Nanoalloys: recent developments and future perspectives

7 September 2022, London Sir Geoffrey Wilkinson Dalton Poster Symposium

21-23 September 2022, London, UK and Online Nanoalloys: recent developments and future perspectives Faraday Discussion #FDNanoalloys

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Introduction

Nanoalloys: recent developments and future perspectives Faraday Discussion is organised by the Faraday Division of the Royal Society of Chemistry This book contains abstracts of the 37 posters presented at Nanoalloys: recent developments and future perspectives Faraday Discussion . All abstracts are produced directly from typescripts supplied by authors. Copyright reserved. Oral presentations and discussions All delegates at the meeting, not just speakers, have the opportunity to make comments, ask questions, or present complementary or contradictory measurements and calculations during the discussion. If it is relevant to the topic, you may give a 5 minute presentation of your own work during the discussion. These remarks are published alongside the papers in the final volume and are fully citable. If you would like to present slides during the discussion please let the session chair know and load them onto the computer in the break before the start of the session. Faraday Discussion Volume Copies of the Discussion Volume will be distributed approximately 6 months after the meeting. To expedite this, it is essential that summaries of contributions to the discussion are received no later than Friday 30th September 2022 for questions and comments and Friday 14th September 2022 for responses. Posters Posters have been numbered consecutively: P01 – P37. The poster sessions will take place on Wednesday 21 September at 17.30. All posters being presented in-person or virtually will be available to view throughout the discussion.

If you are presenting your poster in-person, please ensure you are at your poster during the dedicated poster session.

Posters being presented virtually can be viewed by clicking on the link in the virtual lobby. During the dedicated poster sessions, the authors will be available to use the networking functions in the virtual lobby. Use the inbox in the top light blue bar of the virtual lobby screen to send the poster presenter a message or request a video call with them by clicking on their name in the networking section at the bottom of the screen. If you are a poster presenter, please ensure that you are logged the virtual platform.

Poster Prize The Faraday Discussions poster prize will be awarded to the best student poster as judged by the committee.

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Existing networking rooms will be visible from the virtual lobby. To create a one-to-one chat, simply click on the name of the person you would like to speak to and select if you would like to have a private or public conversation. For a public conversation, other delegates can join your chat room.

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Scientific Committee

Invited Speakers

Pascal Andreazza CNRS, ICMN, Unversité d’Orléans, France Francesca Baletto Università degli Studi di Milano, Italy and Kings College London, United Kingdom Fuyi Chen Northwestern Polytechnical University, China

Miguel Jose Yacaman (Introductory Lecturer) Northern Arizona University, United States Richard Palmer (Closing Remarks Lecturer) University of Swansea, United Kingdom

Christine Aikens Kansas State University, United States

Vincenzo Amendola University of Padova, Italy

Riccardo Ferrando Università degli Studi di Genova, Italy

Beatriz Roldán Cuenya FHI Berlin, Germany

Ewald Janssens, Chair KU Leuven, Belgium

Graham J. Hutchings Cardiff University, United Kingdom Marcelo M. Mariscal University of Cordoba, Argentina

Christine Mottet Université Aix-Marseille, France

Rolf Schäfer TU Darmstadt, Germany

Poster presentations

P01

Oxidation of propane over various supported platinum catalysts Ahlam Almoteiry Cardiff University, UK and Almajaah University, Saudi Arabia Time-resolved investigation of Co-Ag and Ni-Ag nanoalloy formation: effect of the metal deposition sequence Pascal Andreazza ICMN, Université d’Orléans, France Composition-tuned Au-Ag bimetallic cluster-modified TiO 2 films as efficient self-cleaning surfaces under visible light Vana Chinnabathini Chinnabathini KU Leuven, Belgium Au–Pd separation enhances bimetallic catalysis of alcohol oxidation Isaac Daniel Cardiff University, UK Coalescence of pure Pd and AuPd nanoparticles studied by molecular dynamics simulations Edoardo Dighero University of Genoa, Italy Growth pathways of Au, AgAu and PtPd nanoparticles starting from fcc seeds El yakout El koraychy University of Genoa, Italy The NanoParticleLibrary: a python package from the computational studies of Nanoalloys Riccardo Farris Universitat de Barcelona, Spain Anisotropic stress release leads to structural transitions in AuPd nanoalloys Riccardo Ferrando Università degli Studi di Genova, Italy

P02

P03

P04

P05

P06

P07

P08

P09

Size-tunable Ni-Cu Core-Shell nanoparticles: structure, composition, and catalytic activity for the RWGS reaction Maria Heilmann Bundesanstalt für Materialforschung und -prüfung (BAM), Germany

P10

CO 2 activation by Cu-based bimetallic clusters Olga Lushchikova Innsbruck University, Austria

P11

Hydrogenation in water of mono-and disaccharides to polyols using Ni- Fe/SiO 2 catalysts Eric Marceau Unité de Catalyse et Chimie du Solide - CNRS - Université de Lille, France Breaking with the principles of coreduction to form stoichiometric intermetallic PdCu nanoparticles Jette Katja Mathiesen Technical University of Denmark, Denmark Gold nanoparticles modified cobalt iron oxide inverse opals as high- performance oxygen reduction electrocatalyst Trang Nguyen KU Leuven, Belgium Electrocatalytic performance of PtxNi1-x bimetallic clusters prepared by laser ablation cluster beam deposition Yubiao Niu Swansea University, UK Unsupervised learning methods for the identification of nanoparticles structures based on local atomic environments Cesare Roncaglia University of Genoa, Italy

P12

P13

P14

P15

P16

Hydrogen peroxide formation on AuPd nanoparticles Rasmus Svensson Chalmers University of Technology, Sweden

P17

Hot hole mediated catalytic oxidative scission of alkenes using hybrid plasmonic nanoparticles Swathi Swaminathan Indian Institute of Technology Kanpur, India

P18

CO oxidation as a test reaction for PtGe bimetallic nanoalloys Andoni Ugartemendia University of the Basque Country, Spain Selective intercalation – A HR-XPS study of graphene-supported FePt clusters on Rh(111) Natalie Waleska Friedrich-Alexander-Universität Erlangen-Nürnberg, Germany Optical properties of AgAu clusters: effects of mixing, configuration, and size Hans-Christian Weissker CINaM-CNRS & AMU, France

