TY - JOUR
T1 - Single Nanoparticle Activities in Ensemble
T2 - A Study on Pd Cluster Nanoportals for Electrochemical Oxygen Evolution Reaction
AU - Datta, Abheek
AU - Porkovich, Alexander J.
AU - Kumar, Pawan
AU - Nikoulis, Giorgos
AU - Kioseoglou, Joseph
AU - Sasaki, Toshio
AU - Steinhauer, Stephan
AU - Grammatikopoulos, Panagiotis
AU - Sowwan, Mukhles
N1 - Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/10/31
Y1 - 2019/10/31
N2 - Comprehensive understanding of the electrochemical activity of single nanoparticles (NPs) is in critical need for opening new avenues in the broad field of electrochemistry. Published reports on single-NP electrocatalysts typically include complicated and difficult methods of synthesis and characterization; moreover, these methods usually fail to provide a reliable way to measure the activities of individual NPs within larger ensembles of particles, i.e., in real-life nanocatalyst systems. In the present work, we synthesized from the gas phase Pd NPs that act as nanoportals for electron transfer within surface-oxidized Mg thin films. The physical synthesis method provided excellent control over the deposition density and, hence, enabled the design of a system where each individual open nanoportal forms an independent active single-NP electrode (SNPE). Being uncoupled from one another, these SNPEs contribute separately toward the total electrocatalytic activity while simultaneously providing a measure of their average, individual activities. We were thus able to fabricate a stable, steady-state electrode for the electrochemical oxygen evolution reaction (OER) and to study the activity and stability of the SNPEs over a period of 20 days; the former depended on the size of the NPs, while the latter depended on the SNPEs' resistance to aerial oxidation. The remarkable stability of the ensemble catalysts under OER conditions proves that this concept can be used for further studies on the activities of different single NPs in numerous real-life systems.
AB - Comprehensive understanding of the electrochemical activity of single nanoparticles (NPs) is in critical need for opening new avenues in the broad field of electrochemistry. Published reports on single-NP electrocatalysts typically include complicated and difficult methods of synthesis and characterization; moreover, these methods usually fail to provide a reliable way to measure the activities of individual NPs within larger ensembles of particles, i.e., in real-life nanocatalyst systems. In the present work, we synthesized from the gas phase Pd NPs that act as nanoportals for electron transfer within surface-oxidized Mg thin films. The physical synthesis method provided excellent control over the deposition density and, hence, enabled the design of a system where each individual open nanoportal forms an independent active single-NP electrode (SNPE). Being uncoupled from one another, these SNPEs contribute separately toward the total electrocatalytic activity while simultaneously providing a measure of their average, individual activities. We were thus able to fabricate a stable, steady-state electrode for the electrochemical oxygen evolution reaction (OER) and to study the activity and stability of the SNPEs over a period of 20 days; the former depended on the size of the NPs, while the latter depended on the SNPEs' resistance to aerial oxidation. The remarkable stability of the ensemble catalysts under OER conditions proves that this concept can be used for further studies on the activities of different single NPs in numerous real-life systems.
UR - http://www.scopus.com/inward/record.url?scp=85074353069&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcc.9b07824
DO - 10.1021/acs.jpcc.9b07824
M3 - 评论/辩论
AN - SCOPUS:85074353069
SN - 1932-7447
VL - 123
SP - 26124
EP - 26135
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 43
ER -