Journal of the Taiwan Institute of Chemical Engineers
·
2024
·
IF 5.5
Shaodong Jing,Xiaolong Xiao,Zhen Liu,Mengyu Ma,Qian Li
Background In the treatment of organic wastewater, Fenton technology often produces iron sludge due to iron circulation obstruction, which inhibits the treatment efficiency and causes secondary pollution to the actual water. Methods In this study, MoO 2 was used as a cocatalyst to promote the effective cycling of Fe 2+ /Fe 3+ in the Fe 2+ /H 2 O 2 system, thus efficiently degrading total petroleum hydrocarbons (TPHs). The superiority of MoO 2 as co-catalyst was verified under different reaction conditions, and its mechanism was discussed. Findings The degradation rate of TPHs in the Fe 2+ /H 2 O 2 /MoO 2 system (0.069 min −1 ) was about 14 times that of Fe 2+ /H 2 O 2 system (0.005 min −1 ). Compared with the Fe 2+ /H 2 O 2 system, the Fe 2+ /H 2 O 2 /MoO 2 system not only had a wider pH adaptation range, but also could effectively remove TPHs under the interference of co-existing organic and inorganic anions. MoO 2 did not change the types of reactive species in Fenton system, but it enhanced the production of reactive oxygen species (ROS) by promoting the Fe 2+ /Fe 3+ cycling in the reaction system, and ·OH was the main reactive species of TPHs degradation.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
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2024
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IF 9
Yuming Huang,Wei Zhou,Liang Xie,Junfeng Li,Xiaoxiao Meng,Xuewei Zhang,Yang Yu,Miaoting Sun,Jiaxiang Chen,Lijie Wang,Jihui Gao,Guangbo Zhao
Integrating the hydrogen evolution reaction (HER) with the carbon oxidation reaction (COR) is a promising method for producing H₂ with lower energy consumption. However, due to the passivation effect of oxygen functional groups (OFGs) for COR and Fe³⁺, achieving efficient and sustainable carbon oxidation to assist water electrolysis for hydrogen production remains a challenge over the past decades. This study introduced [EDTA·Fe(III)] – as a mediator to promote COR. [EDTA·Fe(III)] – effectively prevented the oxidation layer on the carbon surface from anchoring Fe (III) and reactivated the carbon that had been passivated by the oxidation layer. Density functional theory calculations indicated that the notable COR activity resulted from [EDTA·Fe(III)] – effectively lowering the vertical ionization potential of carbon, without being affected by OFGs. Notably, in the HER||COR-[EDTA·Fe(III)] – system, a cell voltage of merely 0.74 V is sufficient to reach a current density of 10 mA cm −2 , with the corresponding energy consumption being 1.76 kWh Nm −3 (H 2 ). This strategy offers new insights into achieving stable, low-energy hydrogen production via water electrolysis.
研究领域:
能源化学
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Wenbin Gao,Yuzhen Chen,Jiahao Rao,Zhan Hu,Yan Tan,Yujiao Wen,Yifan Wang,Zhi Zhou,Yongfa Zhu,Nan Zhou
Biochar currently served as the support for dispersed metal nanoparticles and cooperated with pyrite to generate more reactive radicals in organic pollution degradation system. But the mechanism of interaction between biochar and pyrite has not been elucidated. In this paper, biochar with oxygen-containing functional groups (OFGs) served as a stable dispersant to prepare nano-Fe x S y loaded biochar materials (BC OFGs @nano-Fe x S y ). BC OFGs coordinated with nano-Fe x S y to overcome its drawbacks, boosting QNC removal efficiency from 28.64% to 100%. The XPS and the linear sweep voltammetry (LSV) results revealed higher Fe(II) content and higher electron transfer rate on used BC OFGs @nano-Fe x S y , further validating that hydroxyl functional groups on biochar surface provided electrons to Fe(III) to achieve efficient Fe(II)/Fe(III) cycling. Based on comparative experiments and studies on the roles of iron, S(II) species and OFGs, we clearly revealed that OFGs on biochar materials surface coordinated with nano-Fe x S y to catalyze the degradation of QNC. The degradation efficiency of BC OFGs @nano-Fe x S y for QNC was still as high as 91.39% after five cycles, providing full demonstrations that OFGs and S(II) as the abundant electron donor coordinated with Fe species for QNC catalytic degradation and further enhanced the catalytic performance and stability of nano-Fe x S y .