P19

P20

P21

Making fullerene cages breathe Wei Zhao King’s College London, UK

P22

Intraocular application of gold nanodisks optically tuned for optical coherence tomography Jeong Hun Kim Seoul National University Hospital, South Korea Size- and composition selected supported subnanometer Cu, Pd and CuPd clusters in the oxidative dehydrogenation of cyclohexene Stanislav Valtera J. Heyrovský Institute of Physical Chemistry, Czech Republic Hydrogen storage and release of single-Nb-atom doped Al clusters in the gas phase investigated by thermal desorption spectrometry Yufei Zhang The University of Tokyo, Japan Finite-temperature structures of Cu, Ag, and Au nanoclusters Manoj Settem Sapienza University of Rome, Italy Core-Shell nanoparticle formation in FeAu and CoAu during laser ablation in liquid synthesis is driven by particle size, melting temperature and surface energy Christoph Rehbock University of Duisburg-Essen, Germany

P23

P24

P25

P26

P27

Optimizing multimetallic nanoparticle compositions with machine learning towards high entropy alloys: case study of PtRuPdRhAu for the CO oxidation reaction Jonathan Quinson Aarhus University, Denmark Phase separation transitions inside Pd-Ir nanoparticles: modeling size- dependent phase diagrams & finite-size scaling Micha Polak Ben-Gurion University of the Negev, Israel Symmetrizing structure and enhancing IR spectra of aluminum clusters by carbon-core doping Fedor Naumkin Ontario Tech University / UOIT, Canada Developing the vapour-solid synthesis of supported, intermetallic nanoparticles for heterogeneous catalysis Daniel Garstenauer University of Vienna, Austria Effect of oxidation on the magnetism of Co and Cr clusters probed by Stern-Gerlach deflection Kobe De Knijf KU Leuven, Belgium

P28

P29

P30

P31

P32

A density functional theory investigation on Au 9 M 2+ (M = Sc - Ni) clusters: structure, stability, electronic properties, and hydrogen

adsorption Ngo Thi Lan Institute of Science and Technology, Vietnam

P33

Solid solution nanoparticles obtained by co-sputter deposition onto liquid polyethylene glycol Mai Thanh Nguyen Hokkaido University, Japan High-index core–shell Ni–Pt nanoparticles as oxygen reduction electrocatalysts Lebohang Macheli University of South Africa, South Africa

P34

P35

Bayesian force fields from first principles for nanoparticle heterogeneous catalysis Cameron Owen Harvard University, USA

P36

Preparing bimetallic nanoparticles supported on activated carbon by sol immobilization: influence of the acid addition Charlie Paris Cardiff University, UK Metal welding at room conditions of CuNi bimetallic nanowire networks Mona Treguer-Delapierre ICMCB-CNRS, U.Bordeaux, France

P37

Oxidation of propane over various supported platinum catalysts Ahlam Almoteiry, James Carter, Stuart Taylor, Graham Hutchings

Cardiff Catalysis Institute, Cardiff University, UK Corresponding author: AlmoteiryAM@cardiff.ac.uk

Pt/CeO2, Pt/ZrO2, Pt/SiO2 and Pt/TiO2 catalysts were employed to catalyse propane oxidation using two preparation methods strong electrostatic adsorption (SEA) and co-precipitation method (CO-P). The catalysts were tested under the same conditions at 450 °C with a molar ratio of 2:1 Propane: oxygen and a total flow rate of 20ml/min. The presence of Pt on the surface of catalysts (SEA) led to an increase in the activity and selectivity for ODH-O2 reaction rather than the bulk method (CO-P) . It was found that the Pt/CeO2 (SEA) catalyst was more active than the Pt/ZrO2 ,Pt/SiO2 and Pt/TiO2 (SEA) catalysts, while it was less selective in propane oxidation towards propene. The different behaviours of these catalysts may relate to the nature of the support, which affected the properties of the active Pt species at the surface of catalysts as well as the reaction mechanisms. Also, we found the reaction of ODH-O2 using Pt catalysts can lead to a combustion reaction (COX product +water) with dehydrogenation reaction (Propene)may be due to availability supply of oxygen which led to direct combustion of propane or propene and react with additional lattice oxygen or surface to produce COX product. References 1. Avila, M., Vignatti, C., Apesteguía, C., & Garetto, T., 2014. Effect of support on the deep oxidation of propane and propylene on Pt-based catalysts. Chemical Engineering Journal, 241, 52–59.

P01

Time-resolved investigation of Co-Ag and Ni-Ag nanoalloy formation: effect of the metal deposition sequence P. Andreazza 1* , A. Coati 2 , Y. Garreau 2 , R. Ferrando 3 , D. Forster 1 , A. Hizi 1 , J. Creuze 4 , C. Andreazza-Vignolle 1 1 Interfaces, Confinement, Matériaux et Nanostructures, ICMN, Université d’Orléans, France, 2 Synchrotron Soleil, L’Orme de Merisiers, France, 3 Università di Genova, Physics Department, Italy, 4 ICMMO, Univ. Paris-Saclay, France As lot of Ag-based binary metallic alloys, Ag-Co and Ni-Ag systems are a very weakly miscible system in wide ranges of temperature and composition. We can distinguish three main driving forces in order to predict the nature and the quantity of the segregating species in a binary alloy: the differences in surface energies and radii of the two elements (mismatch-effect), and their ability to mix in the bulk. In Co-Ag and Ni-Ag systems, we can predict a surface segregation of silver since Ag presents lower surface energy and larger size (to minimize elastic-energy), in addition to the immiscibility behavior [1,2]. At nanoscale, the size reduction favors a segregation behavior by surface and core contraction effects that can be opposed to kinetic trapping effects induced by the growth mode [1]. In this case of UHV atomic deposition and condensation on the surface substrate, the mobility of Ag and Co (or Ni) atoms on the substrate and on the particles must be considered. Consequently, the effect of substrate, growth kinetics and annealing was followed in several configurations of deposition (simultaneous and sequential deposition of metals). Experimentally, morphological and structural evolutions of clusters are studied by HRTEM/EFTEM/HAADF techniques combined with in situ and real time wide- and small-angle X-ray scattering in grazing incidence simultaneously (GIWAXS and GISAXS): the metastable deposition mode at room temperature, i.e. by depositing Co or Ni above an Ag core, and the more stable reverse deposition mode until their equilibrium state obtained by thermal activation. In addition, the quantitative structural analysis of experimental data was facilitated and consolidated using atomistic simulations of the cluster growth by molecular dynamics (MD) to reveal the atom migration leading to phase separation or core-shell formation. In a metastable deposition mode, i.e. by depositing Co above an Ag core, the configuration is complex: Co atoms incorporate the initial Ag core in sub-layer position leading to Janus then core-shell configuration with the Co content [5]. In the more stable reverse deposition mode, unexpected, Ag nucleate in domains on Co core, rather than in shell configuration, due to a combined substrate and kinetic effect. In addition, the Ni-Ag case reveals that Janus configuration is favored rather than core-shell with respect to the same experiment in the Co-Ag case due to several mechanisms. References

