WATER AIR AND SOIL POLLUTION
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2024
·Vol. 235
·期 8
·1-14
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IF 3.8
Wang Weixing,Wang Lei,Lv Yincun,Deng Chenchen,Hu Zehui
Abstract As a broad-spectrum antibiotic, chloramphenicol has an important contribution in resisting bacterial diseases. It has been widely used in medicine and animal husbandry, but it has the disadvantages of long-term unreasonable use and slow degradation in nature. Long-term consumption of food contaminated by chloramphenicol will cause serious side effects to human beings. Therefore, it is urgent to establish an effective method to remove chloramphenicol from wastewater. Co/Ni@ZrO 2 photocatalyst with nanosphere structure was prepared by hydrothermal method and used for the degradation of chloramphenicol (CAP).The structure, morphology and optical properties of the samples were characterized by TEM, SEM, XPS, XRD, FT-IR and UV-Vis. Under visible light, 12% Co/Ni@ZrO 2 has good photocatalytic performance for the degradation of chloramphenicol, which may be due to the synergistic effect and nano-limitation effect between Co/Ni and ZrO 2 . When the optimal dosage of catalyst is 50 mg / L and the initial concentration of chloramphenicol is 20 mg / L, the degradation rate is 98.2 % within 150 min. XPS and Raman results showed that there were appropriate amount of oxygen vacancies on the surface of ZrO 2 , which accelerated the electron transfer rate in the system and inhibited the recombination of photoelectron-hole pairs under visible light, thus improving the activation efficiency of dissolved oxygen in chloramphenicol solution. Free radical capture experiments showed that· O 2 - ,· OH, h + were the main active substances for the degradation of chloramphenicol. The possible mechanism of chloramphenicol degradation under visible light was speculated. The results show that Co/Ni@ZrO 2 is a promising photocatalyst for wastewater treatment. Graphical Abstract A schematic diagram of charge separation and transfer during the degradation of chloramphenicol by 12wt % CoNi @ ZrO2 nanospheres
研究领域:
环境科学
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材料科学
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药学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Leilei Xiao,Jiajia Li,Eric Lichtfouse,Zhenkai Li,Quan Wang,Fanghua Liu
Electroactive microorganisms and electrochemical technologies have been separately used for environmental remediation such as antibiotics removal, yet the efficiency of coupling these two methods for chlorinated antibiotics removal is poorly known. Here we tested the synergy of Geobacter sulfurreducens PCA, an electroactive bacteria, and an electrical field, on chloramphenicol removal. Removal is increased two-fold by increasing the temperature from 30°C to 37°C. The cyclic voltammograms and chronoamperometry tests demonstrated that G. sulfurreducens PCA catalyzed chloramphenicol chemical reduction with electrode as excusive electron donor. A critical voltage, −0.6 to −0.5 V vs. Ag/AgCl, was discovered for chloramphenicol degradation with an increase of removal rate about 2.62-folds, from 31.06% to 81.41%. Combined removal with both G. sulfurreducens PCA and an electrical field increased the apparent rate constant and reached 82.77% removal at −0.5 V. Specially, the combined removal at −0.5 V even presented more robust removal efficiency compared to −0.6 V (78.64%) without G. sulfurreducens PCA. Mass spectrometry of degradation products indicates the reduction of nitro into amine groups, and dechlorination into less toxic compounds. Overall, combined biocatalysis and an electrical field is a promising method to remove antibiotics from polluted environments.
