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Unravelling the effect of charge dynamics at the plasmonic metal/semiconductor interface for CO2 photoreduction
摘要： Sunlight plays a critical role in the development of emerging sustainable energy conversion and storage technologies. Light-induced CO2 reduction by artificial photosynthesis is one of the cornerstones to produce renewable fuels and environmentally friendly chemicals. Interface interactions between plasmonic metal nanoparticles and semiconductors exhibit improved photoactivities under a wide range of the solar spectrum. However, the photo-induced charge transfer processes and their influence on photocatalysis with these materials are still under debate, mainly due to the complexity of the involved routes occurring at different timescales. Here, we use a combination of advanced in situ and time-resolved spectroscopies covering different timescales, combined with theoretical calculations, to unravel the overall mechanism of photocatalytic CO2 reduction by Ag/TiO2 catalysts. Our findings provide evidence of the key factors determining the enhancement of photoactivity under ultraviolet and visible irradiation, which have important implications for the design of solar energy conversion materials.
关键词： Ag/TiO2 catalysts,photocatalysis,plasmonic metal nanoparticles,sustainable energy,solar energy conversion,artificial photosynthesis
更新于2025-10-22 19:40:53
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Conjugated donor-acceptor polymer photocatalysts with electron-output “tentacles” for efficient hydrogen evolution
摘要： The tunable structures and versatile properties for conjugated polymers (CPs) make them viable as a molecular platform for photocatalytic water splitting. Normally, structure design of polymer photocatalyst is focus on tuning its optical band structure or charge-separation ability, the importance of electron-output ability in photocatalytic process is always ignored. This study demonstrates a molecular engineering strategy by introducing an electron-output “tentacle” site, i.e. dibenzothiophene-S,S-dioxide (FSO) unit, into the polymer backbone to construct a series of donor-acceptor type conjugated polymer photocatalysts for efficient hydrogen evolution, which not only results in optimized light absorption ability and excellent exciton-separation, but also leads to the efficient electron-output ability. Detailed DFT calculations further theoretically confirm the vital role of FSO unit as an electron-output “tentacle” site.
关键词： Conjugated polymer,Electron-output “tentacles”,Artificial photosynthesis,Hydrogen evolution,Photocatalysis
更新于2025-09-23 15:23:52
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Artificial Photosynthesis for Carbon Dioxide Reduction and Conversion
摘要： In recent years, solar fuel or chemical production based on the photoreduction or fixation of CO2, the so-called “artificial photosynthesis” has received considerable attention. Thus, the development of an effective catalyst for the conversion of CO2 to useful organic molecules is desirable. Biocatalysts for CO2 reduction and conversion are useful catalyst for the artificial photosynthesis system. In this review, two types of artificial photosynthesis systems for CO2 reduction and conversion consisting of the visible-light sensitizer and biocatalyst are introduced. One is the artificial photosynthesis with visible-light sensitizer and biocatalyst for CO2 photoreduction to formic acid or methanol. The other one is the artificial photosynthesis with visible-light sensitizer, and novel electron carrier molecule and biocatalyst for the carbon-carbon bond formation from CO2 as a feedstock.
关键词： carbon-carbon bond formation,artificial photosynthesis,biocatalyst,CO2 reduction and conversion
更新于2025-09-23 15:23:52
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Recent Improvements in the Production of Solar Fuels: From CO <sub/>2</sub> Reduction to Water Splitting and Artificial Photosynthesis
摘要： This account deals with recent trends and challenges regarding photo(electro)chemical solar fuels produced by CO2 reduction and water splitting. The CO2 reduction process is limited by product selectivity, catalyst stability, and its complex reaction mechanism. A variety of catalysts—including thermocatalysts, photocatalysts, electrocatalysts, and combinations of photo- and electrocatalysts—have been employed to facilitate selective and durable CO2 reduction. In addition, the roles of the supporting electrolyte, pH, reaction temperature, chemical environment, and catalyst surface chemistry in efficient CO2 reduction have been thoroughly studied in recent years. Effective use of solar light is a significant part of realizing efficient solar-to-hydrogen conversion during the water splitting process, and so the response of photo(electro)systems to visible light is key. To this end, several strategies have been studied in detail, including band engineering of photocatalysts, photocatalytic systems that mimic natural photosynthesis, and the development of photoanodes and their combination with photovoltaic systems. Here, we summarize recent developments surrounding the CO2-reduction and water-splitting reactions and progress towards achieving artificial photosynthesis.
