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Surface-Immobilized Conjugated Polymers Incorporating Rhenium Bipyridine Motifs for Electrocatalytic and Photocatalytic CO <sub/>2</sub> Reduction
摘要： The solar-driven conversion of CO2 to value-added products provides a promising route for solar energy storage and atmospheric CO2 remediation. In this report, a variety of supporting electrode materials were successfully modified with a [2,2′-bipyridine]-5,5′-bis(diazonium) rhenium complex through a surface-localized electropolymerization method. Physical characterization of the resulting multilayer films confirms that the coordination environments of the rhenium bipyridine tricarbonyl sites are preserved upon immobilization and that the polymerized catalyst moieties exhibit long-range structural order with uniform film growth. UV?vis studies reveal additional absorption bands in the visible region for the polymeric films that are not present in the analogous rhenium bipyridine complexes. Electrochemical studies with modified graphite rod electrodes show that the electrocatalytic activity of these films increases with catalyst loading up to an optimal value, beyond which electron and mass transport through the material become rate-limiting. Electrocatalytic studies performed at ?2.25 V vs Fc/Fc+ for 2 h reveal CO production with faradaic efficiencies and turnover numbers up to 99% and 3606, respectively. Photocatalytic studies of the modified TiO2 devices demonstrate enhanced activity at low catalyst loadings, with turnover numbers up to 70 during 5 h of irradiation.
关键词： metallopolymers,surface modification,photocatalysis,rhenium bipyridine,solar energy conversion,electrocatalysis
更新于2025-09-23 15:23:52
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Online Policies for Energy Harvesting Receivers With Time-Switching Architectures
摘要： In the real-world, it is virtually impossible to have non-causal knowledge of future events. Research in energy harvesting (EH) systems that assumes knowledge of future energy arrivals falls short in terms of practical utility, pointing to the need for online strategies. In addition, the modeling and analysis for EH transmitter and receiver are inherently different. Compared with EH transmitter, EH receiver has received less attention. In this paper, we formulate Markov decision process problems and perform online optimization to maximize the number of bits decoded for an EH receiver with a time-switching architecture, which harvests energy from both a dedicated transmitter and other sources. We consider both infinite and finite horizon scenarios. For the infinite horizon, we provide an upper bound on the average expected reward. Then, we find an optimal policy which can achieve performance arbitrarily close to this bound. For the finite horizon, we first provide a policy obtained from standard backward induction with space quantization. Its performance can be close to optimal online performance as the number of quantization intervals increases, at the cost of relatively high computational complexity. Then, by carefully restricting the state space, we present a computationally efficient policy, which achieves comparatively good performance.
关键词： Infinite horizon,Markov decision process,Energy harvesting,Online optimization,Finite horizon
更新于2025-09-23 15:23:52
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A review on photoelectrochemical hydrogen production systems: Challenges and future directions
摘要： Water photolysis is a fundamental concept in which solar-driven water splitting is utilized to generate renewable hydrogen fuel using semiconductor-based electrochemical systems. The engineering design principles for each system configuration, including single, dual/tandem photoelectrodes, tandem photoelectrochemical-photovoltaic, and multi-junction designs are reviewed. Modeling and numerical simulation of photoelectrochemical processes based on up-to-date multi-scale analysis are presented and discussed. In addition, the achievements made in semiconductor photoelectrode materials and the rational engineering methods needed to improve the solar to hydrogen efficiency are demonstrated. Furthermore, some key accomplishments in different aspects, such as electron-hole recombination, stability, photocorrosion, energy band gap, and photocurrent density are discussed. Moreover, key points on the challenges, opportunities and future directions towards commercialization of viable photoelectrochemical reactors are discussed.
