CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haiyang Xie,Dan Tang,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Hongbing Ji,Tao Gan
The design of non-noble metal single-atom catalysts (SACs) with superior performance for semi-hydrogenation of alkynol to alkenol is remarkable but challenging. Herein, fluorine-tuned Fe SACs supported on N, F-codoped carbon (Fe 1 -NFC) with a Fe-N 4 F 1 structure is successfully prepared via a complexation method. The axial F-doping can modulate the electronic structure of the metalloporphyrin-like active sites (Fe-N 4 ), promoting the transfer of electrons from Fe atoms to F atoms to form electron-deficient Fe δ+ species. As a result, the Fe 1 -NFC catalyst shows a remarkable activity for the semi-hydrogenation of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol under mild conditions, with a TOF of 9163 h −1 and a selectivity of 96 % at 97 % conversion, both much higher than that of the Fe SACs supported on N-doped carbon (Fe 1 -NC). Density functional theory (DFT) calculations reveal that the excellent catalytic activity is attributed to the interfacial electronic effect of Fe species induced by axial F-doping, thereby enhancing the exothermic adsorption of alkynol on the Fe-N 4 F 1 structures and accelerating the desorption of alkenol to against the overhydrogenation.
研究领域:
催化
·
材料科学
·
化学工程
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hao Xu,Qian Ye,Jing Zhang,Qiansong Li,Meijing Wang,Peng Zhou,Guanyu Zhou,Qingguo Wang
In response to the inherent restriction of low Fe(II) regeneration in the Fenton process, this study demonstrated a mutual-promoting configuration, where oxygen functionalized g-C 3 N 4 (OCN) was applied in Fe(III)/H 2 O 2 system to utilize mild natural solar light (SL) for persistent Fe(II) generation. The constructed OCN/Fe(III)/H 2 O 2 /SL system exhibited strong adaptability to various pollutants, and it well outperformed the g-C 3 N 4 (GCN) modified system and the traditional Fenton system in pollutants degradation efficiency. Compared with GCN, OCN could significantly promote the Fe(II) generation under solar light (SL), leading to more efficient H 2 O 2 activation. The characterization analyses revealed the larger surface area and enhanced charge separation of OCN, which were considered to take main responsibility for its enhanced photoactivity. The complexation of Fe(III) with the carboxyl groups of OCN also benefited the Fe(II) generation. ·OH was detected as the dominant radical responsible for metronidazole (MNZ) degradation, and its production in the OCN modified system was about twice that in the GCN modified system and the Fenton system. Moreover, the precipitation of FeO x on the OCN surface benefited the charge separation of the OCN, so that the improved OCN enabled a slight enhancement of MNZ degradation in the reuse experiments. The intermediates of MNZ degradation were analyzed based on the results of LC-MS, which provided insight into MNZ degradation pathways. This work highlighted the concept of self-improving photocatalyst, the ingenious combination of photocatalysis and Fenton-like system formed a mutual-promoting situation where the OCN and the Fenton-like system could both be improved, which endowed the configuration great potential for green and economical oxidation in environmental remediation.
