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Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要： Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词： metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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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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Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 613-623 doi: 10.1007/s11705-017-1664-9

摘要： Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

关键词： methanation     layered double hydroxide     bimetal Ni-Fe alloy     sintering     carbon deposition    

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Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 24-31 doi: 10.1007/s11705-017-1669-4

摘要： We have successfully prepared a series of Pd-Ni/TiO catalysts by a one-step impregnation-reduction method. Among these catalysts with different compositions of Ni and Pd, the one with the Ni:Pd ratio of 2.95 showed the best activity. Small monodispersed Pd-Ni bimetallic nanoparticles were loaded on the surface of titanium oxide nanopowder as confirmed with TEM and EDS mapping. The XPS analysis demonstrated that Pd exists as 31% Pd(II) species and 69% Pd(0) species and all nickel is Ni(II). The prepared Pd-Ni/TiO exhibited enhanced catalytic activity compared to an equal amount of Pd/TiO for Suzuki-Miyaura reactions together with excellent applicability and reusability.

关键词： Pd-Ni bimetallic nanoparticles     nanocatalysis     Suzuki-Miyaura reaction     titanium oxide    

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Dechlorination of dichlorodiphenyltrichloroethane (DDT) by Fe/Pd bimetallic nanoparticles: Comparison

Kubra Ulucan-Altuntas, Eyup Debik

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1196-2

摘要： DDT undergoes dechlorination via Fe/Pd bimetallic nanoparticle. The oxidation effect of nZVI on DDT is greatly improved when Pd is dopped. The highest concentration to be treated under cancerogenesis limit was 110 mg/L. The dechlorination of DDT is more like to DDE via Fe/Pd but to DDD via nZVI. Degradation products concentrations are lowered via Fe/Pd when compared with nZVI. In this study, the bimetallic Fe/Pd nanoparticle was synthesized using the catalytic element palladium to increase the effect of nano zero valent iron (nZVI), in the light of the information obtained from our previous study, in which the nZVI synthesis method was modified. Dichlorodiphenyltrichloroethane (DDT), one of the most widely used persistent organic pollutant pesticides in the world, was investigated in terms of its degradation by Fe/Pd nanoparticles and the difference with nZVI was determined. During the study, the Fe/Pd concentration, initial DDT concentration, and contact time were selected as variables affecting the treatment. The highest possible initial DDT concentration for the treatment with Fe/Pd bimetallic nanoparticle was investigated to obtain the DDT effluent concentration below the carcinogenesis limit, 0.23 µg/L. The highest concentration that could be treated was found to be 109.95 mg/L with Fe/Pd. It was found that 44.3 min of contact time and 550 mg/L Fe/Pd concentration were needed to achieve this treatment.

关键词： Persistent organic pollutants     nZVI     Bimetallic nanoparticle     Organochlorine pesticides     DDT    

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The kinetic study of light alkene syntheses by CO 2 hydrogenation over Fe-Ni catalysts

Yaling ZHAO, Li WANG, Xiwei HAO, Jiazhou WU,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 153-162 doi: 10.1007/s11705-009-0241-2

摘要： A kinetics model of CO hydrogenation over iron-nickel catalysts was developed based on the detailed mechanism of alkenes re-adsorption and secondary reaction. The corresponding kinetical experiments are conducted in a continuous fixed bed reactor. The effect of reaction conditions on catalyst performance was analyzed according to the results of orthogonal experiments. The results of the experiments show that more methane in products can be obtained with iron-nickel catalysts, the trend of which is consistent with the thermodynamic analysis. However, the content of alkenes in products is equivalent with that of alkanes. This shows that the reaction is controlled by kinetics. In all, the results of the experiments also substantiate that the model can give a good representation of the reaction mechanism of CO hydrogenation over iron-nickel catalysts. The parameters of this model give a better explanation for the question why the iron-nickel catalysts have a higher selectivity toward alkenes compared with other iron-based catalysts.

关键词： representation     corresponding     orthogonal     thermodynamic     consistent    

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Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1519-6

摘要：

• 4-chlorophenol biodegradation could be enhanced in Fe2O3 coupled anaerobic system.

关键词： Dechlorination     Fe2O3 nanoparticles     Electron transfer     Microbial community    

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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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Corrosion behavior of Fe–Cr–Ni based alloys exposed to molten MgCl2–KCl–NaCl salt with over-added

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1608-1619 doi: 10.1007/s11705-023-2349-1

摘要： MgCl2–NaCl–KCl salts mixture shows great potential as a high-temperature (> 700 °C) thermal energy storage material in next-generation concentrated solar power plants. Adding Mg into molten MgCl2–NaCl–KCl salt as a corrosion inhibitor is one of the most effective and cost-effective methods to mitigate the molten salt corrosion of commercial Fe–Cr–Ni alloys. However, it is found in this work that both stainless steel 310 and Incoloy 800H samples were severely corroded after 500 h immersion test at 700 °C when the alloy samples directly contacted with the over-added Mg in the liquid form. The corrosion attack is different from the classical impurity-driven corrosion in molten chloride salts found in previous work. Microscopic analysis indicates that Ni preferentially leaches out of alloy matrix due to the tendency to form MgNi2/Mg2Ni compounds. The Ni-depletion leads to the formation of a porous corrosion layer on both alloys, with the thickness around 204 µm (stainless steel 310) and 1300 µm (Incoloy 800H), respectively. These results suggest that direct contact of liquid Mg with Ni-containing alloys should be avoided during using Mg as a corrosion inhibitor for MgCl2–NaCl–KCl or other chlorides for high temperature heat storage and transfer.