1. I. Parsina, F. Baletto, J. Phys. Chem. C (2010) 114, 1504 2. D. Bochicchio, R. Ferrando, Phys. Rev. B (2013) 87, 165435 3. P. Andreazza, in Nanoalloys , Éd. Springer London, (2012) , p69-112

4. P. Andreazza, V. Pierron-Bohnes, F. Tournus, C. Andreazza-Vignolle, V. Dupuis, Surf. Sci. Rep., (2015) 70, 2, 188 5. P. Andreazza, A. Lemoine, A. Coati, D. Nelli, R. Ferrando, Y. Garreau, J. Creuze, C. Andreazza-Vignolle, Nanoscale (2021) 13, 6096

P02

Composition-tuned Au-Ag bimetallic cluster-modified TiO 2 films as efficient self-cleaning surfaces under visible light Vana Chinnappa Chinnabathini 1,2 , Fons Dingenen 2 , Rituraj Bora 2 , Zviadi Zarkua 1 , Peter Lievens 1 , Didier Grandjean 1 , Sammy W. Verbruggen 2 , and Ewald Janssens 1 1 Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Belgium, 2 Sustainable Energy, Air & Water Technology (DuEL), University of Antwerp, Belgium Surface modification of titanium dioxide photocatalysts with plasmonic metal nanoalloys is a promising way to extend the operation window to the visible light region, corresponding to the maximum output range of the sun’s total irradiance spectrum. 1 These photocatalysts are tested for the degradation of stearic acid (SA) since it is a widely applied method for assessing the photocatalytic activity of self-cleaning materials. SA is a good model compound for organic fouling on glass windows. 2 We studied the stearic acid degradation on TiO 2 decorated with 1.5-2.5 nm AuAg nanoalloy particles of different compositions both under UV and simulated solar light. Mono- and bimetallic Au x Ag 1-x (x=0, 0.1, 0.3, 0.5, 0.7, 0.9 and 1) clusters produced in a noble gas environment were soft-landed using cluster beam deposition (CBD) on TiO 2 P25-coated silicon wafers with a coverage of 4 atomic monolayer equivalents. While the photoactivity of the obtained films towards stearic acid degradation compared to pristine TiO 2 is basically unchanged under UV, a significant enhancement is observed under solar simulator with a very clear composition-dependent volcano-type trend peaking at the Au 0.3 Ag 0.7 composition.This behaviour may originate from their composition-dependent atomic arrangements and electronic structures stemming from their nucleation mechanism. 3,4 These results demonstrate the excellent potential of the CBD technology to fabricate novel and efficient noble metal modified photocatalytic surfaces with a high control over cluster coverage, and composition, without involving potentially hazardous chemical agents. References 1. W. Liao, S.W. Verbruggen, N. Claes, A. Yadav, D. Grandjean, S. Bals, P. Lievens, Nanomaterials 8 (2018) 30 2. W. Verbruggen, M. Keulemans, B. Goris, N. Blommaerts, S. Bals, J.A. Martens, S. Lenaerts, Applied Catalysis B: Environmental 188 (2016) 147-153 3. W. Liao, A. Yadav, K. Hu, J. van der Tol, S. Cosentino, F. D'Acapito, R.E. Palmer, C. Lenardi, R. Ferrando, D. Grandjean, P. Lievens, Nanoscale 10 (2018) 6684-6694 4. Mills, J.S.Wang, J . Photochem. Photobiol. A 182 (2006) 181-186.

P03

Au–Pd separation enhances bimetallic catalysis of alcohol oxidation Xiaoyang Huang 1,7 , Ouardia Akdim 1,7 , Mark Douthwaite 1 , Kai Wang 1 , Liang Zhao 1 , Richard J. Lewis 1 , Samuel Pattisson 1 , Isaac T. Daniel 1 , Peter J. Miedziak 1,2 , Greg Shaw 1 , David J. Morgan 1 , Sultan M. Althahban 3,4 , Thomas E. Davies 1 , Qian He 1,5 , Fei Wang 1 , Jile Fu 1 , Donald Bethell 1 , Steven McIntosh 6 , Christopher J. Kiely 3,6 and Graham J. Hutchings 1 1 Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, UK. 2 School of Applied Sciences, University of South Wales, UK. 3 Department of Materials Science and Engineering, Lehigh University, USA. 4 Department of Mechanical Engineering, Jazan University, Saudi Arabia. 5 Department of Materials Science and Engineering, Faculty of Engineering, National University of Singapore, Singapore. 6 Department of Chemical and Biomolecular Engineering, Lehigh University, USA. 7 These authors contributed equally. Bimetallic Au-Pd catalysts are well known to give significant rate enhancements over their monometallic analogues. This has been demonstrated for a range of reactions including the oxidative dehydrogenation (ODH) of alcohols. 1 The rate of oxygen reduction (ORR) occurring within these systems is crucial, 2 and the opposing activity of supported Au and Pd nanoparticles for ORR is well documented, with Pd known to be very effective. 3 Here, we show that by separating the Au and Pd catalytic sites during the ODH of 5-hydroxymethylfurfural (amongst other alcohols), the activity is almost doubled compared to that of a typical alloy. It is proposed that the bimetallic rate enhancement is due to the coupling of two redox processes occurring over isolated Au and Pd sites. The heightened enhancement when using a physical mixture of monometallic catalysts over that of an alloy is attributed to the ability of the individual metal sites to maintain their full redox capabilities. Using both thermo- and electrocatalytic analysis, ODH is demonstrated to occur over Au sites with ORR catalysed by Pd sites. The conductivity of the support used is proven to be vital, indicating the importance of electron transfer between the two metals. The coupling is further demonstrated by the fact that when the mass of Pd catalyst is increased in a physical mixture system containing a constant amount of Au, the rate of ODH is indirectly increased through an increase in the rate of ORR. This cooperative redox enhancement (CORE) is a novel observation that offers new avenues when considering the design of bimetallic catalytic systems. References 1. Wang, D., Villa, A., Porta, F., Prati, L. & Su, D. Bimetallic gold/palladium catalysts: Correlation between nanostructure and synergistic effects. J. Phys. Chem. C 112 , 8617–8622 (2008). 2. B. N. Zope, D. D. Hibbitts, M. Neurock and R. J. Davis, Science , 2010, 330 , 74–78. 3. A. Kulkarni, S. Siahrostami, A. Patel and J. K. Nørskov, Chemical Reviews , 2018, 118 , 2302–2312.

