Abstract
Abstract One of the most exciting new developments in the plasmonic nanomaterials field is the discovery of their ability to mediate a number of photocatalytic reactions. Since the initial prediction of driving chemical reactions with plasmons in the 1980s, the field has rapidly expanded in recent years, demonstrating the ability of plasmons to drive chemical reactions, such as water splitting, ammonia generation, and CO2 reduction, among many other examples. Unfortunately, the efficiencies of these processes are currently suboptimal for practical widespread applications. The limitations in recorded outputs can be linked to the current lack of a knowledge pertaining to mechanisms of the partitioning of plasmonic energy after photoexcitation. Providing a descriptive and quantitative mechanism of the processes involved in driving plasmon-induced photochemical reactions, starting at the initial plasmon excitation, followed by hot carrier generation, energy transfer, and thermal effects, is critical for the advancement of the field as a whole. Here, we provide a mechanistic perspective on plasmonic photocatalysis by reviewing select experimental approaches. We focus on spectroscopic and electrochemical techniques that provide molecular-scale information on the processes that occur in the coupled molecular-plasmonic system after photoexcitation. To conclude, we evaluate several promising techniques for future applications in elucidating the mechanism of plasmon-mediated photocatalysis.
Highlights
The growing necessity for clean and renewable forms of energy production has had a significant effect on developing new technologies capable of achieving environmentally conscious and energetically efficient methodologies for driving industrial catalytic reactions
Throughout this review, we have provided a discussion and critique of the current literature that is focused on studying plasmon-mediated photocatalysis from a molecular viewpoint
Materials that support surface plasmons have the ability to amplify an electromagnetic wave from free space within an effective volume well below the diffraction limit [27], allowing for a wide range of applications, including fueling photocatalytic reactions [5, 13,14,15,16,17,18, 28,29,30], increasing the efficiency of photovoltaics [31,32,33,34,35,36,37], and serving as vehicles for photothermal therapy [38,39,40,41,42,43,44]
Summary
The growing necessity for clean and renewable forms of energy production has had a significant effect on developing new technologies capable of achieving environmentally conscious and energetically efficient methodologies for driving industrial catalytic reactions. The surface plasmon produces highly enhanced localized electromagnetic fields, creates elevated thermal environments, ejects highly energetic hot carriers, and/or modifies the potential energy landscape of a nearby molecular species [20,21,22] Each of these possible pathways of energy partitioning may contribute to mediating a catalytic process, with the preferential pathway heavily dependent on the targeted chemical reaction and the plasmonic substrate’s design. To make a significant leap in device fabrication, in the absence of an unpredicted technological development, it is imperative to study the individual mechanistic contributions and dynamics during the energy transformation after plasmon excitation With this highly pertinent information in hand, plasmonic substrates may be designed to preferentially dictate the flow of energy as the surface plasmon decays and efficiently channel it into mediating a chemical reaction. Materials that support surface plasmons have the ability to amplify an electromagnetic wave from free space within an effective volume well below the diffraction limit [27], allowing for a wide range of applications, including fueling photocatalytic reactions [5, 13,14,15,16,17,18, 28,29,30], increasing the efficiency of photovoltaics [31,32,33,34,35,36,37], and serving as vehicles for photothermal therapy [38,39,40,41,42,43,44]
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