关键词： Artificial photosynthesis,CO2 reduction,Water splitting
更新于2025-09-23 15:22:29
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Production of Methanol from Aqueous CO <sub/>2</sub> by Using Co <sub/>3</sub> O <sub/>4</sub> Nanostructures as Photocatalysts
摘要： In this work, we report for the first time the photocatalytic activity of Co3O4 nanostructures for the reduction of aqueous CO2 to methanol (MeOH). This could be considered a simple example of artificial photosynthesis. The photocatalysis experiments were developed under simulated solar light of 100 mW/cm2 and without using any sacrificial agent. To carry out this study, nanostructured mixed valence cobalt oxide (Co3O4) powders, with porous nanoparticle aggregates of different morphologies, have been prepared by two synthesis methods. The characterization of structural (PXRD, XPS, SEM, and TEM) and optical (UV-vis-NIR, Raman, and FT-IR) properties, magnetization curves, and surface area (BET) was accomplished.
关键词： Co3O4,photocatalysis,artificial photosynthesis,CO2 reduction,nanostructures,methanol
更新于2025-09-23 15:22:29
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"Two-in-One" Strategy of o-Amino and Aromatic Nitrogen in Biomimetic Metal-Organic Frameworks for Efficient CO2 Photoconversion
摘要： Visible-light driven photoconversion of CO2 into energy carriers is highly important to the natural carbon balance and sustainable development. Herein, we demonstrate the biological nucleobase adenine-dependent CO2 photoreduction performance in green biomimetic metal-organic frameworks. Photocatalytic results indicate that AD-MOF-2 exhibited a very high HCOOH production rate of 443.2 μmol g-1 h-1 in pure aqueous solution, which is more than two times higher than that of AD-MOF-1 (179.0 μmol hour?1 g?1) in acetonitrile solution. Significantly, experimental and theoretical evidences reveal that CO2 photoreduction reaction mainly takes place on biological adenine molecules by unique o-amino assisted active aromatic nitrogen atom rather than traditional metal center. This work not only serves as an important case study for the development of green biomimetic photocatalysts used for artificial photosynthesis, but also proposes a new catalytic strategy for efficient CO2 photoconversion.
关键词： photosensitivity,hydrophobicity,biomimetic catalysis,green MOFs,artificial photosynthesis
更新于2025-09-23 15:22:29
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AIP Conference Proceedings [Author(s) PROCEEDINGS OF THE 3RD INTERNATIONAL SYMPOSIUM ON CURRENT PROGRESS IN MATHEMATICS AND SCIENCES 2017 (ISCPMS2017) - Bali, Indonesia (26–27 July 2017)] - Bismuth vanadate (BiVO4) as counter electrode in the newly developed catalysis zone of modified cadmium sulfide (CdS) sensitized solar cell for hydrogen production
摘要： Recently we developed a modified quantum dot dyes sensitized solar cell (QD-DSSC) having catalysis zone extension for hydrogen production. The DSSC section comprised of CdS sensitized highly order Titanium dioxidenanotube (CdS-HOTN) immobilized on Ti plate, Na2S/S containing electrolyte, and Pt covered SnO-F (fluorine doped tin oxide) glass plate (hence Pt/SnO-F/Glass). While the catalysis zone comprised of an extension of Ti support, as cathode, and the respected counter electrode was an extension of SnO-F glass, which was covered by BiVO4 film, both from respected DSSC section. In this presentation, we will focus on the role of the BiVO4 in our newly developed system. The bismuth vanadate was prepared by co-precipitation method with ammonia and calcination to obtain a fine powder. The BiVO4 fine powder were then deposited onto SnO-F glass plate and characterized by FT-IR, UV–vis diffused reflectance spectroscopy, SEM and X-ray diffraction. The characterization results revealed that the BiVO4 film, typically, has a band gap of 2.35 eV, characteristic of IR peaks represent the –V-O-, and –Bi-O-V- bonds, having a crystal phase as BiVO4 monoclinic scheelite with a typically crystallite size of 74.06 nm. The photo-electro-chemical properties of the BiVO4 film photo-anode was investigated by a linear sweep voltammetry and multi pulse amperometry, which revealed that the current response under the visible light was 0.03 mA/cm2. Further investigation when the BiVO4 film was incorporated into the modified QD-DSSC, the system (catalysis zone section), under solely visible light, was able to split the water into hydrogen and molecular oxygen. A brief discussion of the newly developed modified QD-DSSC, especially on the role of BiVO4 counter electrode in the catalysis zone will be presented, to gain a better insight in our new type artificial photosynthesis.
