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Cadmium removal mechanistic comparison of three Fe-based nanomaterials: Water-chemistry and roles ofFe dissolution

《环境科学与工程前沿（英文）》 2022年 第16卷 第12期 doi: 10.1007/s11783-022-1586-8

摘要：

● nZVI, S-nZVI, and nFeS were systematically compared for Cd(II) removal.

关键词： Nano zero valent iron     Sulfided zero valent iron     FeS     Cd(II) immobilization     Fe dissolution    

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optimization and seismic collapse assessment of shape memory alloy (SMA)-braced frames: Effectiveness of Fe-based

Aydin HASSANZADEH; Saber MORADI

《结构与土木工程前沿（英文）》 2022年 第16卷 第3期   页码 281-301 doi: 10.1007/s11709-022-0807-3

摘要： This paper presents a seismic topology optimization study of steel braced frames with shape memory alloy (SMA) braces. Optimal SMA-braced frames (SMA-BFs) with either Fe-based SMA or NiTi braces are determined in a performance-based seismic design context. The topology optimization is performed on 5- and 10-story SMA-BFs considering the placement, length, and cross-sectional area of SMA bracing members. Geometric, strength, and performance-based design constraints are considered in the optimization. The seismic response and collapse safety of topologically optimal SMA-BFs are assessed according to the FEMA P695 methodology. A comparative study on the optimal SMA-BFs is also presented in terms of total relative cost, collapse capacity, and peak and residual story drift. The results demonstrate that Fe-based SMA-BFs exhibit higher collapse capacity and more uniform distribution of lateral displacement over the frame height while being more cost-effective than NiTi braced frames. In addition to a lower unit price compared to NiTi, Fe-based SMAs reduce SMA material usage. In frames with Fe-based SMA braces, the SMA usage is reduced by up to 80%. The results highlight the need for using SMAs with larger recoverable strains.

关键词： topology optimization     shape memory alloy     Fe-based SMA     steel braced frames     performance-based seismic design     collapse assessment    

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Controllable Fe/HCS catalysts in the Fischer-Tropsch synthesis: Effects of crystallization time

Yifei Wang, Shouying Huang, Xinsheng Teng, Hongyu Wang, Jian Wang, Qiao Zhao, Yue Wang, Xinbin Ma

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 802-812 doi: 10.1007/s11705-019-1866-4

摘要： The Fischer–Tropsch synthesis (FTS) continues to be an attractive alternative for producing a broad range of fuels and chemicals through the conversion of syngas (H and CO), which can be derived from various sources, such as coal, natural gas, and biomass. Among iron carbides, Fe C, as an active phase, has barely been studied due to its thermodynamic instability. Here, we fabricated a series of Fe C embedded in hollow carbon sphere (HCS) catalysts. By varying the crystallization time, the shell thickness of the HCS was manipulated, which significantly influenced the catalytic performance in the FTS. To investigate the relationship between the geometric structure of the HCS and the physic-chemical properties of Fe species, transmission electron microscopy, X-ray diffraction, N physical adsorption, X-ray photoelectron spectroscopy, hydrogen temperature-programmed reduction, Raman spectroscopy, and Mössbauer spectroscopy techniques were employed to characterize the catalysts before and after the reaction. Evidently, a suitable thickness of the carbon layer was beneficial for enhancing the catalytic activity in the FTS due to its high porosity, appropriate electronic environment, and relatively high Fe C content.

关键词： Fischer–Tropsch synthesis     Fe-based catalyst     Fe2C     hollow carbon sphere     crystallization time    

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New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

《能源前沿（英文）》 2021年 第15卷 第2期   页码 421-430 doi: 10.1007/s11708-021-0727-2

摘要： In recent years, Fe-N-C catalyst is particularly attractive due to its high oxygen reduction reaction (ORR) activity and low cost for proton exchange membrane fuel cells (PEMFCs). However, the durability problems still pose challenge to the application of Fe-N-C catalyst. Although considerable work has been done to investigate the degradation mechanisms of Fe-N-C catalyst, most of them are simply focused on the active-site decay, the carbon oxidation, and the demetalation problems. In fact, the 2e pathway in the ORR process of Fe-N-C catalyst would result in the formation of H O , which is proved to be a key degradation source. In this paper, a new insight into the effect of potential on degradation of Fe-N-C catalyst was provided by quantifying the H O intermediate. In this case, stability tests were conducted by the potential-static method in O saturated 0.1 mol/L HClO . During the tests, H O was quantified by rotating ring disk electrode (RRDE). The results show that compared with the loading voltage of 0.4 V, 0.8 V, and 1.0 V, the catalysts being kept at 0.6 V exhibit a highest H O yield. It is found that it is the combined effect of electrochemical oxidation and chemical oxidation (by aggressive radicals like H O /radicals) that triggered the highest H O release rate, with the latter as the major cause.

关键词： proton exchange membrane fuel cells (PEMFCs)     oxygen reduction reaction (ORR)     Fe-N-C catalyst     potential     H2O2     degradation    

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Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive

Chengyuan SU,Weiguang LI,Xingzhe LIU,Xiaofei HUANG,Xiaodan YU

《环境科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 37-45 doi: 10.1007/s11783-014-0729-y

摘要： A study of the decolorization of reactive brilliant blue in an aqueous solution using Fe-Mn-sepiolite as a heterogeneous Fenton-like catalyst has been performed. The Fourier transform infrared (FTIR) spectra of the catalyst showed bending vibrations of the Fe-O. The X-ray diffraction (XRD) patterns of the catalyst showed characteristic diffraction peaks of α-Fe O , γ-Fe O and MnO. A four factor central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables (catalyst addition, hydrogen peroxide dosage, initial pH value and initial dye concentration). When the reaction conditions were catalyst dosage= 0.4 g, [H O ]= 0.3 mL, pH= 2.5, [reactive brilliant blue] = 50 mg·L , and volume of solution= 500 mL at room temperature, the decolorization efficiency of reactive brilliant blue was 91.98% within 60 min. Moreover, the Fe-Mn-sepiolite catalyst had good stability for the degradation of reactive brilliant blue even after six cycles. Leaching of iron ions (<0.4 mg·L ) was observed. The decoloring process was reactive brilliant blue specific via a redox reaction. The benzene ring and naphthalene ring were first oxidized to open ring; these were then oxidized to the alcohol and carboxylic acid. The reactive brilliant blue was decomposed mainly by the attack of ·OH radicals including surface-bound ·OH radicals generated on the catalyst surface.

关键词： Fe-Mn-sepiolite catalyst     heterogeneous Fenton-like     reactive brilliant blue     homogeneous precipitation method     hydroxyl radical    

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Mass Transfer-Promoted Fe2+/Fe3+ Circulation Steered by 3D Flow-Through Co-Catalyst System Toward Sustainable

Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao,

《工程（英文）》 doi: 10.1016/j.eng.2023.06.010

摘要： Realizing fast and continuous generation of reactive oxygen species (ROSs) via iron-based advanced oxidation processes (AOPs) is significant in the environmental and biological fields. However, current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect, giving rise to the sluggish Fe2+/Fe3+ cycle and low dynamic concentration of Fe2+ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with MoS2 to achieve ultra-efficient Fe2+ regeneration (equilibrium Fe2+ ratio of 82.4%) and remarkable stability (more than 20 cycles) via a circulating flow-through process. Unlike the conventional batch-type reactor, experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode, initiated by the convection-enhanced mass/charge transfer for Fe2+ reduction and then strengthened by MoS2-induced flow rotation for sufficient reactant mixing, is crucial for oxidant activation and subsequent ROS generation. Strikingly, the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency. Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology, especially in large-scale complex wastewater treatment.

关键词： Advanced oxidation processes     3D co-catalyst     Flow-through mode     Enhanced mass transfer     Complex wastewater treatment    

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NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要： Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO2 catalyst exhibited exceptional catalytic performance in converting NO to NH3, achieving an NO conversion rate exceeding 80% and an NH3 selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH3 desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词： NO hydrogenation     synthetic ammonia     10Fe-xCu/TiO2     high selectivity    

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ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1322-1

摘要： Abstract • K+ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K+ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NOx in real-world applications.

关键词： Selective catalytic reduction     Cu/SAPO-34 catalyst     Ion-exchanged K     Low-temperature hydrothermal stability     Fe/Beta catalyst    

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Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

《环境科学与工程前沿（英文）》 2019年 第13卷 第2期 doi: 10.1007/s11783-019-1101-z

摘要：

CNTs were incorporated into MIL-88B-Fe to get a new Fenton-like catalyst (C@M).

Fe(II) was introduced in C@M to get a fast initiation of Fenton-like reaction.

Fe(II) content in C@M was related with oxygen-containing functional groups on CNTs.

C@M shows efficient catalytic degradation of pollutants over a wide pH range.