P04

Coalescence of pure Pd and AuPd nanoparticles studied by molecular dynamics simulations Edoardo Dighero, Diana Nelli, Cesare Roncaglia and Riccardo Ferrando Physics Department, University of Genoa, Italy The coalescence of pure Pd nanoparticles and AuPd nanoalloys is studied by molecular dynamics simulations. Different initial geometric structures are considered, namely the fcc truncated octahedron and the icosahedron. In our simulations, an octahedral and an icosahedral nanoparticle collide and merge to form a single large aggregate. The dependence of the final shape of this aggregate on the composition of the initial clusters (pure Pd or alloyed AuPd) is studied. Specifically, for pure Pd nanoparticles the coalescence leads to the formation of fcc final structures, whereas in the case of AuPd the icosahedral geometry is dominant. This is due to the reversal of fcc/icosahedron energetic stability depending on the Au content in AuPd nanoparticles, as found in the experiments and calculations of Ref. [1]. The coalescence process is studied at different temperatures characterising the interdiffusionof atoms belonging to the two initial units. References 1. D. Nelli, C. Roncaglia, R. Ferrando, C. Minnai, J. Phys. Chem. Lett., 2021, 12 , 4609-4615.

P05

Growth pathways of Au, AgAu and PtPd nanoparticles starting from fcc seeds El yakout El koraychy 1 , Cesare Roncaglia 1 , Diana Nelli 1 , Manuella Cerbelaud 2 , Chloé Minnai 3 and Riccardo Ferrando 4 1 Dipartimento di Fisica dell’Università di Genova, Italy, 2 Université de Limoges, France, 3 Molecular Cryo-Electron Microscopy Unit, Okinawa Institute of Science and Technology Graduate University, Japan, 4 Dipartimento di Fisica dell’Università di Genova and CNR-IMEM, Italy The growth of pure Au nanoparticles and of AgAu and PtPd nanoalloys is studied by Molecular Dynamics (MD) simulations.For pure Au,weanalyzethe growth of multiply twinned Au nanoparticles (MTPs), decahedra and icosahedra, from a tetrahedral (Th) initial seed in the gas phase [1]. The existing experimental observations show that MTPs can form from Thviadifferent pathways,butwithoutidentifyingthekeyatomistic mechanisms responsible for these growth pathways. OurMDresults reveal thesemechanisms and give a clear explanation ofthe origin of thetwinning process.In the case of nanoalloys,it is shown thatthe out-of-equilibrium core@shell chemical ordering of AuAg and PtPd can be obtaineddepositing a pure metal on an initial intermixed seed[2].Since in these systems there is no lattice mismatch between the species, the growth leads to quite regular fcc structures resembling those obtained for the pure metals. As for chemical ordering, the purity of the outer shell depends on the mobility of the minority atoms. References 1. El Koraychy, E. Y., Roncaglia, C., Nelli, D., Cerbelaud, M., & Ferrando, R. (2022)Nanoscale horizons 2. El Koraychy, E. Y., Nelli, D., Roncaglia, C., Minnai, C., & Ferrando, R. Eur. Phys. J. Appl. Phys., 97 (2022) 28

P06

The NanoParticleLibrary: a python package from the computational studies of Nanoalloys Riccardo Farris 1 , Konstantin M. Neyman 1,2 and Albert Bruix 1 1 Departament de Ciència de Materials i Química Física and Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, Spain, 2 ICREA (Institució Catalana de Recerca i Estudis Avançats), Spain The understanding of the chemical and physical properties of nanostructured materials is often precluded by the complexity of their structure, which also poses a challenge for constructing representative structural models in computational studies. For nanoalloys, this challenge also involves predicting the most stable arrangement of the two elements, as well as the chemical properties of the resulting surface sites. Stable chemical orderings of bimetallic nanoparticles can be determined with global optimization approaches, which typically evaluate hundreds or thousands of candidate structures algorithmically. Given the unaffordable computational cost of evaluating the stability of such a large number of structures with approximations based on the predominant density functional theory, global optimization algorithms often rely on surrogate energy models that are fit to reproduce energies of bimetallic particles calculated at this accurate level of theory [1, 2]. Similarly, surrogate energy models can be used to approximate the binding energies on a large number of inequivalent sites and thus explore the behavior of nanoalloys under reaction conditions. Here we present an Open Source-Python Package, the NanoParticleLibrary (NPL, https://github.com/reac- nps/NanoParticleLibrary), which has been developed for computational studies of nanoalloys. The library is a wrapper around the popular Atomistic Simulation Environment and includes a flexible energy pipeline for different surrogate energy models of nanoparticles, site recognition algorithms, and various global optimization algorithms. The surrogate energy models can be imported or trained within the library, and used with a Genetic Algorithm, Markov Chain Monte Carlo, and a recently developed Optimal-Exchange algorithm [3]. We showcase the capacity of this library by presenting different case studies involving the optimization of the shape, element ordering, and response to reaction conditions of different technologically relevant bimetallic nanoparticles. References 1. S. M. Kozlov, G. Kovács, R. Ferrando, and K. M. Neyman, “How to determine accurate chemical ordering in several nanometer large bimetallic crystallites from electronic structure calculations,” Chemical Science , vol. 6, no. 7, pp. 3868– 3880, 2015, doi: 10.1039/c4sc03321c. 2. Z. Yan, M. G. Taylor, A. Mascareno, and G. Mpourmpakis, “Size-, Shape-, and Composition-Dependent Model for Metal Nanoparticle Stability Prediction,” Nano Letters , vol. 18, no. 4, pp. 2696–2704, 2018, doi: 10.1021/acs.nanolett.8b00670. 3. Neumann F, Margraf JT, Reuter K, Bruix A. Interplay between shape and composition in bimetallic nanoparticles revealed by an efficient optimal-exchange optimization algorithm. ChemRxiv, doi: 10.26434/chemrxiv-2021-26ztp.

