Enhanced single-nanoparticle collisions for the hydrogen evolution reaction in a confined microchannel

doi:10.1016/S1872-2067(21)64034-2

Abstract

Abstract:

Single nanoparticle (NP) collisions technique has been widely employed in electrocatalysis. However, the short collision duration of single NPs hinders the further improvement in their electrocatalytic performance. Here, to increase the dynamic collision duration of single NPs in the electron tunneling region, enhanced near-wall hindered diffusion is introduced in the stochastic collision process by coupling a Au ultramicroelectrode (UME) with a confined microchannel. In the case of single palladium nanoparticle (Pd NP) collisions for the hydrogen evolution reaction (HER), the hydrodynamic trapping confined in the microchannel effectively permits the activation of the HER on the single Pd NPs. The microchannel-based Au UME is promising in the application of single-NP collisions to energy conversion.

Key words: Single-nanoparticle collisions, Confined microchannel, Hydrodynamic trapping, Collision duration, Hydrogen evolution reaction

Si-Min Lu, Mengjie Chen, Huilin Wen, Hao-Wei Wang, Ziyi Yu, Yi-Tao Long. Enhanced single-nanoparticle collisions for the hydrogen evolution reaction in a confined microchannel[J]. Chinese Journal of Catalysis, 2022, 43(11): 2815-2819.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64034-2

https://www.cjcatal.com/EN/Y2022/V43/I11/2815

Figures/Tables 4

Fig. 1. Schematic illustration of single Pd NP collisions for the HER in a confined microchannel. Diagram of the microchannel-based Au UME device for the stochastic collision electrochemistry of single Pd NPs (left). Raw time-resolved current traces in the presence or absence of Pd NPs in the microchannel (right).

Fig. 2. Transient i-t curves and their magnified images of single Pd NP collisions with the microchannel-based Au UME at biased potentials from -100 to -900 mV vs. Ag/AgCl QRCE. The confined microchannel is filled with 20 nm-diameter Pd NPs suspended in a 10.0 mmol/L HClO4 aqueous electrolyte solution, and the concentration of Pd NPs in the stock solution is 200 pmol/L

Fig. 3. Scatter plots (a-e) and statistical results (f) of collision duration versus integrated charge of single Pd NP collision electrochemistry for the HER using the microchannel-based Au UME at biased potentials ranging from -500 to -900 mV vs. Ag/AgCl QRCE. Shown in the inset in Fig. 3(f) is a configuration image of the microchannel-based Au UME. The confined microchannel is filled with 20 nm-diameter Pd NPs suspended in a 10.0 mmol/L HClO4 aqueous electrolyte solution, and the stock solution has a Pd NP concentration of 200 pmol/L.

Table 1 Statistical results of collision duration, integrated charge, and current amplitude.*

Biased potential (mV vs. Ag/AgCl QRCE)	Duration (ms)	Charge (fC)	Current (pA)
-500	3.1	64	37
-600	2.0	68	63
-700	0.8	13	34
-800	1.3	22	49
-900	1.1	47	83

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