Catalytic Synergies in Bimetallic Ru-Pt Single–Atom Catalysts via Speciation Control

Vera Giulimondi; Andrea Ruiz–Ferrando; Adam H. ClarkSelina K. KaiserFrank KrumeichAntonio J. MartínNúria LópezJavier Pérez–Ramírez

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Catalytic Synergies in Bimetallic Ru-Pt Single–Atom Catalysts via Speciation Control

机译：Catalytic Synergies in Bimetallic Ru-Pt Single–Atom Catalysts via Speciation Control

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Bimetallic single–atom catalysts (b–SACs) have recently gained prominenceby virtue of the unique catalytic cooperative interactions they can exhibit,intertwining electronic and geometric effects. To date, research efforts haveexclusively focused on direct mechanisms such as electron density transfer orsequential reactivity. Herein, the first study on indirect, coordination–inducedcatalytic synergies in carbon-supported Ru-Pt SACs is conducted. To thisend, a holistic approach is developed, combining ⅰ) precision synthesis,ⅱ) advanced characterization, ⅲ) exploration of single–site adsorption propertiesvia the hydrogen evolution reaction, and ⅳ) modeling through densityfunctional theory. Despite the lack of both intermetallic coordination in thefirst or second shell and charge redistribution effects, the RuPt SACs exhibita H_2 formation rate enhanced up to 15–fold compared with their monometalliccounterparts. To unfold the origin of the intermetallic cooperativity,modifications of the structural and catalytic properties induced by the integrationof a second metal species are investigated. Thus, Pt atoms are foundto selectively occupy the most energeticallyfavorable cavities in the support,prompting Ru atoms to assume a distinct, more active, configuration. Thiscontribution unveils a novel principle of bimetallic cooperativity, demonstratingthe key role of integrative experimental and computational analysesin studying b–SACs.

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《Advanced functional materials》 |2022年第51期|2206513.1-2206513.12|共12页
作者
Vera Giulimondi; Andrea Ruiz–Ferrando; Adam H. ClarkSelina K. KaiserFrank KrumeichAntonio J. MartínNúria LópezJavier Pérez–Ramírez;
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Institute for Chemical and BioengineeringDepartment of Chemistry and Applied BiosciencesETH ZurichVladimir–Prelog–Weg 1, 8093 Zurich, Switzerland;

Institute of Chemical Research of Catalonia (ICIQ)The Barcelona Institute of Science and TechnologyAv. Pa?sos Catalans 16, 43007 Tarragona, Spain;

Departament de Química Física I InorgànicaUniversitat Rovira I VirgiliMarcel·lí Domingo s/n, 43007 Tarragona, Spain;

Institute of Chemical Research of Catalonia (ICIQ)The Barcelona Institute of Science and TechnologyAv. Pa?sos Catalans 16, 43007 Tarragona,Paul Scherrer Institute5232 Villigen PSI, Switzerland;

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正文语种英语
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active site coordination; bimetallic systems; cooperativity effects; single–atom catalysts;

Catalytic Synergies in Bimetallic Ru-Pt Single–Atom Catalysts via Speciation Control

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