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JOURNAL OF MATERIALS SCIENCE · 2022 ·Vol. 57 ·期 6 ·4265-4282 · IF 4.682

Construction of S-scheme heterojunction by doping Bi2WO6 into Bi2O3 for efficiently enhanced visible-light photocatalytic performance

Hu Wenna,Wu Fan,Liu Wei

The objective of this study was to construct the S-scheme Bi 2 WO 6 / α- Bi 2 O 3 heterojunctions with high enhanced visible-light photocatalytic performance. The composites loaded various Bi 2 WO 6 mass ratios were prepared by a ball grinding method. The characterization and reaction mechanism of photocatalysts were explored in detail. Remarkably, the results demonstrated that the Bi 2 WO 6 / α- Bi 2 O 3 presented an outstandingly superior performance for photodegradation of nitrobenzene. Among them, the 10%Bi 2 WO 6 / α- Bi 2 O 3 possessed the best photocatalytic property, and it could reach up to 95.7% in 50 min with the top rate constant of 0.06178 min −1 , which was 4.3 and 3.6 times that of bare Bi 2 O 3 and Bi 2 WO 6 , respectively. Simultaneously, the Bi 2 WO 6 / α- Bi 2 O 3 was well stable after five cycling experiments. The efficiently improved photocatalytic performance was primarily attributed to the formation of S-scheme structure between Bi 2 WO 6 and α- Bi 2 O 3 , which enhanced the conspicuous separating efficiency of photogenerated carriers. The present study not only offers a method to solve the unsatisfactory activity of Bi 2 O 3 , but also provides some insights into the design of other novel S-scheme composites with great potential application in clean energy and environmental remediation. Graphical abstract The efficiently improved photocatalytic performance was primarily attributed to the formation of S-scheme structure between Bi 2 WO 6 and α- Bi 2 O 3 , which enhanced the conspicuous separating efficiency of photogenerated carriers.

研究领域: 材料科学 · 环境科学 · 能源科学
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Frontiers in Chemistry · 2025 · IF 4.2

Heterogeneous Fenton-like CuO-CoOx/SBA-15 catalyst for organic pollutant degradation: synthesis, performance, and mechanism

Jinwei Li,Yifei Wei,Qiang Liu,Huanhuan Guan,Chengchun Jiang,Xiaohui Sun

In this study, CuO-CoOx/SBA-15 catalysts were successfully synthesized via ultrasonic impregnation, and their performance in degrading nitrobenzene within a Fenton-like system was investigated. The catalyst materials were characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma mass spectrometry (ICP-MS), scanning electron microscopy (SEM), transmission electron microscope(TEM) and energy-dispersive X-ray spectroscopy (EDS). The CuO-CoOx/SBA-15 catalysts featured well-distributed CuO-CoOx nanoparticles within the mesoporous SBA-15 support. Compared to CuO/SBA-15 and Co3O4/SBA-15 catalysts with similar microstructures, the CuO-CoOx/SBA-15 catalysts exhibited Cu-Co dual active centers and a higher abundance of redox-active sites. During catalytic degradation, H2O2 was continuously activated on the catalyst surface through efficient Cu+/Cu2+ and Co2+/Co3+ redox cycles. The experimental conditions (initial pH, catalyst dosage, and H2O2 dosage) were optimized, resulting in 99% nitrobenzene removal over a wide pH range (3.0–9.0). The primary mechanisms for the oxidation and subsequent removal of nitrobenzene in the CuO-CoOx/SBA-15-H2O2 system were identified as reactions with hydroxyl radicals (·OH).

研究领域: 环境科学 · 催化化学
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Desalination and Water Treatment · 2015 · IF 1.173

Efficient degradation of nitrobenzene by an integrated heterogeneous catalytic ozonation and membrane separation system with active MgO(111) catalyst

Jun Chen,Shuanghong Tian,Lingjun Kong,Yuting Tu,Jiang Lu,Ya Xiong

An integrated heterogeneous catalytic ozonation and membrane separation system was studied for continuous degradation of refractory organic pollutants in water. MgO nanosheets with dominant (111) facets showed large amounts of medium and strong basic sites due to the particular structure of alternating monolayers of exclusively oxygen and exclusively magnesium atoms. MgO(111) acted as the ozonation catalyst for the first time, it was found that efficient degradation of nitrobenzene was achieved with 25.0 mmol/L of MgO(111) catalysts in a wide pH range of 4.0–12.0. In view of practical application, engineering problems to recover fine size catalysts from the treated water were resolved by applying membrane separation technology in the system. Experimental results showed that the membrane could successfully intercept MgO(111) particles in the reactor by the synergistic cooperative sieving of the bare and dynamic membranes. The long-term continuous experiments demonstrated that the removal rate of nitrobenzene could maintain over 90% with a constant flux of 3.92 L m−2 min−1 during the 24 h operation. The continuous system provides a new method for practical application of heterogeneous catalytic ozonation to remove refractory organic pollutants.

