journal article·2024-09-03Open access

Au@AuPd Core-Alloyed Shell Nanoparticles for Enhanced Electrocatalytic Activity and Selectivity under Visible Light Excitation

Kaline N. da Silva, Shwetha Shetty, Sam Sullivan−Allsop, Rongsheng Cai, Shiqi Wang, Jhon Quiroz, Mykhailo Chundak, Hugo L. S. dos Santos, IbrahiM Abdelsalam, Freddy E. Oropeza, Víctor A. de la Peña O’Shea, Niko Heikkinen, Elton Sitta, Tiago V. Alves, Mikko Ritala, Wenyi Huo, Thomas J. A. Slater, Sarah J. Haigh, Pedro H. C. Camargo

ACS Nano· Volume 18· Issue 35

Abstract

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 2 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.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced Photocatalysis Techniques · Advanced Nanomaterials in Catalysis

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, University of Helsinki, A.I. Virtasen aukio 1, PO Box 55, FIN-0014 Helsinki, Finland

Department of Materials, University of Manchester, Manchester M13 9PL, United Kingdom

Photoactivated Processes Unit, IMDEA Energy Institute, Avda. Ramón de la Sagra 3, 28935 Mostoles, Madrid, Spain

VTT Technical Research Centre of Finland, P O Box 1000, FIN-02044 Espoo, Finland

Department of Chemistry, Federal University of Sao Carlos, Rod. Washington Luis, km 235, Sao Carlos 13565−905, Brazil

Departamento de Físico-Química, Instituto de Química, Universidade Federal da Bahia, Rua Barão de Jeremoabo, 14740170-115 Salvador, BA, Brazil

College of Mechanical and Electrical Engineering, Nanjing Forestry University, Nanjing 210037, P. R. China

NOMATEN Centre of Excellence, National Centre for Nuclear Research, Otwock 05-400, Poland

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, United Kingdom

Funding

Engineering and Physical Sciences Research Council · Ministerio de Ciencia, Innovaci?n y Universidades · European Commission · European Regional Development Fund · Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico · Funda??o de Amparo ? Pesquisa do Estado de S?o Paulo · Research Council of Finland · Jane ja Aatos Erkon S??ti? · Horizon 2020 Framework Programme · H2020 European Research Council · Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior

References (61)

Show source-provided references
1. 10.1038/s41929-018-0138-x10.1038/s41929-018-0138-x ↗
2. Camargo P. H. · 202110.1002/9783527826971 ↗
3. 10.1021/acs.chemrev.9b0018710.1021/acs.chemrev.9b00187 ↗
4. 10.1126/science.aat696710.1126/science.aat6967 ↗
5. 10.1021/acsnano.0c0877310.1021/acsnano.0c08773 ↗
6. 10.1002/anie.20221639810.1002/anie.202216398 ↗
7. 10.1021/acscatal.3c0093710.1021/acscatal.3c00937 ↗
8. 10.1021/acs.nanolett.8b0349910.1021/acs.nanolett.8b03499 ↗
9. 10.1016/j.cocis.2019.01.01410.1016/j.cocis.2019.01.014 ↗
10. 10.1073/pnas.160976911310.1073/pnas.1609769113 ↗
11. 10.1038/s41560-019-0517-910.1038/s41560-019-0517-9 ↗
12. 10.1021/acs.nanolett.7b0099210.1021/acs.nanolett.7b00992 ↗
13. 10.1021/acs.nanolett.8b0349910.1021/acs.nanolett.8b03499 ↗
14. 10.1038/nnano.2017.13110.1038/nnano.2017.131 ↗
15. 10.1021/acsenergylett.8b0084110.1021/acsenergylett.8b00841 ↗
16. 10.1021/acsenergylett.0c0211010.1021/acsenergylett.0c02110 ↗
17. 10.1002/smll.20140377710.1002/smll.201403777 ↗
18. 10.1021/jacs.6b0253210.1021/jacs.6b02532 ↗
19. 10.1021/acscatal.3c0056810.1021/acscatal.3c00568 ↗
20. 10.1038/s41467-017-00055-z10.1038/s41467-017-00055-z ↗
21. 10.1038/s41467-023-38982-910.1038/s41467-023-38982-9 ↗
22. 10.1016/S0926-860X(96)00418-810.1016/S0926-860X(96)00418-8 ↗
23. 10.1063/1.48077310.1063/1.480773 ↗
24. 10.1021/jp103833310.1021/jp1038333 ↗
25. 10.1021/acsanm.9b0205610.1021/acsanm.9b02056 ↗
26. 10.1039/C7CY00794A10.1039/C7CY00794A ↗
27. 10.1039/D1NA00489A10.1039/D1NA00489A ↗
28. 10.1039/C7CY02329D10.1039/C7CY02329D ↗
29. 10.1016/j.susc.2018.06.00610.1016/j.susc.2018.06.006 ↗
30. 10.1039/D2NJ01773C10.1039/D2NJ01773C ↗
31. 10.1021/acs.jpcc.9b1047310.1021/acs.jpcc.9b10473 ↗
32. 10.1021/acscatal.7b0054710.1021/acscatal.7b00547 ↗
33. 10.1039/an980050030510.1039/an9800500305 ↗
34. 10.1038/nmat315110.1038/nmat3151 ↗
35. 10.1039/D1CS00237F10.1039/D1CS00237F ↗
36. 10.1021/acsenergylett.0c0098910.1021/acsenergylett.0c00989 ↗
37. 10.1021/jacs.2c0127210.1021/jacs.2c01272 ↗
38. 10.1038/s41467-023-38235-910.1038/s41467-023-38235-9 ↗
39. 10.1021/ja511719g10.1021/ja511719g ↗
40. 10.1021/acsnano.2c0354910.1021/acsnano.2c03549 ↗
41. 10.1021/acsnano.2c1047010.1021/acsnano.2c10470 ↗
42. 10.1002/anie.20221639810.1002/anie.202216398 ↗
43. 10.1002/anie.20190445210.1002/anie.201904452 ↗
44. 10.1038/ncomms1454210.1038/ncomms14542 ↗
45. 10.1021/acsenergylett.9b0168810.1021/acsenergylett.9b01688 ↗
46. 10.1039/D0NR06270G10.1039/D0NR06270G ↗
47. 10.1002/anie.20220607710.1002/anie.202206077 ↗
48. 10.1038/s41467-023-35860-210.1038/s41467-023-35860-2 ↗
49. 10.1002/adma.20230253810.1002/adma.202302538 ↗
50. 10.1002/adfm.20220681710.1002/adfm.202206817 ↗
51. 10.1002/anie.20191312210.1002/anie.201913122 ↗
52. 10.1002/adma.20210530810.1002/adma.202105308 ↗
53. 10.1039/D2EE02151J10.1039/D2EE02151J ↗
54. 10.1002/adma.20190711210.1002/adma.201907112 ↗
55. 10.1002/smll.20220240410.1002/smll.202202404 ↗
56. Hyperspy/Hyperspy: Release v1.6.3, 10.5281/ZENODO.4923970. Accessed on August 5th, 2024.
57. 10.1016/j.theochem.2005.02.01510.1016/j.theochem.2005.02.015 ↗
58. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
59. 10.1063/1.338234410.1063/1.3382344 ↗
60. 10.1021/jp047349j10.1021/jp047349j ↗
61. 10.1021/jp061667w10.1021/jp061667w ↗