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Silica-supported nanostructured copper phyllosilicate: Boosting stability, capacity, and conductivity of Li-ion battery Si-based anodes
(2026-11-01)
Shajan, Minnu Gemini
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Chou, Feng Yuan
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Prasanseang, Warot
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Yimtrakarn, Trakarn
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Sooknoi, Tawan
Explosive demand for large-scale rechargeable batteries has driven the search for alternative electrode materials with higher energy density, lower toxicity, lower cost, and more natural abundance. Si-based materials, e.g., Si, SiO, SiO<inf>2</inf>, and silicates have emerged as promising choices, with extremely high capacities from most cost-effective and abundant sources. However, these compounds still suffer from major issues, such as extreme volume change, poor cycling stability, high manufacturing costs, and low conductivity. Herein, we have prepared low-cost porous nanosized silica-supported copper phyllosilicate, x CuPS/SiO<inf>2</inf>, with different Cu loadings and investigated them as anode material in Li cells. Due to the highly dispersed Cu species strongly interacted with nanosphere SiO<inf>2</inf> support matrix, 20CuPS/SiO<inf>2</inf> has been found to deliver a capacity as high as ∼3550 mAh g‒1 at 500 mA g‒1 with an impressive capacity retention of 99% upon conversion reactions with Li+, and a reversible capacity of 2216 mAh g‒1 at 5000 mA g‒1. These values are among the highest ever reported for Si-, silicate-, silica-, and copper oxide-based anodes. Various phases, i.e., CuO, Li<inf>4</inf>SiO<inf>4</inf>, SiO, Si, Li<inf>2</inf>O, Cu, and Li<inf>x</inf>Si, are formed in the SiO<inf>2</inf> nanodomain, as confirmed by various ex situ characterization techniques, and the redox mechanism has been proposed. The components, particularly Li<inf>4</inf>SiO<inf>4</inf>, Li<inf>2</inf>O, and SiO<inf>2</inf>, are shown to help buffer volumetric or structural changes induced by the redox processes. The nanosized composite and the in situ -formed metallic Cu play a crucial role in rapid charge-transfer kinetics. These synergistic effects ultimately result in an unprecedented electrochemical performance of x CuPS/SiO<inf>2</inf> observed in this work.
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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.
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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
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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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Linear long-chain α-olefins from hydrodeoxygenation of methyl palmitate over copper phyllosilicate catalysts
(2022-04-05)
Prasanseang, Warot
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Choojun, Kittisak
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Poo-arporn, Yingyot
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Huang, Ai Lin
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Lin, Yu Chuan
Copper phyllosilicate (CuPS) was used as a bifunctional catalyst for hydrodeoxygenation of methyl palmitate (MP) to produce long-chain α-olefins without the loss of carbon backbone. The CuPS catalysts were prepared by ammonia evaporation-hydrothermal method. The crystal structure, surface area, reducibility, Cu dispersion, Cu particle size and acidity of the catalysts were examined by XRD, BET, H<inf>2</inf>-TPR, TEM, NH<inf>3</inf>-TPD and Py-IR. The existence of Cu2+ species (octahedral (O<inf>h</inf>)/square planar (Sq)), Cu+ and Cu0 upon calcination/reduction was investigated by in situ TR-XANES. The Cu dispersion was related to the Cu+ fraction in CuPS, while Brønsted acid sites (BAS) depends on Cu0 particles. The MP conversion to 1-hexadecene proceeds via hydrogenation-dehydration promoted by the synergy of Cu0 surface and Brønsted acid sites at the interface. The α-olefin selectivity depends on a balance between Cu+ and Cu loading. The 20CuPS possessing 10% Cu+ fraction, provides a high conversion of 72% with 45% α-olefin selectivity.

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