RSC Advances
·
2018
·Vol. 8
·期 8
·3934-3940
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IF 2.936
Chunyong Zhang,Wei Chen,Jiahui Xian,Degang Fu
In this work, a novel definitive screening design (DSD) was initially used to investigate the in situ chemical oxidation of acid orange-II (AO II) dye using a homogeneous cobalt-catalyzed peroxymonosulfate (Co2+/PMS) system. Experiments were performed in a batch reactor using a synthetic AO II solution containing cobalt ions, humic acid (HA) and five electrolyte salts (NaCl, NaNO3, NaHCO3, Na2SO4 and NaH2PO4). The effects of nine operating variables on AO II degradation: NaCl concentration (0–20 mM), NaH2PO4 concentration (0–20 mM), NaHCO3 concentration (0–20 mM), NaNO3 concentration (0–20 mM), Na2SO4 concentration (0–20 mM), HA concentration (0–40 mg L−1), PMS concentration (2–10 mM), AO II concentration (0–100 mg dm−3) and Co2+ concentration (0–1.36 mM), were investigated. Analysis of a DSD model revealed that only four variables were statistically significant. Besides, our results indicated that there were no significant interactive effects between the five anions employed. Thereafter, a central composite rotatable design (CCRD) was adopted to further optimize these significant variables. A CCRD model describing AO II conversion as a function of PMS concentration, NaCl concentration and Co2+ concentration was then constructed and used to explore the final optimal operating conditions. As a consequence, the combination of DSD and CCRD allowed reducing the number of experiments from over 600 to only 39. Lastly, a plausible reaction sequence concerning the oxidation of AO II in the Co2+/PMS/Cl− system was also proposed. The route of AO II oxidation involved hydroxylation and chlorination, signifying the roles of both sulfate radicals and active chlorine species.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2018
·
IF 3.057
Qingzhuo Ni,Jianfeng Ma,Changhai Fan,Yong Kong,Mingguo Peng,Sridhar Komarneni
A spinel-type Co-Mn oxide was designed and synthesized through a two-step oxidation-precipitation method at modest temperatures. The Co-Mn oxide was applied as the catalyst in the presence of NaHSO 3 under visible light irradiation in order to establish the superiority of heterogeneous photo-chemical catalysis system. In the above system, the Co-Mn catalyst exhibited much better catalytic capability than that in either single photocatalysis or chemocatalysis system, implying that the Co-Mn catalyst could well combine photocatalysis and chemocatalysis to obtain the highest degradation efficiency of up to 94% within 40 min when using Orange II as the target pollutant. Recycling experiments results showed that the as-obtained catalyst has excellent stability and recyclability. Powder X-ray diffraction (XRD) analysis showed that the as-obtained Co-Mn catalyst had a cubic MnCo 2 O 4.5 spinel structure. Because of relatively low temperature (180 ℃) synthesis, the catalyst was formed with nanoparticles (25–65 nm) and high specific surface area as confirmed by SEM and BET analyses. XPS indicated the presence of both manganese and cobalt species that serve as reactive sites for the catalytic oxidation reactions. Rational degradation mechanisms responsible for superior catalytic activity and durability were proposed based on a series of experimental results. The active species such as Mn(III), holes and sulfate and hydroxyl radicals were proposed to be responsible for the outstanding degradation results.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Xiaoyu Yu,Jianliang Sun,Guibiao Li,Yi Huang,Yu Li,Dehua Xia,Feng Jiang
The sulfate radical (•SO 4 − )-based advanced oxidation processes (AOPs) for the degradation of refractory organic pollutants consume a large amount of persulfate activators and often generate toxic organic by-products. In this study, we proposed a novel iron-cycling process integrating •SO 4 − -based AOP mediated by reusable iron particles and a sulfidogenic process to degrade and detoxify Orange II completely. The rusted waste iron particles (Fe 0 @Fe x O y ), which contained Fe II /Fe III oxides (Fe x O y ) on the shell and zero-valent iron (Fe 0 ) in the core, efficiently activated persulfate to produce •SO 4 − and hydroxyl radicals (•OH) to degrade over 95% of Orange II within 120 min. Both •SO 4 − and •OH destructed Orange II through a sequence of electron transfer , electrophilic addition and hydrogen abstraction reactions to generate several organic by-products (e.g., aromatic amines and phenol), which were more toxic than the untreated Orange II. The AOP-generated organic by-products were further mineralized and detoxified in a sulfidogenic bioreactor with sewage treatment together. In a 170-d trial, the organic carbon removal efficiency was up to 90%. The inhibition of the bioreactor effluents on the growth of Chlorella pyrenoidosa became negligible, due to the complete degradation and mineralization of toxic AOP-generated by-products by aromatic-degrading bacteria (e.g., Clostridium and Dechloromonas ) and other bacteria. The sulfidogenic process also well recovered the used Fe 0 @Fe x O y particles through the reduction of surface Fe III back into Fe II by hydrogen sulfide formed and iron-reducing bacteria (e.g., Sulfurospirillum and Paracoccus ). The regenerated Fe 0 @Fe x O y particles had more reactive surface Fe II sites and exhibited much better reactivity in activating persulfate in at least 20 reuse cycles. The findings demonstrate that the integrated process is a promising solution to the remediation of toxic and refractory organic pollutants because it reduces the chemical cost of persulfate activation and also completely detoxifies the toxic by-products.