关键词： Semiconductor materials,Photoelectrochemical process,Hydrogen production,Solar energy
更新于2025-09-23 15:23:52
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Regulating Charge-Transfer in Conjugated Microporous Polymer for Photocatalytic Hydrogen Evolution
摘要： Band gap engineering in donor-acceptor conjugated microporous polymers is a potential way to increase the solar energy harvesting towards photochemical water splitting. Herein, we report design and synthesis of a series of donor-acceptor CMPs [tetraphenylethylene (TPE) = donor and 9-fluorenone (F) = acceptor], F0.1CMP, F0.5CMP and F2.0CMP which exhibit tunable band gaps and photocatalytic hydrogen evolution from water. The donor-acceptor CMPs exhibit intramolecular charge transfer (ICT) absorption in the visible region (λmax=480 nm) and their band gap is finely tuned from 2.8 eV to 2.1 eV by increasing the 9-fluorenone content. Interestingly, they also show charge transfer emissions (in 540 -580 nm range), assisted by the energy transfer from the other TPE segments (not involved in CT interaction) as evidenced from fluorescence lifetime decay analysis. By increasing the 9-fluorenone content the emission color of the polymer is also tuned from green to red. Photocatalytic activities of the donor-acceptor CMPs (F0.1CMP, F0.5CMP and F2.0CMP) are greatly enhanced compared to the 9-fluorenone free polymer (F0.0CMP) which is essentially due to improved visible light absorption and low band gap of donor-acceptor CMPs. Among all the polymers F0.5CMP with an optimum band gap (2.3 eV) shows highest H2 evolution under visible light irradiation. Moreover, all the polymers show excellent dispersibility in organic solvents and also they are easily processed onto solid substrates.
关键词： Visible-light absorption,Conjugated polymers,Photocatalysis,Charge transfer,Energy transfer
更新于2025-09-23 15:23:52
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A New Biscarbazole-Based Metal-Organic Framework for Efficient Host-Guest Energy Transfer
摘要： A new metal–organic framework (MOF), [Zn6L4(Me2NH2+)4·3 H2O] (1) was constructed based on [9,9’-biscarbazole]-3,3’,6,6’-tetracarboxylic acid (H4L) and Zn2+ ions. The porous framework and intense blue fluorescence of the MOF based on the biscarbazole moiety of the ligand could facilitate efficient host to guest energy transfer, which makes it an ideal platform for the tuning of luminescence.
关键词： in situ encapsulation,metal–organic frameworks,energy transfer,host–guest systems,fluorescence
更新于2025-09-23 15:23:52
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Tunable photoluminescence properties and energy transfer of Ca5(BO3)3F: Tb3+/Eu3+ phosphors for solid state lighting
摘要： A series of Ca5(BO3)3F: Tb3+/Eu3+ phosphors have been prepared via solid-state reaction. Phase purity and crystal structure of as-prepared samples are confirmed by X-ray diffraction measurements. The emission intensity of Ca5(BO3)3F: Tb3+ with Li+, Na+, K+ as charge compensators are remarkably enhanced, and the sample in presence of Na+ exhibits the strongest emission intensity. The emission spectra and fluorescence decays confirm the presence of efficient energy transfers from Tb3+ to Eu3+ in Ca5(BO3)3F: Tb3+/Eu3+ phosphors. The energy transfer mechanism between Tb3+ and Eu3+ has been proven to be resonant type via the electric dipole-dipole interaction. The thermal quenching temperature T50 obtained from the temperature-dependent emission spectra is 478 K, demonstrating a high thermal stability of the as-obtained Ca5(BO3)3F: Tb3+/Eu3+ phosphors. Moreover, by increasing the molar ratio of Eu3+ to Tb3+, the emission colors of Ca5(BO3)3F: Tb3+/Eu3+ phosphors can be tuned from green to orange, and then to red. These results demonstrate that the as-obtained Ca5(BO3)3F: Tb3+/Eu3+ phosphors may have potential applications in solid-state lighting fields.
关键词： Energy transfer,Ca5(BO3)3F,Phosphors,Tunable luminescence,Solid-state reaction
更新于2025-09-23 15:23:52
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[Lecture Notes in Computer Science] Hybrid Metaheuristics Volume 11299 (11th International Workshop, HM 2019, Concepción, Chile, January 16–18, 2019, Proceedings) || Optimization of the Velocity Profile of a Solar Car Used in the Atacama Desert
摘要： Global energy demand has undergone a substantial increase in past decades because of the rapid increase of the global population and the energetic consumption of new production technologies. As a result, a change is necessary in the global energy generating matrix, in which the sources originate primarily from renewable energy sources. The main renewable energy source may be solar energy, and one of its applications is solar mobility. A world-class solar racing car exists that requires a rational use of velocity and energy to minimize the time spent in a race. A total of three search metaheuristics were tested to achieve an efficient velocity profile for this car in the Atacama 2018 Solar Race: Genetic Algorithm, Simulated Annealing and Iterated Local Search. The three methods provided similar results, with Simulated Annealing being the one that provided better solutions.
