Processes
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2022
·Vol. 10
·期 4
·751
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IF 3.352
Zixuan Tang,Zehui Bai,Xin Li,Le Ding,Bin Zhang,Xinghua Chang
Cu-based bimetallic materials have been widely reported as efficient catalysts for electrocatalytic nitrate reduction. However, the faradaic efficiency and selectivity are still far from satisfactory. Herein, Cu-Fe bimetallic nanoalloys with adjustable Cu/Fe ratios are successfully prepared through a reactive mechanical milling approach with CuCl2, FeCl3and Na as the starting materials. The optimized Cu3Fe exhibits excellent nitrate conversion efficiency of 81.1% and 70.3% ammonia selectivity at −0.7 V vs. RHE within 6 h under 0.1 M Na2SO4and 100 ppm NO3−. The Fe-introduction-induced upshift of thed-band center is identified to be beneficial for promoting nitrate adsorption on Cu3Fe. Moreover, favorable H generation under the assistance of Fe could effectively accelerate the stepwise hydrogenation during electrocatalytic nitrate reduction, resulting in significantly improved NH4+selectivity. This work supplies valuable insights for the rational design of transition-metal-based bimetallic catalysts for electrocatalytic nitrate reduction.Keywords:Cu-Fe bimetallic catalysts;nitrate to ammonia;d-band center regulation
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Tianze Cong,Hui Huang,Hao Zhang,Chengwei Li,Yongpeng Zhao,Zeng Fan,Lujun Pan
In the surface-enhanced Raman scattering (SERS) measurements, it is very important to fabricate “hot spots” and concentrate the analytes into these regions. In this work, a hybrid structure of Au nanostars (NSs) with high SERS sensitivity and metal-organic framework MIL-101(Fe) with high molecular adsorption capability was constructed as high performance SERS substrate. The MIL-101(Fe) shell between AuNSs is several nanometers, promoting the construct of “hot spots” and the aggregation of target molecules. The as-prepared AuNS/MIL-101(Fe) has achieved high SERS sensitivity, long-time stability, reproducibility, and capability of universal detections. The limit of detection for rhodamine 6 G is down to 0.29 nM. Meanwhile, the SERS activity of AuNS/MIL-101(Fe) is kept for at least 30 days. Furthermore, the relative standard deviations of signals on five substrates are all less than 10 %. The as-prepared AuNS/MIL-101(Fe) also exhibit the SERS activities for various molecules including dyes, organic contaminants, pesticides, and amino acids , indicating that the AuNS/MIL-101(Fe) substrates have wide applications in chemical analysis and environmental monitoring.
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ChemSusChem
·
2022
·Vol. 15
·期 16
·e202200741
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IF 9.14
Ziyuan Xiu,Ming Zheng,Jiadong Li,Feng Wei,Changchang Dong,Mingrui Zhang,Xin Zhou,Xiaojun Han
Graphical Nitrogen reduction : A bionic nitrogen fixation system composed of Fe-VS 2 nanosheets and 1-aminoanthraquinone-functionalized polymethacrylic acid (1-AAQ-PA) matrix is fabricated with 1-AAQ-PA as the electron medium to achieved high NH 3 yield rate of 31.6 μg h −1 mg −1 and faradaic efficiency to NH 3 of 23.1 % in 0.05 m Li 2 SO 4 electrolyte at −0.35 V vs. reversible hydrogen electrode. This work provides inspiration and insights for the development of effective catalyst systems for nitrogen reduction. Electrochemical N 2 fixation is considered to be a promising alternative to Haber–Bosch technology. Inspired by the composition and structure of natural nitrogenase, Fe-doped VS 2 nanosheets were prepared via one-step solvothermal method. The electron transfer system mediated by organic conductive polymer (1-AAQ-PA) was constructed to promote the electron transfer between Fe-VS 2 nanosheets and the electrode in electrocatalytic N 2 reduction reaction (NRR). The obtained 1-AAQ-PA−Fe-VS 2 electrode converted N 2 to NH 3 with a yield of 31.6 μg h −1 mg −1 at −0.35 V vs. reversible hydrogen electrode and high faradaic efficiency of 23.5 %. The introduction of Fe dopants favored N 2 adsorption and activation, while the Li−S bond between Fe-VS 2 and Li 2 SO 4 effectively inhibited hydrogen evolution. The highly efficient electron utilization in the electrocatalytic NRR process was realized using the 1-AAQ-PA as the electron transfer medium. Density functional theory calculations showed that N 2 was preferentially adsorbed on Fe and reduced to NH 3 via both distal and alternating mechanism.