研究领域:
环境科学
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污染治理
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微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2015
·Vol. 6
·期 7
·2296-2304
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IF 5.426
Kaixin Zhu,Junhu Wang,Yanjie Wang,Changzi Jin,Ayyakannu Sundaram Ganeshraja
Refractory and non-biodegradable pollutants produced by industries have inevitably brought great threat to human life. Integrating several kinds of advanced oxidation processes (AOPs) into one system has been proposed to be an efficient strategy to remove such pollutants from the environment at low cost. In this study, magnetic zinc ferrite fine nanoparticles, firstly synthesized by a novel soft chemical solution process, showed super reactivity, good reusability and easy separation ability for visible-light-induced Orange II degradation in an integrated ZnFe2O4/PMS (peroxymonosulfate, 2KHSO5·KHSO4·K2SO4, OXONE) aqueous system. Powder X-ray diffraction, transmission electron microscopy, and 57Fe Mössbauer and X-ray photoelectron spectroscopy were employed to characterize the structure and morphology as well as recognize the physicochemical changes of the fine nanoparticles before and after the reaction. The generated oxidizing intermediates during the degradation process were detected by electron paramagnetic resonance spectroscopy and classic quenching experiments, which confirmed that both sulfate radical (SO4˙−) and hydroxyl radical (˙OH) co-existed in the degradation process. The systematic condition experiments further verified the dual functionality of the ZnFe2O4/PMS system, which actively acted as a photocatalyst and a PMS activator for dye molecule oxidation under visible light irradiation. This study proves that photocatalysis and PMS activation for remediation of organic pollutants in water can be easily integrated into one system by using zinc ferrite nanoparticles as an environmentally friendly catalyst.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Lingli Ji,Qixing Xiao,Lijun Zhu,Sridhar Komarneni,Jianfeng Ma
Carbon dots (CDs)-modified Cr 2 O 3 (CDs@Cr 2 O 3 ) composites were synthesized by solvothermal process followed by calcination to improve their catalytic performance. The physical and chemical properties of the composites were determined by XRD , SEM , TEM, BET and XPS . With the aid of sodium persulfate, the activity of CDs@Cr 2 O 3 to oxidize Orange II by non-radicals was studied under various conditions. The experimental results determined the optimal dosage of PDS to be 0.1 g and the degradation results showed that after 45 min, the degradation rate of Orange II reached to 98.4% with the CDs@Cr 2 O 3 /PDS/Vis system. The adsorption capacity of CDs@Cr 2 O 3 for Orange II was closely related to pH, and this phenomenon is further explained by the isoelectric point. A series of experiments proved that non-free radicals played a crucial role in the oxidation process , in which singlet oxygen ( 1 O 2 ), superoxide radical (O 2 •− ) and photo-generated holes (h + ) were determined as the important reactive oxygen species (ROS). In addition, the present study found that increasing dissolved oxygen could promote the reaction and the catalyst maintained good degradation performance after five cycles suggesting its stability.
