Sooknoi, Tawan

Preferred name

Sooknoi, Tawan

Alternative Name

Sooknoi, T.

Main Affiliation

School of Science

tawan.so@kmitl.ac.th

Now showing 1 - 10 of 59

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Highly Dispersed WOx/SiO2Catalysts Derived from W-TRIS Complex for Efficient Biobutadiene Production from Acetylene-Ethylene Cross-Metathesis
(2025-01-01)
Promchana, Pratya
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Choojun, Kittisak
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Wengwirat, Kanokwan
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Limphirat, Wanwisa
;
Sooknoi, Tawan
Renewable 1,3-butadiene was selectively produced via acetylene-ethylene cross-metathesis over highly dispersed WO<inf>x</inf>/SiO<inf>2</inf>catalysts prepared by a simple impregnation method using the molecular precursor (NH<inf>4</inf>)<inf>2</inf>[W<inf>2</inf>O<inf>6</inf>(TRIS)<inf>2</inf>] (W-TRIS). Compared to catalysts derived from ammonium metatungstate (AMT), the TRIS-derived catalysts exhibited superior WO<inf>x</inf>dispersion and catalytic activity, attributed to stronger W–O–Si interactions as evidenced by XRD, DRUV–vis, Raman spectroscopy, and W L<inf>3</inf>-edge XANES/EXAFS. Systematic variation of WO<inf>3</inf>loading revealed that 5 wt % WO<inf>x</inf>/SiO<inf>2</inf>-TRIS offered the optimal balance of activity and selectivity, achieving 60% acetylene conversion, ∼74% selectivity to 1,3-butadiene, and a turnover frequency (TOF) of 23 h–1. Contact time analysis confirmed that 1,3-butadiene was the primary product, while minor byproducts such as cyclohexene and benzene originated from Diels–Alder cycloaddition followed by dehydrogenation. Reaction temperature screening identified 450 °C as the optimal operating condition; higher temperatures led to increased side reactions. Importantly, long-term testing over 100 h under continuous-flow conditions demonstrated high stability with sustained selectivity and negligible coke formation. These findings underscore the practical advantages of the W-TRIS molecular precursor strategy in designing durable WO<inf>x</inf>/SiO<inf>2</inf>catalysts for efficient and sustainable C<inf>4</inf>chemical production from bioethylene.
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Facile synthesis of the atomically dispersed hydrotalcite oxide supported copper catalysts for the selective hydrogenation of 5–hydroxymethylfurfural into 2,5-bis(hydroxymethyl)furan
(2023-07-15)
Kumar, Raju
;
Lee, Hsin Hui
;
Chen, En
;
Du, Yuan Peng
;
Lin, Chan Yi
The selective hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) using the atomically dispersed supported copper catalyst is investigated. The hydrotalcite oxide supported copper materials (Cu<inf>(x)</inf>HTO) are facilely prepared by coprecipitating metal precursors in a methanolic solution under a tuned pH. The surface characterization involving PXRD, TEM, H<inf>2</inf>/N<inf>2</inf>O-TPR, and XAS reveals unequivocal evidence for the presence of the atomically dispersed copper on HTO surface. XAS specifically indicates the formation of mononuclear copper species, and H<inf>2</inf>/N<inf>2</inf>O-TPR strongly supports the copper atoms of Cu<inf>(5)</inf>HTO are evenly distributed in 99% dispersion. Moreover, the reduced Cu<inf>(5)</inf>HTO (r-Cu<inf>(5)</inf>HTO) enables to completely hydrogenate HMF to BHMF under mild conditions, in comparison to the poor reactivity catalyzed by the hydrotalcite oxide supported copper nanoparticles (r-Cu<inf>(4)</inf>@HTO). The dramatic enhancement of HMF hydrogenation catalyzed by r-Cu<inf>(5)</inf>HTO can be attributed to the fine distribution of copper atoms which are situated homogeneously over HTO surface as well as chemically reactive for the carbonyl group.
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Surface hydrophobicity and catalytic performance of cerium incorporated HZSM-5 zeolite for conversion of bio-ethanol
(2024-05-01)
Ausavasukhi, Artit
;
Sooknoi, Tawan
Cerium incorporated HZSM-5 (CeHZSM-5) catalyst prepared by impregnation method was tested for aqueous ethanol conversion at 200–400 °C. The CeHZSM-5 catalyst was found to be very active (21.02 %Conversion), compared to the parent HZSM-5 catalyst (9.39 %Conversion), especially at low reaction temperatures (200 °C) and when fed with high water content (80 wt% ethanol). FTIR, FT-Raman, DR-UV, NH<inf>3</inf>-TPD, IPA-TPD, DSC and contact angle techniques reveal that the incorporation of cerium species into zeolites results in the acidity and hydrophilic/hydrophobic nature. Cerium species are thought to tend to migrate into ZSM-5 channels and associate with the zeolite framework. As a result, the net electrostatic charge decreases due to the presence of tetrahedral cerium atoms. Therefore, the CeHZSM-5 exhibits a hydrophobic character, compared to the parent one. The decrease in competitive adsorption of water versus ethanol feed at the Brønsted acid site may lead to an increase in CeHZSM-5 catalyst activity.