P07

Anisotropic stress release leads to structural transitions in AuPd nanoalloys D. Nelli 1 , C. Roncaglia 1 , C. Minnai 2 and R. Ferrando 1 1 Physics Department, University of Genoa, Italy, 2 OIST, Onna-son, Kunigami-gun, Japan Shape transformations in Pd-rich AuPd nanoalloys are studied by growth experiments and computer simulations. It is shown that increasing the Au content, a structural transformation from fcc truncated octahedra to icosahedra takes place [1]. The transition is sharper for growth conditions closer to equilibrium. The driving forces of the transition are singled out with the aid of computer simulations, specifically global optimization searches and free energy calculations within the harmonic superposition approximation. These calculations show that there is a reversal of the energetic stability between fcc and icosahedral structures when increasing the Au content. In addition, atomic stress calculations demonstrate that the introduction of Au impurities in the surface causes a better relaxation of the anisotropic surface stress in icosahedra than in fcc nanoparticles, which is at the origin of the observed shape transformation. References 1. D. Nelli, C. Roncaglia, R. Ferrando and C. Minnai, J. Phys. Chem. Lett., 2021, 12 , 4609-4615.

P08

Size-tunable Ni-Cu core-shell nanoparticles: structure, composition, and catalytic activity for the RWGS reaction Maria Heilmann 1,4 , Carsten Prinz 1 , Ralf Bienert 1 , Robert Wendt 2 , Benny Kunkel 3 , Jörg Radnik 1 , Armin Hoell 2 , Sebastian Wohlrab 3 , Ana Guilherme Buzanich 1 and Franziska Emmerling 1,4 1 Bundesanstalt für Materialforschung und -prüfung, Germany, 2 Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Germany, 3 Leibniz-Institut für Katalyse e.V., Germany, 4 Humboldt-Universität zu Berlin, Germany Nanoparticles (NPs) have become important materials for a variety of chemical technologies, including catalysis. One of the main challenges is the reduction of green house gases, such as CO 2 . One opportunity besides the capturing is the conversion to synthesis gas via the reverse water-gas shift reaction.[1,2] A facile and efficient method is described for the solvothermal synthesis of size-tunable, stable, and uniform NiCu core-shell NPs.[3] The diameter of the NPs can be tuned in a range from 6 nm to 30 nm and the Ni:Cu ratio from 30:1 to 1:1. The NPs are structurally characterized with combination of transmission electron microscopy, anomalous small-angle X-ray scattering, X-ray photoelectron spectroscopy, and X-ray absorption fine structure. Using these analytical methods, a core-shell-shell structure their chemical composition is elucidated. A depletion from the core to the shell is observed, with the core consisting of NiCu alloy, surrounded by an inner Ni-rich shell and an outer NiO shell. The SiO 2 -supported NiCu core-shell NPs show pronounced selectivity of >99% for CO in the catalytic reduction of CO 2 to CO using hydrogen as reactant (reverse water–gas shift reaction). References 1. A. Ranjbar, A. Irankhah, S. F. Aghamiri, J. Environ. Chem. Eng . 2018 ,6, 4945. 2. B. Lu, Z. Zhang, X. Li, C. Luo, Y. Xu, L. Zhang, Fuel 2020 ,276. 3. M.Heilmann, C. Prinz, R. Bienert, R. Wendt, B. Kunkel, J. Radnik, A. Hoell, S. Wohlrab, A. Guilherme Buzanich, F. Emmerling, Adv. Eng. Mater. 2022 , 24 (6), 2101308.