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ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Yajie Guo,Xinyu Zhang,Dandan Zhang,Shunlin Li,Hui Wang,Yiyin Peng,Zhaoyong Bian
The present work demonstrates a simple one-step pyrolysis method for the synthesis of a catalytic sludge-based carbon (SBC) biochar containing Fe and Mn from dehydrated sludge with added KMnO 4 and Fe(II). The electrocatalytic degradation of triclosan (TCS) in water was evaluated using an Fe/Mn-SBC cathode to promote a heterogeneous Fenton-like reaction. The catalyst generated at 500 °C exhibited an abundant porous structure and a relatively high surface area, and produced an electrode with better conductivity and electron diffusion . The presence of metal oxides changed the surface structure defects of this biochar and enhanced its catalytic performance while increasing the electrochemically active surface area by 72.68 mF/cm 2 compared with plain SBC. TCS was degraded (91.3%) within 180 min by oxygen species generated in situ on an Fe/Mn-SBC cathode because the activation energy for oxygen reduction was lowered by 4.62 kJ/mol. The degradation of TCS followed pseudo first-order kinetics and was controlled by TCS diffusion and interfacial chemical reactions between adsorbed TCS and the electrode. Possible TCS degradation pathways were devised based on the main intermediates, and 1 O 2 was found to be more important than •OH radicals. Through toxicity test and prediction, the toxicity of degradation was gradually reduced. This study demonstrates a simple and ecofriendly method for the electrocatalytic degradation of organic pollutants.
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Journal of Cleaner Production
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2022
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IF 11.072
Da Liu,Wenyi Gu,Wenqi Zhou,Ying Xu,Wenjia He,Lizheng Liu,Liang Zhou,Juying Lei,Jinlong Zhang,Yongdi Liu
The activation of hydrogen peroxide (H 2 O 2 ) by Fe/carbon composites has been widely used for the removal of antibiotics. However, the secondary pollution of iron ions limits the application of Fe 2+ /H 2 O 2 system. In this work, three kinds of hydrogel materials combining metal-organic framework (MOF)-derived magnetic Fe/porous carbon (MagFePC) with sodium alginate (SA), polyacrylic acid (PAA) and agarose (AG) were prepared by different methods for removal of norfloxacin (NOR) antibiotics in simulated wastewater. After comparison, MagFePC/SA hydrogels synthesized by a titration forming method were found to have the advantages of good toughness, abundant pores and best Fenton activity. MagFePC/SA can effectively activate H 2 O 2 to remove NOR under neutral conditions, and there was almost no leaching of iron ions, causing no secondary pollution to the environment. The effects of pH, ionic strength and surfactants on the degradation performance for NOR were studied. Mechanism study revealed that ·O 2 − and 1 O 2 were the main active species for the degradation of NOR, and the materials still had good stability and reusability after repeated cycles. More important, we built a simple automated unit for wastewater treatment under laboratory conditions that can completely degrade a 5 mg/L NOR solution at a flow rate of 2 mL/min. Current works showed that MagFePC/SA had the advantages of simple synthesis, outstanding degradability , excellent stability and eco-friendly reaction, which was a wastewater treatment material with good prospect for industrial application.
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Environmental Science-Nano
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2022
·Vol. 9
·期 9
·3407-3416
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IF 9.473
Han Song,Xinwen Ou,Mengye Wang,Yan Zhang,Zhang Lin