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Wei Xiang,Hao Chen,Zhenxing Zhong,Chunjie Zhang,Xiejuan Lu,Mingjie Huang,Tao Zhou,Peng Yu,Beiping Zhang
In this study, a novel ultrasound enhanced FeS/persulfate Fenton-like system (US/FeS/PDS) was developed for the synergistic degradation of a typical drug carbamazepine (CBZ) under neutral circumstances. Factors such as FeS dosage, PDS dosage, initial pH and temperature, as well as coexisting anions were investigated. High dosages of FeS and PDS, elevated temperature and acidic circumstances were favorable for the oxidation of CBZ. Presence of HCO 3 − strongly inhibited the CBZ degradation in the US/FeS/PDS system, while slight suppression was observed with either NO 3 − or Cl − . Seven intermediates were identified as the products from the decomposition of CBZ by hydroxyl radicals (OH·) and sulfate radicals (SO 4 − ·). Time-dependent radical examination indicated that homogeneous OH· and SO 4 − · would contribute to the CBZ removal from 22.6 to 34.7% and 12.9 to 50.5%, respectively, while the contribution of solid-liquid interfacial radicals decreased from 64.5 to 20.2%. Meanwhile, the oxidation of S 2− occurred concurrently with reduction of Fe(III) to Fe(II). The reaction mechanism in the US/FeS/PDS system was proposed based on the sonochemical heterogeneous-homogeneous sulfur-iron cycle in the US/FeS/PDS system. US would firstly enhance the interfacial sulfur-iron electron transfer and the disintegration of the passivation layer, and then lead to the overall improvement in both interfacial and bulk sulfur-iron cycle, as well as the degradation of CBZ.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Da Ouyang,Ronghao Wu,Zhaojun Xu,Xiaomin Zhu,Yimin Cai,Ruihuan Chen,Changyin Zhu,Damià Barceló,Haibo Zhang
Advanced oxidation processes (AOPs) based on persulfate (PDS) activation by iron materials have attracted significant attention due to their high organic pollution removal efficiency and relatively low remediation costs. However, one of the iron-based materials’ shortcomings is the weak activation ability of Fe 3+ on PDS and the low sustainability of Fe 2+ in the oxidation environment. In this study, biochar-supported molybdenum dioxide (MoO 2 @BC) was employed as a co-catalyst to enhance the Fe 3+ based PDS activation for Bisphenol A (BPA) degradation. Results showed that >96 % of BPA was removed during 60 min, and the BPA degradation efficiencies only slightly decreased after four reuses of MoO 2 @BC. Electron paramagnetic resonance (EPR) analysis and quenching experiments indicated that reactive oxidation species (ROSs) contributing to the degradation of BPA were SO 4 − , OH and 1 O 2 . Besides, it was found that biochar supporting favours the adsorption of Fe 3+ on the MoO 2 surface and promotes the electron transfer from Mo(IV) to Fe 3+ based on the combination of X-ray photoelectron spectroscopy (XPS) analysis, electrochemical tests and density functional theory calculation (DFT). This work provides a new insight for enhancing the performance of organic contaminants degradation through AOPs based on persulfate activation by iron material.