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CO 2 activation by Cu-based bimetallic clusters Olga V. Lushchikova and Paul Scheier Institut für Ionenphysik und Angewandte Physik, Universität Innsbruck, Austria Among the greenhouse gases responsible for climate change, carbon dioxide (CO 2 ) is the most abundant, accounting for more than 80% of their total amount. Since the industrial revolution, the atmospheric CO 2 concentration has grown rapidly by more than 40% and reached 415 ppm in 2021.[1] Therefore, methods to reduce it are urgently needed. The main challenge of CO 2 utilization is its high thermodynamic stability and kinetic inertness with high dissociation energy exceeding 11 eV. Current industrial conversion of CO 2 to methanol proceeds with the use of a Cu/ZnO/Al 2 O 3 catalyst at elevated temperature and pressure, suggesting high activation barriers of elementary steps in the reaction mechanism.[2] Although an industrial copper-based catalyst thus exists, it has been suggested that the addition of other metals to the copper can modify its catalytic properties, potentially increasing the efficiency of methanol production.[3] This hypothesis is supported by experimental studies that have shown that bimetallic catalysts can outperform conventional industrial catalysts.[4] Despite these promising developments, the exact mechanism of methanol formation remains elusive. Knowledge of the elementary reaction steps at the molecular level is required for a rational design of better catalyst material. Since CO 2 is the prime reactant, its interaction with the active sites of the catalyst needs to be understood. Well- defined metal clusters in the gas phase offer the possibility to model the active sites and explore their interaction with CO 2 in detail. The reaction of CO 2 with metal ions is well studied, but much less information is available about the reaction with larger metal clusters and almost nothing about its reaction with bimetallic clusters, even though they appear to be very promising candidates for methanol synthesis. We are trying to fill this gap by conducting experiments to elucidate structural information of the reaction products formed upon reacting CO 2 with Cu-based bimetallic clusters. Bimetallic clusters are formed and reacted with CO 2 in superfluid helium nanodroplets (HNDs), which act as a nanoreactor. The application of HNDs allows for the highest level of control over cluster charge, size, and copper- to-dopant metal ratio, which will simulate the active sites of the catalyst. Formed complexes can be studied by means of collision-induced dissociation and He-tagging photo fragmentation spectroscopy. In this way, we will obtain detailed information on the binding nature of CO 2 to the cluster and could deduce how it depends on the cluster composition. References 1. NOAA Research. Trends in Atmospheric Carbon Dioxide https://www.esrl.noaa.gov/gmd/ccgg/trends/ (accessed Feb 22, 2021). 2. Artz, J. et al ; Sustainable Conversion of Carbon Dioxide: An Integrated Review of Catalysis and Life Cycle Assessment. Chem. Rev. 2018, 118 (2), 434–504. 3. Yang, Y.; White, M. G.; Liu, P. Theoretical Study of Methanol Synthesis from CO 2 Hydrogenation on Metal-Doped Cu(111) Surfaces. J. Phys. Chem. C 2012, 116 (1), 248–256. 4. Jiang, X. et al; CO 2 Hydrogenation to Methanol on Pd–Cu Bimetallic Catalysts with Lower Metal Loadings. Catal. Commun. 2019, 118, 10–14.

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Hydrogenation in water of mono- and disaccharides to polyols using Ni-Fe/SiO 2 catalysts Achraf Sadier 1 , François Robert 2,3 , Catherine Amiens 2,3 , Karine Philippot 2,3 , Robert Wojcieszak 1 and Eric Marceau 1 1 Univ. Lille, CNRS, Centrale Lille, Univ. Artois, France, 2 CNRS, LCC (Laboratoire de Chimie de Coordination), France, 3 Université de Toulouse, France Besides costly noble metals, Ni is used to catalyze the hydrogenation of sugars to polyols, but is poorly stable. Compared with Ni, supported Ni-Fe alloyed nanoparticles were recently reported to present high conversion and selectivity in the hydrogenation of glucose to sorbitol. [1] Investigating if benefits also exist for the hydrogenation of xylose and maltose to, respectively, xylitol and maltitol, two molecules of interest for the food and pharmaceutical industries, is the purpose of the present work. The activity, selectivity and stability in water of a Ni/SiO 2 catalyst and a bimetallic Ni 62 Fe 38 /SiO 2 catalyst prepared by deposition-precipitation (Ø particles =5-7 nm) were compared as a function of experimental parameters (T=50- 150 °C, P H2 =10-30 bar). For xylose hydrogenation, [2] the only product detected was xylitol, while for maltose, [3] maltitol was the major product, but maltose hydrolysis to glucose occurred in the upper range of temperature. A reaction temperature of 80 °C allowed minimizing nickel leaching at full conversion and unwanted side-reactions. The presence of reduced Fe at the surface of the bimetallic nanoparticles increased the first-order apparent rate constant k and the adsorption constant of the sugar compared with the Ni catalyst, by a factor 2 to 3, indicating a stronger interaction with the oxophilic Ni-Fe surface. However, the rate constant for maltose hydrogenation was lower by a factor 5 to 6 compared with xylose. Another major difference in the case of maltose was a reaction order of 0.5 with respect to P H2 on Ni-Fe/SiO 2 compared with a zero-order on Ni/SiO 2 , stressing significant differences in H 2 coverage of the bimetallic surface. A dilution of Ni domains among Fe atoms can explain the difficulty to find adsorption sites for maltose, a bulky disaccharide, hence the low value of k despite maltose strong adsorption, and the limited coverage in hydrogen atoms apt to ensure the hydrogenation. The presence of Fe also promoted the catalyst stability. The activity of Ni/SiO 2 strongly declined upon formation of a Ni(II) phyllosilicate. No deactivation was found for the Ni-Fe catalyst. Nevertheless, the size of the metal particles and the Fe proportion in the surface layers increased, suggesting a flattening and coalescing of the particles over the silica surface. A comparison with SiO 2 -supported Ni-Fe nanoparticles tailored via an organometallic route (hydrogenation of [Ni(COD) 2 ] and {Fe[N(SiMe 3 ) 2 ] 2 } 2 ; Ø particles =3-4 nm) led to similar results and emphasized the importance of keeping the two metals in their reduced form for an optimum activity, the beneficial role of Fe-enriched surfaces; and the higher performance of a Ni 70 Fe 30 formulation. References

1. Y. Fu et al., Appl. Catal. B 2021 , 288 , 119997. 2. A. Sadier et al., Appl. Catal. B 2021 , 298 , 120564. 3. A. Sadier et al., Appl. Catal. B 2022 , 313 , 121446.