关键词： Heterogeneous Fenton-like catalysts     MIL-88B-Fe     CNTs     Organic pollutants     Mechanism    

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Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 716-725 doi: 10.1007/s11705-022-2265-9

摘要： A Fe2O3−Bi2MoO6 heterojunction was synthesized via a hydrothermal method. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, powder X-ray diffraction, Fourier transform infrared spectroscopy and ultra-violet−visible near-infrared spectrometry were performed to measure the structures, morphologies and optical properties of the as-prepared samples. The various factors that affected the piezocatalytic property of composite catalyst were studied. The highest rhodamine B degradation rate of 96.6% was attained on the 3% Fe2O3−Bi2MoO6 composite catalyst under 60 min of ultrasonic vibration. The good piezocatalytic activity was ascribed to the formation of a hierarchical flower-shaped microsphere structure and the heterostructure between Fe2O3 and Bi2MoO6, which effectively separated the ultrasound-induced electron–hole pairs and suppressed their recombination. Furthermore, a potential piezoelectric catalytic dye degradation mechanism of the Fe2O3−Bi2MoO6 catalyst was proposed based on the band potential and quenching effect of radical scavengers. The results demonstrated the potential of using Fe2O3−Bi2MoO6 nanocomposites in piezocatalytic applications.

关键词： piezocatalysis     Fe2O3−Bi2MoO6     dye decomposition     ultrasonic vibration    

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Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1337-7

摘要：

• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst.

关键词： NOx     Selective catalytic reduction     Iron-based catalyst     Red mud     Monolithic catalyst     Activated carbon    

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Research Trends in Fischer--Tropsch Catalysis for Coal to Liquids Technology

Emiel J. M. Hensen,Peng Wang,Wayne Xu

《工程管理前沿（英文）》 2016年 第3卷 第4期   页码 321-330 doi: 10.15302/J-FEM-2016051

摘要： Fischer–Tropsch Synthesis (FTS) constitutes catalytic technology that converts synthesis gas to synthetic liquid fuels and chemicals. While synthesis gas can be obtained from any carbonaceous feedstock, current industrial FTS operations are almost exclusively based on natural gas. Due to the energy structure of China where cheap coal is abundant, coal to liquids (CTL) technology involving coal gasification, FTS and syncrude upgrading is increasingly being considered as a viable option to convert coal to clean transportation fuels. In this brief paper, we review some pertinent issues about Fe- and Co-based FTS catalysts. Fe is better suited to convert synthesis gas derived from coal gasification into fuels. The authors limit themselves to noting some important trends in the research on Fe-based catalysts. They focus on the preparation of phase-pure carbides and innovative cheap synthesis methods for obtaining active and stable catalysts. These approaches should be augmented by (1) computational investigations that are increasingly able to predict not only mechanism, reaction rates and selectivity but also optimum catalyst composition, as well as (2) characterization of the catalytic materials under conditions close to the operation in real reactors.

关键词： Fischer–Tropsch     FTS     CTL     Fe catalyst     iron carbide     computational modeling    

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Effect of glow discharge plasma on rhodium-based catalyst for oxygenates synthesis

HUANG Lihong, CHU Wei, XU Junqiang, HONG Jingping, YI Min

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 16-19 doi: 10.1007/s11705-007-0004-x

摘要： Rhodium-based catalysts were prepared by impregnation, treated with glow discharge plasma, characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, H2 temperature-programmed desorption and CO temperature-programmed desorption, and investigated for oxygenate synthesis from CO hydrogenation. Based on the characterization results, plasma treatment endowed the samples with smaller particle size, higher dispersion of active components, and an enrichment of active components on the surface as well. As a result, the reducibility and adsorption properties were modified. In catalytic tests, the catalytic activity for CO hydrogenation over the samples treated by plasma was improved remarkably: the conversion of CO and the yield of oxygenates increased at most by a factor of 78.62% and 51.96%, respectively, while the selectivity of ethanol and methanol in the oxygenates was enhanced as well.
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Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 930-941 doi: 10.1007/s11705-023-2309-9

摘要： Membrane technology for wastewater remediation has aroused wide interest owing to its unique properties and potential applications. However, it remains challenging to explore green, efficient and robust membrane material and technique for complex wastewater treatment. Herein, we proposed using a simple electrospinning and in situ seeding method to fabricate a lignin-based electrospun nanofiber membrane (LENM) decorated with photo-Fenton Ag@MIL-100(Fe) heterojunctions for efficient separation of oil/water emulsions and degradation of organic dye. Thanks to the embedded lignin in LENM, an ultrahigh MIL-100(Fe) loading (53 wt %) with good wettability and high porosity was obtained. As a result, the hybrid Ag@MIL-100(Fe)/LENM exhibited excellent oil/water emulsions separation efficiency (more than 97%) without a compromise of water flux. Moreover, the hybrid membrane showed an excellent dye removal with degradation of 99% methylene blue within 30 min under illumination, which is attributed to a synergy of dye adsorption/enrichment and photo-Fenton catalytic degradation from Ag@MIL-100(Fe). Therefore, the lignin-based photo-Fenton hybrid membrane can lay the foundation for the preparation and application of green, sustainable and versatile membrane materials and technologies for efficient complex wastewater remediation.

