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Tailoring Re-loaded core–shell Ni structures embedded in mesoporous silica for the selective transformation of levulinic acid into γ-valerolactone
(2026-05-21)
Maneewong, Yupawan
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Lakhani, Pratikkumar
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Ratchahat, Sakhon
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Sakdaronnarong, Chularat
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Limphirat, Wanwisa
Heterogeneous core–shell catalysts have attracted significant interest because they integrate multiple catalytic functions within a single, precisely engineered architecture. In this work, we report the rational synthesis and catalytic evaluation of a Re-loaded Ni core–shell catalyst embedded in mesoporous silica for the efficient hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). The core–shell configuration enables effective confinement of Ni nanoparticles within the porous silica matrix and stabilizes spatially separated Ni and ReO<inf>X</inf> species with complementary catalytic functions. Comprehensive physicochemical characterization confirmed the successful formation of the core–shell structure, its high structural stability, and the presence of confined metallic Ni sites responsible for H<inf>2</inf> activation and oxophilic ReO<inf>X</inf>-derived acid sites for oxygenate activation. Under optimized conditions, the Ni<inf>12</inf>Re<inf>1.63</inf>-CS catalyst achieved complete LA conversion with a GVL yield exceeding 94% within 2 h, outperforming non-core-shell catalysts. The catalyst also displayed high intrinsic activity, with a turnover frequency of up to ∼36 h−1, and retained an excellent GVL selectivity of approximately 80% during recycling, despite a gradual decrease in LA conversion. These findings demonstrate that spatial separation of hydrogenation and oxophilic adsorption sites within a core–shell architecture is critical for enhancing activity and selectivity in biomass-derived platform molecule upgrading.
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Design of a rhenium-decorated mesoporous nickel phyllosilicate-derived Ni–Re/MCM-41 catalyst for efficient hydrogenation of levulinic acid to γ-valerolactone
(2026-04-27)
Maneewong, Yupawan
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Lakhani, Pratikkumar
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Ratchahat, Sakhon
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Sakdaronnarong, Chularat
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Limphirat, Wanwisa
Herein, Ni and NiRe catalysts supported on mesoporous MCM-41 were synthesized through ammonia evaporation (AE) and impregnation (IM) routes to explore structure–activity correlations in the hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). The AE-derived nickel phyllosilicate (Ni-PS) framework provided strong interactions through Ni–O–Si linkages, leading to high dispersion and stabilization of Ni species. Incorporation of Re significantly improved reducibility, hydrogen activation, and the balance between acidic and metallic sites, resulting in enhanced catalytic efficiency. The optimized NiRe-PS catalyst exhibited a uniform nanostructure, strong Ni–Re synergy, and the highest metallic Ni fraction, which collectively promoted superior activity and stability. Under mild conditions (140 °C, 10 bar H<inf>2</inf>), NiRe-PS achieved complete LA conversion and ∼96% GVL yield within 4 h, with a turnover frequency of 26.3 h−1 (160 °C, 10 bar H<inf>2</inf>) and with an apparent rate constant of 0.0059 min−1. Mechanistic and isotopic investigations confirmed that both molecular and solvent-derived hydrogen contributed to the hydrogenation pathway. The exceptional activity, recyclability, and structural robustness of NiRe-PS demonstrate the potential of phyllosilicate-based bimetallic systems as efficient, non-noble catalysts for sustainable biomass valorization.