研究领域: 环境科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Oxygen vacancies and Lewis sites activating O3/H2O2 at wide pH range via surface electron transfer over CeOx@SiO2 for nitrobenzene mineralization

Weirui Chen,Jinxin Xie,Xukai Li,Laisheng Li

The low efficiency of peroxone (O 3 /H 2 O 2 ) at acidic and neutral pH restrained its application in water purification . To overcome this shortcoming, CeO X @SiO 2 with large surface area, abundant surface oxygen vacancies (V o ), Lewis sites (L sites) and high Ce(III)/Ce(IV) ratio were synthesized to change the traditional electron transfer pathway between O 3 and H 2 O 2 . V o was facile in absorbing H 2 O 2 to form V o -H 2 O 2 and L sites were capable of absorbing O 3 to form L-O 3 . The electron at V o could be donated to V o -H 2 O 2 and generate V o -HO 2 − , which then effectively triggered the decomposition of L-O 3 at CeO X @SiO 2 ’s interface and O 3 in bulk solution. The electron transfer at the solid-liquid interface with the help of Ce 3+ /Ce 4+ redox cycle and V o was pH independent and different from the traditional electron transfer of peroxone reaction. Nitrobenzene (NB) mineralization was promoted to 92.5% in CeO X @SiO 2 -peroxone, but only 63.8% TOC was removed in tradition peroxone process. Moreover, CeO X @SiO 2 -peroxone had a wide pH application range. NB’s degradation in CeO X @SiO 2 -peroxone process followed the co-oxidation mechanism of superoxide free (•O 2 − ) and hydroxyl radical (•OH). The finding of this study could broaden the popularization of peroxone in water treatment and provided a strategy for catalyst design.

研究领域: 环境科学 · 催化化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2023 · IF 5.8

One-step synthesis of Pt-Nd co-doped Ti/SnO2-Sb nanosphere electrodes used to degrade nitrobenzene

Li Yang,Ma Hairun,Li Qianwei,Yan Guangxu,Guo Shaohui

Ti/SnO 2 -Sb electrodes possess high catalytic activity and efficiently degrade nitrobenzene (NB); however, their low service life limits their wide application. In this study, we used one-step hydrothermal synthesis to successfully prepare Pt-Nd co-doped Ti/SnO 2 -Sb nanosphere electrodes. Scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were applied to characterize the surface morphology, microstructure, and chemical composition of the electrodes, respectively. The electrochemical activity and stability of the electrodes were characterized via linear sweep and cyclic voltammetry, electrochemical impedance spectroscopy, and an accelerated service life test; their performance for NB degradation was also studied. An appropriate amount of Pt-Nd co-doping refined the average grain size of SnO 2 and formed a uniform and compact coating on the electrode surface. The oxygen evolution potential, total voltammetric charge, and electron transfer resistance of the Ti/SnO 2 -Sb-Nd-Pt electrodes were 1.88 V, 3.77 mC/cm 2 , and 11.50 Ω, respectively. Hydroxy radical was the main active radical species during the electrolytic degradation of nitrobenzene with Ti/SnO 2 -Sb-Nd-Pt. After Pt-Nd co-doping, the accelerated service life of the electrodes was extended from 8.0 min to 78.2 h (500 mA/cm 2 ); although the NB degradation rate decreased from 94.1 to 80.6%, the total amount of theoretical catalytic degradation of NB in the effective working time increased from 17.4 to 8754.1 mg/cm 2 . These findings reveal good application potential for the electrodes and provide a reference for developing efficient and stable electrode materials.

研究领域: 环境科学 · 材料科学
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Frontiers in Environmental Science · 2022 · IF 5.411

Accelerated catalytic ozonation for aqueous nitrobenzene degradation over Ce-loaded silicas: Active sites and pathways

Wang Qinghong,Ji Yuanyuan,Hu Jingze,Ye Huangfan,Liu Ya,Wang Yuxian,Chen Chunmao,Li Zhuoyu

