Green chemistry and first-principles theory enhance catalysis: synthesis and 6-fold catalytic activity increase of sub-5 nm Pd and Pt@Pd nanocubes

Mastronardi, Valentina; Kim, Junseok; Veronesi, Marina; Pomili, Tania; Berti, Francesco; Udayan, Gayatri; Brescia, Rosaria; Diercks, Justus S.; Herranz, Juan; Bandiera, Tiziano; Fichthorn, Kristen A.; Pompa, Pier Paolo; Moglianetti, Mauro

doi:10.1039/d2nr02278h

Title: Green chemistry and first-principles theory enhance catalysis: synthesis and 6-fold catalytic activity increase of sub-5 nm Pd and Pt@Pd nanocubes

Journal Article · Thu Jun 30 00:00:00 EDT 2022 · Nanoscale

DOI:https://doi.org/10.1039/d2nr02278h· OSTI ID:1975739

Mastronardi, Valentina ^[1]; Kim, Junseok ^[2]; Veronesi, Marina ^[3]; Pomili, Tania ^[1]; Berti, Francesco ^[3]; Udayan, Gayatri ^[4];

^[5]; Diercks, Justus S. ^[6];

^[6];

^[3];

^[2];

^[5];

^[7]

Istituto Italiano di Tecnologia, Genova (Italy); University of Genova (Italy)
Pennsylvania State University, University Park, PA (United States)
Istituto Italiano di Tecnologia, Genoa (Italy)
University of Salento, Lecce (Italy); Istituto Italiano di Tecnologia, Arnesano (Lecce) (Italy)
Istituto Italiano di Tecnologia, Genova (Italy)
Paul Scherrer Institut, Villigen (Switzerland)
Istituto Italiano di Tecnologia, Genova (Italy); Istituto Italiano di Tecnologia, Arnesano (Lecce) (Italy)

Synthesizing metal nanoparticles with fine control of size, shape and surface properties is of high interest for applications such as catalysis, nanoplasmonics, and fuel cells. In this contribution, we demonstrate that the citrate-coated surfaces of palladium (Pd) and platinum (Pt)@Pd nanocubes with a lateral length <5 nm and low polydispersity in shape achieve superior catalytic properties. The synthesis achieves great control of the nanoparticle's physico-chemical properties by using only biogenic reagents and bromide ions in water while being fast, easy to perform and scalable. The role of the seed morphology is pivotal as Pt single crystal seeds are necessary to achieve low polydispersity in shape and prevent nanorods formation. In addition, electrochemical measurements demonstrate the abundancy of Pd{100} surface facets at a macroscopic level, in line with information inferred from TEM analysis. Quantum density functional theory calculations indicate that the kinetic origin of cubic Pd nanoshapes is facet-selective Pd reduction/deposition on Pd(111). Moreover, we underline both from an experimental and theoretical point of view that bromide alone does not induce nanocube formation without the synergy with formic acid. Furthermore, the superior performance of these highly controlled nanoparticles to perform the catalytic reduction of 4-nitrophenol was proved: polymer-free and surfactant-free Pd nanocubes outperform state-of-the-art materials by a factor >6 and a commercial Pd/C catalyst by more than one order of magnitude.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF); USDOE

Grant/Contract Number:: FG02-07ER46414; ACI-1548562; DE FG02-07ER46414

OSTI ID:: 1975739

Alternate ID(s):: OSTI ID: 1875179

Journal Information:: Nanoscale, Vol. 14, Issue 28; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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