研究领域:
环境科学
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微生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Feng Cheng,Yongfei Tong,Yang Liu,Yue Yuan,Zhiqiang Chen,Juan Liang,Yongli Zhang,Peng Zhou,Xiaoguang Duan,Bo Lai
In this study, vanadium powder (V) was employed as a cocatalyst to enhance the Fenton-like system. The V-Fe(III)/H 2 O 2 system can rapidly produce hydroxyl radicals and completely oxidize chloramphenicol with exceptionally high stability for long-term operation. The low-valent vanadium sites on the surface during the stepwise oxidation of vanadium from V 0 to V(IV) can donate electrons for direct H 2 O 2 activation and indirect Fenton reaction by reducing Fe(III) to produce hydroxyl radicals. Meanwhile, density functional theory (DFT) calculation unveils that low-valent vanadium sites of vanadium can lengthen Fe-O bonds of FeOH 2+ to elevate the oxidation potential of Fe(III) and promote Fe(III) reduction induced by H 2 O 2 . The self-cleaning effect of vanadium under acidic conditions can maintain reactive sites for sustainable electron donation and long-lasting enhanced Fenton oxidation. This study provides a novel enhanced Fenton oxidation for water remediation and the first mechanistic insights into the origins of V-based advanced oxidation technologies , it may also be beneficial to treat vanadium-contained wastewater.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xinfei Zhang,Jianhui Zhan,Xiaobo Jia,Jinxing Ma,Bin Han,Zhiliang Wang,Feilong Li,Yitong Wang,Yuan Zhang
In contrast to traditional metal oxides that engage in only two valence state conversions, multivalent metal oxides offer additional electrons, thus accelerating the activation of peroxymonosulfate (PMS) and enhancing catalytic activity. However, the low efficiency of converting between high-valent and low-valent metal ions often limits catalytic performance. In this study, we employed a combined hydrothermal and thermal polymerization strategy to load multivalent vanadium pentoxide (V 2 O 5 ) onto graphitic carbon nitride (g-C 3 N 4 ), thereby constructing a V 2 O 5 /g-C 3 N 4 heterojunction. This heterojunction formed a built-in electric field, facilitating PMS activation and achieving a record-breaking degradation of chloramphenicol (CAP) with a rate constant of 1.13 min −1 . Experimental and theoretical analyses indicated that the synergy between radical and non-radical pathways was the primary mechanism for efficient CAP removal. The built-in electric field altered orbital occupancy, reduced the bandgap, and enhanced electron transfer from g-C 3 N 4 to V 2 O 5 , accelerating the conversion between vanadium valence states and enhancing PMS activation. Furthermore, the V 2 O 5 /g-C 3 N 4 /PMS system exhibited a broad operational pH range (2–10), robust resistance to matrix interference, and exceptional durability, demonstrating its applicability for mitigating ecological toxicity of CAP and treating typical refractory organic pollutants. This study advances the understanding of how built-in electric fields promote PMS activation and introduces a novel approach for addressing emerging pollutants in aquatic environments.
研究领域:
环境科学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Feng Cheng,Peng Zhou,Yang Liu,Xiaowei Huo,Jian Zhang,Yue Yuan,Heng Zhang,Bo Lai,Yongli Zhang
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of H 2 O 2 to produce hydroxyl radicals ( • OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/H 2 O 2 Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that • OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote H 2 O 2 induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/H 2 O 2 systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/H 2 O 2 system with or without visible light shows high potential for application in environmental remediation.
研究领域:
环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
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IF 5.108
Xiaoyan Chen,Wei Miao,Yulin Yang,Sibei Hao,Shun Mao
In this study, an Fe(Ⅱ)/S(IV) system was designed for the degradation of chloramphenicol (CAP). The pseudo-first-order rate constants for CAP degradation under typical conditions with and without air purging were investigated. The greatly enhanced rate of 0.0099 min −1 with air purging compared with 0.0006 min −1 with no air purging indicated that aeration was significant to the degradation of CAP in Fe(Ⅱ)/S(Ⅳ) system. Radical scavenging experiments revealed that SO 4 - was the primary oxidant generated from the activation of S(IV) with Fe(II), accounting for around 70% of degradation under weak acidic and neutral conditions. Increasing Fe(II) and S(IV) doses promoted the degradation of CAP, whereas the overdose of them led to a decreased degradation rate by scavenging radicals. Owing to the participation of oxygen in the formation of ferric sulfite complex and SO 5 - , the increase of dissolved oxygen improved the removal efficiency of CAP. The removal efficiency of CAP was also found to be pH dependent, decreasing from acid condition (initial pH = 4) to basic condition (initial pH = 8). The presence of coexisting anions and water matrix was found inhibiting CAP degradation in Fe(Ⅱ)/S(Ⅳ) system. This work provides an understanding on the working mechanism and possible applications of Fe(Ⅱ)/S(Ⅳ) system in organic compound degradation in wastewater.
