ACS Sustainable Chemistry & Engineering
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2018
·
IF 6.14
Junhui Liu,Anfeng Zhang,Xiao Jiang,Min Liu,Yanwei Sun,Chunshan Song,Xinwen Guo
Conversion of CO2 to sustainable chemical feedstocks and fuels by reacting with renewable hydrogen is considered to be a promising direction in energy research. The selectivity of desired products, such as C2–C4= and C5+, is low over unpromoted iron-based catalysts for CO2 hydrogenation. Therefore, promoters are often used to tailor and optimize the product distribution. In this work, the effect of doping Cu into Fe-based supported catalysts on the catalytic performance for CO2 hydrogenation to hydrocarbons was studied with a particularly focus on the interaction between Fe and Cu. For this purpose, catalysts with different Fe and Cu distribution were prepared by various impregnation methods. It was found that the selectivity of C2–C4= over Cu-promoted catalysts decreased, but a significant improvement was obtained for C5+. This promoting behavior is different from that of other promoters (e.g., K, Mn, Zn, etc.). The secondary conversion of produced olefins on Cu-promoted catalysts, which results from the improvement of olefins adsorption, on Cu-promoted catalysts leads to the decrease of C2–C4= (hydrogenation) but the increase of C5+ (oligomerization). Characterization results demonstrate that the catalytic performance is evidently associated with the strength of the interaction between Fe and Cu in the supported catalysts.
研究领域:
催化化学
·
能源研究
·
化学工程
·
可持续化学
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ACS Omega
·
2022
·
IF 4.132
Liwei Ma,Guoqiang Li,Youqian Wang,Siqi Chai,Guojie Zhang
Fe2+ complexation wet denitrification technology has become a research hotspot. It is very important to achieve efficient regeneration of the absorbent and increase NO absorption in the Fe2+ complexation system. They are the key to the industrial application of the Fe2+ complexation absorption process. In this paper, 2-phosphonate-butane-1,2,4-tricarboxylic acid and ethylenediamine tetraacetic acid were used as ligands to prepare a composite system for the first time. The characteristics of NO removal were investigated under different temperatures, pHs, Fe2+ concentrations, O2 contents, NO concentrations, CO2 contents, and SO2 concentrations. Compared with the single ligand, the results show that the denitrification performance of the solution with a complex ligand is significantly improved. In this system, pH 9, 40 °C temperature, and 20 mmol/L Fe2+ concentration are the economic ideal conditions for NO removal. The system can realize simultaneous removal of NO and SO2, but SO2 in flue gas has a dual effect on the NO removal reaction.
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Chinese Physics B
·
2020
·Vol. 29
·期 12
·127801
·
IF 1.223
Yue Sun,Fenqi Du,Donghang Xie,Dongmei Yang,Yang Jiao,Lichao Jia,Haibo Fan
Iron (Fe) was successfully doped in CuWO4 photoanode films with a combined liquid-phase spin-coating method via the dopant sources of Fe(NO3)3, FeSO4 and FeCl3. The microstructure of the prepared films was characterized by x-ray diffraction, scanning electron microscopy, and atomic force microscopy. The light absorption and photoelectric conversion properties were evaluated by the UV-visible absorption spectra and monochromatic incident photon-to-electron conversion efficiency. The chemical composition and element combination of the samples were examined by x-ray photoelectron spectroscopy. A linear sweep voltammetric and stability test (I–t) were performed with an electrochemical workstation. The results show that the samples are uniform with a thickness of approximately 800 nm and that the photoelectrochemical performance of the doped films is heavily dependent on the Fe source and dopant concentration. Upon optimizing the doping conditions of Fe(NO3)3 and the optimal source, the photocurrent density in the Fe-doped CuWO4 photoanode film is improved by 78% from 0.267 mA/cm2 to 0.476 mA/cm2 at 1.23 V vs reversible hydrogen electrode. The underlying causes are discussed.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Qin He,Yangjie Fu,Xueying Ge,Abdullah M. Al-Enizi,Ayman Nafady,Qi Wang,Shengqian Ma
Novel Fe-BDC/Fe-2MI heterojunction (H 2 BDC: terephthalic acid, 2MI: 2-methylimidazole) was prepared via a one-pot solvothermal method. Herein, mixed ligands (H 2 BDC and 2MI) was applied to form complex with Fe(III). Interestingly, the presence of 2MI can regulate the structure of Fe-BDC. Spindle-like MIL-88B(Fe) was observed in Fe-BDC/Fe-2MI composite, while MIL-53(Fe) was identified in naked Fe-BDC. By employing photoelectrochemical characterizations, Fe-BDC/Fe-2MI was optimized at an initial molar ratio of 1:0.5:10 for Fe(III):H 2 BDC:2MI, which exhibited the highest photocurrent response, lowest charge transfer resistance, and fastest surface reaction kinetics as compared to the individual Fe-BDC and Fe-2MI. Due to the formation of the heterojunction which lead to beneficial photoelectrochemical properties, the as-prepared samples exhibited boosted photocatalytic activity for Cr(VI) reduction. The calculated pseudo-first-order rate constant ( k ) was 0.046 min −1 for Fe-BDC/Fe-2MI, which was 15.3 and 6.6 times that of Fe-BDC (0.003 min −1 ) and Fe-2MI (0.007 min −1 ), respectively. Moreover, the optimized Fe-BDC/Fe-2MI demonstrated superior performance with negligible loss in activity after 4 cyclic runs.