H2 production during the transformation of Fe(OH)2 into magnetite (i.e., Schikorr reaction), has a significant impact on many environmental applications, including the long-term effectiveness of permeable reactive barriers composed of zerovalent iron and the stability of geological radioactive waste repository. However, the reactivity of the Schikorr reaction is not systematically evaluated and its chemical mechanism still remains controversial. Here, we investigate water reduction on the Fe(OH)2 surfaces with the help of an interface-reaction model between water and Fe(OH)2. The Fe(OH)2 hexagonal nanosheets prepared using a coprecipitation method possess dominantly exposed (001) and (100) facets. As unveiled by the DFT simulations, the (001) Fe(OH)2 facet only exposes OH, which is, therefore, inert to water reduction. Moreover, the active Fe-exposed (100) Fe(OH)2 facet is more thermodynamically favourable for water adsorption and dissociation than the (101) and (102) facets. However, the high energy barrier for water dissociation (2.79 eV) may restrict the rate of water reduction on the Fe(OH)2 facet. In addition, the capacity of (100), (101), and (102) Fe(OH)2 facets to adsorb OH− is stronger than that for H2O, which further inhibits water reduction. Furthermore, DOS calculations manifest that Fe d orbitals play a significant role in H2O adsorption, indicating that manipulating the electronic structure of the Fe site is a critical path to mediate water reduction in Fe(OH)2. Our study provides new insights into the understanding of the mechanism of the phase transformation of Fe(OH)2 under anaerobic conditions in environmental and earth sciences.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Hai-Fang Mao,Hong-Qing Fu,Ji-Bo Liu,Yun Zhao
A novel iron-pyridine-based chelate Fe-PYPA was synthesized via a facile and green strategy. The chelate served as a highly efficient catalyst toward CO 2 cycloaddition . A 95.7% PO conversion and a 98.4% PC selectivity were achieved under moderate conditions. Even under solvent-free conditions, Fe-PYPA could achieve a 93.6% conversion and 98.2% selectivity, acting as a robust and efficient catalyst toward CO 2 cycloaddition. Moreover, the as-prepared catalyst showed desirable catalytic activity , good recyclability , remarkable thermo-stability and ideal compatibility to a variety of epoxy substrates. In-situ ATR-IR spectroscopy was used as a powerful tool to gain process understanding for the whole conversion from CO 2 to cyclic carbonate under atmospheric pressure in the presence of TBAI. The process of PO’s ring opening, activation and insertion of CO 2 and the formation of cyclic carbonate were illuminated explicitly through the change of characteristic absorption peaks, providing direct and visual evidence for the mechanism proposed. The present work paves a new way for theoretical and experimental explorations on novel catalyst design and process understanding for highly-efficient greenhouse gas re-utilization.
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Journal of Materials Research and Technology-JMR&T
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2021
·
IF 5.039
Hui Jin,Renjie Ji,Tiancong Dong,Shuo Liu,Fan Zhang,Lilong Zhao,Chi Ma,Baoping Cai,Yonghong Liu
Nickel-iron alloy is broadly utilized in the industrial field due to its fabulous mechanical properties. How to prepare nickel-iron alloy with better corrosion resistance more efficiently is an important concern. Based on this, the WC particles enhanced nickel-iron coatings were fabricated by jet electrodeposition (JED) at a high current density of 100A/dm 2 . It was found that increasing the deposition temperature appropriately during JED is beneficial to obtain Ni-Fe-WC coating with the higher number of hard particles. Specifically, the maximum WC particles proportion reaches 4.47 wt% at 55 °C. The electrochemical corrosion behavior of coating was measured by polarization curve and electrochemical impedance spectroscopy (EIS). The polarization curve test results displayed that the E corr positively shifted from −0.402 to −0.281 V and the i corr reduced from 25.13 to 7.05 μA/cm 2 with the increase of WC particles proportion. Meanwhile, the EIS test results exhibited that the impedance of coating enhanced from 12,720 to 59,140 Ω cm 2 . The neutral salt spray test (NSS) was used to simulate the corrosion of coating in a seawater environment. The NSS results showed that with the increase of WC particles, the corrosion products decreased gradually and the degree of corrosion decreased. The analysis showed that WC particles can help the grain growth and release the internal stress in the coating. Larger grain sizes reduces intergranular corrosion and smaller internal stress help to alleviate stress corrosion cracking. The above research can provide theoretical support for the efficient preparation of particle enhanced composite coating with strong corrosion resistance.