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Tailoring the First Coordination Shell of Isolated Ti(IV) Active Sites in Zeolite Frameworks Boosting Catalytic Activity in Epoxidation
(2025-05-08)
Klinyod, Sorasak
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Yomthong, Krissanapat
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Suttipat, Duangkamon
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Pornsetmetakul, Peerapol
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Kidkhunthod, Pinit
We present a strategy to precisely tune the local structure of the tetrahedrally coordinated titanium (Ti) sites incorporated in the zeolite framework via a one-pot hydrothermal synthesis with the aid of NH<inf>4</inf>F without any further postmodification step. This approach effectively prevents typical issues observed in postsynthetic methods, such as Ti leaching and zeolite framework degradation. By optimizing the NH<inf>4</inf>F concentration in the synthesis precursor, the formation of open Ti(OSi)<inf>3</inf>OH and Ti(OSi)<inf>3</inf>F active species can be precisely controlled. To elucidate the relationship between various Ti active species, including closed Ti(OSi)<inf>4</inf>, open Ti(OSi)<inf>3</inf>OH, and open Ti(OSi)<inf>3</inf>F sites and their catalytic performances in methyl oleate (MO) epoxidation, we employed ultraviolet–visible diffuse reflectance spectroscopy (UV–vis DRS), fluorine X-ray absorption near edge structure spectroscopy (F-XANES), and density functional theory (DFT) calculations. Our findings reveal that increased positive charges on Ti active centers, in the order of closed Ti(OSi)<inf>4</inf> < open Ti(OSi)<inf>3</inf>OH < open Ti(OSi)<inf>3</inf>F, correlate with enhanced catalytic performance in MO epoxidation. However, an excessive proportion of Ti(OSi)<inf>3</inf>F species in the framework can diminish catalytic performance by promoting undesired side reactions. Therefore, we propose an optimized balance between open Ti(OSi)<inf>3</inf>OH and open Ti(OSi)<inf>3</inf>F species in the zeolite structure to maximize the catalytic activity of epoxidation.
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Bio-derived butadiene from cross-metathesis over silanol rich WO3 catalysts obtained from copper phyllosilicate
(2025-03-20)
Wengwirat, Kanokwan
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Choojun, Kittisak
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Promchana, Pratya
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Limphirat, Wanwisa
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Sooknoi, Tawan
Bio-butadiene can be produced from cross-metathesis of bioethanol-derived acetylene/ethylene over supported WO<inf>3</inf> on silanol-rich silica prepared with Cu-leached copper phyllosilicate (CuPS). 20CuPS and 30CuPS were preliminarily reduced before Cu-leaching under an acidic solution (1 M HCl). Compared with fumed SiO<inf>2</inf>29Si CPMAS NMR spectroscopy showed an increase in surface silanols, particularly the isolated silanols (Q<inf>3</inf>), from removing Cu2+ octahedral sites (Cu2+(OSi)<inf>6</inf>) encapsulated within tetrahedral silica layers of CuPS. The surface silanols in fumed SiO<inf>2</inf>, 20CuPS-Le, and 30CuPS-Le adequately accommodate single-site and polymeric WO<inf>3</inf> species, leading to a similar 1,3-butadiene production rate (∼4.7 mmol h−1 g<inf>cat</inf>) at 5 wt% loading. Only 30CuPS-Le sufficiently provides the exposed silanols to disperse 8 wt% WO<inf>3</inf> loading without bulk WO<inf>3</inf> formation. The cross-metathesis activity depends on the relative amounts of exposed silanols. Accordingly, the steady 1,3-butadiene production was obtained in the order of 8WO<inf>3</inf>/30CuPS-Le (6.3 mmol h−1 g<inf>cat</inf>) > 8WO<inf>3</inf>/20CuPS-Le (5.1 mmol h−1 g<inf>cat</inf>) > 8WO<inf>3</inf>/SiO<inf>2</inf> (2.5 mmol h−1 g<inf>cat</inf>).
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Tuning Cu+ species/Brønsted acids of copper phyllosilicate by K+ doping for selective hydrogenation of methyl palmitate to hexadecanol