Cerium oxides loaded silica catalysts were synthesized by an impregnation method by simply mixing Ce precursor with silica spherule (Ce/SS) and ordered MCM-41 zeolites (Ce/MCM-41), followed by a mild calcination. Compared with pure SS and MCM-41, Ce modified Ce/SS and Ce/MCM-41 demonstrate much improved catalytic ozonation activities for mineralization of recalcitrant nitrobenzene (NB). At solution pH of 6, 86 and 97% TOC mineralization rates were achieved within 60 min for Ce/MCM-41 and Ce/SS, respectively. Characterization results suggest that Ce loading significantly increases the surface Lewis acidic sites, which would synergize with Ce3+/Ce4+ redox cycle for the activity improvement. With the aid of in situ electron paramagnetic resonance (EPR) spectra and quenching tests, hydroxyl radical (·OH), superoxide radical (O2•–), and singlet oxygen (1O2) are identified as the O3 catalytic decomposition products, while ·OH mainly accounts for NB mineralization. The detailed degradation route of NB was further investigated by the multi-chromatography analysis. NB is firstly oxidized into polyhydroxy compounds, followed by small molecular organic acids, and finally being mineralized into CO2 and H2O. This study established a facile strategy to synthesize highly active and stable Ce/SiO2 catalysts for catalytic ozonation, and elucidated the in-depth mechanisms for the activity origins of the Ce loaded silica-based materials in catalytic ozonation processes (COP).

CAS / MDL: 106-51-4 98-00-0 75-65-0
研究领域: 环境科学 · 催化化学
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CHEMOSPHERE · 2016 · IF 3.698

Biocatalysis mechanism for p-fluoronitrobenzene degradation in the thermophilic bioelectrocatalysis system: Sequential combination of reduction and oxidation

Yanfeng Wang,Xueqin Zhang,Huajun Feng,Yuxiang Liang,Dongsheng Shen,Yuyang Long,Yuyang Zhou,Qizhou Dai

To verify the potentially synthetic anodic and cathodic biocatalysis mechanism in bioelectrocatalysis systems (BECSs), a single-chamber thermophilic bioelectrocatalysis system (R3) was operated under strictly anaerobic conditions using the biocathode donated dual-chamber (R1) and bioanode donated dual-chamber (R2) BECSs as controls. Direct bioelectrocatalytic oxidation was found to be infeasible while bioelectrocatalytic reduction was the dominant process for p -Fluoronitrobenzene ( p -FNB) removal, with p -FNB removal of 0.188 mM d −1 in R1 and 0.182 mM d −1 in R3. Cyclic voltammetry experiments confirmed that defluorination in the BECSs was an oxidative metabolic process catalyzed by bioanodes following the reductive reaction, which explained the 0.034 mM d −1 defluorination in R3, but negligible defluorination in controls. Taken together, these results revealed a sequentially combined reduction and oxidation mechanism in the thermophilic BECS for p -FNB removal. Moreover, the enrichment of Betaproteobacteria and uniquely selected Bacilli in R3 were probably functional populations for p -FNB degradation.

研究领域: 环境科学 · 微生物学
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CHEMOSPHERE · 2021 · IF 7.086

Activation of sodium persulfate by TiO2@MIL-101(Fe): Boosting the Fenton-like process by interfacial charge transfer

Jiajie Xu,Shengye Wang,Changyu Yan,Hafiz Mohammad Adeel Sharif,Bo Yang

Advanced oxidation processes based on sulfate radicals are considered as a promising approach for environmental remediation. In this study, TiO 2 @MIL-101(Fe) is successfully fabricated by a facile impregnation method and is used for sodium persulfate (SPS) activation. TiO 2 @MIL-101@SPS combines the advantages of photocatalysis and SPS activation, which shows high removal efficiency for nitrobenzene and methyl orange. In addition, the effect of multiple factors, including light source, SPS amount and catalyst amount, on nitrobenzene degradation have been investigated. Results show that the nitrobenzene degradation efficiency is up to 66.53 % while that of TOC removal is 32.21 % under 4-h visible light irradiation with 30 mg catalyst and 1.6 mM SPS. Moreover, LC-MS have been carried out to study the route of nitrobenzene degradation. Besides, ESR analysis reveals that both ● SO 4 − and ● OH radicals are generated sustainably under visible light irradiation, and more ● OH radicals can be detected owing to the synergic effect of photocatalysis and SPS activation. Interfacial charge transfer effect provides photoinduced electrons for the Fe 3+ /Fe 2+ cycle in MIL-101(Fe), which boosts the SPS activation process, resulting in high photocatalytic activity.

研究领域: 环境科学 · 化学工程
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WATER SCIENCE AND TECHNOLOGY · 2019 ·Vol. 80 ·期 5 ·902-910 · IF 1.624

Mesoporous TiO2/carbon catalytic ozonation for degradation of p-chloronitrobenzene

Qun W.,Jingnan Z.,Hong L.,Mengling L.,Xiaohui L.,Zhichao Y.,Tao H.,Pengyu W.