研究领域:
环境科学
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光催化
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水处理
·
高级氧化过程
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
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
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Fei Miao,Zehao Liu,Xin Kang,Cheng Cheng,Xiaoyu Mao,Ruimeng Li,Heng Lin,Hui Zhang
Heterogeneous catalytic oxidation based on iron species for peroxymonosulfate (PMS) activation is considered as one of the most attractive strategies for wastewater treatment. However, the rate-limiting regeneration of Fe(II) from Fe(III) heavily hampers the efficient activation of PMS. In this study, the introduction of electric field to the Fe-supported bentonite (Fe-B) activated PMS process was proposed to enhance the Fe(III)/Fe(II) redox cycle. The Fe-B catalyst performed well in the removal of Acid Orange 7 (AO7) through the synergistic effect of electrolysis and the continuous redox cycle of Fe(III)/Fe(II) for PMS activation. The use of 0.5 g L −1 Fe-B catalyst and 10 mM PMS yielded nearly complete removal of the AO7 (50 mg L −1 ) in 60 min at 2 mA cm −2 of current density. Based on the results of electron paramagnetic resonance (EPR) spectroscopy, chemical quenching tests, X-ray photoelectron spectroscopy (XPS) analysis, and electrochemical measurements, the decolorization of AO7 was dominantly attributed to surface-bound radicals (SO 4 •− ads and • OH ads ) and also the direct electron transfer at DSA anode. Moreover, the electro/Fe-B/PMS system showed an effective pH range from 2.6 to 9.0 and the abatement of AO7 was slightly affected in the presence of natural background anions. This work provides a feasible strategy of PMS activation by cost-effective Fe-B catalyst coupling with electric field and gives an insight into the accelerated oxidation of recalcitrant pollutants.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Ruobai Li,Zhiming Chen,Meixuan Cai,Jiaxing Huang,Ping Chen,Guoguang Liu,Wenying Lv
Metal-organic frameworks (MOFs) have attracted tremendous interest as photocatalysis for the destruction of organic contaminants. Herein, we synthesize a Fe-based MOF namely MIL-53(Fe), combined with Fe(III) and percarbonate, exhibits photocatalytic activity for the destruction of Sulfamethazine (SMT) under visible LED light irradiation. The morphology and physicochemical properties of the MIL-53(Fe) were determined using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectra (EDS), Fourier transform infrared spectroscopy (FTIR) and photoluminescence spectroscopy (PL). The results indicated that the photocatalytic performance of MIL-53(Fe) with unsatisfactory efficiency resulted from the rapid recombination of photogenerated electrons and holes. This may be suppressed through the introduction of an external electron acceptor (e.g., Fe(III) and percarbonate) to the catalytic process. It could be seen that the SMT degradation efficiency in the system of Vis/MIL-53(Fe)/Fe(III)/SPC attained nearly 90% within 60 min, while only 12% achieved in the system of Vis/MIL-53(Fe). The quenching experiments and EPR analysis were employed to illuminate the predominant reactive species in the system of Vis/MIL-53(Fe)/Fe(III)/SPC. It must be mentioned that the higher separation efficiency of photoinduced electron- hole pairs was achieved via the addition of Fe(III). The accelerated photocatalytic degradation of SMT could be attributed to the subsequent formation of reactive species, which were generated from the activation of SPS by Fe(II) reduced from Fe(III) in the Vis/MIL-53(Fe)/Fe(III)/SPC system. Furthermore, the mineralization of SMT was systematically investigated, as well as the effects of operating parameters (e.g., the dose of catalyst, the concentration of Fe(III), and pH). The work has expanded the possibility of MOFs as visible light responsive photocatalysts together with percarbonate for the remediation of contaminated water.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Kunjie Hou,Zhoujie Pi,Fei Chen,Li He,Fubing Yao,Shengjie Chen,Xiaoming Li,Haoran Dong,Qi Yang
The practical application of the traditional Fenton system (Fe(II)/H2O2) is seriously hampered by the sluggish Fe(III)/Fe(II) cycle and the stringent acidic reaction condition. In this work, we found that trace-dissolved S(-II) (DS(-II), 5 μM) could significantly accelerate the Fe(III)/Fe(II) cycle and trigger a rapid H2O2 activation process in the Fe(III)/H2O2 system. Thus, more hydroxyl radicals (·OH) were generated for the rapid removal of various organic pollutants such as bisphenol A (BPA) and sulfamethoxazole (SMX) from water. Besides, the additive DS(-II) effectively broadened the application pH range of the Fenton or Fenton-like system. The constructed Fe(III)/DS(-II)/H2O2 system showed extensive applicability to different water matrices and maintained high BPA removal in the actual water sources. Furthermore, the toxicity assessment revealed that the toxicity of the target contaminant was diminished. The harmless SO42– was the final product of DS(-II) in the Fe(III)/DS(-II)/H2O2 system, and the residual DS(-II) was less than the threshold limit value for fresh or saltwater (0.5 mg/L). This discovery is expected to promote the large-scale practical application of iron-based Fenton or Fenton-like systems in practical organic wastewater purification.