(2023-12-01)
Prasanseang, Warot
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Choojun, Kittisak
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Poo-arporn, Yingyot
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Huang, Ai Lin
;
Lin, Yu Chuan
Selective hydrogenation of methyl palmitate to hexadecanol can be manipulated by tuning Cu+ species and Brønsted acid sites (BAS) of copper phyllosilicate (CuPS) catalysts with K+ doping. The catalysts were prepared by impregnating K+ onto reduced and non-reduced CuPS. The reactions were carried out in a fixed-bed flow reactor at 250 °C under atmospheric H<inf>2</inf>. In situ TR-XANES and Py-IR suggest that the presence of K+ could stabilize Cu+ species and neutralize BAS. As compared to the non-reduced sample, K+ loading (0.01–0.10 wt%) on the reduced CuPS provide higher Cu+ fraction (10–16%), lower BAS (0.82 to 0.16μ mol/g) and lower Cu dispersion (75 to 52%). A balance between Cu0 active surface and Cu+ content provides an optimum hydrogenation activity (up to 80 %). The increased Cu+ species, together with the decreased BAS, does not only enhance the catalyst stability, but also hexadecanol selectivity (from 35 to 60%, at ∼50% conversion).
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Enhanced CO2/CH4 Permselectivity in Partially Hydrolyzed EVA Membranes via Synergistic PEG Plasticization and Amine-Functionalized Silica Incorporation
(2026-03-27)
Ritvirulh, Chonlada
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Wisatsuvan, Patchnakan
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Sooknoi, Tawan
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Rukchonlatee, Suparat
The separation of carbon dioxide (CO2) from methane (CH4) in biogas is essential for increasing the fuel quality. However, conventional membrane-based separation under high pressure is not suitable for household biogas systems due to operational cost and complexity. This study aims to develop low-pressure gas separation membranes based on partially hydrolyzed ethylene vinyl acetate (p-E) copolymers by incorporating poly(ethylene glycol) (PEG) as a plasticizer and amine-functionalized silica (APTES-modified SiO2) as a polar filler. The hydrolysis of EVA improves mechanical strength by increasing hydrogen bonding. PEG addition enhances the free volume and CO2 affinity, while the well-dispersed surface-treated SiO2 increases membrane polarity and suppresses CH4 permeation. Among the tested membranes, the optimal formulation (p-EP400(15)-S0.6) containing 15 wt % PEG400 and 0.6 wt % APTES-SiO2 achieves the highest CO2/CH4 selectivity (∼22) and a high CO2 permeability (∼1400 g/m2·day). These findings demonstrate a promising strategy to develop effective membranes for biogas upgrading under ambient conditions.
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Tubular EVA copolymer/SiO2/PEG composite membrane for CO2 removal from household biogas
(2025-03-01)
Watasit, Prachya
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Ausavasukhi, Artit
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Rukchonlatee, Suparat
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Sooknoi, Tawan
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Ritvirulh, Chonlada
The fuel efficiency of household biogas is generally regulated by its CO<inf>2</inf> content (25%–50%). To improve its heating value, atmospheric CO<inf>2</inf> removal of household biogas using a polymeric membrane was attempted to avoid a complicated separation process. A tubular membrane of poly(ethylene-co-vinyl acetate), composed of 28% and 18% vinyl acetate (E28 and E18) modified with SiO<inf>2</inf> and polyethylene glycol (PEG), was fabricated by blown film extrusion. Model biogas containing CO<inf>2</inf>/CH<inf>4</inf> (40/60 v/v) was separated in an in-house continuous gas separation module, in which CO<inf>2</inf> was mainly permeated out of the tubular membrane at atmospheric pressure. Blending the E28 matrix with E18 (10 wt%) improves the membrane processability and inhibits the CH<inf>4</inf> permeation, leading to enhanced CO<inf>2</inf>/CH<inf>4</inf> selectivity (from ~2.3 to 2.9). Well-dispersed SiO<inf>2</inf> particles (0.5 wt%) increase the membrane modulus and suppress CH<inf>4</inf> loss. However, adding more SiO<inf>2</inf> (0.75–1.0 wt%) leads to higher total gas permeation flux with lower CO<inf>2</inf>/CH<inf>4</inf> selectivity due to particle agglomeration. Incorporation of PEG (0.5–1.5 wt%) increased the membrane polarity and CO<inf>2</inf> permeability. The CO<inf>2</inf>/CH<inf>4</inf> selectivity was also improved (~5.3), only up to 1.0 wt% PEG content. Highlights: Composite EVA/SiO2/PEG membrane separates CO<inf>2</inf>/CH<inf>4</inf> at atmospheric pressure. The concentration gradient across the membrane drives CO<inf>2</inf>/CH<inf>4</inf> permeation. Adding SiO<inf>2</inf> hinders CH<inf>4</inf> permeability and enhances CO<inf>2</inf>/CH<inf>4</inf> selectivity. Increasing PEG content enhances membrane polarity and interaction with CO<inf>2</inf>.