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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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xiaolong Hu,Jingyu Bao,Daiwen Chen,Syed Jalil Shah,Sidra Subhan,Wenxue Gong,Wenyuan Li,Xinqi Luan,Zhongxing Zhao :,Zhenxia Zhao
In the photo-Fenton reactions, fast recombination of photoinduced electrons and holes in Fe-based metal–organic frameworks (Fe-MOFs) slows Fe(III)/Fe(II) cycle, which remains big challenge that significantly retards the overall process. Herein, NH 2 -MIL-88B(Fe) (NM88) was modified with 3,5-diaminobenzoic acid (DB) and TPB-DMTP-COF (COF-OMe) to in situ construct NM88(DB) 0.85 /COF-OMe composite that could strongly harvest the visible light for photo-Fenton degradation of sulfamerazine (SMR). With the addition of DB, electron-donating effect of NM88 was strengthened, which then promoted amino groups to react with aldehyde groups (Schiff-base), and thus highly facilitated the interfacial contact between NM88 and COF-OMe. Such modifications increased the degradation rate constants for NM88(DB) 0.85 /COF-OMe to 15.1 and 17.3 times that of NM88 and COF-OMe respectively with good reusability. Moreover, the catalyst exhibited 32–170 times higher degradation kinetics in comparison to other reported catalysts. Results showed that due to the Schiff-base reaction between NM88(DB) and COF-OMe, electron density on Fe(III) was decreased; and the photogenerated electrons of COF-OMe moved to NM88(DB) to reduce Fe(III), thus resulting in the generation of highly active Fe(II) and ·OH species. Furthermore, the main reactive species were determined to be ·OH and ·O 2 – by trapping experiments, and a possible mechanism of the degradation system followed Z-scheme charge transfer.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2024
·Vol. 59
·期 42
·19811-19824
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IF 3.5
Liu Weinan,Zhang Haiyang,Yuan Hang,Wang Lidong,Li Zhen
Peroxymonosulfate (PMS) is widely used in advanced oxidation processes. Fe(II) is an excellent catalyst for PMS, and organic pollutants in water can be effectively degraded in the Fe(II)/PMS system. However, the pollutant degradation efficiency is limited by the low conversion efficiency of Fe(II). Natural antioxidants exist in the water environment and have strong electron-donating ability. At present, the research on the introduction of natural antioxidants into the advanced oxidation processes to degrade pollutants focuses on a few polyphenols, and the effects of other natural antioxidants on the removal of pollutants are worth studying. In this study, natural antioxidants, proanthocyanidins (PCs), saponins (SPs), and Lycium barbarum polysaccharides (LBPs), were introduced into the Fe(III)/PMS system. The reduction ability of natural antioxidants was used to improve the conversion efficiency of Fe(III) to Fe(II), and PMS was more effectively activated to produce ROS, which promoted the degradation of ofloxacin (OFL). After the introduction of PC in the Fe(III)/PMS system, 80% of OFL was degraded at 20 min, and 90% of OFL was degraded at 120 min after the introduction of SP. The experimental results showed that the degradation of OFL was affected by the amount of antioxidants, PMS and Fe(III), pH value, and coexisting anions. Free radical quenching experiments showed that 1 O 2 , SO 4 − ·, and ·OH play an important role in the degradation of OFL in the Fe(III)/antioxidant/PMS system. This paper proves that the introduction of proanthocyanidins and saponins into the advanced oxidation processes can remove organic pollutants more efficiently. Graphical
研究领域:
环境科学
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化学工程
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水处理技术
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Ying Gao,Qinqin Chen,Xinhao Shen,Shuang Yao,Zhiwen Jiang,Sanjian Ma,Hailiang Yang,Juanhong Li,Zixia Lin,Xin Liu
Both the sluggish kinetics of Fe(II) regeneration and usage restriction of H2O2 have severely hindered the scientific progress of the Fenton reaction toward practical applications. Herein, a reduction strategy of activated hydrogen, which was used to simultaneously generate H2O2 and accelerate the regeneration of ferrous in a Fenton-like reaction based on the reduction of activated hydrogen derived from H2, was proposed. Two types of composite catalysts, namely, Pd/UiO-66(Zr)-2OH and Pd@UiO-66(Zr)-2OH, were successfully prepared by loading nano-Pd particles onto the outer and inner pores of UiO-66(Zr)-2OH in different loading modes, respectively. They were used to enhance the reduction of activated hydrogen. The characterization results based on the analysis of scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy revealed that the materials were successfully prepared. By using a trace amount of ferrous iron and without adding H2O2, trimethoprim (C0 = 20 mg·L–1), as a target pollutant, could be nearly 100% degraded within 180 min in the reaction system composed of these two materials. The cycle of iron and the self-generation of H2O2 were verified by the detection of ferrous H2O2 in the system. Density functional theory calculation results further confirmed that the pore-filled Pd0 NPs, as the main catalytic site for Pd@UiO-66(Zr)-2OH, could produce H2O2 under the combined action of hydrogen and oxygen. The Pd@UiO-66(Zr)-2OH system had excellent stability after multiple applications (at least 6 cycles), all of which resulted in 100% removal of trimethoprim. The degradation efficiency of the Pd/UiO-66(Zr)-2OH system for TMP gradually decreased from 97 to 80% after six cycles. The results of electron paramagnetic resonance combined with classical radical burst experiments revealed the degradation pathways in the reaction system with hydroxyl radicals and singlet oxygen as the main reactive oxygen particles.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Huiwang Dai,Xiaozeng Miao,Jianxi Zhu,Jianxin Chen
