Electrochemical Activation of Single-Walled Carbon Nanotubes with Pseudo-Atomic-Scale Platinum for the Hydrogen Evolution Reaction

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@article{31cad6fb054c4fc6bb2eff8ec9f060f8,
title = "Electrochemical Activation of Single-Walled Carbon Nanotubes with Pseudo-Atomic-Scale Platinum for the Hydrogen Evolution Reaction",
abstract = "The development of effective and inexpensive hydrogen evolution reaction (HER) electrocatalysts for future renewable energy systems is highly desired. Platinum-based materials are the most active electrocatalysts for catalyzing HER, but reducing the use of Pt is required because of the high price and scarcity of Pt. Here, we achieve pseudo-atomic-scale dispersion of Pt, i.e. individual atoms or subnanometer clusters, on the sidewalls of single-walled carbon nanotubes (SWNTs) with a simple and readily upscalable electroplating deposition method. These SWNTs activated with an ultralow amount of Pt exhibit activity similar to that of commercial Pt/C with a notably higher (∼66–333-fold) Pt loading for catalyzing the HER under the acidic conditions required in proton exchange membrane technology. These catalysts resemble pseudo-atomic-scale Pt systems which are mainly composed of a few to tens of Pt atoms dispersed on the sidewalls of the SWNTs. The Pt loading is only 0.19–0.75 atom {\%} at the electrode surface, and characteristic peaks for Pt cyclic voltammograms are undetectable. The atomic dispersion increases the portion of the surface active-atom sites, and therefore, notably lower Pt loading is needed to attain a high catalytic activity. Density functional theory (DFT) calculations suggest higher ability for SWNTs, in comparison to graphene, as a catalyst support for immobilizing Pt atoms, thus providing an atomic dispersion. Moreover, a high HER activity for the SWNTs activated with Pt atoms, similar to that of bulk Pt, is predicted.",
keywords = "carbon nanotube, DFT calculation, electroplating, hydrogen evolution, pseudo-atomic-scale Pt",
author = "Mohammad Tavakkoli and Nico Holmberg and Rasmus Kronberg and Hua Jiang and Jani Sainio and Esko Kauppinen and Tanja Kallio and Kari Laasonen",
year = "2017",
doi = "10.1021/acscatal.7b00199",
language = "English",
volume = "7",
pages = "3121–3130",
journal = "ACS Catalysis",
issn = "2155-5435",
publisher = "AMERICAN CHEMICAL SOCIETY",
number = "5",

}

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TY - JOUR

T1 - Electrochemical Activation of Single-Walled Carbon Nanotubes with Pseudo-Atomic-Scale Platinum for the Hydrogen Evolution Reaction

AU - Tavakkoli, Mohammad

AU - Holmberg, Nico

AU - Kronberg, Rasmus

AU - Jiang, Hua

AU - Sainio, Jani

AU - Kauppinen, Esko

AU - Kallio, Tanja

AU - Laasonen, Kari

PY - 2017

Y1 - 2017

N2 - The development of effective and inexpensive hydrogen evolution reaction (HER) electrocatalysts for future renewable energy systems is highly desired. Platinum-based materials are the most active electrocatalysts for catalyzing HER, but reducing the use of Pt is required because of the high price and scarcity of Pt. Here, we achieve pseudo-atomic-scale dispersion of Pt, i.e. individual atoms or subnanometer clusters, on the sidewalls of single-walled carbon nanotubes (SWNTs) with a simple and readily upscalable electroplating deposition method. These SWNTs activated with an ultralow amount of Pt exhibit activity similar to that of commercial Pt/C with a notably higher (∼66–333-fold) Pt loading for catalyzing the HER under the acidic conditions required in proton exchange membrane technology. These catalysts resemble pseudo-atomic-scale Pt systems which are mainly composed of a few to tens of Pt atoms dispersed on the sidewalls of the SWNTs. The Pt loading is only 0.19–0.75 atom % at the electrode surface, and characteristic peaks for Pt cyclic voltammograms are undetectable. The atomic dispersion increases the portion of the surface active-atom sites, and therefore, notably lower Pt loading is needed to attain a high catalytic activity. Density functional theory (DFT) calculations suggest higher ability for SWNTs, in comparison to graphene, as a catalyst support for immobilizing Pt atoms, thus providing an atomic dispersion. Moreover, a high HER activity for the SWNTs activated with Pt atoms, similar to that of bulk Pt, is predicted.

AB - The development of effective and inexpensive hydrogen evolution reaction (HER) electrocatalysts for future renewable energy systems is highly desired. Platinum-based materials are the most active electrocatalysts for catalyzing HER, but reducing the use of Pt is required because of the high price and scarcity of Pt. Here, we achieve pseudo-atomic-scale dispersion of Pt, i.e. individual atoms or subnanometer clusters, on the sidewalls of single-walled carbon nanotubes (SWNTs) with a simple and readily upscalable electroplating deposition method. These SWNTs activated with an ultralow amount of Pt exhibit activity similar to that of commercial Pt/C with a notably higher (∼66–333-fold) Pt loading for catalyzing the HER under the acidic conditions required in proton exchange membrane technology. These catalysts resemble pseudo-atomic-scale Pt systems which are mainly composed of a few to tens of Pt atoms dispersed on the sidewalls of the SWNTs. The Pt loading is only 0.19–0.75 atom % at the electrode surface, and characteristic peaks for Pt cyclic voltammograms are undetectable. The atomic dispersion increases the portion of the surface active-atom sites, and therefore, notably lower Pt loading is needed to attain a high catalytic activity. Density functional theory (DFT) calculations suggest higher ability for SWNTs, in comparison to graphene, as a catalyst support for immobilizing Pt atoms, thus providing an atomic dispersion. Moreover, a high HER activity for the SWNTs activated with Pt atoms, similar to that of bulk Pt, is predicted.

KW - carbon nanotube

KW - DFT calculation

KW - electroplating

KW - hydrogen evolution

KW - pseudo-atomic-scale Pt

U2 - 10.1021/acscatal.7b00199

DO - 10.1021/acscatal.7b00199

M3 - Article

VL - 7

SP - 3121

EP - 3130

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 5

ER -

ID: 13071754