Au@AuPd Core-Alloyed Shell Nanoparticles for Enhanced Electrocatalytic Activity and Selectivity under Visible Light Excitation
Plasmonic catalysis has been employed to enhance molecular transformations under visible light excitation, leveraging the localized surface plasmon resonance (LSPR) in plasmonic nanoparticles. While plasmonic catalysis has been employed for accelerating reaction rates, achieving control over the reaction selectivity has remained a challenge. In addition, the incorporation of catalytic components into traditional plasmonic-catalytic antenna-reactor nanoparticles often leads to a decrease in optical absorption. To address these issues, this study focuses on the synthesis of bimetallic core@shell Au@AuPd nanoparticles (NPs) with ultralow loadings of palladium (Pd) into gold (Au) NPs. The goal is to achieve NPs with an Au core and a dilute alloyed shell containing both Au and Pd, with a low Pd content of around 10 atom %. By employing the (photo)electrocatalytic nitrite reduction reaction (NO<sub>2</sub>RR) as a model transformation, experimental and theoretical analyses show that this design enables enhanced catalytic activity and selectivity under visible light illumination. We found that the optimized Pd distribution in the alloyed shell allowed for stronger interaction with key adsorbed species, leading to improved catalytic activity and selectivity, both under no illumination and under visible light excitation conditions. The findings provide valuable insights for the rational design of antenna-reactor plasmonic-catalytic NPs with controlled activities and selectivity under visible light irradiation, addressing critical challenges to enable sustainable molecular transformations.
Authors
- Thomas J. A. Slater (ORCID: https://orcid.org/0000-0003-0372-1551)
- Elton Sitta (ORCID: https://orcid.org/0000-0003-3181-0076)
- Hugo L. S. Santos (ORCID: https://orcid.org/0000-0003-0187-6250)
- Shwetha Shetty (ORCID: https://orcid.org/0000-0002-8608-0472)
- IbrahiM Abdelsalam (ORCID: https://orcid.org/0009-0007-5280-9337)
- Pedro H. C. Camargo (ORCID: https://orcid.org/0000-0002-7815-7919)
- Kaline N. da Silva (ORCID: https://orcid.org/0000-0001-8077-146X)
- Tiago Vinicius Alves (ORCID: https://orcid.org/0000-0001-9129-3272)
- Rongsheng Cai (ORCID: https://orcid.org/0000-0002-2148-0563)
- Mykhailo Chundak (ORCID: https://orcid.org/0000-0003-4417-1832)
- Niko Heikkinen (ORCID: https://orcid.org/0000-0002-9788-1291)
- Jhon Quiroz (ORCID: https://orcid.org/0000-0002-8626-7210)
- Sarah J. Haigh (ORCID: https://orcid.org/0000-0001-5509-6706)
- Mikko Ritala (ORCID: https://orcid.org/0000-0002-6210-2980)
- Víctor A. de la Peña O’Shea (ORCID: https://orcid.org/0000-0001-5762-4787)
- Wenyi Huo (ORCID: https://orcid.org/0000-0001-8297-9045)
- Sam Sullivan Allsop (ORCID: https://orcid.org/0000-0002-8697-6922)
- Shiqi Wang (ORCID: https://orcid.org/0000-0003-2010-0132)
- F. Palacio (ORCID: https://orcid.org/0000-0001-7222-9603)
Institutions
- Madrid Institute for Advanced Studies (ES)
- Universidade Federal da Bahia (BR)
- University of Helsinki (FI)
- Nanjing Forestry University (CN)
- Universidade Federal de São Carlos (BR)
- University of Manchester (GB)
- IMDEA Energy Institute (ES)
- National Centre for Nuclear Research (PL)
- Cardiff University (GB)
- VTT Technical Research Centre of Finland (FI)
Publication Details
- Journal
- ACS Nano
- Published
- 2024-08-20
- DOI
- https://doi.org/10.1021/acsnano.4c07076
- Citations
- 17
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 1.74
Funders
- Ministerio de Ciencia, Innovación y Universidades
- Henry Royce Institute
- European Commission
- Fundação de Amparo à Pesquisa do Estado de São Paulo
- Fundacja na rzecz Nauki Polskiej
- Coordenação de Aperfeiçoamento de Pessoal de Nível Superior
- Academy of Finland
- Conselho Nacional de Desenvolvimento Científico e Tecnológico
- Jane ja Aatos Erkon Säätiö
- Horizon 2020 Framework Programme
- Engineering and Physical Sciences Research Council
- European Regional Development Fund
- Agencia Estatal de Investigación
- Interreg
- H2020 European Research Council