Selina K. Kaiser

Harvard University

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Javier Pérez‐Ramírez

ETH Zurich

Frank Krumeich

Bioengineering (Switzerland)

Adam H. Clark

Paul Scherrer Institute

Núria López

Institut Català d'Investigació Química

Edvin Fako

Robert Bosch (Germany)

Ronghe Lin

Zhejiang Normal University

ОV

Оlga V. Safonova

Paul Scherrer Institute

Vera Giulimondi

ETH Zurich

Sharon Mitchell

ETH Zurich

Antonio J. Martín

ETH Zurich

Cooperative Institutions

ETH Zurich

Harvard University

Freie Universität Berlin

Harvard University Press

Institut Català d'Investigació Química

University of California, Los Angeles

Centre National de la Recherche Scientifique

Lawrence Berkeley National Laboratory

Charles Humbert 8

Bioengineering (Switzerland)

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Controlled Formation of Dimers and Spatially Isolated Atoms in Bimetallic Au-Ru Catalysts via Carbon-Host Functionalization

Zenodo (CERN European Organization for Nuclear Research) (2022)

Vera Giulimondi Selina K. Kaiser Antonio J. Martín Simon Büchele Frank Krumeich

Enclosed we report the data in the article: "Controlled Formation of Dimers and Spatially Isolated Atoms in Bimetallic Au-Ru Catalysts via Carbon-Host Functionalization" by Pérez-Ramírez et al.

Bimetallic strip

Surface Modification

Carbon fibers

10.5281/zenodo.6325284

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Citations (0)

Cover Picture: Design of Single Gold Atoms on Nitrogen‐Doped Carbon for Molecular Recognition in Alkyne Semi‐Hydrogenation (Angew. Chem. Int. Ed. 2/2019)

Angewandte Chemie International Edition (2018)

Ronghe Lin Davide Albani Edvin Fako Selina K. Kaiser Оlga V. Safonova

Single atoms of gold stabilized on nitrogen-doped carbon are studied as heterogeneous catalysts by J. Pérez-Ramírez, N. López, et al. in their Communication on page 504 ff. The cover is inspired by the van Gogh masterpiece “Starry night over the Rhône”. Gold atoms with tailored oxidation state and coordination sphere (stars) exhibit different spectroscopic fingerprints (reflections on water) and an unprecedented volcano-type performance for the hydrogenation of functionalized alkynes (pier). The couple on the shore show that experiments and theory should go hand in hand to achieve a rational catalyst design. Single atoms of gold stabilized on nitrogen-doped carbon are studied as heterogeneous catalysts by J. Pérez-Ramírez, N. López, et al. in their Communication on page 504 ff. The cover is inspired by the van Gogh masterpiece “Starry night over the Rhône”. Gold atoms with tailored oxidation state and coordination sphere (stars) exhibit different spectroscopic fingerprints (reflections on water) and an unprecedented volcano-type performance for the hydrogenation of functionalized alkynes (pier). The couple on the shore show that experiments and theory should go hand in hand to achieve a rational catalyst design. Point-of-Care Testing Single Nanoparticle Spectroscopy Soft Matter

Alkyne

Carbon fibers

Coordination sphere

10.1002/anie.201813083

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Nanoparticle proximity controls selectivity in benzaldehyde hydrogenation

Nature Catalysis (2024)

Kang Rui Garrick Lim Selina K. Kaiser Haichao Wu Sadhya Garg Marta Perxés Perich

Benzyl alcohol

Benzaldehyde

Hydrogenolysis

Reactivity

10.1038/s41929-023-01104-1

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Citations (21)

Sustainable Synthesis of Bimetallic Single Atom Gold‐Based Catalysts with Enhanced Durability in Acetylene Hydrochlorination

Small (2021)

Selina K. Kaiser Adam H. Clark Lucrezia Cartocci Frank Krumeich Javier Pérez‐Ramírez

Abstract Gold single‐atom catalysts (SACs) exhibit outstanding reactivity in acetylene hydrochlorination to vinyl chloride, but their practical applicability is compromised by current synthesis protocols, using aqua regia as chlorine‐based dispersing agent, and their high susceptibility to sintering on non‐functionalized carbon supports at >500 K and/or under reaction conditions. Herein, a sustainable synthesis route to carbon‐supported gold nanostructures in bimetallic catalysts is developed by employing salts as alternative chlorine source, allowing for tailored gold dispersion, ultimately reaching atomic level when using H 2 PtCl 6 . To rationalize these observations, several synthesis parameters (i.e., pH, Cl‐content) as well as the choice of metal chlorides are evaluated, hinting at the key role of platinum in promoting a chlorine‐mediated dispersion mechanism. This can be further extrapolated to redisperse large gold agglomerates (>70 nm) on carbon carriers into isolated atoms, which has important implications for catalyst regeneration. Another key role of platinum single atoms is to inhibit the sintering of their spatially isolated gold‐based analogs up to 800 K and during acetylene hydrochlorination, without compromising the intrinsic activity of Au(I)‐Cl active sites. Accordingly, exploiting cooperativity effects of a second metal is a promising strategy towards practical applicability of gold SACs, opening up exciting opportunities for multifunctional single‐atom catalysis.

