Single-atom photocatalysts have shown their compelling potential and arguably become the most active research direction in photocatalysis due to their fascinating strengths in enhancing light-harvesting, charge transfer dynamics, and surface reactions of a photocatalytic system. While numerous comprehensions about the single-atom photocatalysts have recently been amassed, advanced characterization techniques and vital theoretical studies are strengthening our understanding on these fascinating materials, allowing us to forecast their working mechanisms and applications in photocatalysis. In this review, we begin by describing the general background and definition of the single-atom photocatalysts. A brief discussion of the metal-support interactions on the single-atom photocatalysts is then provided. Thereafter, the current available characterization techniques for single-atom photocatalysts are summarized. After having some fundamental understanding on the single-atom photocatalysts, their advantages and applications in photocatalysis are discussed. Finally, we end this review with a look into the remaining challenges and future perspectives of single-atom photocatalysts. We anticipate that this review will provide some inspiration for the future discovery of the single-atom photocatalysts, manifestly stimulating the development in this emerging research area.

Heterogeneous Single-Atom Photocatalysts: Fundamentals and Applications.

Solar energy is a major source of renewable energy with the potential to meet the energy demand and to support the sustainable development of the world. The efficient harvesting and conversion of solar energy is one of the key factors to maximize the utilization of solar energy. In general, solar energy can be harnessed and converted into various kinds of energy, including electricity, fuels and thermal energy, through photovoltaic, photochemical and photothermal processes, respectively. Among these technologies, photothermal conversion is a direct conversion process that has attained the highest achievable conversion efficiency. The photothermal effect has been used as a novel strategy to augment vaporization and catalysis performance. In this review, we look into the basis of the photothermal conversion process, the design of efficient photothermal conversion materials in terms of both light harvesting and thermal management, a fundamental understanding of various system schemes, and the recent progress in photothermal evaporation and catalysis applications. This review aims to afford researchers with a better understanding of the photothermal effect and provide a guide for the rational design and development of highly efficient photothermal materials in energy and environmental fields.

Solar-driven photothermal nanostructured materials designs and prerequisites for evaporation and catalysis applications

Photo-thermal catalysis has recently emerged as an alternative route to drive chemical reactions using light as an energy source. Through the synergistic combination of photo- and thermo-chemical contributions of sunlight, photo-thermal catalysis has the potential to enhance reaction rates and to change selectivity patterns, even under moderate operation conditions. This review provides the fundamentals of localized surface plasmon resonance (LSPR) that explain the photo-thermal effect in plasmonic structures, describes the different mechanistic pathways underlying photo-thermal catalysis, suggests methodologies to disentangle the reaction mechanisms and proposes material design strategies to improve photo-thermal performance. Ultimately, the goal is to pave the way for the wide implementation of this promising technology in the production of synthetic fuels and chemicals.

/pdf/fundamentals-and-applications-of-photo-thermal-catalysis-532tbwjn5y.pdf

Fundamentals and applications of photo-thermal catalysis.

Localized surface plasmon resonance (LSPR) is a physical phenomenon exhibited by nanoparticles of metals including coinage metals, alkali metals, aluminum, and some semiconductors which translates into electromagnetic, thermal, and chemical properties. In the past decade, LSPR has been taken advantage of in the context of catalysis. While plasmonic nanoparticles (PNPs) have been successfully applied toward enhancing catalysis of inorganic reactions such as water splitting, they have also demonstrated exciting performance in the catalysis of organic transformations with potential applications in synthesis of molecules from commodity to pharmaceutical compounds. The advantages of this approach include improved selectivity, enhanced reaction rates, and milder reaction conditions. This review provides the basics of LSPR theory, details the mechanisms at play in plasmon-enhanced nanocatalysis, sheds light onto such nanocatalyst design, and finally systematically presents the breadth of organic reactions hence catalyzed.

Applications of Plasmon-Enhanced Nanocatalysis to Organic Transformations.

Water splitting represents a promising technology for renewable energy conversion and storage, but it is greatly hindered by the kinetically sluggish oxygen evolution reaction (OER). Here, using Au-nanoparticle-decorated Ni(OH)2 nanosheets [Ni(OH)2–Au] as catalysts, we demonstrate that the photon-induced surface plasmon resonance (SPR) excitation on Au nanoparticles could significantly activate the OER catalysis, specifically achieving a more than 4-fold enhanced activity and meanwhile affording a markedly decreased overpotential of 270 mV at the current density of 10 mA cm–2 and a small Tafel slope of 35 mV dec–1 (no iR-correction), which is much better than those of the benchmark IrO2 and RuO2, as well as most Ni-based OER catalysts reported to date. The synergy of the enhanced generation of NiIII/IV active species and the improved charge transfer, both induced by hot-electron excitation on Au nanoparticles, is proposed to account for such a markedly increased activity. The SPR-enhanced OER catalysis co...

Promoting Active Species Generation by Plasmon-Induced Hot-Electron Excitation for Efficient Electrocatalytic Oxygen Evolution

Harnessing surface plasmon of metal nanostructures to promote catalytic organic synthesis holds great promise in solar-to-chemical energy conversion. High conversion efficiency relies not only on broadening the absorption spectrum but on coupling the harvested energy into chemical reactions. Such coupling undergoes hot-electron transfer and photothermal conversion during the decay of surface plasmon; however, the two plasmonic effects are unfortunately entangled, making their individual roles still under debate. Here, we report that in a model system of bimetallic Au–Pd core–shell nanostructures the two effects can be disentangled through tailoring the shell thickness at atomic-level precision. As demonstrated by our ultrafast absorption spectroscopy characterizations, the achieved tunability of the two effects in a model reaction of Pd-catalyzed organic hydrogenation offers a knob for enhancing energy coupling. In addition, the two intrinsic plasmonic modes at 400–700 and 700–1000 nm in the bar-shaped na...

Unraveling Surface Plasmon Decay in Core-Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis.

The origin of the Rayleigh scattering ring effect has been experimentally examined on a quantum dot/metal film system, in which CdTe quantum dots embedded in PVP are spin-coated on a thin Au film. On the basis of the angle-dependent, optical measurements under different excitation schemes (i.e., wavelength and polarization), we demonstrate that sur-face plasmon assisted directional radiation is responsible for such an effect. Moreover, an interesting phase-shift behavior is addressed.

Surface Plasmon Assisted Directional Rayleigh Scattering

The fluorescence quenching of Rhodamine 6G (R6G) by graphene oxide (GO) was interrogated by R6G fluorescence measurements using a set of controlled GO samples with varied C/O ratios as the quencher.The carbonyl groups on the GO nanosheet turned to play a dominant role in quenching the R6G fluorescence.The quenching in the static regime can be described by the 'sphere of action' model.The significant absorption of the R6G fluorescence by the ground-state complex formed between R6G and GO was identified to be responsible for the static quenching.This work offers helpful insights into the fluorescence quenching mechanisms in the R6G/GO system.

Mechanistic Insights into the Fluorescence Quenching of Rhodamine 6G by Graphene Oxide

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Papers

Unraveling Surface Plasmon Decay in Core-Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis.

Surface Plasmon Assisted Directional Rayleigh Scattering

Mechanistic Insights into the Fluorescence Quenching of Rhodamine 6G by Graphene Oxide