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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS · 2020 · IF 3.442

Enhanced catalytic performance with Fe@α-Fe2O3 thin nanosheets by synergistic effect of photocatalysis and Fenton-like process

Deqiang Feng,Jie He,Lingcheng Zheng,Wenjun Jiang,Ce Zhang,Long Li,Jian Song,Wei Yao

Developing novel catalysts and catalysis processes are highly attractive in environmental protection and energy utilization. Photocatalysis-Fenton combinational process is an environmentally friendly technology and has broad application prospects. In this work, thin Fe@α-Fe 2 O 3 nanosheets with thickness of 2–5 nm were designed by oxidation of Fe metal nanostructure synthesized using a modified solution reaction method. The nanosheet structure with thin thickness has short diffusion distance for the photogenerated carriers and prolongs the carriers' life. Simultaneously, the presence of Fe can reduce the resistance of system and further promote the transport and transfer of photogenerated carriers from the bulk to the surface, causing less carrier recombination and better photocatalytic performance. What's more, the Fe@α-Fe 2 O 3 composite can induce the Fenton-like reaction to generate active • OH radicals, which significantly improve the degradation rate . The synergistic effect of photocatalysis and Fenton processes makes the system show an enhanced photodegradation performance: 96.5% of RhB is degraded after 60 min visible light irradiation , especially, 84.3% of RhB is degraded within the first 10 min, which are much higher than that of the pure α-Fe 2 O 3 sample. This work demonstrates that the conjunction of photocatalysis and Fenton processes based on the Fe@α-Fe 2 O 3 nanosheets provides a potential application for pollutants degradation.

研究领域: 环境化学 · 材料科学 · 催化化学 · 纳米科技 · 物理化学
✓ 已验证 DOI 高影响因子
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RSC Advances · 2016 ·Vol. 6 ·期 92 ·89821-89826 · IF 3.289

p-Nitrophenol degradation and microbial community structure in a biocathode bioelectrochemical system

Xinyu Wang,Defeng Xing,Nanqi Ren

The biocathode bioelectrochemical system (bioc-BES) was used for p-nitrophenol (PNP) degradation with sodium bicarbonate as the carbon source. The PNP degradation efficiency in bioc-BES with applied voltage of 0.5 V reached 96.1% ± 0.5% within 72 h, which was much higher than that obtained in the biocathode BES without applied voltage (bioc-BES-NAP), open circuit biocathode BES (OC-bioc-BES) or abiotic cathode BES (abioc-BES). With the increase in the PNP concentration from 20 mg L−1 to 60 mg L−1, the PNP concentration of the effluent decreased from 21.66 ± 2.94 mg L−1 to 0.38 ± 0.1 mg L−1 in 48 h. The final reductive product of PNP was p-aminophenol (PAP) in the biocathode chamber. High-throughput 454 pyrosequencing showed that predominant populations in the biocathode biofilm of bioc-BES were affiliated with electrochemically active Delftia and Diaphorobacter, while Aminobacter was the predominant population in the biocathode biofilm of the bioc-BES-NAP and OC-bioc-BES. These results suggested that microbial electrocatalysis and electrochemically active bacteria on the cathodic electrode accelerated PNP degradation in the biocathode BES (bioc-BES). The biocathode BES will be a promising treatment technology for PNP-containing wastewater.

研究领域: 环境微生物学 · 环境工程 · 生物电化学 · 污染物降解 · 废水处理 · 微生物生态学
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Chemical Engineering and Processing-Process Intensification · 2018 · IF 2.826

Electrogeneration of H2O2 using a porous hydrophobic acetylene black cathode for electro-Fenton process

Linchao Li,Huili Hu,Xiangguo Teng,Yuanchun Yu,Yongming Zhu,Xiaoqiang Su

The aim of this work is to prepare a hydrophobic cathode equipped with quite a few cracks for gas transfer, which can prepare H 2 O 2 in the course of electro-Fenton process. Scanning electron microscopy (SEM) and optical digital microscope are used to characterize the morphology of electrode, and an electrochemical workstation (CHI660e) is used to carry out all electrochemical studies with a conventional three-electrode system. The results demonstrate that the porous electrode is conducive to gas transmission with these cracks which can avoid the formation of bubbles. Additionally, the reaction is almost not affected by the content of dissolved oxygen and the gas flow with this structure. Under the conditions of 300 mA/cm 2 (current density), the H 2 O 2 concentration is up to 14.4 mmol/L after 30 min electrolysis with current efficiency beyond 90%. Furthermore, the cathode is successfully applied to electro-Fenton process which reduced catalyst loading. The results indicate that total degradation of MO is observed at the first 10 min, and 81% of TOC can be removed when the dosage of catalyst is 0.4 mmol/L within 60 min.