关键词： water splitting,titanium dioxide nanotubes,cadmium sulfide,artificial photosynthesis,modified dyes sensitized solar cell,Bismuth vanadate
更新于2025-09-23 15:21:21
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Strong pH-Dependent Near-Infrared Fluorescence in a Microbial Rhodopsin Reconstituted with a Red-Shifting Retinal Analogue
摘要： Near-infrared (NIR)-driven rhodopsins are of great interest in optogenetics and other optobiotechnological developments such as artificial photosynthesis and deep-tissue voltage imaging. Here we report the proton pump proteorhodopsin (PR) containing a NIR-active retinal analogue (PR:MMAR) exhibits intense NIR fluorescence at a quantum yield of 3.3%. This is 130 times higher than native PR (Lenz, M. O.; et al. Biophys J. 2006, 91, 255?262) and 3?8 times higher than the QuasAr and PROPS voltage sensors (Kralj, J.; et al. Science 2011, 333, 345?348; Hochbaum, D. R.; et al. Nat. Methods 2014, 11, 825?833). The NIR fluorescence strongly depends on the pH in the range of 6?8.5, suggesting potential application of MMAR-binding proteins as ultrasensitive NIR-driven pH and/or voltage sensors. Femtosecond transient absorption spectroscopy showed that upon near-IR excitation, PR:MMAR features an unusually long fluorescence lifetime of 310 ps and the absence of isomerized photoproducts, consistent with the high fluorescence quantum yield. Stimulated Raman analysis indicates that the NIR-absorbing species develops upon protonation of a conserved aspartate, which promotes charge delocalization and bond length leveling due to an additional methylamino group in MMAR, in essence providing a secondary protonated Schiff base. This results in much smaller bond length alteration along the conjugated backbone, thereby conferring significant single-bond character to the C13C14 bond and structural deformation of the chromophore, which interferes with photoinduced isomerization and extends the lifetime for fluorescence. Hence, our studies allow for a molecular understanding of the relation between absorption/emission wavelength, isomerization, and fluorescence in PR:MMAR. As acidification enhances the resonance state, this explains the strong pH dependence of the NIR emission.
关键词： stimulated Raman analysis,fluorescence,voltage sensor,rhodopsins,optogenetics,artificial photosynthesis,proteorhodopsin,femtosecond transient absorption spectroscopy,pH sensor,Near-infrared,voltage imaging
更新于2025-09-23 15:21:01
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All-in-one photosynthetic assemblies for solar fuels
摘要： Converting solar energy into chemical fuel using an all-in-one photosynthetic assembly requires novel concept and cutting-edge technologies. Up to now, a series of new concepts have been suggested for designing of the assembly. It is thus important to examine present physics and research status of the assembly to glean the design guidelines for future devices. Here we introduce the concept of all-in-one photosynthetic assembly, which including photoelectrochemical diodes, all-in-one membranes and monolithic photovoltaic-photoelectrolysis cells. Key physical aspects are examined to identify the state-of-the-art in device design. We then discuss the device configurations, requirements and practical implications. Key features of the assemblies are also highlighted with their photosynthetic performance. Finally, a potential design that can be scalable to large area is projected for a more complete picture of the field. These concepts and their successful realization will be an important contribution towards realization of artificial photosynthesis.
关键词： Photochemical cells,All-in-one,Device,Artificial photosynthesis,Solar fuels
更新于2025-09-23 15:21:01
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Spin-Controlled Charge Recombination Pathways across the Inorganic/Organic Interface
摘要： Charge transfer and recombination across the inorganic/organic interface in nanocrystal or quantum dot (QD)-molecule hybrid materials has been extensively studied. Principles of controlling charge transfer and recombination via energetics and electronic coupling have been established. However, the use of electron spin to control transfer and recombination pathways in such systems remains relatively underexplored. Here we use CdS QD-alizarin (AZ) as a model system to demonstrate this principle. Using time-resolved spectroscopy, we found that the charge separated states (QD--AZ+) created by selectively exciting AZ molecules mostly recombined to regenerate ground state complexes, whereas the apparently “same” charge separated states created by exciting QDs recombined to produce AZ molecular triplet states. Such a difference can be traced to the distinct spin configurations between excited QDs (QD*, with an ill-defined spin) and AZ (1AZ*, spin singlet) and the asymmetric electron and hole spin-flip rates in II-VI group QDs. The transferability of such a principle was confirmed by similar observations obtained for CdS QD-tetracene complexes. Opening an avenue of controlling charge transfer and recombination pathways via electron spin is potentially important for applications such as artificial photosynthesis.
关键词： CdS QD-alizarin,artificial photosynthesis,quantum dot,inorganic/organic interface,triplet states,electron spin,recombination,time-resolved spectroscopy,Charge transfer
更新于2025-09-23 15:19:57