of Materials Chemistry A

Sustainable photonics applications of solid-state triplet-triplet annihilation photon upconversion (TTA-UC) are limited by a small UC spectral window, low UC efficiency in air, and non-recyclability of polymeric materials used. In a step to overcome these issues, we have developed new recyclable TTA-UC bioplastics by encapsulating TTA-UC chromophores liquid inside the semicrystalline gelatin films showing broad-spectrum upconversion (red/far-red to blue) with high UC efficiency in the air. For this, we synthesized a new anionic annihilator, sodium-TIPS-anthracene-2-sulfonate (TIPS-AnS), that combined with red/ far-red sensitizers (PdTPBP/Os(m-peptpy) 2 (TFSI) 2 ), a liquid surfactant triton X-100 reduced (TXr) and protein gelatin (G) formed Red/ far-red to blue TTA-UC bioplastic films just by air drying of their aqueous solutions. The G-TXr-TIPS-AnS-PdTPBP film showed record red to blue (633 to 478 nm) TTA-UC quantum yield of 8.5% in air. The high UC quantum yield has been obtained due to the fluidity of dispersed TXr containing chromophores and oxygen blockage by gelatin fibers that allowed efficient diffusion of triplet excited chromophores. Further, the G-TXr-TIPS-AnS-Os( m -peptpy) 2 (TFSI) 2 bioplastic film displayed far-red to blue (700-730 nm to 478 nm) TTA-UC, demonstrating broad-spectrum photon harvesting. Finally, we demonstrated the recycling of G-TXr-TIPS-AnS-PdTPBP bioplastics by developing a downstream approach that gives new directions for designing future recyclable photonics bioplastic materials. of detection films at approximately 30° to the direction of the excitation light to yield front-face detection. The absolute fluorescence quantum yields of G-TXr-TIPS-AnS-cresyl violet (λ ex = 633 nm), and G-TXr-TIPS-AnS-PdTPBP (λ ex = 415 nm) films were measured in the integrated sphere using FLS1000 Photoluminescence Spectrometer, Edinburgh instrument. The measurements were carried out by putting sample or reference films cast on a glass plate horizontally on a sample stage, followed by 90 o excitation with respect to the detector. Before the sample measurements, photoluminescence spectra (PL) of empty glass plates were recorded as reference. For G-TXr-TIPS-AnS-cresyl violet film the PL spectra were recorded between 613 nm to 800 nm (λ ex = 633 nm). The absolute quantum was calculated using instrument inbuilt software by subtracting the reference spectrum between 640 to 800 nm. The absolute quantum yield value of cresyl violet was calculated to be 0.31. The data wasn’t corrected for reabsorption. The same wavelength range of cresyl violet’s PL spectra in the G-TXr-TIPS-AnS-cresyl violet film measured at different excitation intensities of 633 nm laser was used for relative UC quantum yield measurement. For G-TXr-TIPS-AnS-PdTPBP film the PL spectra were recorded between 395 nm to 650 nm (λ ex = 415 nm). The Q. yield was measured between 420 to 650 nm. The samples were not corrected for reabsorption. The phosphorescence lifetime was measured using Varian Eclipse 1 fluorescence spectrophotometer with 633 nm excitation. film in half with hands. DMA analysis was performed on TAinstrument DMAQ800 in tensile film mode at a strain of 0.05% and frequency of 1 Hz and temperature of 30 o C. Prior to the measurement, a strain sweep was performed on G film to ensure that the applied strain is within the linear viscoelastic region.