关键词： lignin     electrospinning     heterojunctions     photo-Fenton catalysis     wastewater remediation    

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Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

《能源前沿（英文）》 2023年 第17卷 第1期   页码 123-133 doi: 10.1007/s11708-022-0849-1

摘要： High cost has undoubtedly become the biggest obstacle to the commercialization of proton exchange membrane fuel cells (PEMFCs), in which Pt-based catalysts employed in the cathodic catalyst layer (CCL) account for the major portion of the cost. Although non-precious metal catalysts (NPMCs) show appreciable activity and stability in the oxygen reduction reaction (ORR), the performance of fuel cells based on NPMCs remains unsatisfactory compared to those using Pt-based CCL. Therefore, most studies on NPMC-based fuel cells focus on developing highly active catalysts rather than facilitating oxygen transport. In this work, the oxygen transport behavior in CCLs based on highly active Fe-N-C catalysts is comprehensively explored through the elaborate design of two types of membrane electrode structures, one containing low-Pt-based CCL and NPMC-based dummy catalyst layer (DCL) and the other containing only the NPMC-based CCL. Using Zn-N-C based DCLs of different thickness, the bulk oxygen transport resistance at the unit thickness in NPMC-based CCL was quantified via the limiting current method combined with linear fitting analysis. Then, the local and bulk resistances in NPMC-based CCLs were quantified via the limiting current method and scanning electron microscopy, respectively. Results show that the ratios of local and bulk oxygen transport resistances in NPMC-based CCL are 80% and 20%, respectively, and that an enhancement of local oxygen transport is critical to greatly improve the performance of NPMC-based PEMFCs. Furthermore, the activity of active sites per unit in NPMC-based CCLs was determined to be lower than that in the Pt-based CCL, thus explaining worse cell performance of NPMC-based membrane electrode assemblys (MEAs). It is believed that the development of NPMC-based PEMFCs should proceed not only through the design of catalysts with higher activity but also through the improvement of oxygen transport in the CCL.

关键词： proton exchange membrane fuel cells (PEMFCs)     non-precious metal catalyst (NPMC)     cathode catalyst layer (CCL)     local and bulk oxygen transport resistance    

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标题 作者 时间 类型 操作

Cadmium removal mechanistic comparison of three Fe-based nanomaterials: Water-chemistry and roles ofFe dissolution

期刊论文

optimization and seismic collapse assessment of shape memory alloy (SMA)-braced frames: Effectiveness of Fe-based

Aydin HASSANZADEH; Saber MORADI

期刊论文

Controllable Fe/HCS catalysts in the Fischer-Tropsch synthesis: Effects of crystallization time

Yifei Wang, Shouying Huang, Xinsheng Teng, Hongyu Wang, Jian Wang, Qiao Zhao, Yue Wang, Xinbin Ma

期刊论文

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

期刊论文

Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive

Chengyuan SU,Weiguang LI,Xingzhe LIU,Xiaofei HUANG,Xiaodan YU

期刊论文

Mass Transfer-Promoted Fe2+/Fe3+ Circulation Steered by 3D Flow-Through Co-Catalyst System Toward Sustainable

Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao,

期刊论文

NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

期刊论文

ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

期刊论文

Carbon nanotubes-incorporated MIL-88B-Fe as highly efficient Fenton-like catalyst for degradation of

Hang Zhang, Shuo Chen, Haiguang Zhang, Xinfei Fan, Cong Gao, Hongtao Yu, Xie Quan

期刊论文

Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

期刊论文

Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst

期刊论文

Research Trends in Fischer--Tropsch Catalysis for Coal to Liquids Technology

Emiel J. M. Hensen,Peng Wang,Wayne Xu

期刊论文

Effect of glow discharge plasma on rhodium-based catalyst for oxygenates synthesis

HUANG Lihong, CHU Wei, XU Junqiang, HONG Jingping, YI Min

期刊论文

Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

期刊论文

Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

期刊论文