SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jianhui Xu,Xin Fu,Yufeng Liu,Yunfei Zhang,Shenggui Chen,Dan Li,Chunhui Zhang,Jiale Gao,Yibo Fu
Electrocatalytic hydrodechlorination technology provides an attractive strategy to effectively eliminate the biotoxicity of halogenated organic pollutants (HOPs). Herein, we demonstrated a highly dispersed Pd loaded on blue TiO 2 nanotube arrays (Pd x -BTNA) cathode that can achieve efficient dechlorination and detoxification toward florfenicol (FLO). Characterization results indicated that strong interaction between Pd and BTNA was achieved through Pd-O bonds, which facilitated the electron transfer rate. Pd x -BTNA significantly outperformed other cathodes (i.e., BTNA, Pd x -TNA and Pd x -Ti) in the electrocatalytic dechlorination of FLO due to enhanced utilization of active H*. The dechlorination performances of FLO well followed the pseudo-first-order kinetic, and the reaction constant rate on Pd x -BTNA cathode (0.035 min −1 ) was 17.5, 1.94, 7.0 times higher than that on BTNA, Pd x -TNA and Pd x -Ti cathodes, respectively. Quenching experiments and electrochemical characterization indicated that both direct electron transfer and indirect reduction process mediated by H* were involved in the dechlorination of FLO. The optimal dechlorination efficiency of 98.79% was obtained by Pd x -BTNA cathode within 120 min at 1 mM PdCl 2 , applied cathode potential of −1.2 V. In addition, Pd x -BTNA exhibited superior stability and durability with almost no Pd leaching (0.0011 mg/L) during five dechlorination cycles. Our research proposed a novel strategy to design low noble Pd-loaded cathode material for efficient dechlorination and detoxification of HOPs.
研究领域:
环境科学
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材料科学
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电化学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2023
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IF 7.1
Yuqing Su,Zhen Yu,Ruonan Gu,Wei Wu,Shaoling Dai,Shaoan Cheng
Blue TiO2 exhibited excellent electrocatalytic activity for degrading various organic pollutants in wastewater. However, its crystal structure and morphology considerably affected the electrocatalytic activity of blue TiO2. In this study, a blue hierarchical TiO2 nanotube array (B-HTNA) was synthesized utilizing Ti foam by ice–water bath anodic oxidation and cathodic reduction. Benefiting from a higher concentration of doped Ti3+, the prepared B-HTNA exhibited greater electron transport capability. B-HTNA effectively degraded tetracycline with a high removal rate of more than 90% within 60 min under 20 mA cm–2. The results of free radical quenching experiments revealed the effects induced under different experimental conditions, wherein the electrochemical oxidation of pollutants with B-HTNA mainly relied on the oxidation of hydroxyl radicals. In addition, B-HTNA exhibited a longer service life of up to 85.4 h, surpassing other anodes with a bare and fragile nanotube array. B-HTNA displayed enhanced stability owing to the hierarchical structure with uniform nanoparticles adhering to a porous layer, which could prevent chemical erosion of the anode and charge leakage from the top of the nanotube during cathodic polarization, thereby enhancing self-doping and stability.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
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2023
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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
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产品关联
DOI
高影响因子
RSC Advances
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2023
·Vol. 13
·期 40
·28299-28306
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IF 3.9
Jun Guo,Wei Gan,Ruixin Chen,Miao Zhang,Zhaoqi Sun
TiO2 nanorod arrays have been widely used in photocatalytic processes, but their poor visible light absorption and rapid carrier recombination limit their application. Both introducing oxygen vacancies and using precious metals as surface plasmon resonance (SPR) stimulators are effective strategies to enhance their photocatalytic performance. Herein, Au nanoparticle sensitized blue TiO2 nanorod arrays (Au/B-TiO2) were successfully fabricated for efficient Gatifloxacin photodegradation. The degradation efficiency of Gatifloxacin was up to 95.0%. Moreover, the corresponding reaction rate constant (Ka) was up to 0.02007 min−1. Additionally, it was suggested that Gatifloxacin could be subject to three different degradation pathways. The superior catalytic activity of Au/B-TiO2 is a result of the combined effect of the two components. Firstly, TiO2 nanorod arrays provide a larger surface area for Au deposition and act as efficient transfer channels. Secondly, the presence of oxygen vacancies in blue TiO2 nanorod arrays enhances the catalytic activity. Thirdly, Au acts as a SPR activator, providing a large number of high-energy electrons in the photocatalysis process. Lastly, the improved light capture capabilities are essential for efficient removal of Gatifloxacin. This work provides a new approach for the construction of a high-performance heterojunction photocatalyst in advanced oxidation processes.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Jianhui Xu,Yufeng Liu,Dan Li,Chunhui Zhang,Xin Fu,Yunfei Zhang,Pengxu Wang,Jincheng Lu,Shenggui Chen,Lei Li
Electrocatalytic technology (EC) is a promising strategy for peroxymonosulfate (PMS) activation due to its environmental safety and energy conservation. Herein, 3D printed blue TiO 2 nanotube arrays (3DP-BTNAs) reactive electrochemical membranes (REM) were designed as anode and cathode in EC and EC/PMS systems. EC/PMS system displayed superior performance for acetaminophen (ACT) degradation and detoxication. The ACT degradation in EC/PMS system was 3.70 times faster than that in EC system. Quenching experiments suggested that singlet oxygen ( 1 O 2 ) mediated nonradical pathway was responsible for ACT degradation in EC/PMS system, while hydroxyl radical (•OH) was the predominant reactive oxygen species (ROS) in EC system. Our study first provided direct evidence that PMS activation on cathode was mainly triggered by superoxide radical (O 2 •- ). PMS was reduced by O 2 •- derived from O 2 reduction on cathode, and subsequently converted into ROS for organics oxidation . However, PMS tended to adsorb on anode and formed 3DP-BTNAs-PMS* complex for organics degradation. The influencing factors (e.g., PMS dosage, flow rate) on ACT degradation in EC/PMS system were evaluated, and the obtained optimal kinetic constant and lowest energy consumption were 0.135 min −1 and 0.27 Wh/L, respectively. In addition, eight degradation products were identified and possible degradation pathways of ACT were proposed to be the cleavage of C-N bonds and benzene ring. This study is dedicated to the rational design of highly porous REM material by 3DP technology for wastewater treatment and the in-depth mechanism of PMS activation over BTNAs electrode in EC/PMS system.
研究领域:
环境科学
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化学工程
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材料科学
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水处理
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产品关联
DOI
高影响因子
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