研究领域: 环境化学 · 电化学工程 · 水处理技术 · 反应器设计 · 污染物降解
✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

Enhancement of oxygen diffusion process on a rotating disk electrode for the electro-Fenton degradation of tetracycline

Yan Zhang,Ming-Ming Gao,Xin-Hua Wang,Shu-Guang Wang,Rui-Ting Liu

An electro-Fenton process was developed for wastewater treatment in which hydrogen peroxide was generated in situ with a rotating graphite disk electrode as cathode. The maximum H 2 O 2 generation rate for the RDE reached 0.90   mg/L/h/cm 2 under the rotation speed of 400   rpm at pH 3, and −0.8   V vs SCE. The performance of this electro-Fenton reactor was assessed by tetracycline degradation in an aqueous solution. Experimental results showed the rotation of disk cathode resulted in the efficient production of H 2 O 2 without oxygen aeration, and excellent ability for degrading organic pollutants compared to the electro-Fenton system with fixed cathode. Tetracycline of 50   mg/L was degraded completely within 2   h with the addition of ferrous ion (1.0   mM). The chronoamperometry analysis was employed to investigate the oxygen diffusion on the rotating cathode. The results demonstrated that the diffusion coefficients of dissolved oxygen is 19.45   ×   10 −5   cm 2 /s, which is greater than that reported in the literature. Further calculation indicated that oxygen is able to diffuse through the film on the rotating cathode within the contact time in each circle. This study proves that enhancement of oxygen diffusion on RDE is benefit for H 2 O 2 generation, thus provides a promising method for organic pollutants degradation by the combination of RDE with electro-Fenton reactor and offers a new insight on the oxygen transform process in this new system.

研究领域: 环境科学 · 电化学 · 水处理技术 · 污染物降解 · 反应工程
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2015 · IF 4.321

Activated carbon fibers as an effective metal-free catalyst for peracetic acid activation: Implications for the removal of organic pollutants

Fengya Zhou,Chao Lu,Yuyuan Yao,Lijie Sun,Fei Gong,Daiwen Li,Kemei Pei,Wangyang Lu,Wenxing Chen

The development of an efficient and green catalytic system for recalcitrant pollutant removal is an attractive yet challenging research topic in the field of environmental catalysis. In the present work, the use of activated carbon fibers (ACFs) as a novel and excellent metal-free catalyst is proposed for peracetic acid (PAA) activation, constructing a pro-environmental and efficient catalytic system for the removal of organic pollutants. In this system, ACFs could effectively activate PAA to remove the dye Reactive Brilliant Red X-3B (RR X-3B) over a wide pH range (3–11), exhibiting a remarkable pH-tolerant performance. Moreover, the ACFs also displayed excellent sustained catalytic ability and regeneration capability, avoiding secondary contamination. A hybrid method that combines various radical scavengers with electron paramagnetic resonance (EPR) technology has been used to confirm that both hydroxyl radicals (HO ) and alkoxyl radicals (CH 3 C(O)O ) were generated in the ACFs/PAA catalytic system. Furthermore, a combination of EPR with density functional theory calculations has been employed to evaluate the role of ACFs in the ACFs/PAA system. The results suggested that the introduction of ACFs facilitated homolytic cleavage of the O–OH bond, resulting in the generation of HO and CH 3 C(O)O for the effective removal of organic dyes. Based on these results and analyses, a possible mechanism is proposed.

研究领域: 环境催化 · 高级氧化过程 · 材料科学 · 污染物降解
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Solar-assisted electrooxidation process for enhanced degradation of bisphenol A: Performance and mechanism

Jing Ding,Qingwei Gao,Bingxin Cui,Qingliang Zhao,Guanshu Zhao,Shan Qiu,Lingjun Bu,Shiqing Zhou

Comparisons of solar-assisted electrooxidation process (SEOP), electrooxidation (EO), and solar photolysis have been addressed to evaluate the performance of bisphenol A (BPA) removal and mineralization. The results presented the BPA removal efficiency of 100% in SEOP was higher than that of 2.8% and 88% at 90 min in direct photolysis and EO process, respectively, indicating the synergistic effect of EO and solar light in SEOP. The investigation of corresponding active species indicated that ·OH and 1 O 2 played the predominant role in SEOP. The introduction of solar light in the EO process could promote the generation of ·OH, 1 O 2 , and SO 4 ·- and enhance the degradation performance, explaining the synergistic removal mechanism. The density functional theory (DFT) results pointed out the main active sites of BPA attacked by electrophilic reagent based on the calculation of the energy barrier, Fukui index, and molecular orbitals, etc. Taking into account of the identification of intermediates, the possible degradation pathways of BPA mainly included C-C bond cleavage, ring hydroxylation, and ketonization process. The effects of anode materials, illumination intensity, current density, and electrolyte for the degradation efficiency in SEOP were explored. These results exhibited that the efficient removal of BPA in SEOP was achieved with a relatively lower electricity consumption of 1.21 kWh·(m 3 ·order) -1 , which provided new insights into the synergistic mechanism and enhanced removal of contaminants.

