Plasmonic materials convert light into hot carriers and heat to mediate catalytic transformation. The participation of hot carriers (photocatalysis) remains a subject of vigorous debate, often argued on the basis that carriers have ultrashort lifetime incompatible with drive photochemical processes. This study utilises plasmon hot electrons directly in the photoelectrocatalytic reduction of CO to CO via a Ppasmonic nanohybrid.
View Article and Find Full Text PDFPlasmonic systems convert light into electrical charges and heat, mediating catalytic transformations. However, there is ongoing controversy regarding the involvement of hot carriers in the catalytic process. In this study, we demonstrate the direct utilisation of plasmon hot electrons in the hydrogen evolution reaction with visible light.
View Article and Find Full Text PDFJ Phys Chem Lett
July 2023
Optical upconversion via a multiphoton absorption process converts incoherent low-energy photons to shorter wavelengths. In this contribution, we report a solid-state thin film for infrared-to-visible upconversion composed of plasmonic/TiO interfaces. When excited at λ = 800 nm, three photons are absorbed, leading to the excitation of TiO trap states into an emissive state in the visible domain.
View Article and Find Full Text PDFBacteria organized in biofilms show significant tolerance to conventional antibiotics compared to their planktonic counterparts and form the basis for chronic infections. Biofilms are composites of different types of extracellular polymeric substances that help in resisting several host-defense measures, including phagocytosis. These are increasingly being recognized as a passive virulence factor that enables many infectious diseases to proliferate and an essential contributing facet to anti-microbial resistance.
View Article and Find Full Text PDFThe growing energy demand with the widespread use of smart portable electronics, as well as an exponential increase in demand for smart batteries for electric vehicles, entails the development of efficient portable batteries with high energy density and safe power storage systems. Li-ion batteries arguably have superior energy density to all other traditional batteries. Developing mechanically robust solid-state electrolytes (SSEs) for lithium-ion conduction for an efficient portable energy storage unit is vital to empower this technology and overcome the safety constraints of liquid electrolytes.
View Article and Find Full Text PDFCrystalline two-dimensional organic nanosheets (2D-ONs) having atomic or near-atomic thickness with infinite lateral dimensions are of crucial significance for their possible application as a material for energy storage. The presence of nanofluidic channels with a designed array of molecular interlayers in such 2D-ONs, for a favorable lithium-ion transport, has special significance for improving the efficacy of lithium-ion batteries. However, the rational design of crystalline 2D-ONs remains a challenge because of the lack of appropriate monomers and convenient preparation methods.
View Article and Find Full Text PDFPurpose-built molecules that follow the fundamental process of photosynthesis have significance in developing better insight into the natural photosynthesis process. Quinones have a significant role as electron acceptors in natural photosynthesis, and their reduction is assisted through H-bond donation or protonation. The major challenge in such studies is to couple the multielectron and proton-transfer process and to achieve a reasonably stable charge-separated state for the elucidation of the mechanistic pathway.
View Article and Find Full Text PDFBiofouling refers to the undesirable process that leads to the accumulation of microorganisms such as bacteria or fungi on substrates. This is one of the major concerns associated with several components of our regular life such as food, health, water and energy. In the healthcare sector, biofouling on medical devices is known to cause infections, which are often resistant to conventional antibiotics and lead to increase in the number of hospital and surgery-related deaths.
View Article and Find Full Text PDFDespite the recent surge of interest in two-dimensional (2D) inorganic nanosheets derived from photoactive coordination polymers of lanthanide ions having interesting optical properties, research in this area is still in its infancy. Luminescent lanthanide ions, Eu(iii) or/and Tb(iii), as well as a bis-terpyridine ligand (L), were used in this study as the building blocks for the synthesis of the archetypical layered structure of coordination polymers (CPs) (L·Eu/L·Tb). 2D-nanosheets were obtained through exfoliation of the layered precursor of CPs in a suitable solvent system following a sonication-assisted strategy.
View Article and Find Full Text PDFQuinones play a significant role as primary electron acceptors in the natural photosynthetic system of photosystem II, and their reduction is known to be facilitated by hydrogen-bond donors or protonation. In this study, a ruthenium(ii) polypyridyl complex 1 coupled to an anthraquinone (AQ) functionality through a rigid imidazole (Im) spacer has been synthesized to examine the effect of H-bonding on both the thermal and photoinduced electron transfer reactions. The anthraquinone moiety of complex 1 is fused to a benzi-imidazole system bearing C[double bond, length as m-dash]OAQHNIm based H-bonding at one side of the anthraquinone moiety so that intramolecular hydrogen bonding from the imidazole group to the nearby quinone carbonyl can occur.
View Article and Find Full Text PDFWe report here a smart functional low molecular weight gelator (LMWG) L, containing an unusual metal ion coordination site, i.e. "half-crown/two carbonyl".
View Article and Find Full Text PDFSelf-assembly of suitable molecular building blocks is an efficient and convenient approach to generate nanomaterials with various morphologies and functions. Moreover, understanding the nature of molecules and controlling factors of their self-assembly process is crucial in fundamental aspects of molecular self-assembly which provide insights into the design of new assemblies with functional nano-architectures. To this end, the present study reports water induced self-assembled multifaceted morphology formation and the plausible pathway of the morphology transformation of a single poly(aryl ether) dendron amphiphile 1(D).
View Article and Find Full Text PDFThe proton-coupled electron-transfer (PCET) reaction is investigated for a newly synthesized imidazole-anthraquinone biomimetic model with a photoactive Ru -polypyridyl moiety that is covalently coupled to the imidazole fragment. Intramolecular H-bonding interactions between imidazole and anthraquinone moieties favor the PCET process; this can be correlated to an appreciable positive shift in the one-electron reduction potential of the coordinated anthraquinone moiety functionalized with the imidazole fragment. This can also be attributed to the low luminescence quantum yield of the Ru -polypyridyl complex used.
View Article and Find Full Text PDFBinary pseudorotaxane formation between an aza crown derivative as host (H) and two different imidazolium derivatives as guests (G and G) have been studied in detail by NMR (H NMR, 2D NOESY), optical (steady state electronic and emission spectroscopy), and mass spectroscopy. Binding stoichiometry (1:1), association constant for the respective [2]pseudorotaxane formation (K = (2.61 ± 0.
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