu,Lei Xu,Hua Yin,Junfeng Niu

Tris (2-butoxyethyl) phosphate (TBOEP) has gained significant attention due to its widespread presence and potential toxicity in the environment. In this study, the degradation of TBOEP in aquatic media was investigated using electrochemical oxidation technology . The anode Ti/SnO 2 –Sb/La–PbO 2 demonstrated effective degradation performance, with a reaction constant ( k ) of 0.6927 min −1 and energy consumption of 1.24 kW h/m 3 at 10 mA/cm 2 . CV tests, EPR tests, and quenching experiments confirmed that indirect degradation is the main degradation mechanism and ·OH radicals were the predominant reactive species, accounting for up to 93.8%. The presence of various factors, including Cl − , NO 3 − , HCO 3 − and humic acid (HA), inhibited the degradation of TBOEP, with the inhibitory effect dependent on the concentrations. A total of 13 intermediates were identified using UPLC-Orbitrap-MS/MS, and subsequent reactions led to their further degradation. Two main degradation pathways involving bond breaking, hydroxylation, and oxidation were proposed. Both Flow cytometry and the ECOSAR predictive model indicated that the intermediates exhibited lower toxic than the parent compound, resulting in a high detoxification rate of 95.9% for TBOEP. Although the impact of TBOEP on the phylum-level microbial community composition was found to be insignificant, substantial alterations in bacterial abundance were noted when examining the genus level. The dominant genus Methylotenera , representing 17.4% in the control group, decreased to 6.9% in the presence of TBOEP and slightly increased to 8.7% in the 4-min exposure group of degradation products . Electrochemical oxidation demonstrated its effectiveness for the degradation and detoxification of TBOEP in aqueous solutions, while it is essential to consider the potential impact of degradation products on sediment microbial communities.

研究领域: 环境科学 · 化学工程 · 分析化学 · 毒理学 · 微生物学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Strategies for controlling gas evolution reactions to boost the divergent paired electrochemical upgrading of furfural in acidic environment

Xinxin Li,Linchuan Cong,Yupeng Wu,Nan Lin,Fangbing Liu,Deyuan Xin,Fuyu Han,Jin Yang,Weitong Chen,Haibo Lin

Electrochemical methods for catalytic furfural conversion have drawn significant interest in both academic and industrial research communities. Paired electrocatalytic conversion has been identified as a promising strategy for reducing energy consumption and promoting carbon neutrality. To optimize product distribution and conversion efficiency, we have developed a divergent paired electrochemical upgrading approach for furfural in acidic environments, with a focus on prioritizing strong gas evolution reactions and product transformations. The high electrocatalytic activity of CuSn/CuF@Cu prepared by electrodeposition can effectively inhibit the hydrogen evolution. The performance of the electrocatalysts and the pathways of electrocatalytic hydrogenation (ECH) of furfural to 2-methylfuran (MF) were investigated by combination of experiments and the density functional theory (DFT) calculations. A stable Ti/PbO 2 electrode with high oxygen evolution overpotential was prepared for anodic electrocatalytic oxidation (ECO) and the product transformation route was described. The conversion of furfural to maleic acid (MA) and MF in acidic environment was successfully achieved. In the paired electrosynthesis system, the electrons generated from anodic ECO of furfural are utilized in valuable and controllable cathodic ECH. It significantly and continuously reduces the power cost associated with renewable energy sources and further promotes the development of biomass electrochemical conversion.

研究领域: 电化学 · 催化 · 可再生能源 · 生物质转化 · 材料科学
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