研究领域:
环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 21
·59366-59381
·
IF 5.8
Xiong Huixin,Shi Kun,Han Jie,Cui Can,Liu Yang,Zhang Bailin
Discharge of the untreated dye-containing wastewaters will induce water source pollution and further harm aquatic organisms. In this study, the akaganéite/polyaniline catalyst (β-FeOOH/PANI, about 1.0 μm) could be successfully composed by polyaniline (PANI, (C 6 H 7 N) n , 200–300 nm) and akaganéite (β-FeOOH, FeO(OH) 1−x Cl x , less than 200 nm), according to the identification and characterization results of XRD, Ramon, FTIR, XPS, SEAD, EDS, and FESEM (or HRTEM). Due to PANI providing more photogenerated electrons, the β-FeOOH/PANI composite (compared with β-FeOOH) in photo-Fenton system had the more highly catalytic degradation capacity to Acid Orange II (AOII) under an optimal condition (7.5 mmol/L of H 2 O 2 oxidant, 40 mg/L of AOII, 0.2 g/L of catalyst dosage, and pH 4.0). The AOII degradation kinetics could be well fitted by pseudo-first-order model. In photo-Fenton catalytic process of AOII dye, the ∙OH and h + were the main reaction substances. The AOII in solutions could be gradually mineralized into non-toxic inorganic H 2 O molecule and CO 2 . The β-FeOOH/PANI catalyst also had a good reusable ability of about 91.4% AOII degradation after 4 runs. These results can provide a reference for synthesis of catalyst used in photo-Fenton system and the applications in degradation removal of organic dye from wastewaters.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2017
·
IF 4.217
Lixuan Duan,Xuejun Zhou,Siting Liu,Penghui Shi,Weifeng Yao
We report a 3D-hierarchically Co 3 O 4 /graphene hydrogel (CGH) composite as a catalyst activator of peroxymonosulfate (PMS) for sulfate radical-based degradation of Orange II in a heterogeneous system. The physicochemical performance of the composite is analyzed by X-ray diffraction spectra, scanning electron microscopy, Raman spectroscopy, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The results demonstrate that the samples are prepared resoundingly. The CGH hybrid composite completely removes Orange II wastewater within 6 min; furthermore, after five runs, the catalyst activity remains essentially unchanged and the macrostructure is followed consistently. This unusual macrostructure hydrogel of supported cobalt oxide indicates a high feasibility of commercial promotion to remove the azo dye.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 11
·1-12
·
IF 2.9
Wang Xilin,Sun Xiaojing,Dai Ping,Xu Dongyan
This study focuses on preparation of a novel Fe 3 O 4 @C/RM composite by carbothermal reduction of red mud (RM) with scrap tire-derived carbon black and its application for the degradation of orange II in water by activating PMS. X-ray diffraction (XRD) measurements revealed that hematite (Fe 2 O 3 ) was reduced to Fe 3 O 4 in the pyrolysis process above 600 o C. The reduction pathway of Fe 2 O 3 was inferred by detecting the gas emissions during carbothermal reduction. Morphology analysis indicates that Fe 3 O 4 nanoparticles were encapsulated in a carbon matrix, forming a composite with the residual components of RM. The as-prepared Fe 3 O 4 @C/RM composite exhibited high performance toward orange II degradation with 95.9% removal of orange II within 90 min. Electron paramagnetic resonance (EPR) and quenching tests were applied to illustrate the activation processes of peroxymonosulfate. Both radical and non-radical oxygen species are responsible for the efficient degradation of orange II in the Fe 3 O 4 @C/RM/PMS system.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
·
IF 5.774
Shuo Feng,Bing Xiao,Meng Wu,Yun Wang,Rufen Chen,Hui Liu
In this study, copper phosphide (Cu 3 P) was used as a heterogeneous catalyst for peroxydisulfate (PDS) activation and Orange II degradation. This catalyst functions over a broad pH range, from 3.0 to 9.0 and the degradation rate of Orange II is 95.2% at 15 min under optimal conditions. The rapid degradation kinetics can be described by the Behnajady-Modirshahla-Ghanbery (BMG) equation. Sulfate radical, the main reactive oxidizing species, along with OH and O 2 − , were responsible for pollutant degradation. The Cu 3 P catalyst exhibited good stability and excellent anti-interference performance toward Cl − , NO 3 − , and HCO 3 − anions. The removal efficiency of Orange II remained close to 100%, even after five rounds of recycling reactions. The rapid catalytic mechanism of Cu 3 P is attributed to the dual-catalysis center in Cu 3 P (Cu and P) and simultaneous existence of three cycles ( Cu II → Cu III → Cu II , Cu I → Cu II → Cu I , and Cu δ+ → Cu 1+δ+ → Cu δ+ ) on the surface and interior of Cu 3 P. This study sheds new light on the fabrication of high-performance heterogeneous catalysts to solve the environmental problems.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Jun Chen,Layun Zhu,Shangqing Xia,Zhaoming Chen,Xue Li,Xiaohong Yang,Zihui Song,Yutong Wang,Zongsheng Zhan,Dongliang Shao
