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1.
Phys Chem Chem Phys ; 26(25): 17456-17466, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38888144

RESUMO

While model studies with small nanoparticles offer a bridge between applied experiments and theoretical calculations, the intricacies of working with well-defined nanoparticles in electrochemistry pose challenges for experimental researchers. This perspective dives into nanoparticle electrochemistry, provides experimental insights to uncover their intrinsic catalytic activity and draws conclusions about the effects of altering their size, composition, or loading. Our goal is to help uncover unexpected contamination sources and establish a robust experimental methodology, which eliminates external parameters that can overshadow the intrinsic activity of the nanoparticles. Additionally, we explore the experimental difficulties that can be encountered, such as stability issues, and offer strategies to mitigate their impact. From support preparation to electrocatalytic tests, we guide the reader through the entire process, shedding light on potential challenges and crucial experimental details when working with these complex systems.

2.
J Am Chem Soc ; 146(3): 2015-2023, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38196113

RESUMO

Understanding the size-dependent behavior of nanoparticles is crucial for optimizing catalytic performance. We investigate the differences in selectivity of size-selected gold nanoparticles for CO2 electroreduction with sizes ranging from 1.5 to 6.5 nm. Our findings reveal an optimal size of approximately 3 nm that maximizes selectivity toward CO, exhibiting up to 60% Faradaic efficiency at low potentials. High-resolution transmission electron microscopy reveals different shapes for the particles and suggests that multiply twinned nanoparticles are favorable for CO2 reduction to CO. Our analysis shows that twin boundaries pin 8-fold coordinated surface sites and in turn suggests that a variation of size and shape to optimize the abundance of 8-fold coordinated sites is a viable path for optimizing the CO2 electrocatalytic reduction to CO. This work contributes to the advancement of nanocatalyst design for achieving tunable selectivity for CO2 conversion into valuable products.

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