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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    

In situ formation of bimetallic FeNi nanoparticles on sand through green technology: Application for

Ravikumar KVG, Debayan Ghosh, Mrudula Pulimi, Chandrasekaran Natarajan, Amitava Mukherjee

《环境科学与工程前沿(英文)》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1195-3

摘要: • In situ preparation of FeNi nanoparticles on the sand via green synthesis approach. • Removal of tetracycline using GS-FeNi in batch and column study. • Both reductive degradation and sorption played crucial role the process. • Reusability of GS-FeNi showed about 77.39±4.3% removal on 4th cycle. • TC by-products after interaction showed less toxic as compared with TC. In this study, FeNi nanoparticles were green synthesized using Punica granatum (pomegranate) peel extract, and these nanoparticles were also formed in situ over quartz sand (GS-FeNi) for removal of tetracycline (TC). Under the optimized operating conditions, (GS-FeNi concentration: 1.5% w/v; concentration of TC: 20 mg/L; interaction period: 180 min), 99±0.2% TC removal was achieved in the batch reactor. The removal capacity was 181±1 mg/g. A detailed characterization of the sorbent and the solution before and after the interaction revealed that the removal mechanism(s) involved both the sorption and degradation of TC. The reusability of reactant was assessed for four cycles of operation, and 77±4% of TC removal was obtained in the cycle. To judge the environmental sustainability of the process, residual toxicity assay of the interacted TC solution was performed with indicator bacteria (Bacillus and Pseudomonas) and algae (Chlorella sp.), which confirmed a substantial decrease in the toxicity. The continuous column studies were undertaken in the packed bed reactors using GS-FeNi. Employing the optimized conditions, quite high removal efficiency (978±5 mg/g) was obtained in the columns. The application of GS-FeNi for antibiotic removal was further evaluated in lake water, tap water, and ground water spiked with TC, and the removal capacity achieved was found to be 781±5, 712±5, and 687±3 mg/g, respectively. This work can pave the way for treatment of antibiotics and other pollutants in the reactors using novel green composites prepared from fruit wastes.

关键词: GS-FeNi nanoparticles     Tetracycline removal     Re-usability     Residual toxicity     Column studies    

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    

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    

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

《化学科学与工程前沿(英文)》 2010年 第4卷 第4期   页码 476-480 doi: 10.1007/s11705-010-0512-y

摘要: A co-precipitation method was employed to prepare Ni/Al O -ZrO , Co/Al O -ZrO and Ni-Co/Al O -ZrO catalysts. Their properties were characterized by N adsorption (BET), thermogravimetric analysis TGA , temperature-programmed reduction (TPR), temperature-programmed desorption (CO -TPD), and temperature-programmed surface reaction (CH -TPSR and CO -TPSR). Ni-Co/Al O -ZrO bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO adsorption sites (C+ CO = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH -CO -TPSR, there were 80.9% and 81.5% higher CH and CO conversion over Ni-Co/Al O -ZrO catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al O -ZrO catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.

关键词: Ni-Co bimetallic catalyst     composite support     CH4 reforming with CO2    

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1581-1592 doi: 10.1007/s11705-023-2327-7

摘要: Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al2O3, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including SO4•‒, OH •, and O2•‒) and singlet oxygen (1O2) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al2O3 promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

关键词: Cu–Al bimetallic oxides     mesoporous silica spheres     peroxydisulfate     bisphenol A    

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

《化学科学与工程前沿(英文)》   页码 1623-1631 doi: 10.1007/s11705-022-2202-y

摘要: The number of active components and their dispersion degree are two key factors affecting the performance of adsorbents. Here, we report a simple but efficient strategy for dispersing active components by using a confined space, which is formed by mesoporous silica walls and templates in the as-prepared SBA-15 (AS). Such a confined space does not exist in the conventional support, calcined SBA-15, which does not contain a template. The Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination, during which the template was also removed. The results show that up to 5 mmol·g–1 of CuO and ZnO can be well dispersed; however, severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same loading. Confined space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and ZnO. The bimetallic materials were employed for the adsorptive separation of propene and propane. The samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.

关键词: bimetallic adsorbents     confined space     mesoporous silica     propene/propane separation    

Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 1962-1972 doi: 10.1007/s11705-023-2359-z

摘要: Within the “hydrogen chain”, the high-temperature water gas shift reaction represents a key step to improve the H2 yield and adjust the H2/COx ratio to fit the constraints of downstream processes. Despite the commercial application of the high-temperature water gas shift, novel catalysts characterized by higher intrinsic activity (especially at low temperatures), good thermal stability, and no chromium content are needed. In this work, we propose bimetallic iron-copper catalysts supported on ceria, characterized by low active phase content (iron oxide + copper oxide < 5 wt %). Fresh and used samples were characterized by inductively coupled plasma mass spectrometry, X-ray diffraction, nitrogen physisorption, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, and temperature programmed reduction in hydrogen to relate physicochemical features and catalytic activity. The sample with iron/copper ≈ 1 and 4 wt % active phase content showed the best catalytic properties in terms of turnover frequency, no methane formation, and stability. Its unique properties were due to both strong iron-copper interaction and strong metal-support interaction, leading to outstanding redox behavior.

