scholarly journals Zn Promoted Mg-Al Mixed Oxides-Supported Gold Nanoclusters for Direct Oxidative Esterification of Aldehyde to Ester

2021 ◽  
Vol 22 (16) ◽  
pp. 8668
Author(s):  
Jie Li ◽  
Shiyi Wang ◽  
Huayin Li ◽  
Yuan Tan ◽  
Yunjie Ding
Keyword(s):  
Photoelectron Spectroscopy ◽  
Mixed Oxides ◽  
Physical Adsorption ◽  
Gold Nanoclusters ◽  
Precipitation Method ◽  
Esterification Reaction ◽  
X Ray ◽  
Oxidative Esterification ◽  
Molar Ratios ◽  
Supported Gold

The synthesis of ester compounds is one of the most important chemical processes. In this work, Zn-Mg-Al mixed oxides with different Zn2+/Mg2+ molar ratios were prepared via co-precipitation method and supported gold nanoclusters to study the direct oxidative esterification of aldehyde and alcohol in the presence of molecular oxygen. Various characterization techniques such as N2-physical adsorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and CO2 temperature programmed desorption (TPD) were utilized to analyze the structural and electronic properties. Based on the results, the presence of small amounts of Zn2+ ions (~5 wt.%) provoked a remarkable modification of the binary Mg-Al system, which enhanced the interaction between gold with the support and reduced the particle size of gold. For oxidative esterification reaction, the Au25/Zn0.05MgAl-400 catalyst showed the best performance, with the highest turnover frequency (TOF) of 1933 h−1. The active center was believed to be located at the interface between metallic gold with the support, where basic sites contribute a lot to transformation of the substrate.

scholarly journals Efficient Synthesis of Methyl Methacrylate by One Step Oxidative Esterification over Zn-Al-Mixed Oxides Supported Gold Nanocatalysts

Catalysts ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 162
Author(s):  
Huayin Li ◽  
Yuan Tan ◽  
Xingkun Chen ◽  
Wenshao Yang ◽  
Chuanqi Huang ◽  
...  
Keyword(s):  
Methyl Methacrylate ◽  
Mixed Oxides ◽  
Gold Catalyst ◽  
Co Adsorption ◽  
Gold Catalysts ◽  
Esterification Reaction ◽  
X Ray ◽  
Oxidative Esterification ◽  
One Step ◽  
Supported Gold

Methyl methacrylate (MMA) is an important monomer in fine chemicals. The synthesis of MMA by one-step oxidative esterification from methacrolein with methanol over a heterogeneous catalyst with high activity, selectivity and stability is highly desirable. Herein, Zn-Al-hydrotalcites (HTs)-supported atomically precise Au25 nanoclusters with different molar ratios of Zn2+/Al3+ were prepared and used as the precursors for this reaction. They exhibited good performances in comparison with the gold catalysts prepared by the deposition precipitation method. The structural and electronic properties were evaluated by various characterization technologies, including X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) of CO adsorption, X-ray photoelectron spectroscopy (XPS), and CO2 temperature-programmed desorption (TPD). The combined characterization results suggested that the adsorption property of gold and the basicity of the catalyst contributes to their high activities. Substrates extended experiments and stability tests implied the potential application of Zn-Al-mixed oxides supported gold catalysts, which paves a new way for supported gold catalyst in the one-step oxidation esterification reaction.

scholarly journals Improved Water–Gas Shift Performance of Au/NiAl LDHs Nanostructured Catalysts via CeO2 Addition

Nanomaterials ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 366
Author(s):  
Margarita Gabrovska ◽  
Ivan Ivanov ◽  
Dimitrinka Nikolova ◽  
Jugoslav Krstić ◽  
Anna Maria Venezia ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Nanostructured Catalysts ◽  
Water Gas Shift ◽  
Precipitation Method ◽  
Conversion Degree ◽  
Pure Hydrogen ◽  
Medium Temperature ◽  
X Ray ◽  
Supported Gold ◽  
Water Gas