研究领域:
环境科学
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水处理
·
污染控制
✓ 已验证
DOI
Journal of Environmental Sciences
·
2023
·
IF 6.9
Ting He,Jie Sun,Liangwei Deng,Jialin Ming,Changwei Hu
Due to its high efficiency, Fe(II)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants. A lot of chemical Fe sludge along with various refractory pollutants was concomitantly produced, which may cause secondary environmental problems without proper disposal. We here innovatively proposed an effective method of achieving zero Fe sludge, reusing Fe resources (Fe recovery = 100%) and advancing organics removal (final TOC removal > 70%) simultaneously, based on the in situ formation of magnetic Ca-Fe layered double hydroxide (Fe 3 O 4 @CaFe-LDH) nano-material. Cations (Ca 2+ and Fe 3+ ) concentration (≥ 30 mmol/L) and their molar ratio (Ca:Fe ≥ 1.75) were crucial to the success of the method. Extrinsic nano Fe 3 O 4 was designed to be involved in the Fe(II)-catalytic wastewater treatment process, and was modified by oxidation intermediates/products (especially those with COO − structure), which promoted the co-precipitation of Ca 2+ (originated from Ca(OH) 2 added after oxidation process) and by-produced Fe 3+ cations on its surface to in situ generate core-shell Fe 3 O 4 @CaFe-LDH. The oxidation products were further removed during Fe 3 O 4 @CaFe-LDH material formation via intercalation and adsorption. This method was applicable to many kinds of organic wastewater, such as bisphenol A, methyl orange, humics, and biogas slurry. The prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported CaFe-LDHs. This work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(II)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.
研究领域:
环境工程
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废水处理
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 73
·46215-46220
·
IF 3.108
Youzhi Wang,Yurun Feng,Xue Guo,Yu Liu,Hongyu Gong
Fe-doped polymer-derived SiCN ceramics were synthesized by a precursor conversion method with different contents of nano-Fe2O3. The phase composition and microstructure were characterized by XRD, SEM and TEM. The results revealed that α-Fe and graphite phases were generated during the synthetic process. The electromagnetic and wave absorbing properties of the Fe-doped SiCN ceramics were analyzed with different amounts of nano-F2O3 over the frequency range of 2–18 GHz. The existence of α-Fe and graphite phases improved the electromagnetic properties of the materials greatly. The reflectance and electromagnetic attenuation coefficient of Fe-doped SiCN ceramics (15 wt% F2O3) reached −11 dB and 325 at 10.5 GHz, respectively, which indicated that the Fe-doped SiCN ceramics possessed excellent absorbing properties.
研究领域:
材料科学
·
电磁学
✓ 已验证
DOI
高影响因子
Energy Advances
·
2024
·
IF 3.2
Kunpeng Liu,Xu Wang,Nan Wang,Ruiyong Zhang,Meinan Yang,Baorong Hou,Wolfgang Sand
Rationally designing high-efficiency catalysts for electrochemical two-electron water oxidation reaction (2e− WOR) to produce hydrogen peroxide (H2O2) is extremely important, while designing bimetallic metal–organic frameworks (MOFs) is of great significance for effective 2e− WOR. Herein, MIL-53(Fe) and different proportions of Co-doped MIL-53(Fe) were prepared by a hydrothermal method. The structural characterization and elemental analysis showed that the Co ions were successfully doped into MIL-53(Fe) to form a MIL-53(Fe/Co) bimetallic MOF, and the morphology of MIL-53(Fe/Co) became more regular after Co doping. We found that the optimized MIL-53(Fe/Co) exhibits remarkable 2e− WOR performance, which gave an overpotential of 150 mV at 1 mA cm−2. The overpotential of MIL-53(Fe/Co) was approximately 220 mV (at 1 mA cm−2) lower than that of MIL-53(Fe), which may be attributed to the change of microstructure of MIL-53(Fe) after Co doping and the synergistic effect between Fe/Co. Our work introduces a strategy for designing bimetallic MOF-based electrocatalysts, opening up new possibilities for efficient 2e− WOR systems.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Yiyang Lin,Tao Lin,Han Chen,Junding Yin
The effect of N , N -bis(carboxymethyl)glutamic acid (GLDA) on the removal of organic pollutants by Fe(II)-mediated periodate (PI) advanced oxidation process at neutral pH was investigated, in which N-(1,3-dimethylbutyl)- N ′-phenyl- p -phenylenediamine quinone (6PPD-Q) was used as the model pollutant. The results showed that the Fe(II)-GLDA complex formed by mixing GLDA with Fe(II) in a 1:1 ratio reacted with PI can degrade 6PPD-Q effectively. The presence of GLDA alters the redox potential of Fe(II)/Fe(III), which allows for a better utilization of Fe(II) under the synergistic effect of ultraviolet (UV) irradiation. Based on quenching experiments, sulfoxide probe transformation and electron spin resonance (ESR) signals, the reactive species that play a major role in this process are Fe IV O and IO 3 . The degradation products of 6PPD-Q were detected by Ultra Performance Liquid Chromatography-Tandem Mass Spectrometry (UPLC-MS/MS) and two possible degradation pathways were proposed based on density functional theory (DFT) calculations. The toxicity of 6PPD-Q was found to be effectively reduced after degradation by Ecological Structure Activity Relationships (ECOSAR) software analysis and zebrafish experiments. This study provides some fundamental insights for the removal of organic pollutants by GLDA-enhanced Fe(II)/PI system under neutral conditions.