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Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 7
·3988-3994
·
IF 7.443
Xiang Li,Fangyuan Gai,Buyuan Guan,Ye Zhang,Yunling Liu,Qisheng Huo
Fe@C core–shell particles were successfully synthesized by coating Fe2O3 particles with resorcinol–formaldehyde resins (RFs) and then calcining to make the RFs carbonize, and at the same time to reduce the core to Fe. Furthermore, we designed and synthesized Fe@C yolk–shell particles to increase the number of active sites on the Fe surface. Compared with pure Fe material, the Fe in these particles possesses a high surface area without serious aggregation. Tests to remove 4-chlorophenol suggest that both these kinds of particles can degrade chlorophenol rapidly and thoroughly based on a Fenton-like reaction. Using Fe@C yolk–shell particles, the chlorophenol can be degraded to a concentration below the HPLC detection limit (<0.5 mg l−1) within 12 minutes. The magnetic properties and good stability of Fe@C endow it with promising potential for water treatment.
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CATALYSIS COMMUNICATIONS
·
2017
·
IF 3.33
Zhiming Chen,Bo Xu,Xiaomei Wang,Li Zhang,Xiaoqing Yang,Cuncheng Li
Separation and recycling of noble metal nanoparticles after catalytic reaction is critical to promote its application efficiency and cut down the cost. This work presents a facile synthesis strategy for the fabrication of sandwich-like MIL-100(Fe)@Pt@MIL-100(Fe) (denoted as S-Pt) nanoparticles with high stability and improved catalytic activity for hydrogenation of nitrophenol. MIL-100(Fe) acts as both carrier to make the catalyst easily separated and shield to protect the tiny Pt nanoparticles from leaching or aggregation during reaction. Moreover, mass transfer effect of the porous MIL-100(Fe) with its pore structure serving as nano-reactor is also benefit for promoting the catalytic efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ke Lu,Mingyue Xia,Chaojun Chen,Hao Yuan,Jianping Liang,Hongli Wang,Zhi Zheng,Qinghua Liu,Junfeng Gao,Dezheng Yang
Plasma-synergistic catalysis is considered an effective method for degrading aromatic organic pollutants in water. However, the underlying synergistic catalytic mechanism between plasma and catalysts remains poorly understood. Here, we propose a plasma-metal organic frameworks (MOFs) synergistic strategy to investigate the mechanism of plasma-synergistic catalysts for phenol degradation. The results show that Fe-doped Zeolitic Imidazolate Framework-8 (Fe x -ZIF8, x = 0, 0.1, 0.2, 0.4) undergoes the plasma-induced transformation into an Fe-N 3 C structure (P-Fe-N 3 C), leading to a 4.5-fold enhancement in the phenol degradation rate compared to only plasma discharge. Density functional theory (DFT) calculations indicate that the plasma-induced structural transformation of Fe x -ZIF8 promotes the redistribution of point charges and space charges around the Fe center, thereby lowering the activation energy barrier in the rate-determining step (*C 6 H 4 (OH) 2 ). These findings not only provide theoretical support for the degradation of water pollutants via plasma-synergistic catalysts but also offer a novel strategy for constructing MOFs-derived materials.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 4.3
Ruxin Liu,Tao Yu,Xingwang Niu,Jinsheng Li,Xuefei Lei,Zhaobo Wang,Rui Guo
Antibiotic pollution from compounds such as tetracycline hydrochloride (TC-HCl) is a growing concern due to its persistence in the environment and potential to promote antimicrobial resistance. Conventional treatment methods for such wastewater often suffer from low efficiency and high operational costs. In this study, a bimetallic FeMn-BTC material with a two-dimensional sheet-like morphology was synthesized via a facile one-pot ultrasonic method for the efficient degradation of TC-HCl. By precisely selecting the Fe/Mn molar ratio to 7:3, a high density of accessible Fe(II) active sites was achieved. Under visible-light irradiation, FeMn-BTC degraded 92% of high-concentration TC-HCl (100 mg/L) with a reaction rate constant of 0.06703 min −1 , which is 10.5 times higher than that of the monometallic Fe-BTC. This remarkable enhancement is attributed to the incorporation of manganese, which facilitates the Fe(III)/Fe(II) redox cycle and extends the visible-light absorption range. Density functional theory (DFT) calculations further verify that manganese doping lowers both the adsorption and O-O bond cleavage energy barriers of H 2 O 2 . Mechanistic studies identify hydroxyl radicals (·OH) as the primary reactive species, with the synergistic interaction between iron and manganese promoting H 2 O 2 activation and charge-carrier separation. The catalyst also exhibits excellent stability over a wide pH range (3–9) and shows universal degradation activity toward various pollutants (methylene blue, rhodamine B, and malachite green) as well as in real water matrices containing common anions such as Cl − and SO 4 2− . After four consecutive recycling runs, the material retains over 75% of its initial degradation efficiency, outperforming most reported metal–organic framework-based catalysts. This work offers theoretical insights and a practical strategy for designing highly efficient photocatalysts for Fenton-like reactions.