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Highly active and stable Ni–W/SiO2 catalyst derived from W incorporated on Ni phyllosilicate for deoxygenation of triglycerides into green biofuel range hydrocarbons
(2025-10-01)
Praikaew, Wanichaya
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Prameswari, Jedy
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Ratchahat, Sakhon
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Chaiwat, Weerawut
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Sakdaronnarong, Chularat
Highly active and stable Ni–W/SiO<inf>2</inf> catalyst derived from W incorporated into Ni phyllosilicate (Ni-PS) was prepared by the ammonia evaporation (AE) method, and benchmarked with the catalyst prepared by the impregnation method (IM). Their catalytic activities were evaluated for deoxygenation of triglycerides into green biofuel-range hydrocarbons. The Ni-PS structure demonstrated a large surface area with strong interaction between Ni2+ and SiO<inf>2</inf>, resulting from the incorporation of Ni2+ into the silica framework, which led to highly dispersed Ni⁰ after H<inf>2</inf> reduction. Additionally, the H<inf>2</inf> adsorption and desorption capabilities, together with a substantial quantity of Lewis acid sites, were advantageous features of Ni-PS catalysts compared to Ni-IM and 5 W/Ni-IM catalysts. Ex situ and in situ structural characterizations revealed the generation of Ni⁰ and W⁰ states, along with remaining W4+ species after H<inf>2</inf> reduction. The 5 W/Ni-AE catalyst exhibited stable performance up to 60 h on stream, producing consistent yields of 30 % jet fuel and 40 % diesel, which was attributed to its high porosity, small Ni⁰ particle sizes, enhanced H<inf>2</inf> adsorption–desorption capacities, and abundant Lewis acid sites. Consequently, the heterogeneous 5 W/Ni-AE catalyst shows significant practical relevance for generating green biofuel from oil-derived feedstock in sustainable biorefineries.
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Nanoarchitectonics of carbon-based electrodes via activated carbon/carbon composite xerogels by CO2
(2025-09-01)
Sirichan, Kasawan
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Kraiwattanawong, Kriangsak
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Bumroongsakulsawat, Palang
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Assabumrungrat, Suttichai
Carbon/carbon (C/C) composites, characterized by trimodal porous structures and highly tunable surfaces, offer promising prospects for electrochemical applications within the framework of nanoarchitectonics. However, recent research lacks systematic investigations into property-controlled performance. This study explores the effects of functional groups, surface area, and pore architecture in CO<inf>2</inf>-activated C/C composite xerogels synthesized from resorcinol-formaldehyde (RF) sol and cotton fibers (CFs). Increased activation time and CF content enhanced porosity, functional group density (O[sbnd]H and C[dbnd]O), and structural disorder. The macropores introduced by CFs facilitated deeper CO<inf>2</inf> penetration, thereby increasing meso‑ and microporosity, surface area, and specific capacitance. Electrochemical performance measured through cyclic voltammetry and charge/discharge analysis revealed that capacitance was governed primarily by surface area rather than pore geometry. Specific capacitance and surface area increased from 144 to 344 F g⁻¹ and from 575 to 1471 m² g⁻¹, respectively, under 0.5 A g⁻¹ discharge.
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Comparative CFD modeling of foam and conventional pellet catalysts in glycerol steam reforming
(2025-07-15)
Simasatitkul, Lida
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Phitchayakorn, Chattharika
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Amornraksa, Suksun
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Anantpinijwatna, Amata
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Assabumrungrat, Suttichai
A novel approach to glycerol valorization via steam reforming was investigated through computational fluid dynamics (CFD) modelling. The performance characteristics of conventional pellet catalysts were compared with foam catalysts in a 6-inch diameter packed bed reactor. A two-dimensional pseudo-homogeneous steady-state model was employed to evaluate catalyst configurations ranging from 10 to 30 pores per inch (PPI). The foam catalyst structures exhibited superior performance across key metrics, achieving maximum hydrogen yield (60 %) at one-third of the reactor length whilst reducing pressure drop by 95 % compared to conventional pellets. Within the foam configurations, the 10PPI variant demonstrated optimal performance characteristics, with an 80 % reduction in normalized pressure drop compared to 30PPI, whilst maintaining comparable product yields. The enhanced performance was attributed to the open-cell architecture, which facilitated improved mass transfer and reduced diffusion limitations. These findings suggest that foam catalysts represent a promising alternative to conventional pellet configurations for glycerol steam reforming processes.
