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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第5期   页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction     Fe-N-C     active sites     Fe addition     second heat treatment    

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Sinks of steel in China–addition to in-use stock, export and loss

Hua GUO,Tianzhu ZHANG

《环境科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 141-149 doi: 10.1007/s11783-014-0696-3

摘要： China has become the largest producer of crude steel in the world since 1996, which places the country under huge pressure in terms of resources, energy, and the environment. Examining the driver of steel demand is of great significance to the structural adjustment and sustainable development of the steel industry. The researchers calculate the steel demand in China from 2000 to 2009 based on three sinks (steel stock, export, and loss) by taking the four stages of steel life cycle (production, fabrication and manufacturing, use, and waste management and recycling) as the study object. The researchers conclude that addition to in-use stock is the main driver of steel demand and that the 10-year average addition to in-use stock accounted for 77% of the steel sinks, in which 55% of the addition occurs in the building sector, and the steel for this segment is of low strength with large consumption. Based on the analysis of existing policies, the researchers propose that the steel demand structure will develop toward diversification and that the building sector will realize the upgrade of products as soon as possible to improve construction quality. Under the pressure of rising cost for imported resources, the export ratio of steel products should be controlled appropriately. Thus, recycling economy should be developed to reduce steel losses.

关键词： steel demand     driver     Material Flow Analysis (MFA)     Substance Flow Analysis (SFA)     addition to in-use stock     steel policy    

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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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Effect of short-term atrazine addition on the performance of an anaerobic/anoxic/oxic process

Changyong WU, Xiaoling LI, Zhiqiang CHEN, Yongzhen PENG,

《环境科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 150-156 doi: 10.1007/s11783-010-0020-9

摘要： In this study, an anaerobic/anoxic/oxic (AO) wastewater treatment process was implemented to treat domestic wastewater with short-term atrazine addition. The results provided an evaluation on the effects of an accidental pollution on the operation of a wastewater treatment plant (WWTP) in relation to Chemical Oxygen Demand (COD) and biological nutrient removal. Domestic wastewater with atrazine addition in 3 continuous days was treated when steady biological nutrient removal was achieved in the AO process. The concentrations of atrazine were 15, 10, and 5mg·L on days 1, 2 and 3, respectively. The results showed that atrazine addition did not affect the removal of COD. The specific NH NO reduction rate decreased slightly due to the short-term atrazine addition. However, it did not affect the nitrogen removal due to the high nitrification and denitrification capacity of the system. Total nitrogen (TN) removal was steady, and more than 70% was removed during the period studied. The phosphorus removal rate was not affected by the short-term addition of atrazine under the applied experimental conditions. However, more poly-hydroxy-alkanoate (PHA) was generated and utilized during atrazine addition. The results of the oxygen uptake rate (OUR) showed that the respiration of nitrifiers decreased significantly, while the activity of carbon utilizers had no obvious change with the atrazine addition. Atrazine was not removed with the AO process, even via absorption by the activated sludge in the process of the short-term addition of atrazine.

关键词： biological nutrient removal     atrazine     anaerobic/anoxic/oxic (A2O) process     oxygen demand removal     oxygen uptake rate (OUR)    

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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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Hydration, microstructure and autogenous shrinkage behaviors of cement mortars by addition of superabsorbent

Beibei SUN, Hao WU, Weimin SONG, Zhe LI, Jia YU

《结构与土木工程前沿（英文）》 2020年 第14卷 第5期   页码 1274-1284 doi: 10.1007/s11709-020-0656-x

摘要： Superabsorbent Polymer (SAP) has emerged as a topic of considerable interest in recent years. The present study systematically and quantitively investigated the effect of SAP on hydration, autogenous shrinkage, mechanical properties, and microstructure of cement mortars. Influences of SAP on hydration heat and autogenous shrinkage were studied by utilizing TAM AIR technology and a non-contact autogenous shrinkage test method. Scanning Electron Microscope (SEM) was employed to assess the microstructure evolution. Although SAP decreased the peak rate of hydration heat and retarded the hydration, it significantly increased the cumulative heat, indicating SAP helps promote the hydration. Hydration promotion caused by SAP mainly occurred in the deceleration period and attenuation period. SAP can significantly mitigate the autogenous shrinkage when the content ranged from 0 to 0.5%. Microstructure characteristics showed that pores and gaps were introduced when SAP was added. The microstructure difference caused by SAP contributed to the inferior mechanical behaviors of cement mortars treated by SAP.