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WATER RESEARCH
·
2023
·
IF 12.8
Yuan Gao,Yun Luo,Zhao Pan,Zhu Zeng,Wenxia Fan,Jingyu Hu,Zhong Zhang,Jinxing Ma,Yang Zhou,Jun Ma
As a widely used feed additives, p-arsanilic acid (p-AsA) frequently detected in the environment poses serious threats to aquatic ecology and water security due to its potential in releasing more toxic inorganic arsenic. In this work, the efficiency of Fe(II)/sulfite, Fe(II)/PDS and Fe(II)/PMS systems in p-AsA degradation and simultaneous arsenic removal was comparatively investigated for the first time. Efficient p-AsA abatement was achieved in theses Fe-based systems, while notable discrepancy in total arsenic removal was observed under identical acidic condition. By using chemical probing method, quenching experiments, isotopically labeled water experiments, p-AsA degradation was ascribed to the combined contribution of high-valent Fe(IV) and SO 4 •− in these Fe(II)-based system. In particular, the relative contribution of Fe(IV) and SO 4 •− in the Fe(II)/sulfite system was highly dependent on the molar ratio of [Fe(II)] and [sulfite]. Negligible arsenic removal was observed in the Fe(II)/sulfite and Fe(II)/PDS systems, while ∼80% arsenic was removed in the Fe(II)/PMS system under identical acidic condition. This interesting phenomenon was due to that ferric precipitation only occurred in the Fe(II)/PMS system. As(V) was further removed via adsorption onto the iron precipitate or the formation of ferric arsenate-sulfate compounds, which was confirmed by particle diameter measurements, fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. Through tuning solution pH, complete removal of total arsenic could achieve in all three systems. Among these three Fe-based technologies, the hybrid oxidation-coagulation Fe(II)/PMS system demonstrated potential superiority for arsenic immobilization by not requiring pH adjustment for coagulation and facilitating the in-situ generation of ferric arsenate-sulfate compounds with comparably low solubility levels like scorodite. These findings would deepen the understanding of these three Fe-based Fenton-like technologies for decontamination in water treatment.
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Catalysis Science & Technology
·
2019
·Vol. 10
·期 5
·1431-1443
·
IF 5.726
Zhaohui Teng,Shan Huang,Liang Fu,Heng Xu,Na Li,Qulan Zhou
In our research, rice husk ash (RHA) was employed as a catalyst support and Fe–Cu bimetallic compounds were employed as catalysts in the reduction of NO by CO. Rice husk ash contains abundant amorphous SiO2 and it would be a good catalyst support as indicated by the characterization results. Different combustion conditions were tested to obtain the appropriate rice husk ash. Characterization methods were employed to study its physical properties. The results of the catalytic activity testing experiment were highly in accordance with the characterization results. Fe2Cu1 based on rice husk ash had approximately 100% conversion rates for both NO and CO, which indicated the superiority of the rice husk ash and Fe–Cu oxides. Moreover, the O2 content, CO/NO ratio and SO2 had little influence on this new combination. This remarkable performance was due to the strong interaction between the rice husk ash and metal species. The results of our research will provide some instructions for the improvement of industrial denitrification.
研究领域:
环境科学
·
催化化学
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Qian Guo,Zuxin Xu,Wenhai Chu,Yingying Zhou,Xiaoting Gao,Cheng Ye
Sewer overflows are a potential source of emerging contaminants to urban waters, posing a threat to ecosystems and human health. Herein, the performance and mechanism of ferrate(Ⅵ) (Fe(Ⅵ))/peroxymonosulfate (PMS), Fe(Ⅵ)/peroxydisulfate (PDS), and Fe(Ⅵ)/percarbonate (SPC) for the degradation of ofloxacin (OFL) in overflows were comparatively investigated. These systems achieved efficient degradation of OFL and the removal of conventional pollutants. Particularly, Fe(Ⅵ)/PMS showed better degradation performance for OFL with a degradation efficiency of 98.8 %. The dominant reactive oxygen species for OFL degradation in the Fe(Ⅵ)/PMS, Fe(Ⅵ)/PDS, Fe(Ⅵ)/SPC systems were singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 · - ), and hydroxyl radical (·OH), respectively. High-valent iron species played an important role in the Fe(Ⅵ)/PMS and Fe(Ⅵ)/PDS systems. Notably, the synergistic effect of oxidation and in-situ coagulation played a key role in OFL degradation, which determined the superior performance of Fe(Ⅵ)/PMS. The formed flocs with Fe-O-P bond acted as a highway to promote the electron transfer from OFL to PMS, resulting in the efficient degradation of OFL in Fe(Ⅵ)/PMS system. Moreover, a same degradation pathway of OFL was found, and the toxicity of the degradation products was reduced, especially in the Fe(Ⅵ)/PMS system. This study provided a new strategy for overflows treatment.
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