Teerawatananond, Thapong

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College of Innovation and Industrial Management

thapong.te@kmitl.ac.th

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Sustainable Liquid-Phase Selective Hydrogenation of CO2 to C1–C3 Alcohols over Mg-, Zn-, and Pt-Modified Copper Phyllosilicate Catalysts: Insight Reaction Pathways
(2026-07-27)
Poson, Suttiporn
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Teerawatananond, Thapong
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Shoosri, Tanyarat
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Miyake, Takanori
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Panpranot, Joongjai
The sustainable conversion of carbon dioxide (CO<inf>2</inf>)into value-added chemicals remains a major challenge, particularly for the selective formation of C<inf>1</inf>–C<inf>3</inf> alcohols. Herein, bimetallic copper phyllosilicate catalysts (1%X-20%CuPS, X = Zn, Mg, Pt) were developed and systematically evaluated for the liquid-phase hydrogenation of CO<inf>2</inf> to alcohols compared with monometallic 20%CuPS as a benchmark. Among these catalysts, 1%Mg-20%CuPS exhibited the highest activity, excellent stability, and good reusability, highlighting the beneficial role of earth-abundant metal promotion. The enhanced performance is attributed to increased surface basicity and stronger CO<inf>2</inf> adsorption, which facilitated the formation and stabilization of formate intermediates. Concurrently, in situ reduction of Cu+/Cu0 sites promotes efficient H<inf>2</inf> dissociation and subsequent hydrogenation steps. A high surface Mg/Si ratio further stabilizes CO-derived intermediates and promotes CO-mediated C–C coupling, favoring C<inf>2</inf><inf>+</inf> alcohol formation. Zn incorporation induced similar but less pronounced effects, whereas Pt altered the reaction network, leading to increased byproduct formation and lower alcohol selectivity. After 24 h, the total alcohol selectivity followed the order 1%Mg-20%CuPS (98%) > 1%Zn-20%CuPS (88%) > 1%Pt-20%CuPS (73%) > 20%CuPS (67%). Overall, second metal modification effectively tunes catalyst properties and reaction pathways, with Mg emerging as a sustainable and industrially viable promoter for CO<inf>2</inf> valorization to C<inf>1</inf>–C<inf>3</inf> alcohols.
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Synergistic NiCo-BTC Catalysts for the Catalytic Transfer Hydrogenation of Furfural to γ-Valerolactone: Insights from Monometallic Cu-, Ni-, and Co-BTC Comparison
(2026-10-01)
Thansirisunthorn, Sudarat
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Teerawatananond, Thapong
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Shoosri, Tanyarat
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Rungtaweevoranit, Bunyarat
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Miyake, Takanori
A series of monometallic Cu-BTC, Ni-BTC, and Co-BTC catalysts was successfully synthesized via the solvothermal method to evaluate their performance in the catalytic transfer hydrogenation of furfural (FF) to γ-valerolactone (GVL). The Co-BTC and Ni-BTC catalysts exhibited higher FF conversion, selectivity, and GVL yield than Cu-BTC due to favorable redox properties of Co2+ and Ni2+ and stronger acidity that enhance substrate activation and key ring-opening and lactonization steps. To further enhance performance, bimetallic NiCo-BTC catalysts with different Ni/Co mole ratios (0.25, 0.50, 0.75, 1.00) were developed. All bimetallic NiCo-BTC catalysts outperformed the monometallic counterparts, with 0.50NiCo-BTC achieving complete FF conversion and the highest GVL selectivity and yield of 89% at 200 °C after 24 h. TEM, XPS, XANES, and NH<inf>3</inf>-TPD analyses indicated that the enhanced catalytic activity and selectivity arise from synergistic Ni-Co interactions and increased surface acidity. Time-resolved product analysis confirmed a sequential pathway with furfuryl alcohol (FA) as a key intermediate. Moreover, the 0.50NiCo-BTC catalyst exhibited good reusability over three cycles with minimal activity loss, demonstrating structural stability under reaction conditions. These results highlighted the importance of metal synergy and acid site tuning in designing highly efficient metal organic framework catalysts for biomass upgrading via catalytic transfer hydrogenation.