关键词： Superabsorbent Polymer     mechanical properties     hydration heat     autogenous shrinkage     microstructure    

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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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Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要： Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

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Mass loss and nutrient dynamics during litter decomposition in response to warming and nitrogen addition

Haiyan REN, Jie QIN, Baolong YAN, Alata, Baoyinhexige, Guodong HAN

《农业科学与工程前沿（英文）》 2018年 第5卷 第1期   页码 64-70 doi: 10.15302/J-FASE-2017194

摘要： Plant litter decomposition has been studied extensively in the context of both warming and increased atmospheric nitrogen deposition. However, the temporal patterns of mass loss and nutrient release in response to warming and nitrogen addition remain unclear. A 2-year decomposition experiment aimed to examine the effects of warming and nitrogen addition on decomposition rate, and nitrogen and phosphorus dynamics. The effects of warming and nitrogen addition on decomposition of litter of , a dominant species in a desert steppe of northern China, were studied. Warming and nitrogen addition significantly enhanced litter mass loss by 10% and 16%, respectively, and moreover promoted nitrogen and phosphorus release from the litter in the first year of decomposition, followed by an immobilization period. The interactive effects of warming and nitrogen addition on mass loss, nitrogen and phosphorus concentrations of litter were also found during the decomposition. This study indicates that warming and nitrogen addition increased litter mass loss through altering litter quality. These findings highlight that interactions between climate change and other global change factors could be highly important in driving decomposition responses.

关键词： climate warming     grassland     litter decomposition     nitrogen deposition     nutrient release    

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Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)

Ehsan Rahmani, Mohammad Rahmani

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1100-1111 doi: 10.1007/s11705-019-1891-3

摘要： A solvothermal method was used to synthesize MIL-101(Fe) and MIL-88(Fe), which were used for alkylation of benzene. The synthesized catalysts were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, field emission scanning electron microscope, dynamic light scattering, and BET techniques. Metal-organic frameworks (MOFs) were modeled to investigate the catalytic performance and existence of mass transfer limitations. Calculated effectiveness factors revealed absence of internal and external mass transfer. Sensitivity analysis revealed best operating conditions over MIL-101 at 120°C and 5 bar and over MIL-88 at 142°C and 9 bar.

关键词： MOFs     alkylation     ethylbenzene     catalysts pellet model     kinetic model     sensitivity analysis    

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Effect of Fe on NO release during char combustion in air and O

Ying GU, Xiaowei LIU, Bo ZHAO, Minghou XU

《能源前沿（英文）》 2012年 第6卷 第2期   页码 200-206 doi: 10.1007/s11708-012-0181-2

摘要： The chemistry of char was probed by studying nitrogen release under the reactions with air and oxy-fuel combustion. The experiments were conducted in a drop tube furnace and a fixed bed flow reactor. NO was observed during those experiments. The results show that the particle size of char generated at 1073 K in CO is larger than that in N . However, at 1573 K, it is smaller in CO atmosphere due to particle breaking by gasification of char and CO . The Fe addition increases the NO conversion ratio, and the effect of Fe rises steeply with the process going until it becomes stable in the end. The results also indicate that the release of NO increases more significantly with the Fe addition in oxy-fuel environment.

关键词： NO     Fe     char     combustion     CO2    

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电沉积Zn-Fe-SiO2复合镀层研究

张英杰,范云鹰,董鹏,罗少林

《中国工程科学》 2008年 第10卷 第3期   页码 93-96

摘要：

报告了电沉积Zn-Fe-SiO2复合镀层的研究结果，论述了电流密度、极间距、搅拌方式、阳极数量及排布方式、添加剂等对Zn-Fe-SiO2复合镀层的影响及试验所取得的技术指标试验结果表明，Zn-Fe-SiO2复合镀层工艺具有过程稳定性好，维护措施简单方便，生产的环保及安全性好等优点。

关键词： 电沉积     复合镀层     Zn-Fe-SiO2    

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Fabrication of recyclable Fe chelated aminated polypropylene fiber for efficient clean-up of phosphate

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 840-852 doi: 10.1007/s11705-022-2253-0

