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Analysis of institutional authors

Ruiz-Ferrando, AAuthorLopez, NAuthor

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September 22, 2024
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Convergent Active Site Evolution in Platinum Single Atom Catalysts for Acetylene Hydrochlorination and Implications for Toxicity Minimization

Publicated to: Acs Catalysis. 14 (18): 13652-13664 - 2024-08-29 14(18), DOI: 10.1021/acscatal.4c03533

Authors: Giulimondi V; Vanni M; Damir S; Zou T; Mitchell S; Krumeich F; Ruiz-Ferrando A; López N; Gata-Cuesta JJ; Guillén-Gosálbez G; Smit JJ; Johnston P; Pérez-Ramírez J

Affiliations

Inst Chem Res Catalonia ICIQ CERCA, Tarragona 43007, Spain - Author
Johnson Matthey Catalyst Technol, Billingham TS23 1LB, England - Author
Johnson Matthey Catalyst Technol, London W2 6LG, England - Author
Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland - Author
Univ Rovira i Virgili, Tarragona 43002, Spain - Author
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Abstract

Platinum single atoms anchored onto activated carbon enable highly stable Hg-free synthesis of vinyl chloride (VCM) via acetylene hydrochlorination. Compared to gold-based alternatives, platinum catalysts are in initial phases of development. Most synthetic approaches rely on chloroplatinic acid, presenting opportunities to explore other precursors and their impact on catalyst structure, reactivity, and toxicity aspects. Here, we synthesize platinum single atom catalysts (Pt SACs, 0.2-0.8 wt % Pt) employing diverse Pt2+ and Pt4+ complexes with ammine, hydroxyl, nitrate, and chloride ligands, following a scalable impregnation protocol on activated carbon extrudates. X-ray absorption spectroscopy (XAS) reveals that Pt4+ species reduce to Pt2+ upon deposition onto the support. Despite similar oxidation states, the initial activity is precursor dependent, with tetraammine-derived Pt SACs displaying 2-fold higher VCM yield than chlorinated counterparts, linked to superior hydrogen chloride binding abilities by density functional theory (DFT) simulations. Their activity gradually converges due to dynamic active site restructuring, delivering remarkable precursor-independent stability over 150 h. Operando XAS and DFT studies uncover reaction-induced ligand exchange, generating common active and stable Pt-Cl-x (x = 2-3) species. Convergent active site evolution enables flexibility in metal precursor selection and thus toxicity minimization through multiparameter assessment. This study advances safe-by-design catalysts for VCM synthesis, highlighting the importance of toxicity analyses in early-stage catalyst development programs.

Keywords

Acetylene hydrochlorinationActive site dynamicsDesigKinetic modelinKinetic modelingPlatinumSingle atom catalysisTotal-energy calculationsToxicity

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal Acs Catalysis due to its progression and the good impact it has achieved in recent years, according to the agency WoS (JCR), it has become a reference in its field. In the year of publication of the work, 2024 there are still no calculated indicators, but in 2023, it was in position 21/185, thus managing to position itself as a Q1 (Primer Cuartil), in the category Chemistry, Physical.

Independientemente del impacto esperado determinado por el canal de difusión, es importante destacar el impacto real observado de la propia aportación.

Según las diferentes agencias de indexación, el número de citas acumuladas por esta publicación hasta la fecha 2025-12-06:

  • Scopus: 10

Impact and social visibility

From the perspective of influence or social adoption, and based on metrics associated with mentions and interactions provided by agencies specializing in calculating the so-called "Alternative or Social Metrics," we can highlight as of 2025-12-06:

  • The use, from an academic perspective evidenced by the Altmetric agency indicator referring to aggregations made by the personal bibliographic manager Mendeley, gives us a total of: 12.
  • The use of this contribution in bookmarks, code forks, additions to favorite lists for recurrent reading, as well as general views, indicates that someone is using the publication as a basis for their current work. This may be a notable indicator of future more formal and academic citations. This claim is supported by the result of the "Capture" indicator, which yields a total of: 11 (PlumX).

With a more dissemination-oriented intent and targeting more general audiences, we can observe other more global scores such as:

  • The Total Score from Altmetric: 5.
  • The number of mentions on the social network X (formerly Twitter): 8 (Altmetric).

It is essential to present evidence supporting full alignment with institutional principles and guidelines on Open Science and the Conservation and Dissemination of Intellectual Heritage. A clear example of this is:

  • The work has been submitted to a journal whose editorial policy allows open Open Access publication.

Leadership analysis of institutional authors

This work has been carried out with international collaboration, specifically with researchers from: Switzerland; United Kingdom.

Awards linked to the item

This publication was supported by NCCR Catalysis (grant number 180544), a National Centre of Competence in Research funded by the Swiss National Science Foundation. The Spanish Ministry of Science and Innovation is acknowledged for financial support (PID2021-122516OB-I00 and Severo Ochoa Grant MCIN/AEI/10.13039/501100011033CEX2019-000925-S) and the Barcelona Supercomputing Center-MareNostrum (BSC-RES) for providing generous computer resources. A.R.-F. acknowledges funding from the Generalitat de Catalunya and the European Union under Grant 2023 FI-3 00027. The Swiss-Norwegian beamlines (SNBL, ESRF) are acknowledged for provision of beamtime and its staff for invaluable support. The Scientific Center for Optical and Electron Microscopy (ScopeM) at the ETH Zurich and Swiss Federal Laboratories for Materials Science and Technology (EMPA) are thanked for access to their facilities. We thank Constance Ko for contributions to some of the illustrations.