Supported gold on co-precipitated nanosized NiAl layered double hydroxides (LDHs) was studied as an effective catalyst for medium-temperature water–gas shift (WGS) reaction, an industrial catalytic process traditionally applied for the reduction in the amount of CO in the synthesis gas and production of pure hydrogen. The motivation of the present study was to improve the performance of the Au/NiAl catalyst via modification by CeO2. An innovative approach for the direct deposition of ceria (1, 3 or 5 wt.%) on NiAl-LDH, based on the precipitation of Ce3+ ions with 1M NaOH, was developed. The proposed method allows us to obtain the CeO2 phase and to preserve the NiAl layered structure by avoiding the calcination treatment. The synthesis of Au-containing samples was performed through the deposition–precipitation method. The as-prepared and WGS-tested samples were characterized by X-ray powder diffraction, N2-physisorption and X-ray photoelectron spectroscopy in order to clarify the effects of Au and CeO2 loading on the structure, phase composition, textural and electronic properties and activity of the catalysts. The reduction behavior of the studied samples was evaluated by temperature-programmed reduction. The WGS performance of Au/NiAl catalysts was significantly affected by the addition of CeO2. A favorable role of ceria was revealed by comparison of CO conversion degree at 220 °C reached by 3 wt.% CeO2-modified and ceria-free Au/NiAl samples (98.8 and 83.4%, respectively). It can be stated that tuning the properties of Au/NiAl LDH via CeO2 addition offers catalysts with possibilities for practical application owing to innovative synthesis and improved WGS performance.

scholarly journals Zn-Al Mixed Oxides Decorated with Potassium as Catalysts for HT-WGS: Preparation and Properties

Catalysts ◽  
2020 ◽  
Vol 10 (9) ◽  
pp. 1094 ◽  
Author(s):  
Katarzyna Antoniak-Jurak ◽  
Paweł Kowalik ◽  
Kamila Michalska ◽  
Wiesław Próchniak ◽  
Robert Bicki
Keyword(s):  
Photoelectron Spectroscopy ◽  
Mixed Oxides ◽  
Catalyst Activity ◽  
Molar Ratio ◽  
X Ray ◽  
Molar Ratios ◽  
Mixed Oxide Catalysts ◽  
Wgs Reaction ◽  
Temperature Programmed ◽  
Co Precipitation

A set of ex-ZnAl-LDHs catalysts with a molar ratio of Zn/Al in the range of 0.3–1.0 was prepared using co-precipitation and thermal treatment. The samples were characterized using various methods, including X-ray fluorescence spectroscopy (XRF), X-ray photoelectron spectroscopy (XPS), X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy FT-IR, N2 adsorption, Temperature-programmed desorption of CO2 (TPD-CO2) as well as Scanning electron microscopy (SEM-EDS). Catalyst activity and long-term stability measurements were carried out in a high-temperature water–gas shift (HT-WGS) reaction. Mixed oxide catalysts with various Zn/Al molar ratios decorated with potassium showed high activity in the HT-WGS reaction within the temperature range of 330–400 °C. The highest activity was found for the Zn/Al molar ratio of 0.5 corresponding to spinel stoichiometry. However, the catalyst with a stoichiometric spinel molar ratio of Zn/Al (ZnAl_0.5_K) revealed a higher tendency for surface migration and/or vaporization of potassium during overheating at 450 °C. The correlation of the activity results and TPD-CO2 data show that medium basic sites enhance the progress of the HT-WGS reaction.

scholarly journals Promotional Effect of Gold on the WGS Activity of Alumina-Supported Copper-Manganese Mixed Oxides

Catalysts ◽  
2018 ◽  
Vol 8 (11) ◽  
pp. 563 ◽  
Author(s):  
Tatyana Tabakova ◽  
Ivan Ivanov ◽  
Yordanka Karakirova ◽  
Daniela Karashanova ◽  
Anna Venezia ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Mixed Oxides ◽  
Precipitation Method ◽  
Molar Ratio ◽  
X Ray ◽  
Promotional Effect ◽  
Production Of Hydrogen ◽  
Copper Manganese ◽  
Highly Dispersed

The water-gas shift (WGS) reaction is a well-known industrial process used for the production of hydrogen. During the last few decades, it has attracted renewed attention due to the need for high-purity hydrogen for fuel-cell processing systems. The aim of the present study was to develop a cost-effective and catalytically efficient formulation that combined the advantageous properties of transition metal oxides and gold nanoparticles. Alumina-supported copper- manganese mixed oxides were prepared by wet impregnation. The deposition-precipitation method was used for the synthesis of gold catalysts. The effect of the Cu:Mn molar ratio and the role of Au addition on the WGS reaction’s performance was evaluated. Considerable emphasis was put on the characterization of the as-prepared and WGS-tested samples by means of a number of physicochemical methods (X-ray powder diffraction, high-resolution transmission electron microscopy, electron paramagnetic resonance, X-ray photoelectron spectroscopy, and temperature-programmed reduction) in order to explain the relationship between the structure and the reductive and WGS behavior. Catalytic tests revealed the promotional effect of gold addition. The best performance of the gold-promoted sample with a higher Cu content, i.e., a Cu:Mn molar ratio of 2:1 might be related to the beneficial role of Au on the spinel decomposition and the highly dispersed copper particle formation during the reaction, thus, ensuring the presence of two highly dispersed active metallic phases. High-surface-area alumina that was modified with a surface fraction of Cu–Mn mixed oxides favored the stabilization of finely dispersed gold particles. These new catalytic systems are very promising for practical applications due to their economic viability because the composition mainly includes alumina (80%).

