Plasmon coupling inside 2D-like TiB2 flakes for water splitting half reactions enhancement in acidic and alkaline conditions
Graphical abstract
Introduction
Excitation of plasmon on the surface of metal nanostructures allows focusing light into a nanospace with a “deep” sub-diffraction limit [1]. This effect makes possible to reach the spatially restricted gigantic local concentration of energy which find wide applications in surface-enhanced Raman scattering (SERS) and chemical transformation initiation [2], [3], [4], [5]. In the last case, the plasmon triggering ensures the activation of surrounding dielectric molecules or materials, leading to their direct chemical transformation or to the enhancement of their catalytic properties [6], [7], [8], [9], [10]. Plasmonics is involved in various relevant areas of photo- of photo-electrochemical water splitting, CO2 and nitrogen reduction as well as pollutant degradation [11], [12], [13], [14], [15], [16], [17]. Plasmon assistance in these processes allows to increase in the overall efficiency and expand the range of “useful” light wavelengths [18], [19]. As for the structure design plasmon active nanostructures are coupled with redox-active or catalytically-active materials, and an enhancement of the catalytic activity proceeds through the direct charge carrier injection, inner charge carriers excitation, or plasmon heating [20], [21], [22].
The hybridization of the most previously reported structures includes the deposition of plasmon active nanostructures on the surface of catalytic materials (including 2D flakes), with previously known HER or OER activities, like the TiO2, g-C3N4, WO3, or MXene flakes [23], [24], [25], [26], [27], [28], [29], [30], [31], [32], [33]. In this case, the redox active material is subjected to a plasmonic field excited on the surface of metal nanostructures [34], [35], [36]. However, there exists an additional possibility to increase the plasmonic efficiency by several orders of magnitude by creating plasmonic hot spots [37], [38], [39], [40]. These hot spots can be exited in the close, vicinity of symmetric (e.g. two similar metal nanoparticles) or asymmetric (e.g. metal nanoparticles nearby of a thin metal film or grating) coupled plasmon active nanostructures [41], [42], [43], [44], [45]. Plasmon coupling creates much higher local energy and electric field values and, actually find wide application in SERS. However, its usage for triggering of chemical transformation has been rarely reported [46], [47], [48].
In this work, we propose the utilization of plasmon coupling (in particular SPP-LSP coupling) for triggering of catalytic activity of “quasi” 2D flakes of TiB2 for the first time. TiB2 was previously reported as a medium water splitting catalyst, favorable for its availability and preparation simplicity. However, its catalytic activity in both HER and OER processes is not satisfactory. At the beginning of this work, we supposed that the utilization of coupled plasmonic triggering and exposure of TiB2 to gigantic energy in plasmonic hot spots could significantly increase the flakes' catalytic activity.
Section snippets
Chemical and materials
Titanium boride (titanium boride powder < 10 μm) precursor was supplied by Sigma-Aldrich. Au target (purity of 99.99 %) was provided by Safina. Gold (III) chloride trihydrate (≥99.9 %), potassium hydroxide, sulfuric acid (96.0 %), deionized water, and methanol were purchased from Sigma-Aldrich. All chemical reagents were used as received without further purification.
Samples preparation
Exfoliation of TiB2. Few-layer titanium diboride sheets were prepared using a high-intensity cavitation field in an ultrasound
Proposed experimental concept: LSP-SPP coupling inside TiB2
The scheme of our experimental concept is shown in Fig. 1. In the first step, the previously developed procedure, based on ultrasonic-assisted liquid-phase exfoliation was used to produce TiB2 flake-like structures from bulk powder [54], [55]. Then, the AuNPs, ensuring the LSP excitation, were synthesized on the basal planes of flakes. Simultaneously, we created the periodically patterned grating-like polymer template, which was further covered by a thin gold layer. In both cases we used the Au
Conclusion
In this work, we propose the utilization of LSP-SPP plasmonic coupling for the efficient triggering of TiB2 flakes' catalytic activity. For this purpose, the AuNPs were deposited on the flakes to provide the LSP excitation. Then the TiB2@AuNPs flakes were deposited on the surface of Au grating, providing the excitation of SPP. As a result, the TiB2 flakes were situated in the place of coupled LSP-SPP plasmonic hot spots, where the gigantic concentration of plasmonic energy occurs. This
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgment
This work was supported by the GACR under the project No. 21-09277S.
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