关键词： Metaheuristics,Energy management,Solar competition,Hybrid electric vehicle
更新于2025-09-23 15:23:52
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Thermoluminescent behavior of UV and γ rays irradiated Eu2+ and Er3+doped silicate phosphors
摘要： This paper reports the structural, morphological and thermoluminescent studies of Eu2+ and Er3+ ions activated ASiO3 (A= Ca, Ba, Sr) phosphors synthesized via conventional solid state reaction method. The impurity ions concentration of both Eu2+ and Er3+ ions varies from 0 mol% to 1 mol%. The study of crystallographic traits of the synthesized phosphors is done by Powder X-Ray Diffraction (PXRD) analysis. The crystalline nature, phase purity and appreciable homogeneity of the synthesized phosphors were confirmed by this study. The distinct morphological and topographical features were studied through Field Emission Scanning Electron Microscopy (FESEM) and Transmission Electron Microscopy (TEM). The thermoluminescent (TL) behavior of ultraviolet (UV) irradiated and gamma irradiated ASiO3:Eu2+, Er3+ (A= Ca, Ba, Sr) phosphors were studied here and the various kinetic parameters were estimated by Computerised glow curve deconvolution (CGCD) technique and peak shape method. The UV and gamma irradiated phosphors exhibit second order kinetics. The high values of activation energy (~ 3 eV) confirm the trapping of electrons in deep trap centers. The incorporation of doping ions into the host lattice causes non-valence substitutions at the substitutional sites. This increases the number of defects and vacancies in the phosphors and more trap centers were generated. The increased TL intensity and high temperature glow peaks confirm the same. The synthesized phosphors show enhanced TL characteristics, efficient trapping mechanism and low fading effects. These characteristics confirm the suitability of the synthesized phosphors for TL mapping and sensing applications.
关键词： Alkaline earth silicates,Thermoluminscence,Activation energy,Trap depth,Order of kinetics.
更新于2025-09-23 15:23:52
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NIR-Fluorescent Multidye Silica Nanoparticles with Large Stokes Shifts for Versatile Biosensing Applications
摘要： We have synthesized and characterized of a series of single and multidye copolymerized nanoparticles with large to very large Stokes shifts (100 to 255 nm) for versatile applications as standalone or multiplexed probes in biological matrices. Nanoparticles were prepared via the St?ber method and covalently copolymerized with various combinations of three dyes, including one novel aminocyanine dye. Covalently encapsulated dyes exhibited no significant leakage from the nanoparticle matrix after more than 200 days of storage in ethanol. Across multiple batches of nanoparticles with varying dye content, the average yields and average radii were found to be highly reproducible. Furthermore, the batch to batch variability in the relative amounts of dye incorporated was small (relative standard deviations <2.3%). Quantum yields of dye copolymerized nanoparticles were increased 50% to 1000% relative to those of their respective dye-silane conjugates, and fluorescence intensities were enhanced by approximately three orders of magnitude. Prepared nanoparticles were surface modified with polyethylene glycol and biotin and bound to streptavidin microspheres as a proof of concept. Under single wavelength excitation, microsphere-bound nanoparticles displayed readily distinguishable fluorescence signals at three different emission wavelengths, indicating their potential applications to multicolor sensing. Furthermore, nanoparticles modified with polyethylene glycol and biotin demonstrated hematoprotective qualities and reduced nonspecific binding of serum proteins, indicating their potential suitability to in vivo imaging applications.
关键词： Fluorescent silica nanoparticles,Biocompatible nanoparticles,Large stokes shift,Near-infrared fluorescence,Multicolor assay,Resonance energy transfer
更新于2025-09-23 15:23:52
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Efficient degradation of phenol using Sn4+ doped FeOCl as photo-Fenton catalyst
摘要： Sn4+ doped FeOCl has been successfully synthetized as a sunlight-driven photo-Fenton catalyst, which shows that the catalytic activity of Sn4+/FeOCl (1.08% Sn4+ in the Sn4+/FeOCl) is a factor of 11.8 time higher than that of FeOCl. The doping of Sn4+ in FeOCl increases the optical adsorption and surface area of FeOCl. The decreased chemical bond strength of Fe-Cl in Sn4+/FeOCl effectively increases the number of exposed active sites (Fe-site and Sn-site), which boosts the production of ·OH radicals. The Sn-site shows higher catalytic activity than Fe-site. A synergistic mechanism for Sn4+/FeOCl is proposed for the enhanced catalytic performance.
关键词： Solar energy materials,FeOCl,Phenol,Nanocomposites,Fenton reaction,Sn4+
更新于2025-09-23 15:23:52