scholarly journals Photocatalytic Reduction of CO2 to Methanol Using a Copper-Zirconia Imidazolate Framework

Catalysts ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 346
Author(s):  
Sonam Goyal ◽  
Maizatul Shima Shaharun ◽  
Ganaga Suriya Jayabal ◽  
Chong Fai Kait ◽  
Bawadi Abdullah ◽  
...  
Keyword(s):  
Photoelectron Spectroscopy ◽  
Catalyst Support ◽  
Oxidation Potential ◽  
Molar Ratio ◽  
X Ray Diffraction ◽  
X Ray ◽  
Molar Ratios ◽  
Optimum Parameters ◽  
Reduction Of Co2 ◽  
Enhanced Yield

A set of novel photocatalysts, i.e., copper-zirconia imidazolate (CuZrIm) frameworks, were synthesized using different zirconia molar ratios (i.e., 0.5, 1, and 1.5 mmol). The photoreduction process of CO2 to methanol in a continuous-flow stirred photoreactor at pressure and temperature of 1 atm and 25 °C, respectively, was studied. The physicochemical properties of the synthesized catalysts were studied using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and photoluminescence (PL) spectroscopy. The highest methanol activity of 818.59 µmol/L.g was recorded when the CuZrIm1 catalyst with Cu/Zr/Im/NH4OH molar ratio of 2:1:4:2 (mmol/mmol/mmol/M) was employed. The enhanced yield is attributed to the presence of Cu2+ oxidation state and the uniformly dispersed active metals. The response surface methodology (RSM) was used to optimize the reaction parameters. The predicted results agreed well with the experimental ones with the correlation coefficient (R2) of 0.99. The optimization results showed that the highest methanol activity of 1054 µmol/L.g was recorded when the optimum parameters were employed, i.e., stirring rate (540 rpm), intensity of light (275 W/m2) and photocatalyst loading (1.3 g/L). The redox potential value for the CuZrIm1 shows that the reduction potential is −1.70 V and the oxidation potential is +1.28 V for the photoreduction of CO2 to methanol. The current work has established the potential utilization of the imidazolate framework as catalyst support for the photoreduction of CO2 to methanol.

scholarly journals Study on Adsorption Properties of Modified Corn Cob Activated Carbon for Mercury Ion

Energies ◽  
2021 ◽  
Vol 14 (15) ◽  
pp. 4483
Author(s):  
Yuyingnan Liu ◽  
Xinrui Xu ◽  
Bin Qu ◽  
Xiaofeng Liu ◽  
Weiming Yi ◽  
...  
Keyword(s):  
Activated Carbon ◽  
Photoelectron Spectroscopy ◽  
Adsorption Process ◽  
Physical Adsorption ◽  
Raw Material ◽  
Order Kinetic ◽  
Mercury Ions ◽  
Corn Cob ◽  
Adsorption Time ◽  
X Ray

In this study, corn cob was used as raw material and modified methods employing KOH and KMnO4 were used to prepare activated carbon with high adsorption capacity for mercury ions. Experiments on the effects of different influencing factors on the adsorption of mercury ions were undertaken. The results showed that when modified with KOH, the optimal adsorption time was 120 min, the optimum pH was 4; when modified with KMnO4, the optimal adsorption time was 60 min, the optimal pH was 3, and the optimal amount of adsorbent and the initial concentration were both 0.40 g/L and 100 mg/L under both modified conditions. The adsorption process conforms to the pseudo-second-order kinetic model and Langmuir model. Scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDS), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and Zeta potential characterization results showed that the adsorption process is mainly physical adsorption, surface complexation and ion exchange.

scholarly journals Synthesis of Exosome-Based Fluorescent Gold Nanoclusters for Cellular Imaging Applications

2021 ◽  
Vol 22 (9) ◽  
pp. 4433
Author(s):  
Eun Sung Lee ◽  
Byung Seok Cha ◽  
Seokjoon Kim ◽  
Ki Soo Park
Keyword(s):  
Photoelectron Spectroscopy ◽  
Low Cost ◽  
Stokes Shift ◽  
Gold Nanoclusters ◽  
Human Colon ◽  
Cellular Imaging ◽  
Metal Nanoclusters ◽  
Human Colon Cancer ◽  
X Ray ◽  
High Concentrations