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Potential of advanced microporous zeolites and mesoporous materials derived from natural precursors as supports for iron phosphide catalysts in bio-jet fuel production from palm oil (Elaeis guineensis)
(2025-06-10)
Tanwongwan, Worapak
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Sartsamai, Ruttasart
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Kaewmeesri, Rungnapa
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Faungnawakij, Kajornsak
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Chollacoop, Nuwong
Iron phosphide (FeP) has emerged as an efficient catalyst for converting palm oil, a biomass-derived feedstock, into bio-jet fuel through the hydrocracking process. The catalytic performance of FeP is strongly influenced by the choice of support material. In this study, microporous MWW-type zeolites (MCM-22 and MCM-36) and mesoporous materials (MCM-41 and MCM-48) were successfully synthesized from entirely natural precursors, silica derived from rice husk and aluminosilicate gel extracted from kaolin clay, via a hydrothermal method, and employed as supports for FeP catalysts. Among these materials, MCM-22 zeolite exhibited the highest microporosity, followed by zeolite MCM-36, resulting in superior acidity compared to the mesoporous materials, MCM-41 and MCM-48. FeP supported on MCM-22 (FeP/MCM-22) demonstrated the best catalytic performance, liquid hydrocarbon yield (∼33%), and bio-jet selectivity (∼78%) were obtained, outperforming FeP/MCM-36, FeP/MCM-41, and FeP/MCM-48. This is due to its high surface area of micropores (∼187 m2 g−1) and the excellent acidity of this zeolite, which helped prevent FeP overloading and promote uniform metal distribution. Furthermore, it exhibited remarkable stability and reusability, with performance improving over three consecutive reaction cycles, LHCs yield increasing to 50% and bio-jet selectivity stabilizing at about 83%, attributed to enhanced acidity accessibility and progressive formation of the FeP active phase.
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Process Improvement and Economic and Environmental Evaluation of Bio-Hydrogenated Diesel Production from Refined Bleached Deodorized Palm Oil
(2025-01-01)
Anantpinijwatna, Amata
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Simasatitkul, Lida
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Yooyen, Kanokporn
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Amornraksa, Suksun
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Assabumrungrat, Suttichai
The co-production of BHD with other renewable fuels (i.e., using a novel process involving carbon dioxide utilization to achieve the global sustainability goal) is presented. The three configurations of BHD production from refined bleached deodorized palm oil (RBDPO), including (1) the conventional BHD process with hydrogen recovery (BHD process), (2) the BHD process coupled with the Fischer–Tropsch process (BHD-FT process), and (3) the BHD process coupled with the bio-jet fuel and methanol processes (BHD-BIOJET-MEOH process) are investigated using the process model developed in Aspen Plus. The effect of the operating parameters is studied, and the condition of each process offering the highest BHD yield is proposed. Then, the pinch analysis and heat exchanger network (HEN) design of each proposed process are performed to find the highest energy-efficient configuration. The economic and environmental analysis is later performed to investigate the sustainability performance of each configuration. The conventional BHD process requires less hydrogen and consumes less energy than the others. The BHD-BIOJET-MEOH process is the most economically feasible, offering the highest net present value (NPV) of USD 7.93 million and the shortest payback period of 3 years and 1 month. However, it offers the highest carbon footprint of 0.820 kgCO<inf>2</inf> eq./kg of BHD, and it presented the highest potential environmental impact (PEI) in all categories.
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Nanoporous Carbon-Supported Bimetallic (Ni, Cu, and Fe)-Mo Catalysts for Partial Hydrogenation of Biodiesel
(2024-10-15)
Jaruwat, Dolrudee
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Kaewtrakulchai, Napat
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Siriorarnroj, Siwat
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Srifa, Atthapon
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Kiatkittipong, Worapon
Upgrading biodiesel or hydrogenated fatty acid methyl esters (H-FAMEs) by partial hydrogenation is a second-generation biofuel with high specific fuel characteristics, such as superior cold flow properties, higher oxidative stability, and lower hazardous gas emissions, allowing this biofuel to provide excellent fuel properties, over conventional biodiesel. This study assessed the potential of using nanoporous carbon produced from cattail leaves (CL) as an alternative catalyst support. We synthesized various catalysts including monometallic Mo/NPC, Ni/NPC, Ce/NPC, and Fe/NPC catalysts, as well as bimetallic molybdenum-based catalysts doped with nickel, copper, or iron for the partial hydrogenation of soybean biodiesel. The NPC support demonstrated a surface area (S<inf>BET</inf>) of approximately 1,323 m2g-1, which greatly increases the catalytic activity through the efficient dispersion of catalyst active sites. The partial hydrogenation reaction of soybean FAME over the MoNi/NPC catalyst obtained the highest catalytic activity with enhanced oxidation stability from 3 to 14 h, and the cloud point and pour point increased from 2 to 13 °C and −1 to 10 °C, respectively. Hence, the selection of catalysts is crucial due to their impact on the feasibility of the process and its economic viability. This article focuses on highlighting the effectiveness of a highly promising catalyst for partial hydrogenation as well as examining the variables that influence the primary reaction pathway.