In this study, a mesoporous TiO 2 /carbon catalyst (TiO 2 /C) was prepared by a facile impregnation-carbonization approach to catalyze ozonation of p -chloronitrobenzene ( p -CNB). The catalyst was well characterized and the catalytic efficiency under various conditions was systematically evaluated. TiO 2 /C has a disordered mesostructure with a high specific surface area. 92.8% of p -CNB (2 μmol/L) can be degraded within 20 min in the TiO 2 /C/O 3 system in the presence of 1 mg/L O 3 , 100 mg/L catalyst, at pH = 5. Based on the evaluation of the effect of basic parameters, it could be deduced that the removal of p -CNB relied on the synthetic effect of catalysis by TiO 2 /C and the autocatalytic induction of p -CNB. The removal efficiency of p -CNB, the structure change and the leaching of Ti ions were also evaluated in five cycles, indicating TiO 2 /C is stable and recyclable for catalytic ozonation in water treatment.

研究领域: 环境科学 · 催化化学 · 水处理技术 · 材料科学 · 环境工程 · 纳米材料应用
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

A novel thermosensitive persulfate controlled-release hydrogel based on agarose/silica composite for sustained nitrobenzene degradation from groundwater

Shuxuan Wu,Sheng Deng,Fu Xia,Xu Han,Tianyu Ju,Han Xiao,Xiangjian Xu,Yu Yang,Yonghai Jiang,Beidou Xi

The increasing risk of organic contamination of groundwater poses a serious threat to the environment and human health, causing an urgent need to develop long-lasting and adaptable remediation materials. Controlled-release materials (CRMs) are capable of encapsulating oxidants to achieve long-lasting release properties in aquifers and considered to be effective strategies in groundwater remediation . In this study, novel hydrogels (ASGs) with thermosensitive properties were prepared based on agarose and silica to achieve controlled persulfate (PS) release. By adjusting the composition ratio, the gelation time and internal pore structure of the hydrogels were regulated for groundwater application, which in turn affected the PS encapsulated amount and release properties. The hydrogels exhibited significant temperature responsiveness, with 6.8 times faster gelation rates and 2.8 times longer controlled release ability at 10 ℃ than at 30 ℃. The ASGs were further combined with zero-valent iron to achieve long-lasting degradation of the typical nitrobenzene compound 2,4-dinitrotoluene (2,4-DNT), and the degradation performance was maintained at 50 % within 14 PV, which was significantly improved compared with that of the PS/ZVI system. This study provided new concepts for the design of controlled-release materials and theoretical support for the remediation of organic contamination.

研究领域: 环境科学 · 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Synergistic reduction and oxidation system using 4,7-dihydroxycoumarin as a green photocatalyst for efficient nitrobenzene degradation

Jiajie Xu,Changyu Yan,Zhaojiang Wu,Miaoling Xu,Tuo Wei,Tingchao He,Wenhua Zhou,Yi Zhang,Junmin Zhang,Bo Yang

In this study, a synergistic reduction–oxidation process was proposed using natural organic matters (NOMs) as an organic photocatalyst for complete degradation of nitrobenzene (NB) that was difficult to oxidative decomposition directly. It has been verified by electron spin resonance (ESR) that both reductive organic free radical (4H-chromene-2,4,7-triol radical, S 2 ) and oxidative OH radicals could be generated sustainably by using 4,7-dihydroxycoumarin (4,7-DHC) as a green photocatalyst under UV light irradiation, and 95.07% of NB degradation efficiency was achieved after 4-h irradiation with 40 µM 4,7-DHC. The formation of aniline as a reductive product was convenient for the attack of OH radicals, making it easier for the complete degradation of NB. In addition, 4,7-DHC showed high photocatalytic activity in a wide range of pH from 1 to 13, and the best photocatalytic activity was achieved with a pH value of 4.56. Besides, the effect of common coexisted ions (SO 4 2− , Cl − and NO 3 − ) on the NB degradation was discussed, and the highest k value was obtained with SO 4 2− (80 µM), NO 3 − (120 µM) or Cl − (20 µM). Moreover, 4,7-DHC exhibited extensive degradability to the frequently coexisted pollutants in NB-contaminated wastewater including humic acid (HA), aniline (AN) and m-dinitrobenzene (m-DNB), which might be extended into a potential approach for environmental remediation of NB-contaminated water due to its low cost and accessibility of 4,7-DHC as NOMs.

研究领域: 环境科学 · 化学工程 · 光催化
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