In recent years, fluorescent metal nanoclusters have been used to develop bioimaging and sensing technology. Notably, protein-templated fluorescent gold nanoclusters (AuNCs) are attracting interest due to their excellent fluorescence properties and biocompatibility. Herein, we used an exosome template to synthesize AuNCs in an eco-friendly manner that required neither harsh conditions nor toxic chemicals. Specifically, we used a neutral (pH 7) and alkaline (pH 11.5) pH to synthesize two different exosome-based AuNCs (exo-AuNCs) with independent blue and red emission. Using field-emission scanning electron microscopy, energy dispersive X-ray microanalysis, nanoparticle tracking analysis, and X-ray photoelectron spectroscopy, we demonstrated that AuNCs were successfully formed in the exosomes. Red-emitting exo-AuNCs were found to have a larger Stokes shift and a stronger fluorescence intensity than the blue-emitting exo-AuNCs. Both exo-AuNCs were compatible with MCF-7 (human breast cancer), HeLa (human cervical cancer), and HT29 (human colon cancer) cells, although blue-emitting exo-AuNCs were cytotoxic at high concentrations (≥5 mg/mL). Red-emitting exo-AuNCs successfully stained the nucleus and were compatible with membrane-staining dyes. This is the first study to use exosomes to synthesize fluorescent nanomaterials for cellular imaging applications. As exosomes are naturally produced via secretion from almost all types of cell, the proposed method could serve as a strategy for low-cost production of versatile nanomaterials.

A Label-Free Electrochemical Aptasensor for the Rapid Detection of Tetracycline Based on Ordered Mesoporous Carbon–Fe3O4

2018 ◽  
Vol 71 (3) ◽  
pp. 170 ◽  
Author(s):  
Xuejia Zhan ◽  
Guangzhi Hu ◽  
Thomas Wagberg ◽  
Dongwei Zhang ◽  
Pei Zhou
Keyword(s):  
Photoelectron Spectroscopy ◽  
Mesoporous Carbon ◽  
Physical Adsorption ◽  
Differential Pulse ◽  
Ordered Mesoporous Carbon ◽  
Label Free ◽  
X Ray Diffraction ◽  
X Ray ◽  
Ordered Mesoporous ◽  
Modification Procedure

A novel aptasensor based on a tetracycline (TET) aptamer immobilized by physical adsorption on an ordered mesoporous carbon–Fe3O4 (OMC-Fe3O4)-modified screen-printed electrode surface was successfully fabricated. OMC-Fe3O4 was characterized by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The modification procedure of the aptasensor was characterized by cyclic voltammetry. Interaction between the TET aptamer and target was determined by differential pulse voltammetry. Under optimal conditions, the proposed aptasensor exhibited good electrochemical sensitivity to TET in a concentration range of 5 nM to 10 μM, with a detection limit of 0.8 nM (S/N = 3). This aptasensor exhibited satisfactory specificity, reproducibility, and stability.

Gold nanoclusters reductively deposited on porous silicon: morphology and electronic structures

1998 ◽  
Vol 76 (11) ◽  
pp. 1707-1716 ◽  
Author(s):  
I Coulthard ◽  
S Degen ◽  
Y -J Zhu ◽  
T K Sham
Keyword(s):  
Gold Nanoparticles ◽  
Porous Silicon ◽  
Photoelectron Spectroscopy ◽  
Gold Nanoclusters ◽  
Gold Complex ◽  
X Ray Diffraction ◽  
Complex Ions ◽  
X Ray ◽  
Preparation Conditions ◽  
P Type

Utilizing porous silicon as a reducing agent and a substrate, gold complex ions [AuCl4]- were reduced from aqueous solution to produce nanoparticles of gold upon the surface of porous silicon. Scanning electron microscopy (SEM) was utilized to study the morphology of the porous silicon layers and the deposits of gold nanoparticles. It is found that preparation conditions have a profound effect on the morphology of the deposits, especially on porous silicon prepared from a p-type wafer. The gold nanoparticles, varying from micrometric aggregates of clusters of the order of 10 nm, to a distribution of nearly spherical clusters of the order of 10 nm, to strings of ~10 nm were observed and compared to bulk gold metal using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS). These techniques confirm and complement the SEM findings. The potential for this reductive deposition technique is noted.Key words: gold nanostructures, reductive deposition, porous silicon, morphology, X-ray spectroscopy.

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