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Bimetallic copper- and nickel-rich Cu-Ni phyllosilicate catalysts for the liquid phase selective hydrogenation of furfural to furfuryl alcohol
(2024-12-02)
Shoosri, Tanyarat
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Chotiwilaiwan, Pisacha
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Rattanapornchaiwat, Tanisorn
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Teerawatananond, Thapong
;
Miyake, Takanori
Bimetallic Cu-Ni phyllosilicates (Cu-NiPS) with various Ni/Cu ratios (5 : 15, 10 : 10, 15 : 5 wt%) were synthesized using ammonia evaporation hydrothermal method to obtain copper-rich or nickel-rich Cu-Ni alloys. These catalysts were evaluated for the selective hydrogenation of furfural (FF) to furfuryl alcohol (FA) in the liquid phase under relatively mild conditions (100 °C, 20 bar H<inf>2</inf>). The bimetallic Cu-NiPS catalysts exhibited excellent dispersion of the Ni-Cu alloy with average particle sizes ranging from 3.8 to 4.8 nm and demonstrated significantly enhanced catalytic performance over the monometallic nickel phyllosilicate (20% NiPS). The copper-rich Ni-Cu alloy (15% Cu-5% NiPS) exhibited the highest FF conversion efficiency (88%) and FA selectivity (90%). This superior performance is attributed to its smallest particle size, higher proportion of Cu0 and the synergistic interactions between Ni and Cu. This synergy effectively stabilizes the carbonyl group while promoting efficient H<inf>2</inf> dissociation and FA desorption, thereby facilitating the hydrogenation of FF to FA. Furthermore, the catalyst exhibited excellent recyclability and maintained high conversion efficiency and selectivity over multiple cycles.
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Role of Copper Species in Copper Phyllosilicate Catalysts for the Catalytic Transfer Hydrogenation of Furfural to γ-Valerolactone
(2025-02-17)
Shoosri, Tanyarat
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Thongratkaew, Sutarat
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Rungtaweevoranit, Bunyarat
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Kraithong, Wasawat
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Faungnawakij, Kajornsak
Copper phyllosilicate (CuPS) catalysts were synthesized and evaluated for the catalytic transfer hydrogenation of furfural to γ-valerolactone (GVL). Various copper loadings (10–30 wt.%) were studied to elucidate the impact of copper species on catalytic performance. Notably, a high dispersion of copper (%D<inf>Cu</inf> ≈ 70%) and a substantial BET surface area (620 m2/g) were achieved, even at the maximum copper loading of 30 wt.%. TR-XANEs and XPS analyses identified the two geometric structures of Cu2⁺ on the CuPS catalysts; square planar and octahedral alongside Cu⁺/Cu⁰ species were formed upon reduction at temperatures exceeding 200 °C. The reduced 30% CuPS-R catalyst, enriched in metallic Cu⁰, achieved complete conversion of furfural, but exhibited low GVL selectivity (22%). Conversely, the as-synthesized 30% CuPS, predominantly composed of Cu2⁺, showed a lower furfural conversion (14%) but higher selectivity for GVL (37%). The physical mixing of 30% CuPS-R and 30% CuPS in a 50:50 ratio yielded the best catalytic performance, resulting in 100% furfural conversion and 86% GVL selectivity. The findings suggest that metallic Cu⁰ is essential for initiating the conversion of furfural, while Cu2⁺ plays a critical role in GVL formation. An optimal Lewis/Brønsted acidity (L/B) ratio of 5.7 is proposed for the mixed catalysts. The proposed reaction mechanism underscores the complex interplay between different copper species and acid sites, emphasizing the need for optimizing both metal and acid functionalities in catalyst design.

Teerawatananond, Thapong

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