摘要： Herein, a Fe3+-loaded aminated polypropylene fiber has been reported as an efficient phosphate adsorbent. The remarkable phosphate removal ability of the fiber is due to Fe3+ immobilization, and it demonstrates a maximum adsorption capacity of 33.94 mg·P·g–1. Adsorption experiments showed that the fiber is applicable over a wide pH range from 2 to 9. Furthermore, the adsorption kinetics and isotherm data were consistent with the pseudo-second-order and Langmuir adsorption models, respectively. The adsorption equilibrium of the fiber for phosphate was reached within 60 min, indicating an efficient monolayer chemisorption process. Moreover, the adsorbent maintained prominent phosphate removal in the presence of competitive ions such as NO3– and Cl–, exhibiting high selectivity. More importantly, the fiber demonstrated excellent reusability (5 times) and low adsorption limit below 0.02 mg·P·g–1. In addition, the phosphate removal efficiency of the fiber can exceed 99% under continuous flow conditions. The adsorption mechanism was studied by X-ray photoelectron spectroscopy, showing that the adsorption of phosphate on the fiber mainly depended on the chemical adsorption of the modified Fe3+. Overall, this study proves that the fiber possesses many advantages for phosphate removal, including high adsorption efficiency, lower treatment limit, good recyclability, and environmental friendliness.

关键词： phosphate adsorption     aminated polypropylene fiber     Fe3+     ligand exchange     reusability    

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Asymmetric transfer hydrogenation of prochiral ketone catalyzed over Fe-CS/SBA-15 catalyst

XUE Ping, WU Tao

《化学科学与工程前沿（英文）》 2007年 第1卷 第3期   页码 251-255 doi: 10.1007/s11705-007-0045-1

摘要： A heterogeneous chiral catalyst Fe(III)-CS (chitosan) complex/mesoporous molecular sieve SBA-15 (Santa Barbara Amorphous) was prepared. The asymmetric transfer hydrogenations of prochiral acetophenone and 4-methyl-2-pentanone to corresponding chiral alcohols were carried out on Fe-CS/SBA-15 at atmosphere pressure using 2-propanol as hydrogen donor. Effects of Fe content in catalyst, reaction temperature, reaction time and promoter KOH concentration on the conversion of substrates and enantioselectivity were investigated. Fe-CS/SBA-15 with 2.2% mass fraction Fe exhibits considerable enantioselectivity and catalytic activity for the asymmetric transfer hydrogenations of aromatic ketone and aliphatic ketone. Under optimal reaction conditions: KOH concentration 0.03 mol/L, reaction temperature 70ºC and reaction time 4 h, enantiomer excess (ee) of ()-1-phenylethanol and conversion of acetophenone can reach 87.4% and 27.7%, respectively. Under the above KOH concentration and reaction temperature and reaction time of 8 h, the ee of ()-4-methyl-2-pentanol and conversion 4-methyl-2-pentanone amounted to 50.2% and 25.5%, respectively.

关键词： asymmetric transfer     enantioselectivity     Fe-CS/SBA-15     aliphatic     aromatic    

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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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标题 作者 时间 类型 操作

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

Sinks of steel in China–addition to in-use stock, export and loss

Hua GUO,Tianzhu ZHANG

期刊论文

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

期刊论文

Effect of short-term atrazine addition on the performance of an anaerobic/anoxic/oxic process

Changyong WU, Xiaoling LI, Zhiqiang CHEN, Yongzhen PENG,

期刊论文

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

期刊论文

Hydration, microstructure and autogenous shrinkage behaviors of cement mortars by addition of superabsorbent

Beibei SUN, Hao WU, Weimin SONG, Zhe LI, Jia YU

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

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

期刊论文

Mass loss and nutrient dynamics during litter decomposition in response to warming and nitrogen addition

Haiyan REN, Jie QIN, Baolong YAN, Alata, Baoyinhexige, Guodong HAN

期刊论文

Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)

Ehsan Rahmani, Mohammad Rahmani

期刊论文

Effect of Fe on NO release during char combustion in air and O

Ying GU, Xiaowei LIU, Bo ZHAO, Minghou XU

期刊论文

电沉积Zn-Fe-SiO2复合镀层研究

张英杰,范云鹰,董鹏,罗少林

期刊论文

Fabrication of recyclable Fe chelated aminated polypropylene fiber for efficient clean-up of phosphate

期刊论文

Asymmetric transfer hydrogenation of prochiral ketone catalyzed over Fe-CS/SBA-15 catalyst

XUE Ping, WU Tao

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