研究领域:
环境科学
·
废水处理
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yaqian Pang,Junpeng Zhou,Xiaoli Yang,Yeqing Lan,Cheng Chen
In this study, the Co 3 O 4 -SnO 2 composite derived from bimetallic oxalates was rationally fabricated and utilized as a catalyst for peroxymonosulfate (PMS) activation towards the destruction of chloramphenicol (CAP). The physicochemical properties of the Co 3 O 4 -SnO 2 were systematically characterized to discover the relationship between its structure and catalytic performance. SnO 2 as a cocatalyst with high conductivity and stability immensely improved the activity of Co 3 O 4 in the Co 3 O 4 -SnO 2 composite. Approximately 98% of CAP (10 mg/L) was eliminated by the Co 3 O 4 -SnO 2 (0.1 g/L) activated PMS (1.0 mmol/L) at initial pH 7 within 20 min. The rationally designed Co 3 O 4 -SnO 2 composite exhibited higher catalytic activity than Co 3 O 4 , SnO 2 , and other cobalt-based bimetallic oxides (such as Co-Fe, Co-Mn, and Co-Cu) in the PMS activation for the CAP degradation. The synergistic effect of Co 3 O 4 and SnO 2 endowed the Co 3 O 4 -SnO 2 composite with higher conductivity and more electron transfer, which was proved by the electrochemical tests. The presence of SO 4 •− , • OH, O 2 •− , and 1 O 2 during the CAP degradation was testified by both quenching experiments and electron paramagnetic resonance (EPR) spectroscopy. In addition, the catalytic mechanism and degradation pathways were further proposed via the characterization of X-ray photoelectron spectroscopy (XPS) and the identification of transformation products, respectively. This work provides a new insight into the preparation of novel catalysts and their application in wastewater treatment.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Su Yan,Siqin Li,Sicheng Zhang,Lina Qian,Xiaoyu Yong,Xueying Zhang,Jun Zhou
Layered double hydroxides (LDHs) is one of the popular catalysts for peroxymonosulfate (PMS) activation, but LDHs has a challenge in particles aggregation that impacts their catalytical activity. Biochar carrier could effectively disperse LDH particles on its surface. This study for the first time used petrochemical sludge biochar (PSC) to prepare CoFe-LDH@PSC x composites, the catalytic performances of which were evaluated by PMS activation towards chloramphenicol (CAP) degradation. Results suggested CoFe-LDH@PSC 1:2 had a sponge-like surface with high surface area (188.53 m 2 g −1 ). CoFe-LDH@PSC 1:2 /PMS system could quickly degrade 97 % of 20 mg L −1 CAP from bulk solution within 20 min under the optimal reaction conditions (0.12 g L −1 CoFe-LDH@PSC 1:2 , 0.6 mM PMS, and pH 3.0). TOC removal in this system could reach 73.3 % at the same time. CAP degradation kinetic constant ( k obs ) of CoFe-LDH@PSC 1:2 /PMS system reached 0.129 min −1 that was 2.8 and 4.4 times higher than that of CoFe-LDH/PMS and PSC/PMS system, respectively. The excellent degradation performance was attributed to the fast redox cycle of ≡Co(II)/≡Co(III), ≡Fe(II)/≡Fe(III) and redox-active groups of C=C/C=O on catalyst, facilitating electron transfer for PMS activation to more reactive species ( OH, SO 4 − , O 2 − or 1 O 2 ) for CAP degradation. Fe 0 in catalyst was also beneficial for promoting ≡Co/≡Fe redox cycle. CAP degradation pathways were proposed based on intermediates identified by LC-MS. Overall, this work demonstrated CoFe-LDH@PSC 1:2 was a promising catalyst for PMS activation towards antibiotics degradation. Converting hazardous petrochemical sludge to “green” catalyst followed the concept of substantiable development.