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Breaking with the principles of coreduction to form stoichiometric intermetallic PdCu nanoparticles Jette K. Mathiesen 1 , Espen D. Bøjesen 2 , Jack K. Pedersen 3 , Emil T. S. Kjær 3 , Mikkel Juelsholt 4 , Susan Cooper 3 , Jonathan Quinson 3 , Andy Anker 3 , Geoff Cutts 5 , Dean S. Keeble 5 , Maria S. Thomsen 3 , Jan Rossmeisl 3 and Kirsten M. Ø. Jensen 3 1 Department of Physics,Technical University of Denmark,Denmark, 2 Interdisciplinary Nanoscience Center & Aarhus University Centre for Integrated Materials Research, Aarhus University, Denmark, 3 Department of Chemistry and Nano-Science Center, University of Copenhagen, Denmark, 4 Department of Materials, University of Oxford,UK, 5 Diamond Light Source, Harwell Campus, UK Intermetallic nanoparticles (NPs), defined by an atomically ordered structure with high stability, have shown enhanced catalytic properties as compared to their disordered alloy counterparts. 1,2 The enhancement in catalytic properties is partially attributed to changes in the nature of available surface sites, which are induced by changes in the crystal structure. 3,4 To advance green energy solutions and pave the way for new improved catalytic materials comprised of intermetallic NPs, it is therefore crucial that we understand what controls the formation of intermetallic NPs to synthetically promote these structures. By carefully selecting the additives used in a PdCu NP synthesis, we show that monodisperse, intermetallic PdCu NPs can be synthesized in a controllable manner. In this synthesis, the additives iron(III) chloride and ascorbic acid are used to control both the morphology and polymorph of the intermetallic NPs. Ascorbic acid provides a fast reduction of the ionic metal precursor species, while iron(III) chloride facilitates ligand exchange with the metal ion complexes and can assist in oxidative etching. Combined, ascorbic acid and iron(III) chloride provide a synergetic effect resulting in precursor reduction and defect-free growth; ultimately leading to monodisperse intermetallic PdCu NPs. Using in situ X-ray total scattering and pair distribution function analysis, we follow the disorder-order transformation all the way from the initial precursor structure to the formation of intermetallic PdCu NPs. We report a hitherto unknown transformation pathway that diverges from the commonly reported co-reduction disorder-order transformation. A Cu-rich structure initially forms, followed by incorporation of Pd(0) into the structure to obtain the disordered alloy PdCu structure. The formation of a Cu-rich structure suggests that it is not essential that the metallic species reduce at the same rate to ultimately form stoichiometric intermetallic PdCu NPs, as previously believed. These findings underpin the importance and strength of performing further combined multi-technique studies to uncover the driving force of intermetallic NP formation. When we understand how intermetallic NPs are formed, these mechanistic insights might open new opportunities to expand our library of intermetallic NPs by exploiting synthesis by design . References 1. Loukrakpam, R., Shan, S., Petkov, V., Yang, L., Luo, J. & Zhong, C.-J., The Journal of Physical Chemistry C 117 , 20715- 20721 (2013). 2. Jiang, K., Wang, P., Guo, S., Zhang, X., Shen, X., Lu, G., Su, D. & Huang, X.,Angewandte Chemie International Edition 55 , 9030-9035 (2016). 3. Gamler, J. T., Ashberry, H. M., Skrabalak, S. E. & Koczkur, K. M., Advanced Materials 30 , 1801563 (2018). 4. Antolini, E., Applied Catalysis B: Environmental 217 , 201-213 (2017).

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Gold nanoparticles modified cobalt iron oxide inverse opals as high-performance oxygen reduction electrocatalyst Thi Hong Trang Nguyen * , Chinnabathini Vana Chinnappa, Didier Grandjean and Ewald Janssens Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Belgium *thihongtrang.nguyen@kuleuven.be Exploration of competitive electrocatalysts to replace high-performance but high-cost Pt-based catalysts for oxygen reduction reaction (ORR) in fuel cells is an important strategy to confront energy and environmental crises. Although Fe, Co, and Ni-based catalysts have demonstrated good ORR catalytic activity, they generally lack stability in harsh environments as these metals can dissolve in an acidic or basic solution. Using their oxides 1,2 and carbides/nitrides 3,4 compounds instead has allowed significant improvements for the ORR by reducing metal dissolution. Introducing gold in these systems can also significantly enhance their activity, long-term durability and mitigate their dissolution. 5,6 We have recently produced mesoporous cobalt iron oxide inverse opals ( m -CFO IO) directly grown on nickel foam using polystyrene beads as a hard template followed by calcination in air. Their mesoporous structure featuring a high surface area demonstrated promising performance in the ORR. The performance of m -CFO IO can be significantly enhanced by modifying their surface with well- defined gas-phase Au NPs. Preformed Au nanoparticles of ca. 2 nm diameter have been deposited in soft landing mode using the cluster beam deposition (CBD) technology on m -CFO IO with loadings ranging from 4 to 10 atomic monolayers (ML). As-prepared m -CFO/Au IO samples were characterized with scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical methods. m -CFO/Au IO catalysts with an optimal gold loading of 7 ML exhibit an excellent ORR performance with the highest onset potential of 0.87 V and halfwave potential of 0.79 V vs. RHE. A remarkable three-time increase of the kinetic current density at 0.7 V and a halfwave potential shift of 180 mV are reported compared with their non- modified counterparts with long-term stability in both half-cell and single-cell accelerated degradation tests. The observed catalytic behavior enhancements that strongly depend on the Au mass loading deposited on the m -CFO IO are expected to arise from the sample’s large surface area and the synergistic effect of Au NPs and the m -CFO that guarantee a large number of accessible catalytic sites and rapid mass-transfer kinetics. References 1. Cheng, J. Shen, B. Peng, Y. Pan, Z. Tao and J. Chen, Nat. Chem., 2011, 3, 79–84

2. Wang, Y. Li, T. Jin, J. Meng, L. Jiao, M. Zhu and J. Chen, Nano Lett., 2017, 17, 7989–7994. 3. Hu, X. Y. Yu, F. Chen, Y. Wu, Y. Hu and X. W. Lou, Adv. Energy Mater., 2017, 1702476 4. Fan, Z. Peng, R. Ye, H. Zhou and X. Guo, ACS Nano, 2015, 9, 7407–7418 5. Gatalo, P. Jovanovic, G. Polymeros, M. Gabersc. ACS Catal. 2016, 6 (3), 1630−1634 6. Choi, C. W. Roh, B. S. Kim, H. Lee. Appl. Catal., B 2019, 247, 142−149