The redox cycle of iron is a well-known rate-determining step for hydroxyl radical generation in photo-Fenton system. In this study, oxalate was employed as regulator to enhance the degradation of Orange II in Fe 3 O 4 magnetic nanoparticles (NPs)-catalyzed heterogeneous UV-Fenton system. Results showed that the oxalate could interact with the surface ≡Fe III species of catalyst, which weakened the bond of ≡Fe III –O and promoted the leaching of iron ions. Then the redox cycle of iron and generation of HO· would be accelerated via the homogeneous UV-Fenton reaction. The degradation rate constant of Orange II reached 0.220 min −1 when additional oxalate concentration was 0.4 mM, which was 2.5 times as high as that without oxalate in heterogeneous UV-Fenton system. In this case, the removal efficiencies of color and TOC were 99.3% and 92.0% after 30 and 120 min treatment, respectively. In addition, based on the results of XRD and XPS characterization, it could be deduced that the crystal structure and elemental configuration of Fe 3 O 4 magnetic nanoparticles could be maintained after reaction. Besides, the results of FTIR and magnetization characterization indicated that the C 2 O 4 2− on surface of catalyst could be degraded and the catalyst could be easily separated from aqueous by applying an external magnetic field. The Fe 3 O 4 magnetic nanoparticles showed high catalytic stability and reusability under the regulation of oxalate due to the fact that the leached iron ions could be re-adsorbed on the catalyst after treatment.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Hanjie Zhang,Linghan Li,Na Chen,Haijie Ben,Guangming Zhan,Hongwei Sun,Qin Li,Jie Sun,Lizhi Zhang
Heterogeneous-homogeneous coupled Fenton (HHCF) processes compromise the merits of rapid degradation and catalyst reusability, thus are very attractive for environmental remediation and water treatment. However, the development of HHCF processes suffers from the lack of desirable catalysts and Fe(III)/Fe(II) redox cycle (iron cycle) mediators. Herein we demonstrate the combination of hydrogen peroxide, ferric phosphate and hydroxylamine offers a promising HHCF process, where ferric phosphate and hydroxylamine serve as the catalyst and iron cycle mediator, respectively. Hydroxylamine can realize suitable iron release from ferric phosphate, effective iron cycle, and •OH consumption, resulting in efficient conversion of H 2 O 2 to •OH for sulfamethazine removal. More importantly, the phosphorus release from ferric phosphate and nitrogen residual during this HHCF process are limited to reduce the risk of secondary pollution. This study clarifies the importance of iron dissolution and iron cycle on highly efficient Fenton processes, and also provides a promising antibiotic pollutant removal strategy.
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Sheng-Song Yu,Jie-Jie Chen,Rui-Fen Cheng,Yuan Min,Han-Qing Yu
The biogeochemical cycle of iron is of great importance to living organisms on Earth, and dissimilatory metal-reducing bacteria (DMRB) with the capability of reducing hematite (α-Fe2O3) by outer-membrane (OM) cytochromes play a great role in the iron cycle. However, the dynamic binding of cytochromes to α-Fe2O3 at the molecular level and the resulting impact on the photon-to-electron conversion of α-Fe2O3 for the iron cycle are not fully understood. To address these issues, two-dimensional IR correlation analysis coupled with molecular dynamics (MD) simulations was conducted for an OmcA–Fe2O3 system as OmcA bonds stronger with hematite in a typical DMRB,Shewanella. The photoelectric response of α-Fe2O3 with the OmcA coating was evaluated at three different potentials. Specifically, the binding groups from OmcA to α-Fe2O3 were in the sequence of carboxyl groups, amide II, and amide I. Further MD analysis reveals that both electrostatic interactions and hydrogen bonds played essential roles in the binding process, leading to the structural changes of OmcA to facilitate iron reduction. Moreover, the OmcA coating could store the photogenerated electrons from α-Fe2O3 like a capacitor and utilize the stored electrons for α-Fe2O3 reduction in dark and anoxic environments, further driving the biogeochemical cycle of iron. These investigations give the dynamic information on the OM protein/hematite interaction and provide fundamental insights into the biogeochemical cycle of iron by taking the photon-induced redox chemistry of iron oxide into consideration.
研究领域:
微生物学
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生物地球化学
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环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）