研究领域:
环境科学
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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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2024
·
IF 8.1
Bincheng Xu,Zexi Luo,Tao Tao,Ying Wang
Co-based nanomaterials have been proven as excellent catalysts in activating peroxymonosulfate (PMS), owing to the high adsorption ability and efficient electron transfer toward PMS molecules. However, the slow Co sites regeneration induced by HSO 5 − /SO 5 – redox cycle alone not only deteriorates the utilization efficiency of PMS, but also restricts the overall catalytic reaction rate. Herein, we report a novel S-FeCoO nano-catalyst to active PMS for chloramphenicol (CAP) degradation. As a result, up to 97.73 % of removal efficiency was achieved within 30 min even with an initial CAP concentration of 50 mg/L, which is substantially superior to other Co or Fe-based PMS activation systems. More importantly, synergistic effects arising from the coexisting Fe and S species were identified by the control experiments and characterization results. Co served as the primary active site, while Fe(II) and S 2− /S 2 2− greatly accelerated Co(III)/Co(II) redox cycle by donating electrons. The proposed strategy of dual acceleration of Co(III)/Co(II) redox cycle, as well as its mechanism insights, is expected to provide important implications on the rational design of advanced catalysts for PMS activation.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ningjie Du,Ying Liu,Qiuju Li,Wei Miao,Dandan Wang,Shun Mao
Single-atom catalysts have drawn increasing attention in advanced oxidation due to their unique structure and significant promise in heterogeneous catalysis. Herein, single-atom iron anchored on nitrogen-doped carbon (SAFe-N-C) was synthesized with iron phthalocyanine (FePc) and metal-organic framework (ZIF-8). With thermal treatment and acid leaching, atomically-dispersed Fe-N x sites were successfully formed on the surface of N-C support derived from ZIF-8. The prepared catalyst was demonstrated to activate peroxydisulfate (PDS) for chloramphenicol (CAP) degradation. Compared with N-C, the SAFe-N-C shows 6 times enhanced removal efficiency (from 15.3% to 93.1%) for CAP. Moreover, the catalyst shows high catalytic activity in a wide pH range of 5 to 9 and good resistance to inorganic anions, in which a singlet oxygen-dominated process is found. This study reveals the role of single-atom site in singlet oxygen evolution and offers a new catalytic approach for selective removal of organic pollutants in complex water matrix.
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
RARE METALS
·
2024
·
IF 9.6
Fan Yu-Ning,Zhang Yun-Qiu,Gao San-Shuang,Bi Zeng-Hui,Wang Yin,Zhou Shu-Xing,Liu Qian,Lv Tian-Ping,Hu Guang-Zhi
The use of transition metal-activated peroxymonosulfate (PMS) as an advanced oxidation technology has gained recognition. This study developed a catalyst using cobalt–lanthanum bimetallic oxide supported on layered molybdenum disulfide (MoS 2 ) as a carrier. The Co–La/MoS 2 catalyst was synthesised through coprecipitation, followed by calcination with an optimised metal ratio of Co:La = 2:1 to activate PMS and degrade trace chloramphenicol (CAP) in water. The chemical composition of the catalyst was confirmed using X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). At catalyst and PMS dosages of 0.1 and 0.5 g·L −1 , respectively, the degradation rate of CAP was 95% within 30 min. The catalyst exhibited strong resistance to most interfering anions and maintained a high degradation rate at pH 3–11. Liquid chromatography–mass spectrometry analysis revealed the potential degradation pathways of CAP in the Co–La/MoS 2 (2:1)/PMS system. For other pollutants, such as oxytetracycline, complete degradation was achieved within 20 min, demonstrating the broad applicability of the Co–La/MoS 2 (2:1)/PMS system for the degradation and removal of antibiotic organic contaminants. This study offers a feasible approach for the degradation of antibiotic organic pollutants, including CAP, in natural water bodies. Graphical abstract
研究领域:
环境科学
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化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Liu-Xi Yang,Jia-Cheng E. Yang,Ming-Lai Fu
In this study, porous magnetic CoFe 2 O 4 nanocrystals (NCs) were successfully synthesized by using bimetal-organic framework (MOF) as a precursor, and used as catalysts to activate peroxymonosulfate (PMS) for the removal of chloramphenicol (CAP) in the solution. The structure and physicochemical properties of CoFe 2 O 4 NCs were thoroughly examined by a series of characterization techniques. The results revealed as-synthesized CoFe 2 O 4 had a nanorod-shaped structure with high specific surface area (83.00 m 2 g −1 ) and pore volume (0.31 cm 3 g −1 ). Furthermore, the degradation efficiency (100%) and the removal of total organic carbon (68.09%) were achieved after 120 min with 0.1 g/L CoFe 2 O 4 NCs, 2 mM PMS and 10 mg/L CAP at pH of 8.20. In addition, effects of catalyst dosage, PMS dosage, initial pH values, CAP concentration and co-existing anions as well as natural organic matters in the solution on the degradation efficiencies were studied and all the removal can be well fitted with pseudo-first-order kinetic model (R 2 > 0.96). Sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO•) were proved to be two main reactive species for CAP removal in CoFe 2 O 4 /PMS system based on quenching experiments. CAP was degraded by the main pathways of dichlorination, denitration, decarboxylation , hydroxylation, ring cleavage and chain cleavage on CoFe 2 O 4 /PMS system through high performance liquid chromatograph-mass spectrometry analysis. We believe that this study would be very meaningful to promote the applications of MOFs-derived catalysts on the SO 4 •− based advanced oxidation processes (SR-AOPs) for the environmental remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）