Energy transfer properties of novel coumarin-perylene bisimide dendrimer are studied by means of steady state and time-resolved UV/vis spectroscopy. At low donor excitation density fast (transfer rate approximately 10 ps(-1)) and efficient (quantum yield approximately 99.5%) donor-acceptor energy transfer is observed. The random distributions of donor-acceptor orientations and distances result in nonexponential energy transfer kinetics. The energy transfer remains independent of excitation density up to densities corresponding to one absorbed photon per 10 dendrimer molecules. At higher excitation densities the transfer rate is found to increase due to excitation of multiple donors per dendrimer. Control of the donor-acceptor energy transfer rate is achieved by pre-excitation of the acceptor and monitored by prepump-pump-probe experiments, which show that the energy transfer rate can be decreased by a factor of 2. The relative orientations of transition dipole moments in the donor and acceptor molecules are found to be one of the key factors determining the energy transfer dynamics at high excitation densities.
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Adv Mater
January 2025
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, SAR, 999077, P. R. China.
Electrochemically converting nitrate (NO ) to value-added ammonia (NH) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH electrosynthesis.
View Article and Find Full Text PDFAdv Mater
January 2025
Extreme Materials Research Center, Korea Institute of Science and Technology, 14-gil 5 Hwarang-ro, Seongbuk-gu, Seoul, 02792, Republic of Korea.
Hydrogen peroxide (HO) electrosynthesis via the 2e oxygen reduction reaction (ORR) is considered as a cost-effective and safe alternative to the energy-intensive anthraquinone process. However, in more practical environments, namely, the use of neutral media and air-fed cathode environments, slow ORR kinetics and insufficient oxygen supply pose significant challenges to efficient HO production at high current densities. In this work, mesoporous B-doped carbons with novel curved BC active sites, synthesized via a carbon dioxide (CO) reduction using a pore-former agent, to simultaneously achieve excellent 2e ORR activity and improved mass transfer properties are introduced.
View Article and Find Full Text PDFSmall
January 2025
College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, P. R. China.
Nickel hydroxide (Ni(OH)) is considered to be one of the most promising electrocatalysts for urea oxidation reaction (UOR) under alkaline conditions due to its flexible structure, wide composition and abundant 3D electrons. However, its slow electrochemical reaction rate, high affinity for the reaction intermediate *COOH, easy exposure to low exponential crystal faces and limited metal active sites that seriously hinder the further improvement of UOR activities. Herein it is reported electrocatalyst composed of rich oxygen-vacancy (O) defects with amorphous SeO-covered Ni(OH) (O-SeO/Ni(OH)).
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Department of Physics, Assam University, Silchar-788011, India.
Density functional theory has been employed to study indolo[3,2,1-]carbazole donor-based dyes, incorporating one and two units of 2,4-dimethoxybenzene auxiliary donors. Electrostatic potential analysis highlights the dye with one auxiliary donor (D2) as having the highest charge-donating capability. Structural analysis shows that auxiliary donors enhance planarity, reduce steric hindrance, and improve π-conjugation.
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January 2025
School of Physics and Electronic Science, East China Normal University, Shanghai, 200062, P. R. China.
Multiple resonance (MR)-type thermally activated delayed fluorescence (TADF) emitters have garnered significant interest due to their narrow full width at half maximum (FWHM) and high electroluminescence efficiency. However, the planar structures and large singlet-triplet energy gaps (ΔEs) characteristic of MR-TADF molecules pose challenges to achieving high-performance devices. Herein, two isomeric compounds, p-TPS-BN and m-TPS-BN, are synthesized differing in the connection modes between a bulky tetraphenylsilane (TPS) group and an MR core.
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