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Molecular Catalysis
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2021
·
IF 5.062
Yu Guan,Yinhe Liu,Qiang Lv,Bo Wang
The selective catalytic reduction of nitrogen oxides (NO x ) by carbon monoxide (CO-SCR) is a promising way to deal with exhaust gasses. And Effective redox cycle and NO dissociation ability are crucial factors for catalytic reduction of NO x . Herein, Fe decorated CeO 2 microsphere catalysts with surface oxygen defect were synthesized by solvothermal and calcination method. Among all catalysts, 0.5Fe-CeO 2 sample showed excellent catalytic performance with efficiency near 96% for NO reduction under the condition of 550 ppmv NO, 1200 ppmv CO, and 40,000 h − 1 of GHSV. It was found that Fe doping could efficiently regulate Ce 4+ /Ce 3+ redox couple and oxygen vacancy for catalytic activity. XRD, Raman, XPS, EPR and H 2 -TPR etc. were employed to explore the physicochemical properties of samples. The results showed that Fe had been incorporated into CeO 2 by XRD, and the results of Raman spectrum and XPS indicated that Ce 4+ /Ce 3+ redox couple existed in 0.5Fe-CeO 2 catalyst. Furthermore, the H 2 -TPR spectrum displayed the formation of oxygen vacancy in the samples. N 2 adsorption-desorption isotherms indicated that the doping of Fe could enlarge the specific surface area, pore volume and pore dimeter of the samples, and thus greatly enhanced the NO adsorption and further NO catalytic reduction on catalysts. In addition, other characterization of physicochemical properties and density functional theory (DFT) calculation were performed to reveal the mechanism of NO + CO reaction. As a result, a mechanism was proposed to elucidate highly efficient NO reduction over the catalysts of Fe decorated CeO 2 microspheres. Finally, the synergistic effects of redox center and oxygen vacancy on catalytic activity enhancement were revealed. This work provides a promising way to the design of efficient catalysts for NO reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Ruihao Tang,Wei Hong,C. Srinivasakannan,Xuelin Liu,Xin Wang,Xinhui Duan
Silica aerogel and Fe doped silica aerogel composite were synthesized by sol–gel method adopting ambient pressure drying method. The crystal structure, surface morphology, pore structure, surface functional groups and elemental composition of silica aerogel prepared with different concentrations of Fe 3+ were characterized by XRD, SEM, TEM, BET, FTIR, XPS and Zeta potential analysis. The specific surface area of the composite aerogel was found to decrease with the increase addition amount of FeCl 3 . The optimal composite aerogel adsorbent had a surface area of 240 m 2 /g with well-developed mesoporous network, which possessed a maximum malachite green(MG) adsorption capacity of 1592 mg/g, as compared to virgin silica aerogel of 1250 mg/g. Adsorption capacity for large molecules like MG is very low for the most popular adsorbent such as high surface area activated carbon, which is usually the first-choice adsorbent for wastewater treatment. Such high adsorption capacitiy of the silica aerogel composite is highly promising as it is on the classification of low-cost adsorbents, which can serve to be far better alternative for waste water treatment applications.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2021
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IF 6.158
Longjie Liu,Qingping Wang,Jiajiang Lin,Gary Owens,Zuliang Chen
Recently, estrogen has attracted widespread concern because it is increasing being detected in wastewater treatment plants. While techniques for estrogen removal have been reported, these have mostly focused on exploring the effect on removal using simple single-factor experiments, rather than applying more complex multifactor mathematical models to wastewater treatment. In this study, reduced graphene oxide-based iron nanoparticles (rGO@Fe NPs) were used for 17α-estradiol (αE 2 ) removal based on adsorption and Fenton oxidation . A response surface methodology , based on a Box-Behnken design, was used to determine the relationships between critical operation factors (pH, temperature, αE 2 concentration, rGO@Fe NPs dose and H 2 O 2 concentration) and removal efficiency to establish the optimal conditions for 1 mg L −1 αE 2 removal. Under the determined optimal reaction condition of pH 6.0, temperature 40 °C, 0.08 g L −1 rGO@Fe NPs dose and 6 mM H 2 O 2 , a maximum removal efficiency of 99.9% was obtained. Subsequently, the presence of co-existing anions (Cl − , SO 4 2− and NO 3 − ) significantly decreased the removal efficiency of αE 2 . However, αE 2 removal from domestic wastewater could be increased by 38.0% when applying RSM results. Moreover, αE 2 removal by rGO@Fe NPs remained stable over five reuse cycles indicating that rGO@Fe NPs would be an efficient and practical advanced materials for αE 2 removal.
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LANGMUIR
·
2021
·
IF 3.882
Shabab Hussain,Xinyi Wan,Zhou Fang,Xinsheng Peng
Separation and purification of surfactant-stabilized oil-in-water nanoemulsions is a great environmental challenge. Membrane-based separation strategies are more effective over conventional methods in the treatment of nanoemulsion waste water. In this paper, we construct a superhydrophilic membrane by coating a thin photothermal-responsive iron tetrakis(4-carboxyphenyl)porphyrin (Fe-TCPP) nanofibrous metal organic framework (MOF) selective layer on a macroporous polyethersulfone membrane. The as-prepared membrane exhibits high separation performance of oil-in-water nanoemulsions with permeance of 46.4 L·m–2·h–1·bar–1 and separation efficiency of 99%. It also demonstrates nice anti-oil/ionic-fouling property, good recyclability, and desirable stability. The high separation performance is accredited to the superhydrophilicity, highly charged surface, and nanometer pore sizes of the Fe-TCPP nanofibrous membrane. Due to the unique photothermal property of Fe-TCPP nanofibers, the permeance can be enhanced more than 50% by visible light without deteriorating the rejection. This photo-stimuli MOF-based thin-layer membrane offers great potential for the generation of point-of-use water treatment devices.
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