Bimetallic strip

Acetylene

Aqua regia

Reactivity

Carbon fibers

10.1002/smll.202004599

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Citations (38)

Preserved in a Shell: High‐Performance Graphene‐Confined Ruthenium Nanoparticles in Acetylene Hydrochlorination

Angewandte Chemie (2019)

Selina K. Kaiser Ronghe Lin Frank Krumeich Оlga V. Safonova Javier Pérez‐Ramírez

Abstract The potential implementation of ruthenium‐based catalysts in polyvinyl chloride production via acetylene hydrochlorination is hindered by their inferior activity and stability compared to gold‐based systems, despite their 4‐fold lower price. Combining in‐depth characterization and kinetic analysis we reveal the superior activity of ruthenium nanoparticles with an optimal size of 1.5 nm hosted on nitrogen‐doped carbon (NC) and identify their deactivation modes: 1) nanoparticle redispersion into inactive single atoms and 2) coke formation at the metal sites. Tuning the density of the NC carrier enables a catalytic encapsulation of the ruthenium nanoparticles into single layer graphene shells at 1073 K that prevent the undesired metal redispersion. Finally, we show that feeding O 2 during acetylene hydrochlorination limits coke formation over the nanodesigned ruthenium catalyst, while the graphene layer is preserved, resulting in a stability increase of 20 times, thus rivalling the performance of gold‐based systems.

Acetylene

10.1002/ange.201906916

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Citations (6)

Preserved in a Shell: High‐Performance Graphene‐Confined Ruthenium Nanoparticles in Acetylene Hydrochlorination

Angewandte Chemie International Edition (2019)

Selina K. Kaiser Ronghe Lin Frank Krumeich Оlga V. Safonova Javier Pérez‐Ramírez

Acetylene

10.1002/anie.201906916

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Citations (70)

Single-Atom Catalysts across the Periodic Table

Chemical Reviews (2020)

Selina K. Kaiser Zupeng Chen Dario Faust Akl Sharon Mitchell Javier Pérez‐Ramírez

Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although the concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials have similar functions to ligands in homogeneous catalysts, determining the stability, local environment, and electronic properties of isolated atoms and thus providing a platform for tailoring heterogeneous catalysts for targeted applications. Within just a decade, we have witnessed many examples of SACs both disrupting diverse fields of heterogeneous catalysis with their distinctive reactivity and substantially enriching our understanding of molecular processes on surfaces. To date, the term SAC mostly refers to late transition metal-based systems, but numerous examples exist in which isolated atoms of other elements play key catalytic roles. This review provides a compositional encyclopedia of SACs, celebrating the 10th anniversary of the introduction of this term. By defining single-atom catalysis in the broadest sense, we explore the full elemental diversity, joining different areas across the whole periodic table, and discussing historical milestones and recent developments. In particular, we examine the coordination structures and associated properties accessed through distinct single-atom–host combinations and relate them to their main applications in thermo-, electro-, and photocatalysis, revealing trends in element-specific evolution, host design, and uses. Finally, we highlight frontiers in the field, including multimetallic SACs, atom proximity control, and possible applications for multistep and cascade reactions, identifying challenges, and propose directions for future development in this flourishing field.

Characterization

Reactivity

Flourishing

Periodic Table

10.1021/acs.chemrev.0c00576

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Citations (961)

Catalytic Synergies in Bimetallic RuPt Single–Atom Catalysts via Speciation Control (Adv. Funct. Mater. 52/2022)

Advanced Functional Materials (2022)

Vera Giulimondi Andrea Ruiz‐Ferrando Adam H. Clark Selina K. Kaiser Frank Krumeich

Bimetallic strip

10.1002/adfm.202270298

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Citations (0)

CCDC 1983602: Experimental Crystal Structure Determination

The Cambridge Structural Database (2021)

Erlin Yue Lea Dettling Julian A. W. Sklorz Selina K. Kaiser Manuela Weber

10.5517/ccdc.csd.cc24l351

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Nitrogen‐Doped Carbons with Hierarchical Porosity via Chemical Blowing Towards Long‐Lived Metal‐Free Catalysts for Acetylene Hydrochlorination

Zenodo (CERN European Organization for Nuclear Research) (2019)

Selina K. Kaiser Kyung Seob Song Sharon Mitchell Prof. Ali Coskun Prof. Javier Pérez‐Ramírez

Porous nitrogen-doped carbons (NCs) are sustainable alternatives to the toxic mercury-based acetylene hydrochlorination catalysts applied in the manufacture of polyvinyl chloride. However, the application of NCs as metal-free catalysts is hampered by their insufficient durability under industrially relevant process conditions. In particular, pore blockage leads to accelerated deactivation of NCs compared to the state-of-the-art precious metal-based systems. Herein, we develop a salt template-assisted synthesis strategy coupled with chemical blowing to tune the textural properties of NCs, while preserving the N-content and speciation. The addition of metal salts (i.e., Mg(OAc)2 or CaCO3) enhances gas evolution, leading to an increased formation of micro- and mesopores, while the in-situ generated CaO/CaCl2 and MgO/MgCl2 develop auxiliary pore networks. Micropores are easily blocked during acetylene hydrochlorination, but meso- and macropores are structurally stable, enhancing the lifetime of hierarchical NCs by ca. 50 times compared to their non-templated analogues, rivalling the stability of benchmark metal-based catalysts.

Acetylene

10.5281/zenodo.3625195

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