Journal of Fuel Chemistry and Technology•2026•DOI: 10.1016/S1872-5813(26)60643-3
The adsorption behavior and electron transfer mechanism of CO on Ptn/γ-Al2O3 catalysts (n = 4, 13) were systematically investigated using density functional theory (DFT) calculations, complemented by infrared (IR) spectroscopy, electron difference density (EDD), and charge decomposition analysis (CDA). The study reveals that Pt cluster size critically governs the adsorption configuration, electron transfer, and C–O vibrational frequency. For small Pt4 sub-nanometric clusters, highly unsaturated Pt atoms exhibit strong d-electron back-donation, leading to substantial filling of CO π* antibonding orbitals, significant weakening of the C–O bond, and a redshift in IR frequency. Conversely, large Pt13 clusters, characterized by dense structures and electron delocalization, exhibit weakened back-donation, enhanced C–O bonding, and a blueshift. The electron transfer intensity follows the order: linear < bridge < multi-terminal adsorption. Bridge adsorption is most sensitive to cluster size, displaying an IR blueshift of 81 cm−1 when Pt atoms increase from 4 to 13. Multi-terminal adsorption shows stable frequencies due to a 'saturation effect'. This study establishes a comprehensive correlation among Pt size, electronic structure, adsorption properties, and infrared response, providing atomic-scale theoretical guidance for designing efficient Pt-based catalysts with optimized CO adsorption strength and resistance to poisoning.
SCIENCE CHINA Materials•2026•DOI: 10.1007/s40843-025-4079-4
Utilization of ultrahigh-nickel LiNi_xCo_yMn_1-x-yO_2 (NCM) (x > 0.97) in Li-ion batteries can distinctively boost energy density through enhanced discharge capacity. However, capacity and thermal stability deteriorate as Ni content approaches the limit. Here, we propose a facile strategy by introducing high-valence tungsten (W) into ultrahigh-nickel polycrystalline LiNi_0.98Co_0.01Mn_0.01O_2 (PCNCM98). W-doped PCNCM98 (W-PCNCM98) exhibits refined, compactly stacked primary particles, whereas PCNCM98 shows equiaxial, non-uniform larger particles. The refined microstructure enhances mechanical strength: average particle hardness of W-PCNCM98 is 104 MPa, 1.5 times higher than PCNCM98 (68 MPa). This improved mechanical property suppresses lattice volume changes and relieves microcrack formation from H2–H3 phase transition. Consequently, cycling performance in pouch-type full cells is significantly enhanced, with capacity retention of 73% after 2000 cycles at 1 C and 25 °C, 54% higher than PCNCM98. Enhanced structural stability and strong electron affinity of W6+ also improve thermal stability: exothermic peak for W-PCNCM98 is postponed to 203 °C with heat generation of 1287 J g−1, versus 190 °C and 1528 J g−1 for PCNCM98. This high-valent doping strategy stabilizes ultrahigh-nickel NCM cathodes, accelerating large-scale EV applications.
SCIENCE CHINA Materials•2025•DOI: 10.1007/s40843-025-3522-7
Scalable printing of stretchable conjugated polymer films is essential for low-cost, large-area wearable electronics, yet achieving optimal film morphology that simultaneously enhances energy dissipation and charge transport remains a critical challenge. This study demonstrates large-area stretchable conjugated polymer films with low crystallinity but strong chain alignment, fabricated by simultaneously regulating fluid field and solidification dynamics during bar-coating. The strong fluid field aligns polymer chains in the coating direction and promotes solution aggregation in the initial wet layer, while sequential rapid solidification restricts crystallization and facilitates aggregate alignment, forming highly-aligned nanofiber networks within the elastomer phase. These elastomer-constrained nanofiber networks maintain connectivity under strain, providing efficient charge transport channels. The resulting films exhibit high charge mobilities of 6.11 and 2.98 cm2 V−1 s−1 at 0% and 100% strains, respectively, among the highest reported for stretchable conjugated polymer films. The films also achieve a high X-ray sensitivity of 1757.2 μC Gyair−1 cm−2 and an ultralow detection limit of 72.5 nGyair s−1, with maintained imaging capability before and after stretching. This work establishes a robust morphology control strategy for high-performance, large-area stretchable conjugated polymer films, advancing their practical application in wearable electronics.