ABSTRACT The activated cyanobacterial carbon (ACC) prepared from Chaohu Lake cyanobacteria was used as a carrier for nitrogen doping to synthesize nitrogen-doped activated cyanobacterial carbon (N@ACC), a highly efficient activation material. N@ACC was found to be an effective catalyst for the degradation of Orange II (OII) dye by activating peroxymonosulfate (PMS). Characterization of N@ACC showed that it had a larger specific surface area (159.12 m 1 /g) than ACC and an average particle size of 3.28 nm. N@ACC also contained various functional groups such as C=O, C=N, and –OH. To optimize the degradation of OII, the reaction conditions of the N@ACC activated PMS system were adjusted. The N@ACC activated PMS system was able to achieve a degradation rate of 98.8% for OII (100 mg/L) within 35 min, which was significantly higher than the rate achieved by the ACC activated PMS system (19.5%). The degradation reaction followed first-order kinetics and indicated a combined free radical mechanism. Compared to ACC, N@ACC contained a higher content of nitrogen, specifically pyridinic and graphitic nitrogen. The results showed that introducing nitrogen would refactor the structure of raw carbon, regulate its properties, and create new active sites for the degradation of pollutants. Moreover, N@ACC does not need metallic elements to improve PMS degradation efficiency. Therefore, the synthesis of N@ACC could be used as a new way to activate PMS.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Qinzhi Wang,Zhan Shi,Zhi Wang,Yijian Zhao,Jianuo Li,Huifan Hu,Yaowen Bai,Zhihao Xu,Hui Zhangsun,Li Wang
Acid orange II (AO II), a typical azo pigment, is strictly controlled by legislation and prohibited in foodstuffs. Herein, we prepared gold nanoparticles decorated amino-functionalized Cr-based metal-organic frameworks [NH 2 -MIL-101(Cr)@Au] via an in-situ reduction method as a surface-enhanced Raman scattering (SERS) substrate for simultaneous adsorption and detection of AO II. Gold nanoparticles are uniformly dispersed on the surface of NH 2 -MIL-101(Cr) owing to its three-dimensional (3D) structure and the interaction between –NH 2 and Au ions , providing more SERS-active “hot spots”. These NH 2 -MIL-101(Cr)@Au nanocomposites exhibited selective and high adsorption performance (419.85 mg g −1 ) for AO II, and could be used as superior SERS substrates for the detection of AO II with a low limit of detection (LOD) of 0.05 mg L −1 and wide detection range of 0.05–50 mg L −1 using portable Raman spectrometer. Furthermore, this SERS assay has been successfully used to determine AO II in orange juice and chili powder with good sensitivities.
研究领域:
材料科学
·
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Yu Lei,Yixing Hao,Hao Cheng,Jianfeng Ma,Yong Qin,Yong Kong,Sridhar Komarneni
Fe 2 O 3 @CeO 2 nanocomposites were synthesized by water bath heating method to activate NaHSO 3 for Orange II dye (50 mg L −1 ) degradation, which reached up to 98.2% within 120 min. The Fe 2 O 3 @CeO 2 and NaHSO 3 dosages and the molar ratios of Ce and Fe in Fe 2 O 3 @CeO 2 were investigated to obtain the optimum conditions as follows: 0.02 g Fe 2 O@CeO 2 , 0.1 g NaHSO 3 and the molar ratio of Ce and Fe was 5:2 (designated as Ce-Fe-1, or simply Fe 2 O 3 @CeO 2 ). In addition, Fe 2 O 3 @CeO 2 catalyst displayed superior catalytic performance to those materials that were previously reported, as verified by the good stability (reached 90.9% after three cycles) and high degradation rate of Orange II (98.2%) of the currently developed material. Existence of · SO 4 – and · OH radicals were verified by Electron Spin Resonance Spectroscopy during degradation, and these radicals are proposed to have high degradation efficiency of Orange II. On the basis of the detected radicals, a possible degradation mechanism was proposed to provide more choices for the application of sulfite in advanced oxidation processes (AOPs).
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）