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Electrocatalytic performance of PtxNi1-x bimetallic clusters prepared by laser ablation cluster beam deposition Yubiao Niu 1 , Anupam Yadav 2 , Ting-Wei Liao 2 , Xian-Kui Wei 3 , Marc Heggen 3 , Ewald Janssens 2 , Peter Lievens 2 , Andrew J Wain 4 and Richard E Palmer 1 1 Nanomaterials Lab, Mechanical Engineering, Faculty of Science and Engineering, Swansea University, UK, 2 Quantum Solid State Physics, Department of Physics and Astronomy, KU Leuven, Belgium, 3 Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grunberg Institute, Germany, 4 National Physical Laboratory, UK Electrolyser technologies offer an environmentally friendly route to the production of hydrogen gas, which can be used as an energy carrier in a variety of applications [1, 2]. Electrolysis of water involves using electricity to split water into oxygen at the anode and hydrogen at the cathode, with catalysts required on each electrode in order to make these reactions energetically feasible. Due to the slow kinetics of the oxygen evolution reaction, a substantial amount of research effort has been focused on improving the design of the anode catalyst [3]. However, the cathode catalyst still presents problems: whilst platinum, the benchmark catalyst for the hydrogen evolution reaction (HER), is both highly active and stable, it is an expensive, rare earth metal. Therefore, the amount of Pt in the cathode catalyst needs to be reduced or replaced with cheaper, earth abundant alternatives to improve sustainability and reduce device costs. Alloying platinum with non-noble transition metals is one route to achieving these objectives. In this work, the catalytic reactivity of Pt-Ni nanoclusters, synthesised by laser ablation cluster beam deposition technique, towards electrochemical HER was investigated. Pt 70 Ni 30 and Pt 50 Ni 50 have effectively achieved equivalent performance to the Pt disk. An anti-contamination effect was also revealed for Pt x Ni 1-x Bimetallic Clusters. References 1. Ifkovits, Z. P., Evans, J. M., Meier, M. C., Papadantonakis, K. M., & Lewis, N. S. Energy & Environmental Science, 2021. 2. Escalera-López, D., Niu, Y., Park, S. J., Isaacs, M., Wilson, K., Palmer, R. E., & Rees, N. V. (2018). Applied Catalysis B: Environmental, 235, 84-91. 3. Wei, C., Rao, R. R., Peng, J., Huang, B., Stephens, I. E., Risch, M., & Shao‐Horn, Y. (2019). Advanced Materials, 31(31), 1806296.

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Unsupervised learning methods for the identification of nanoparticles structures based on local atomic environments

Cesare Roncaglia and Riccardo Ferrando Physics Department, University of Genoa, Italy

We propose a scheme for the automatic separation of data sets composed of several nanoparticles (NPs) structures by means of Machine Learning techniques. These data sets originate from atomistic simulations, such as global optimizations and molecular dynamics (MD), which are well known to produce large outputs that are often difficult to inspect by hand. By combining a description of NPs based on their local atomic environment with unsupervised learning algorithms, such as K-Means and Gaussian mixture model, we are able to distinguish between different structural motifs (for example icosahedra, decahedra, polyicosahedra, fcc fragments and twins). We show that this method is able to improve over the results obtained in Ref. [1] thanks to the successful implementation of a more detailed description of NPs, especially for systems showing a large variety of structures, including disordered ones. References 1. C. Roncaglia, D. Rapetti and R. Ferrando, Phys. Chem. Chem. Phys., 2021, 23 , 23325-23335.

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Hydrogen peroxide formation on AuPd nanoparticles Rasmus Svensson and Henrik Grönbeck Department of Physics and Competence Centre for Catalysis, Chalmers University of Technology, Sweden Hydrogen peroxide, H 2 O 2 , is an important industrial chemical, thanks to its mild oxidizing character and small environmental impact [1]. The desire for green, energy-efficient, small-scale synthesis of H 2 O 2 has sparked theneed for efficient catalysts for the direct formation of H 2 O 2 from O 2 and H 2 . In this work we have explored,and kinetically analyzed, critical steps for the heterogeneous catalytic formation of H 2 O 2 over single atomalloy palladium doped gold nanoparticles. In particular, density functional theory (DFT) calculations havebeen performed to establish the potential energy landscape and kinetic Monte Carlo simulations using scalingrelations have been applied to determine the reaction kinetics. The reaction is investigated with respect toparticle shape, size and degree of alloying. Gold alloys exothermically with palladium for all Au:Pd-ratios [2], entailing the possibility of high ratios of palladium monomers in dilute palladium gold nanoparticles. However, due to the low surface energy of gold, the probability of finding palladium at the surface of the particle is reduced under vacuum conditions. The situation is different under high oxygen and hydrogen pressures, where the presence of adsorbates stabilize palladium at the surface. In the catalytic formation of H 2 O 2 , several critical steps have been identified, of which, both palladium and gold play crucial parts. Firstly, oxygen should adsorb, but not dissociate, on the surface. This can be done on the palladium monomers, whereas larger patches of palladium results in scission of the O-O bond. Secondly, hydrogen should adsorb and dissociate over palladium atoms. This is an important role of the palladium atoms on the surface, as hydrogen does not dissociate on pure gold surfaces. Moreover, atomic hydrogen may diffuseover gold surfaces without being desorbed, owing to a large desorption barrier. The fact that hydrogen maydiffuse over the gold surface enables the possibility for reaction paths where multiple palladium monomersare involved during the formation of H 2 O 2 . The cleavage of the O–O, O–OH and HO–OH bonds must beprevented along the reaction path, as it leads to irreversible formation of water. The inert properties of gold playsin this respect an important role as, for example, desorption of H 2 O 2 is preferred with respect to dissociationinto 2OH. We found that the desorption energy of H 2 O 2 from the gold surfaces are clearly lower than thecorresponding palladium rich surfaces [3]. This work highlights the different roles of different sites in a catalytic reaction. The work stresses that it is the ensemble of sites rather than one active site that determines the activity of alloy nanoparticles. References 1. J. M. Campos-Martin, G. Blanco-Brieva, and J. L. Fierro, Angewandte Chemie International Edition, vol. 45, no. 42, pp. 6962–6984, 2006.

2. H. Okamoto and T. Massalski, Bulletin of Alloy Phase Diagrams, vol. 6, no. 3, pp. 229–235, 1985. 3. L. Chen, J. W. Medlin, and H. Grönbeck, ACS Catalysis, vol. 11, no. 5, pp. 2735–2745, 2021.

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