关键词: water gas shift     iron     copper     bimetallic catalysts     ceria     hydrogen    

Mechanistic understanding of Cu-based bimetallic catalysts

You Han, Yulian Wang, Tengzhou Ma, Wei Li, Jinli Zhang, Minhua Zhang

《化学科学与工程前沿(英文)》 2020年 第14卷 第5期   页码 689-748 doi: 10.1007/s11705-019-1902-4

摘要: Copper has received extensive attention in the field of catalysis due to its rich natural reserves, low cost, and superior catalytic performance. Herein, we reviewed two modification mechanisms of co-catalyst on the coordination environment change of Cu-based catalysts: (1) change the electronic orbitals and geometric structure of Cu without any catalytic functions; (2) act as an additional active site with a certain catalytic function, as well as their catalytic mechanism in major reactions, including the hydrogenation to alcohols, dehydrogenation of alcohols, water gas shift reaction, reduction of nitrogenous compounds, electrocatalysis and others. The influencing mechanisms of different types of auxiliary metals on the structure-activity relationship of Cu-based catalysts in these reactions were especially summarized and discussed. The mechanistic understanding can provide significant guidance for the design and controllable synthesis of novel Cu-based catalysts used in many industrial reactions.

关键词: copper     bimetallic catalyst     coordination     modification mechanism     catalytic application    

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要: Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词: catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

《化学科学与工程前沿(英文)》 2021年 第15卷 第5期   页码 1111-1124 doi: 10.1007/s11705-020-2031-9

摘要: The hydroisomerization of -hexadecane over Pt-Pd bimetallic catalysts is an effective way to produce clean fuel oil. This work reports a useful preparation method of bimetallic bifunctional catalysts by a co-impregnation or sequential impregnation process. Furthermore, monometallic catalysts with loading either Pt or Pd are also prepared for comparison. The effects of the metal species and impregnation order on the characteristics and catalytic performance of the catalysts are investigated. The catalytic test results indicate that the maximum -hexadecane yield over different catalysts increases as follows: Pt/silicoaluminophosphate SAPO-41

关键词: SAPO-41 molecular sieve     Pt-Pd bimetallic site     bifunctional catalysts     n-hexadecane     hydroisomerization    

Translocation and biotoxicity of metal (oxide) nanoparticles in the wetland-plant system

《环境科学与工程前沿(英文)》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1432-4

摘要:

• Aquatic plants are more likely to absorb TiO2 NPs that are beneficial to them.

关键词: Constructed wetlands     Aquatic plants     Nanoparticles     Physiological activity     Biomass    

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    

Gold nanoparticles/single-stranded DNA-reduced graphene oxide nanocomposites based electrochemical biosensor

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1572-1582 doi: 10.1007/s11705-021-2112-4

摘要: High density and uniform distribution of the gold nanoparticles functionalized single-stranded DNA modified reduced graphene oxide nanocomposites were obtained by non-covalent interaction. The positive gold nanoparticles prepared by phase inversion method exhibited good dimensional homogeneity and dispersibility, which could readily combine with single-stranded DNA modified reduced graphene oxide nanocomposites by electrostatic interactions. The modification of single-stranded DNA endowed the reduced graphene oxide with favorable biocompatibility and provided the preferable surface with negative charge for further assembling of gold nanoparticles to obtain gold nanoparticles/single-stranded DNA modified reduced graphene oxide nanocomposites with better conductivity, larger specific surface area, biocompatibility and electrocatalytic characteristics. The as-prepared nanocomposites were applied as substrates for the construction of cholesterol oxidase modified electrode and well realized the direct electron transfer between the enzyme and electrode. The modified gold nanoparticles could further catalyze the products of cholesterol oxidation catalyzed by cholesterol oxidase, which was beneficial to the enzyme-catalyzed reaction. The as-fabricated bioelectrode exhibited excellent electrocatalytic performance for the cholesterol with a linear range of 7.5‒280.5 μmol·L‒1, a low detection limit of 2.1 μmol·L‒1, good stability and reproducibility. Moreover, the electrochemical biosensor showed good selectivity and acceptable accuracy for the detection of cholesterol in human serum samples.

关键词: reduced graphene oxide     gold nanoparticles     electrochemical biosensor     cholesterol oxidase     cholesterol    

polymeric substances from activated sludge on the aggregation kinetics of silver and silver sulfide nanoparticles

《环境科学与工程前沿(英文)》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1450-2

摘要:

• The NPs aggregation in the electrolyte solution is consistent with the DLVO theory.

关键词: Silver nanoparticles     Silver sulfide nanoparticles     Extracellular polymeric substances     Aggregation kinetics     Influence mechanisms    

标题 作者 时间 类型 操作

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

Kubra Ulucan-Altuntas, Eyup Debik

期刊论文

In situ formation of bimetallic FeNi nanoparticles on sand through green technology: Application for

Ravikumar KVG, Debayan Ghosh, Mrudula Pulimi, Chandrasekaran Natarajan, Amitava Mukherjee

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

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

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

期刊论文

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

期刊论文

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

期刊论文

Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

期刊论文

Mechanistic understanding of Cu-based bimetallic catalysts

You Han, Yulian Wang, Tengzhou Ma, Wei Li, Jinli Zhang, Minhua Zhang

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

期刊论文

Translocation and biotoxicity of metal (oxide) nanoparticles in the wetland-plant system

期刊论文

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

期刊论文

Gold nanoparticles/single-stranded DNA-reduced graphene oxide nanocomposites based electrochemical biosensor

期刊论文

polymeric substances from activated sludge on the aggregation kinetics of silver and silver sulfide nanoparticles

期刊论文