研究领域: 环境科学 · 化学工程 · 水处理技术 · 高级氧化技术 · 污染物降解 · 理论化学
✓ 已验证 DOI 高影响因子
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2019 · IF 7.149

Polyaniline: A New Metal-Free Catalyst for Peroxymonosulfate Activation with Highly Efficient and Durable Removal of Organic Pollutants

Bojing Sun,Wenjie Ma,Na Wang,Ping Xu,Leijiang Zhang,Bianna Wang,Honghong Zhao,Kun-Yi Andrew Lin,Yunchen Du

Metal-free heterogeneous catalysts are receiving more and more attention for wastewater remediation by activating peroxymonosulfate (PMS) due to their environmental benign. However, carbon-based materials as the most typical metal-free heterogeneous always suffer from poor durability. Inspired by the fact that a conjugated system may facilitate the electron transfer during PMS activation, we innovatively select polyaniline (PANI) as a new PMS activator and investigate its catalytic performance in detail. It is found that PANI can display better catalytic performance than traditional metal-based catalysts and popular N-doped carbocatalysts in methyl orange (MO) degradation. More importantly, PANI is not only universal for various pollutants degradation but also maintains its catalytic performance in repeated degradation experiments. The stable N sites in the conjugated chains and the oxidation-resistance benzene rings as the building units are considered to be responsible for such an excellent durability. In addition, the influences of some routine factors and actual water backgrounds are comprehensively checked and analyzed. The quenching experiments and electron paramagnetic resonance confirm that MO degradation is achieved through both radical and nonradical pathways, where SO4•– and 1O2 are primary reactive species. The reaction mechanism is also proposed with the assistance of X-ray photoelectron spectroscopy.

研究领域: 环境化学 · 材料科学 · 催化 · 水处理 · 污染物降解
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2013 · IF 3.473

Reductive degradation of chlorinated organic pollutants-contaminated water by bimetallic Pd/Al nanoparticles: Effect of acidic condition and surfactants

Bo Yang,Yunfei Zhang,Shubo Deng,Gang Yu,Yonghong Lu,Jinhua Wu,Jianzhong Xiao,Gang Chen,Xiaobing Cheng,Lili Shi

The Pd/Al nanoparticles (NPs) prepared by aqueous cementation were employed to probe hydrodechlorination (HDC) efficiencies of 4-chlorophenol (4-CP) in aqueous solution and 2-chlorobiphenyl (2-PCB) in surfactant solution. Major factors affecting HDC performance were investigated including acidic types, pH conditions, and surfactant types and their concentrations. Among HCl, H 2 SO 4 , H 3 PO 4 , formic acid, and acetic acid, only HCl was the proper pH adjustor to initiate HDC reaction of 4-CP with Pd/Al NPs at pH 3.0 due to the particular penetration function of active Cl − on the compact oxide film of Al. Aqueous pH states obviously influenced HDC efficiency and its values stable at pH 3–4 were the optimum range for HDC with HCl adjustor. 0.389   mM of 4-CP could be almost completely dechlorinated into phenol after 30-min reaction using 2   g/L of Pd/Al NPs with 1.2   wt.% of Pd loading. In addition, the effect of surfactants on HDC process of highly hydrophobic 2-PCB was explored, which were employed for its better solubilization. The addition of surfactants including SDS, CTAB, Tween 80, or Brij 30 had adverse effect on HDC activity of Pd/Al NPs due to their inhibiting effect on Al corrosion. The adverse effect was closely related with the concentrations of surfactants especially for each CMC level and molecular structures.

研究领域: 环境化学 · 纳米修复 · 水处理 · 催化 · 污染物降解
✓ 已验证 DOI 高影响因子
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Desalination and Water Treatment · 2024 · IF 1

UVC photolysis of phenanthrene in cyclodextrin solutions generated from contaminated soil washing

Luojing Xiang,Xu Zhang

Ultraviolet-C (UVC; 254 nm) photolysis was applied to achieve simultaneous removal of phenanthrene and recovery of the extraction ability of cyclodextrin (CD) in soil washing solutions. β-cyclodextrin (β-CD) and hydroxypropyl-β-cyclodextrin (HPCD) were found to have comparable abilities to solubilize phenanthrene in aqueous solutions and extract phenanthrene from spiked agricultural soil or kaolinite. Only loosely bound phenanthrene is extractable to CDs, and approximately 30% of initially spiked phenanthrene is non-extractable. β-CD and HPCD showed comparable retardation effects on the UVC photolysis of phenanthrene, and HPCD was more persistent than β-CD during UVC photolysis of soil extraction solutions. After three extraction–UVC photolysis cycles, the extraction efficiency of the regenerated β-CD and HPCD solutions were 77% and 93% of the corresponding fresh CD solutions. In contrast, the apparent photolysis kinetic constant of phenanthrene in regenerated HPCD extraction solutions decreased significantly more than that in regenerated β-CD extraction solutions. 9,10-Phenanthrenequinone and its hydroxylation derivate, and three other oxygenated products were the detected intermediates that were generated during the UVC photolysis of phenanthrene, and CD or leached soil organic matter did not alter the degradation pathway. A combination of enhanced extraction and UVC photolysis is a promising method for treatment of extraction solutions from soil contaminated by phenanthrene or other polycyclic aromatic hydrocarbons.

研究领域: 环境科学 · 土壤修复 · 光化学 · 污染物降解 · 废水处理
✓ 已验证 DOI 高影响因子
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