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Huihui Liu,Jiaying Yan,Yanlin Wu,Caixia Yan,Minghua Nie,Wenbo Dong
Sinapic acid (SA) as an environmentally friendly natural phenolic acid, has the properties of antioxidant because of containing –OH and –OCH 3 on the benzene ring and it is safe. The Fe(III)/peroxymonosulfate (PMS) system modified by SA for enhancing micropollutant degradation had been studied, while weather SA could improve micropollutant degradation in other Fe(III)/oxidants systems was still unclear. The Fe(III)/hydrogen peroxide (H 2 O 2 ) and Fe(III)/peroxydisulfate (PDS) systems modified by SA for micropollutants degradation were studied, the results indicated that SA could enhancing micropollutants degradation by accelerating the Fe(III)/Fe(II) cycle in both systems. In addition, the PMS, the H 2 O 2 and the PDS systems were compared, and ten micropollutants commonly present in natural water were selected to evaluate the oxidation capacity of different systems. The PMS and PDS systems have higher oxidation degradation capacity for ten micropollutants than that of H 2 O 2 system, attributed to the SO 4 •− , HO • and Fe(IV) all contributing to micropollutants degradation. However, in the H 2 O 2 system, ten micropollutants degradation almost entirely relied on HO • . In the PMS and PDS systems, the SO 4 •− played a dominated role for micropollutants removal, attributed to its higher steady-state concentration than HO • and its higher second-order reaction rate with micropollutants than Fe(IV). Economic evaluation indicted that the H 2 O 2 system was more cost-effective than the PMS and PDS systems for micropollutants removal. This was because the cost of H 2 O 2 was lower than PMS and PDS, and concentration of Fe(III), oxidants and SA requirements in the H 2 O 2 system were lower than that in the PMS and PDS systems. Overall, this study provided an economical and environmental-friendly method for the efficient treatment of harmful micropollutants in wastewater.
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
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Bin Nie,Haojun Dong,Jincan Yan,Shengyu Zhang,Shuang Zhong
The activation of peroxymonosulfate (PMS) by heterogeneous catalysts presents an exciting but challenging strategy for degrading persistent organic pollutants in water. Iron oxychloride (FeOCl) is considered a promising heterogeneous catalyst due to its unique oxygen bridge structure, which could render it more active by facilitating the iron valence transitions between Fe(II) and Fe(III). However, the limited Fe(II)/Fe(III) conversion cycle rate hinders its catalytic activity, leading to unsatisfactory PMS activations in practical applications. Herein, we demonstrated the performance and the mechanistic pathway of enhanced FeOCl (CNFeOCl) catalytic activation using a graphitic carbon nitride (g-C 3 N 4 ) with a unique electronic structure as a carrier employing 2,4-dichlorophenol (2,4-DCP) as a representative pollutant. The CNFeOCl/PMS system achieved complete degradation of 2,4-DCP (30 mg/L) in a short time (<5 min), whereas the FeOCl/PMS system degraded only 35.98% under the same conditions. The high 2,4-DCP degradation rate of CNFeOCl was due to its improved Fe(II)/Fe(III) ratio (34.34%/40.03%), increased specific surface area (30.32 m 2 /g), and reduced charge-transfer resistance. Combining a series of characterizations, electron spin resonance (ESR) detection, and quenching experiments, the investigations elucidated the enhanced catalytic activation mechanism of CNFeOCl which includes dominant reactive oxygen species (ROS) generation and some key factors that generally affected the efficiency of oxidative degradation. We believe this study offers new insights into the intrinsic role of g-C 3 N 4 supported FeOCl for PMS activation and provides theoretical support to guide the rational design for developing efficient iron-based catalysts toward heterogeneous catalysis.
研究领域:
环境科学
·
催化化学
✓ 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）