Hot carriers (HCs) and thermal effects, stemming from plasmon decays, are crucial for most plasmonic applications. However, quantifying these two effects remains extremely challenging due to the experimental difficulty in accurately measuring the temperature at reaction sites. Herein, we provide a novel strategy to disentangle HCs from photothermal effects based on the different traits of heat dissipation (long range) and HCs transport (short range), and quantitatively uncover the dominant and potential‐dependent role of photothermal effect by investigating the rapid‐ and slow‐response currents in plasmon‐mediated electrochemistry at nanostructured Ag electrode. Furthermore, the plasmoelectric surface potential is found to contribute to the rapid‐response currents, which is absent in the previous studies.
Platinum-based catalysts are widely used in hydrogen evolution reactions; however, their applications are restricted because of the cost-efficiency trade-off. Here, we present a thermodynamics-based design strategy for synthesizing an Al
73
Mn
7
Ru
20
(atomic %) metal catalyst via combinatorial magnetron co-sputtering. The new electrocatalyst is composed of ~2 nanometers of medium-entropy nanocrystals surrounded by ~2 nanometers of amorphous regions. The catalyst exhibits exceptional performance, similar to that of single-atom catalysts and better than that of nanocluster-based catalysts. We use aluminum rather than a noble metal as the principal element of the catalyst and ruthenium, which is cheaper than platinum, as the noble metal component. The design strategy provides an efficient route for the development of electrocatalysts for use in large-scale hydrogen production. Moreover, the superior hydrogen reaction evolution created by the synergistic effect of the nano-dual-phase structure is expected to guide the development of high-performance catalysts in other alloy systems.
Plasmon-mediated chemical reactions (PMCRs) possess desirable opportunities for manipulating the reaction outcomes due to the unique impact from surface plasmons. However, achieving PMCR product selectivity by tuning the light wavelength has rarely been demonstrated and the underlying mechanism of product selectivity remains elusive. This work studies the reaction mechanism of one classical type of PMCR, plasmon-aided reduction of p-nitrothiophenol (PNTP), and discovers that the reduction product of PNTP can be easily manipulated by adjusting the excitation light wavelength due to the different thermal and hot-electron effects induced by the different wavelengths. Specifically, the sole product of p,p′-dimercaptoazobenzene is obtained under 514 nm light due to the dominant thermal effect thus created, whereas p-aminothiophenol is more favorably produced under 785 nm light, which enables more efficient generation of hot electrons.
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