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Reversible Hydrogenation-Dehydrogenation of Acetylpyridine-Pd-MIL-101(Cr) for Chemical Hydrogen Storage
(2020-10-07)
Makmeesub, Nuttapong
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Ritvirulh, Chonlada
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Choojun, Kittisak
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Chen, Teng Hao
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Poo-Arporn, Yingyot
3-Acetylpyridine (AcP), as an organic hydrogen carrier, and Pd nanoparticles, as a catalyst, were incorporated into MIL-101(Cr) for chemical hydrogen storage. AcP was first grafted into MIL-101(Cr), and then Pd (0.5-4.0 wt %) was encapsulated by a double-solvent adsorption process. Thermogravimetric analysis, inductively coupled plasma-optical emission spectrometry, X-ray photoelectron spectroscopy, transmission electron microscopy, in situ X-ray adsorption near-edge structure analysis, 1H nuclear magnetic resonance (NMR), and elemental analysis suggested the existence of AcP and Pd nanoparticles (NPs) inside the MIL-101(Cr) cages. The chemical hydrogen storage of samples was evaluated by H2 temperature-programmed reaction. In situ Fourier transform infrared and 1H NMR techniques verified the hydrogenated and dehydrogenated forms of AcP upon hydrogen uptake. Reversible hydrogenation/dehydrogenation can be readily regulated by H2 partial pressure and temperature. The chemical hydrogen storage could be accomplished only when AcP and Pd NPs were adjacently present. The chemical hydrogen storage was enhanced with an increased Pd loading up to 0.33 mmol H2·g-1 per cycle. With the manipulation of hydrogenation and dehydrogenation temperatures at 150 °C, the chemical hydrogen storage can be maintained for up to 10 cycles. The material reported herein is one of the noncryogenic chemical hydrogen storages that can be operated at constant temperature and atmospheric pressure.
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Cu encapsulated in hierarchical MFI zeolites for ethanol dehydrogenation to acetaldehyde
(2026-04-09)
Saenluang, Kachaporn
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Maineawklang, Narasiri
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Prasertsab, Anittha
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Sooknoi, Tawan
;
Kegnæs, Søren
In this contribution, we report the design of Cu nanoparticles encapsulated within both hierarchical and conventional MFI frameworks for the dehydrogenation of ethanol to acetaldehyde. The encapsulated catalysts were successfully synthesized via a hydrothermal method, using tetrabutylammonium hydroxide (TBAOH) and tetrapropylammonium hydroxide (TPAOH) as structure-directing agents (SDAs) for hierarchical and conventional frameworks, respectively. Characterization results showed that the hierarchical silicalite-1 zeolite (Cu@hieS-1) exhibited the simultaneous presence of mesopores and uniform Cu nanoparticles (∼2.3 nm), with high Cu dispersion (82.6%), thereby significantly improving active-site accessibility and reducing diffusion path lengths, eventually enhancing catalytic efficiency. Catalytic testing demonstrated that Cu@hieS-1 achieved 96% ethanol conversion and 82% acetaldehyde yield at 400 °C, outperforming conventional zeolites (15% ethanol conversion and 12% acetaldehyde yield). The reason for the improved catalytic activity over Cu@hieS-1 compared to the conventional ones relates to the fact that Cu@hieS-1 contains a higher proportion of Cu+ species compared with the others, eventually leading to promoting acetaldehyde formation. Additionally, hierarchical zeolites exhibited enhanced catalytic stability, maintaining ∼80% conversion and 82% acetaldehyde yield. This work illustrates the benefits of the encapsulated catalyst in optimizing catalytic performances for sustainable acetaldehyde production.

Sooknoi, Tawan

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