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

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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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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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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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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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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Downregulation effects of beta-elemene on the levels of plasma endotoxin, serum TNF-alpha, and hepatic

null

《医学前沿（英文）》 2011年 第5卷 第1期   页码 101-105 doi: 10.1007/s11684-011-0111-4

摘要：

It has been demonstrated that β-elemene could protect against carbon tetrachloride (CCl4)-induced liver fibrosis in our laboratory work, and the aim of this paper is to reveal the protective mechanisms of β-elemene. The hepatic fibrosis experimental model was induced by the hypodermical injection of CCl4 in Wistar male rats. β-elemene was intraperitoneally administered into rats for 8 weeks (0.1 mL/100 g bodyweight per day), and plasma endotoxin content was assayed by biochemistry. The serum TNF-α level was detected using radioactive immunity. CD14 expression in rat livers was measured by immunohistochemistry and Western blot. The results showed that β-elemene can downregulate the levels of plasma endotoxins, serum TNF-α, and hepatic CD14 expression in rats with liver fibrosis. β-elemene plays an important role in downregulating the lipopolysaccharide signal transduction pathway, a significant pathway in hepatic fibrosis development.

关键词： liver fibrosis     beta-elemene     endotoxin     CD14    

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Beta-cyclodextrin adsorbents to remove water pollutants—a commentary

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1407-1423 doi: 10.1007/s11705-022-2146-2

摘要： Beta-cyclodextrin-based adsorbent is a promising adsorbent because it has unique characteristics and able to form host-guest complexes with various organic compounds. Adsorption using beta-cyclodextrin-based adsorbent has continuously improved by various preparation strategies and crosslinking agents. This commentary aims to highlight the preparation strategies, properties, and adsorption mechanisms of beta-cyclodextrin-based adsorbents. The adsorbents can be generally classified according to the preparation methods and display high adsorption capacity especially for dyes. Particularly, composite/nanocomposite beta-cyclodextrin-based adsorbents exhibit outstanding adsorption capacity even though the surface area is lower than that of porous and magnetic beta-cyclodextrin-based adsorbents. The beta-cyclodextrin/chitosan functionalized graphene oxide hydrogel with specific surface of 17.6 m2·g–1 yields an extraordinarily maximum adsorption capacity of 1499 mg·g–1 methylene blue, while beta-cyclodextrin/chitosan modified with iron(II, III) oxide nanoparticles displays a much greater maximum adsorption capacity at 2780 mg·g–1. The hydrophobic interaction, functional groups, hydrogen bonding, and electrostatic interaction govern the adsorption to a greater capacity. Although this commentary is not exhaustive, the preparation strategies and illustrated mechanisms provide useful insights into the adsorbent–adsorbate interactions, cost-effective analysis, challenges, and future directions of beta-cyclodextrin-based adsorbents in wastewater treatment.

关键词： beta-cyclodextrin adsorbent     adsorption     inclusion complex     mechanism     water pollutant     wastewater treatment    

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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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The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1366-2

摘要：

•Bacterially-mediated coupled N and Fe processes examined in incubation experiments.

关键词： Denitrification     N2O emission     Fe(II) oxidation     Fe/N ratio     Fe minerals    

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Ni-Bi 助剂用于α-Fe2O3 Letter

党珂,王拓,李澄澄,张冀杰,刘珊珊,巩金龙

《工程（英文）》 2017年 第3卷 第3期   页码 285-289 doi: 10.1016/J.ENG.2017.03.005

摘要：

本文提出了镍-硼酸(Ni-Bi) 助催化剂负载于α 型三氧化二铁(Fe2O3) 具有提升表面动力学和钝化表面态的双重作用Ni-Bi助剂的负载使Fe2O3 光电阳极的光电流起始电位产生230 mV 的负移，1.23 V(vs.

关键词： 镍-硼酸     &alpha     型三氧化二铁     产氧反应     助催化剂    

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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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Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 102-115 doi: 10.1007/s11705-022-2179-6

摘要： High-performance and stable electrocatalysts are vital for the oxygen evolution reaction (OER). Herein, via a one-pot hydrothermal method, Ni/Fe/V ternary layered double hydroxides (NiFeV-LDH) derived from Ni foam are fabricated to work as highly active and durable electrocatalysts for OER. By changing the feeding ratio of Fe and V salts, the prepared ternary hydroxides were optimized. At an Fe:V ratio of 0.5:0.5, NiFeV-LDH exhibits outstanding OER activity superior to that of the binary hydroxides, requiring overpotentials of 269 and 274 mV at 50 mA·cm–2 in the linear sweep voltammetry and sampled current voltammetry measurements, respectively. Importantly, NiFeV-LDH shows extraordinary long-term stability (≥ 75 h) at an extremely high current density of 200 mA·cm–2. In contrast, the binary hydroxides present quick decay at 200 mA·cm–2 or even reduced current densities (150 and 100 mA·cm–2). The outstanding OER performance of NiFeV-LDH benefits from the synergistic effect of V and Fe while doping the third metal into bimetallic hydroxide layers: (a) Fe plays a crucial role as the active site; (b) electron-withdrawing V stabilizes the high valence state of Fe, thus accelerating the OER process; (c) V further offers great stabilization for the formed intermediate of FeOOH, thus achieving superior durability.

关键词： oxygen evolution reaction     electrocatalysts     ternary layered double hydroxides     long-term stability    

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标题 作者 时间 类型 操作

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

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

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

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

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

Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

期刊论文

Downregulation effects of beta-elemene on the levels of plasma endotoxin, serum TNF-alpha, and hepatic

null

期刊论文

Beta-cyclodextrin adsorbents to remove water pollutants—a commentary

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

The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The

期刊论文

Ni-Bi 助剂用于α-Fe2O3

党珂,王拓,李澄澄,张冀杰,刘珊珊,巩金龙

期刊论文

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

期刊论文

Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable

期刊论文