Covalent functionalisation with alkyl tails is a common method for supporting molecular catalysts and photosensitisers onto lipid bilayers, but the influence of the alkyl chain length on the photocatalytic performances of the resulting liposomes is not well understood. In this work, we first prepared a series of rhenium-based CO 2 -reduction catalysts [Re(4, 9, 12, 15, 17, and 19). We then prepared a series of PEGylated DPPC liposomes containing RuC n and ReC n , hereafter noted C n , to perform photocatalytic CO 2 reduction in the presence of sodium ascorbate. The photocatalytic performance of the C n liposomes was found to depend on the alkyl tail length, as the turnover number for CO (TON) was inversely correlated to the alkyl chain length, with a more than fivefold higher CO production (TON = 14.5) for the C 9 liposomes, compared to C 19 (TON = 2.8). Based on immobilisation efficiency quantification, diffusion kinetics, and time-resolved spectroscopy, we identified the main reason for this trend: two types of membranebound RuC n species can be found in the membrane, either deeply buried in the bilayer and diffusing slowly, or less buried with much faster diffusion kinetics. Our data suggest that the higher photocatalytic performance of the C 9 system is due to the higher fraction of the more mobile and less buried molecular species, which leads to enhanced electron transfer kinetics between RuC 9 and ReC 9 .
Contemporary devices for glucose monitoring predominantly
rely
on finger-pricked blood through an enzyme-catalyzed reaction. However,
the enzymes are highly expensive, unstable, and require complex procedures
for integration with the sensing matrix, rendering strategic replacement
by nonenzymatic sensors. Here, a nonenzymatic glucose sensor is developed
based on surface engineering of laser scribed graphene (LSG)an
immerging 3D patterned graphenethat combines binder-free,
highly porous, conducting graphitic carbon network. An easy and green
method is developed to engineer the LSG surface by conformal anchoring
of copper oxide nanoparticles (CuO NPs) of optimized NP size for enhancing
its catalytic efficacy. The device shows excellent nonenzymatic glucose
sensing performance (0.4 V detection potential vs printed Ag/AgCl
reference electrode, <0.2 s response time, 0.1 μM detection
limit, 1 μM-5 mM linearity, and high selectivity). Noteworthy,
the device exhibits high stability and reproducibility for glucose
in human body fluids (whole blood, serum, sweat, and urine). In addition,
conformal transfer of LSG to commercial Scotch brand tape (LSGST) enables wearability of the device on curvilinear body parts,
exemplified through miniaturized devices monitoring glucose in sweat
directly. These findings pave a new path for a comprehensive personalized
healthcare strategy by accurate nonenzymatic detection of glucose
from human body fluids.
BODIPY heterochromophores, asymmetrically substituted with perylene and/or iodine at the 2 and 6 positions were prepared and investigated as sensitizers for triplet‐triplet annihilation up conversion (TTA‐UC). Single‐crystal X‐ray crystallographic analyses show that the torsion angle between BODIPY and perylene units lie between 73.54 and 74.51, though they are not orthogonal. Both compounds show intense, charge transfer absorption and emission profiles, confirmed by resonance Raman spectroscopy and consistent with DFT calculations. The emission quantum yield was solvent dependent but the emission profile remained characteristic of CT transition across all solvents explored. Both BODIPY derivatives were found to be effective sensitizers of TTA‐UC with perylene annihilator in dioxane and DMSO. Intense anti‐Stokes emission was observed, and visible by eye from these solvents. Conversely, no TTA‐UC was observed from the other solvents explored, including from non‐polar solvents such as toluene and hexane that yielded brightest fluorescence from the BODIPY derivatives. In dioxane, the power density plots obtained were strongly consistent with TTA‐UC and the power density threshold, the Ith value (the photon flux at which 50 % of ΦTTAUC is achieved), for B2PI was observed to be 2.5x lower than of B2P under optimal conditions, an effect ascribed to the combined influence of spin‐orbit charge transfer intersystem crossing (SOCT‐ISC) and heavy metal on the triplet state formation for B2PI.
Herein, we report a single step, anionic surfactant-assisted, low temperature-hydrothermal synthetic strategy of CoO nanoparticles anchored on β-Co(OH) nanosheets which show a low overpotential (295 mV @ 10 mA cm) for the oxygen evolution reaction (OER). They also demonstrate much better kinetic parameters compared to the state-of-the-art RuO. Interestingly, under the OER operational conditions (in alkaline medium), the topotactic transformation of α-Co(OH) to a stable Brucite-like β-Co(OH) phase leads to a synergistic interaction between the β-Co(OH) sheets on the CoO nanoparticles for enhancing the OER electrocatalytic activity.
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