Issue 2, 2020

Photon-induced synthesis of ultrafine metal nanoparticles on graphene as electrocatalysts: impact of functionalization and doping

Abstract

Utilizing reducing species generated by high-energy photons offers an alternative strategy to prepare metal nanoparticles (NPs) in the absence of a foreign reductant. However, fine control of the NP size and dispersity remains a big challenge. Herein, we report that by properly selecting the solvent, precursor concentration and carbon support, ultrafine palladium (Pd) NPs with an average size of 3.0 nm uniformly distributed on nitrogen-doped graphene (NG) are radiolytically prepared. Control experiments demonstrate that ethylene glycol with moderate reducibility is a superior solvent to water. Among four graphene-based supports with distinct functionalization or doping, nitrogen dopants outperform oxygen functional groups in anchoring the NPs and controlling their size and dispersity. Pd/NG also affords the lowest η10 (overpotential at a current density of 10 mA cm−2) toward the hydrogen evolution reaction (HER). Comparison of Pd/NG with varied Pd loadings indicates that the HER activity nearly reaches a plateau once the loading increases to 2.6 wt%, which is limited by the nitrogen content of NG. X-ray photoelectron spectroscopy unambiguously reveals the electron transfer from electron-rich Pd to electron-deficient nitrogen, especially graphitic nitrogen, corroborating the decisive role of doped nitrogen in stabilizing the Pd NPs on NG. Extending this synthesis to platinum (Pt) yields Pt/NG that presents even lower η10 than the commercial 10 wt% Pt/carbon black due to the smaller NP size. These results collectively highlight the potential of high-energy photons for green, versatile and scalable synthesis of heterogeneous nanostructures.

Graphical abstract: Photon-induced synthesis of ultrafine metal nanoparticles on graphene as electrocatalysts: impact of functionalization and doping

Supplementary files

Article information

Article type
Paper
Submitted
24 sen 2019
Accepted
22 noy 2019
First published
25 noy 2019

J. Mater. Chem. A, 2020,8, 714-723

Photon-induced synthesis of ultrafine metal nanoparticles on graphene as electrocatalysts: impact of functionalization and doping

K. Guo, L. J. Rowland, L. H. Isherwood, G. Glodan and A. Baidak, J. Mater. Chem. A, 2020, 8, 714 DOI: 10.1039/C9TA10518B

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements