Plasmon-Assisted Ammonia Electrosynthesis

Contreras, Enrique; Nixon, Rachel; Litts, Chloe; Zhang, Wenxin; Alcorn, Francis M.; Jain, Prashant K.

doi:10.1021/jacs.2c01272

Cited by 68 publications

(62 citation statements)

References 70 publications

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“…energies exceeding 340 meV (Fig.3D, S12). Notably, the ensemble average plasmon generated potential measured in this study is approximately two orders of magnitude less than measured values in other recent work (32,46,47). For example, Yu and coworkers have recently reported a hot electron energy of 0.32 eV generated from continuous wave excitation of a gold nanosphere array.…”

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confidence: 70%

Quantifying the Ultrafast and Steady-State Molecular Reduction Potential of a Plasmonic Photocatalyst

Warkentin

Frontiera

2022

Preprint

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Plasmonic materials are promising photocatalysts as they are well-suited to convert light into hot carriers and heat. Hot electron transfer is suggested as the driving force in many plasmon-driven reactions. However, to date there are no direct molecular measures of the rate and yield of plasmon-to-molecule electron transfer, or energy of these electrons on the timescale of plasmon decay. Here, we use ultrafast and spectroelectrochemical surface-enhanced Raman spectroscopy to quantify electron transfer from a plasmonic substrate to adsorbed methyl viologen molecules. We observe a reduction yield of 2.4 - 3.5 % on the picosecond timescale, with plasmon-induced potentials ranging from -3.1 to -4.5 mV. Excitingly, some of these reduced species are stabilized and persist for tens of minutes. This work provides concrete metrics toward optimizing material-molecule interactions for efficient plasmon-driven photocatalysis.

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confidence: 70%

Quantifying the Ultrafast and Steady-State Molecular Reduction Potential of a Plasmonic Photocatalyst

Warkentin

Frontiera

2022

Preprint

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“…Notably, if the LSPR occurs in the visible region, solar energy can be effectively utilized. So far, the relevant reports were mostly focused on the synthesis of various plasmonic nanostructures with a primary target to increase the catalytic activity. − In contrast, the plasmon effects on regulating electrocatalytic pathways as well as the underlying mechanism have been least investigated. , …”

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confidence: 99%

Plasmon-Enhanced C–C Bond Cleavage toward Efficient Ethanol Electrooxidation

Yan

Mao

et al. 2022

J. Phys. Chem. Lett.

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Ethanol, as a sustainable biomass fuel, is endowed with the merits of theoretically high energy density and environmental friendliness yet suffers from sluggish kinetics and low selectivity toward the desired complete electrooxidation (C1 pathway). Here, the localized surface plasmon resonance (LSPR) effect is explored as a manipulating knob to boost electrocatalytic ethanol oxidation reaction in alkaline media under ambient conditions by appropriate visible light. Under illumination, Au@Pt nanoparticles with plasmonic core and active shell exhibit concurrently higher activity (from 2.30 to 4.05 A mg Pt −1 at 0.8 V vs RHE) and C1 selectivity (from 9 to 38% at 0.8 V). In situ attenuated total reflection−surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) provides a molecular level insight into the LSPR promoted C−C bond cleavage and the subsequent CO oxidation. This work not only extends the methodology hyphenating plasmonic electrocatalysis and in situ surface IR spectroscopy but also presents a promising approach for tuning complex reaction pathways.

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“…Photocatalysis with hot carriers has been studied extensively because the energetic electron–hole pairs from LSPR excitation can boost the catalytic performance. , Furthermore, plasmonic photocatalysis exhibits a superlinear function of photon flux and temperature in photocatalytic activity and quantum efficiency . To enhance the efficiency of hot carrier-induced photocatalysis, we focus on M–S photocatalysis that can form a Schottky barrier at the plasmonic M–S junction, leading to the inhibition of an undesirable recombination of hot carriers.…”

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confidence: 99%

Surface Plasmon-Induced Hot Carriers: Generation, Detection, and Applications

et al. 2022

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Metrics & MoreArticle RecommendationsCONSPECTUS: During surface plasmon-mediated light−matter interactions, external energies on plasmonic metal nanostructures undergo energy dissipation via elastic e−e scattering, radiative luminescence, and nonradiative processes such as thermal relaxation (phonon) and electronic excitation (electron−hole pairs). In this process, surface plasmon decays dominantly through nonradiative recombination when the metal is smaller than 25 nm, forming hot carriers, including hot electrons and hot holes, with high kinetic energy of 1−3 eV. Although the ultrafast dynamics of hot carriers are on time scales ranging from femtoseconds to picoseconds, these fast-disappearing hot carriers can be collected as the steady-state photocurrent or chemicurrent by adopting the metal−semiconductor (M−S)based platform for detecting hot carrier flow. Plasmonic hot carriers, especially as they convert to an electrochemical signal, are a promising topic, and their energy conversion mechanisms are being actively studied in the fields of renewable energy, optoelectronics, and photocatalysis. Recent studies have demonstrated that these hot carriers can both improve the performance of solar energy conversion and control the catalytic activity or selectivity by directly participating in the photoelectrochemical (PEC) reaction.In this Account, we describe the inherent relationship between hot carriers and surface plasmon as well as what role hot carriers play throughout the catalytic reaction. The recent experimental work and the theoretical analysis of in situ hot carrier generation on Au nanostructures were conducted with photoconductive atomic force microscopy and finite-difference time-domain (FDTD) simulations, respectively. We highlight the recent nanoscale visualization of hot carrier flow occurring through light−matter interactions and that the localized surface plasmon field surrounding the Au nanostructure leads to boosted hot carrier generation. In addition, we highlight the recent demonstration that plasmonic hot carriers prolong the lifetime of photoexcited carriers in the MAPbI 3 /Au/TiO 2 hybrid nanodiode by the synergistic effect between plasmonic Au and perovskites. From this work, the solar-toelectron conversion performance of this nanodiode significantly increases due to the amplification of light absorption, which helps to design hybrid platforms for efficient hot carrier photovoltaics. We discuss the application of surface plasmon-driven hot electron generation, including hot electron-based photovoltaic devices and photocatalysts. We highlight the recent photoelectrochemical measurements on the Au/p-GaN heterostructures that are controlled by participating plasmonic hot carriers in the water splitting reaction. Furthermore, controlling the flow of both hot electrons and holes by developing hybrid platform configurations for hot carrier applications has promising opportunities for regulating the catalytic activities of hot carrier-based photocatalysis and improving the photoconversion efficie...

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Plasmon-Assisted Ammonia Electrosynthesis

Cited by 68 publications

References 70 publications

Quantifying the Ultrafast and Steady-State Molecular Reduction Potential of a Plasmonic Photocatalyst

Quantifying the Ultrafast and Steady-State Molecular Reduction Potential of a Plasmonic Photocatalyst

Plasmon-Enhanced C–C Bond Cleavage toward Efficient Ethanol Electrooxidation

Surface Plasmon-Induced Hot Carriers: Generation, Detection, and Applications

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