scholarly journals Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production

PLoS ONE ◽  
2021 ◽  
Vol 16 (7) ◽  
pp. e0255002
Author(s):  
Caroline Supplis ◽  
Jérémi Dauchet ◽  
Victor Gattepaille ◽  
Fabrice Gros ◽  
Thomas Vourc’h ◽  
...  

Most chemical reactions promoted by light and using a photosensitizer (a dye) are subject to the phenomenon of luminescence. Redistribution of light in all directions (isotropic luminescence emission) and in a new spectral range (luminescence emission spectrum) makes experimental and theoretical studies much more complex compared to a situation with a purely absorbing reaction volume. This has a significant impact on the engineering of photoreactors for industrial applications. Future developments associated with photoreactive system optimization are therefore extremely challenging, and require an in-depth description and quantitative analysis of luminescence. In this study, a radiative model describing the effect of luminescence radiation on the calculation of absorptance is presented and analyzed with the multiple inelastic-scattering approach, using Monte Carlo simulations. The formalism of successive orders of scattering expansion is used as a sophisticated analysis tool which provides, when combined with relevant physical approximations, convenient analytical approximate solutions. Its application to four photosensitizers that are representative of renewable hydrogen production via artificial photosynthesis indicates that luminescence has a significant impact on absorptance and on overall quantum yield estimation, with the contribution of multiple scattering and important spectral effects due to inelastic scattering. We show that luminescence cannot be totally neglected in that case, since photon absorption lies at the root of the chemical reaction. We propose two coupled simple and appropriate analytical approximations enabling the estimation of absorptance with a relative error below 6% in every tested situation: the zero-order scattering approximation and the gray single-scattering approximation. Finally, this theoretical approach is used to determine and discuss the overall quantum yield of a bio-inspired photoreactive system with Eosin Y as a photosensitizer, implemented in an experimental setup comprising a photoreactor dedicated to hydrogen production.

2017 ◽  
Vol 5 (38) ◽  
pp. 9979-9985 ◽  
Author(s):  
Jiao Liu ◽  
Xin-Xin Yuan ◽  
Hong-Wei Li ◽  
Yuqing Wu

AMP-capped gold and silver bimetal nanoclusters, Au–AgNCs@AMP, showing strong luminescence emission with a high quantum yield (QY = 8.46%) and novel photosensitivity, have been prepared using the hydrothermal synthesis method.


2021 ◽  
Author(s):  
WEN-SHUO KUO ◽  
Chia-Yuan Chang ◽  
Ping-Ching Wu ◽  
Jiu-Yao Wang

Abstract BackgroundNitrogen doping and amino-group functionalization, which result in strong electron donation, can be achieved through chemical modification. Large π-conjugated systems of graphene quantum dot (GQD)-based materials acting as electron donors can be chemically manipulated with low two-photon excitation energy in a short photoexcitation time for improving the charge transfer efficiency of sorted nitrogen-doped amino acid–functionalized GQDs (sorted amino-N-GQDs). ResultsIn this study, a self-developed femtosecond Ti-sapphire laser optical system (222.7 nJ pixel−1 with 100-170 scans, approximately 0.65-1.11 s of total effective exposure times; excitation wavelength: 960 nm in the near-infrared II region) was used for chemical modification. The sorted amino-N-GQDs exhibited enhanced two-photon absorption, post-two-photon excitation stability, two-photon excitation cross-section, and two-photon luminescence through the radiative pathway. The lifetime and quantum yield of the sorted amino-N-GQDs decreased and increased, respectively. Furthermore, the sorted amino-N-GQDs exhibited excitation-wavelength-independent photoluminescence in the near-infrared region and generated reactive oxygen species after two-photon excitation. An increase in the size of the sorted amino-N-GQDs boosted photochemical and electrochemical efficacy and resulted in high photoluminescence quantum yield and highly efficient two-photon photodynamic therapy. ConclusionThe sorted dots can be used in two-photon contrast probes for tracking and localizing analytes during two-photon imaging in a biological environment and for conducting two-photon photodynamic therapy for eliminating infectious microbes.


2018 ◽  
Vol 43 (31) ◽  
pp. 14439-14450 ◽  
Author(s):  
Cheng Ziming ◽  
Wang Fuqiang ◽  
Liang Huaxu ◽  
Hu Shengpeng ◽  
Lin Bo ◽  
...  

2020 ◽  
Vol 8 (26) ◽  
pp. 13142-13149 ◽  
Author(s):  
Ping-Yen Hsieh ◽  
Tatsuya Kameyama ◽  
Takayuki Takiyama ◽  
Ko Masuoka ◽  
Takahisa Yamamoto ◽  
...  

Alloyed ZnSe–AgInSe2 quantum dots were used as a photocatalyst for H2 production, showing an apparent quantum yield of 3.4% at 600 nm.


2015 ◽  
Vol 51 (70) ◽  
pp. 13496-13499 ◽  
Author(s):  
Tiantian Jia ◽  
Molly M. J. Li ◽  
Lin Ye ◽  
Sam Wiseman ◽  
Guoliang Liu ◽  
...  

Single layer MoS2synthesized by exfoliation with Li is demonstrated to take up the dye molecule, Eosin Y, with strong binding affinityviasulfur vacancies.


1962 ◽  
Vol 40 (6) ◽  
pp. 1134-1139 ◽  
Author(s):  
Arthur R. Knight ◽  
Harry E. Gunning

The reaction of isopropanol vapor with Hg 6(3P1) atoms has been investigated under static conditions at 25 °C under continuous and intermittent illumination. The effect of added inert gas and isolation of the 2537 Å Hg resonance line were also studied.The products of the reaction are H2 (0.72), CH3COCH3 (0.25), CO, CH4, C2H6, CH3CHO, and H2O, with the numbers in parentheses representing the quantum yields at zero exposure time. The non-volatile product remaining in the cell was a mixture of C6-glycols, containing 98.6% pinacol, 1.2% 2-methyl-2,4-pentanediol, and ca. 0.2% or less of 2,5-hexanediol.Under intermittent illumination, the quantum yield of hydrogen production, measured as a function of light period, tL, rose linearly with log tL, and had a constant value of unity for tL < 0.45 msec. A mechanism is proposed involving the primary formation with perfect efficiency of isopropoxy radicals and H atoms.


2012 ◽  
Vol 41 (15) ◽  
pp. 4536 ◽  
Author(s):  
Hanzhong Ke ◽  
Wenbin Li ◽  
Tao Zhang ◽  
Xunjin Zhu ◽  
Hoi-Lam Tam ◽  
...  

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