关键词： concentrated solar power (CSP)     Mg corrosion inhibitor     Mg–Ni intermetallic     salt purification     thermal energy storage (TES)    

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Effects of iron oxide nanoparticles on phenotype and metabolite changes in hemp clones ( L.)

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1569-9

摘要：

● Fe3O4 NPs increased the biomass and chlorophyll content of hemp clones.

关键词： Fe3O4 nanoparticle     Hemp     Growth enhancement     THC     Metabolite    

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铝电解用Fe-Ni-Co-Al2O3金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

《中国工程科学》 2004年 第6卷 第8期   页码 35-39

摘要：

研制了一种新型铝电解金属陶瓷惰性阳极，阳极基体由Fe-Ni-CoAl2O3构成。;15 mm，石墨阴极尺寸大小为120 mm×40 mm×20 mm，通入的直流电为100～300 A，电解时间各为10 h；实验所得的电解铝产品纯度达到98%以上，杂质主要为Fe，Ni，Co；电解后的阳极外观尺寸无明显变化，阳极气体中氧气质量分数达到98%～99%。

关键词： 铝电解     惰性阳极     反电动势    

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Characteristics and energy distribution of modulated multi-pulse injection modes based diesel HCCI combustion

LIU Bin, SU Wanhua, WANG Hui, HUANG Haozhong

《能源前沿（英文）》 2007年 第1卷 第4期   页码 420-427 doi: 10.1007/s11708-007-0061-7

摘要： Cycle fuel energy distribution and combustion characteristics of early in-cylinder diesel homogenous charge compression ignition (HCCI) combustion organized by modulated multi-pulse injection modes are studied by the engine test.

关键词： combustion     compression     homogenous     in-cylinder     modulated multi-pulse    

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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed Ni

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H2), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes     room-temperature hydrogenation     Ni nanoparticles     nitrogen-doped carbon nanoneedles     metal–organic-framework    

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Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 832-839 doi: 10.1007/s11783-015-0778-x

摘要： Polybrominated diphenyl ethers (PBDEs) have been widely used as fire-retardants. Due to their high production volume, widespread usage, and environmental persistence, PBDEs have become ubiquitous contaminants in various environments.Nanoscale zero-valent iron (ZVI) is an effective reductant for many halogenated organic compounds. To enhance the degradation efficiency, ZVI/Palladium bimetallic nanoparticles (nZVI/Pd) were synthesized in this study to degrade decabromodiphenyl ether (BDE209) in water. Approximately 90% of BDE209 was rapidly removed by nZVI/Pd within 80 min, whereas about 25% of BDE209 was removed by nZVI. Degradation of BDE209 by nZVI/Pd fits pseudo-first-order kinetics. An increase in pH led to sharply decrease the rate of BDE209 degradation. The degradation rate constant in the treatment with initial pH at 9.0 was more than 6.8 × higher than that under pH 5.0. The degradation intermediates of BDE209 by nZVI/Pd were identified and the degradation pathways were hypothesized. Results from this study suggest that nZVI/Pd may be an effective tool for treating polybrominated diphenyl ethers (PBDEs) in water.

关键词： degradation     bimetallic nanoparticles     nanoscale zero-valent iron     polybrominated diphenyl ethers    

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标题 作者 时间 类型 操作

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

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

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

期刊论文

Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

期刊论文

Dechlorination of dichlorodiphenyltrichloroethane (DDT) by Fe/Pd bimetallic nanoparticles: Comparison

Kubra Ulucan-Altuntas, Eyup Debik

期刊论文

The kinetic study of light alkene syntheses by CO 2 hydrogenation over Fe-Ni catalysts

Yaling ZHAO, Li WANG, Xiwei HAO, Jiazhou WU,

期刊论文

Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

期刊论文

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

期刊论文

Corrosion behavior of Fe–Cr–Ni based alloys exposed to molten MgCl2–KCl–NaCl salt with over-added

期刊论文

Effects of iron oxide nanoparticles on phenotype and metabolite changes in hemp clones ( L.)

期刊论文

铝电解用Fe-Ni-Co-Al2O3金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

期刊论文

Characteristics and energy distribution of modulated multi-pulse injection modes based diesel HCCI combustion

LIU Bin, SU Wanhua, WANG Hui, HUANG Haozhong

期刊论文

Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed Ni

期刊论文

Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

期刊论文