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Bimetallic PdNi catalyst on cattail Leaves-Derived nanoporous carbon support for synthesis of partially hydrogenated fatty acid methyl ester (H-FAME)
(2024-06-01)
Longprang, Tripob
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Kaewtrakulchai, Napat
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Kiatkittipong, Worapon
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Srifa, Atthapon
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Chollacoop, Nuwong
Cattail leaves (CL) have been used as a carbon source to synthesize nanoporous carbon (NPC) support with high surface area (S<inf>BET</inf> = 2002.12 m2g−1) via hydrothermal carbonization and potassium hydroxide (KOH) activation. The studied catalysts, including monometallic Pd/NPC and Ni/NPC, and bimetallic PdNi/NPC, were synthesized and characterized by using several techniques (e.g., scanning electron microscopy, transmission electron microscopy, nitrogen sorption, Fourier transform infrared spectroscopy, thermogravimetric analysis, and X-ray diffraction). Their catalytic activity toward partial hydrogenation of palm biodiesel to H-FAME was tested, and the liquid product composition, cloud point, and oxidation stability were determined. The studied catalysts have a high porosity with the S<inf>BET</inf> of approximately 2037.34–2187.96 m2g−1 led to excellent metal dispersion. Although Ni did not show high catalytic activity compared to Pd, Ni incorporated with Pd as PdNi/NPC catalyst significantly increased the cis-C18:1 selectivity and prevented the catalytic deactivation during the partial hydrogenation. The oxidation stability of palm biodiesel feedstock was increased from 13.69 to 17.12 h while the cloud points adversely increased by only 3 degrees from 12 to 15 °C (still lower than 16 °C of the Thai industrial recommendation) with bimetallic PdNi/NPC catalyst. The main benefit of bimetallic PdNi/NPC over monometallic Pd/NPC and Ni/NPC is shown through not only higher C18:2 conversion but also much higher cis-to-trans ratio of C18:1 resulting in higher oxidation stability with acceptable compromise on the cloud point increasing. Consequently, the produced palm H-FAME can be used at a high blend ratio.
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Biofuel upgrading via catalytic deoxygenation in trickle bed reactor: Crucial issue in selection of pressure regulator type
(2024-01-01)
Pongsiriyakul, Kanokthip
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Kiatkittipong, Worapon
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Lim, Jun Wei
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Najdanovic-Visak, Vesna
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Wongsakulphasatch, Suwimol
Trickle bed reactors (TBRs) are commonly used in various chemical and associated processes. The selection of a proper back pressure regulator (BPR) is crucial for maintaining the system's upstream pressure. In this study, we investigate the impact of BPR selection on deoxygenation reaction in a TBR with two typical types of BPR, including gas-phase type back pressure regulator (Gas-BPR) and multiphase type back pressure regulator (Multi-BPR). Notably, Gas-BPR introduces interruptions and pressure drops during the sampling step, impacting the hydrogen flow rate, while Multi-BPR ensures more consistent hydrogen flow. To examine the performance of BPR systems, hydrotreating experiments were conducted at 330 °C, 50 bar of hydrogen over Ni/γ-Al<inf>2</inf>O<inf>3</inf> catalyst using crude Pongamia pinnata oil as a feedstock and refined palm olein as a benchmark. Insignificant difference in the reaction performance between Multi-BPR and Gas-BPR systems was observed when using refined palm olein. Interestingly, there was a significant difference between the two systems when feeding with crude Pongamia pinnata oil. The multi-BPR system demonstrated superior performance, achieving 100% conversion of the feedstock over a prolonged period compared to the interrupted hydrogen flow in the Gas-BPR system. Further characterization of fresh and spent catalysts using N<inf>2</inf> sorption, XRD, SEM-EDS and TGA-DTG-DSC techniques revealed that a gum and coke formation was a reason for the rapid catalyst deactivation. Furthermore, the interrupted flow in the Gas-BPR system led to substantial gum production, ultimately causing a blockage in the reactor bed. Consequently, for feedstocks with high impurities, a robust continuous flow of hydrogen is essential. Thus, the study strongly recommends selecting Multi-BPR for continuous operation in TBRs to enhance efficiency and avoid catalyst deactivation.

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