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Role of Metallic Nanoclusters in Catalysis for Fuel Cell Feed Gas Purification and Hydrogen Storage

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Role of Metallic Nanoclusters in Catalysis for Fuel Cell Feed Gas Purification and Hydrogen Storage Role of metallic nanoclusters in catalysis for fuel cell feed gas purification and hydrogen storage Krstić, Marjan Doctoral thesis / Disertacija 2016 Degree Grantor / Ustanova koja je dodijelila akademski / stručni stupanj: University of Split, University of Split, Faculty of science / Sveučilište u Splitu, Prirodoslovno-matematički fakultet Permanent link / Trajna poveznica: https://urn.nsk.hr/urn:nbn:hr:166:827385 Rights / Prava: In copyright Download date / Datum preuzimanja: 2021-10-04 Repository / Repozitorij: Repository of Faculty of Science University of Split Faculty of Science Biophysics Doctoral Programme Marjan Krsti´c Role of metallic nanoclusters in catalysis for fuel cell feed gas purification and hydrogen storage Doctoral thesis Split, 2016 Sveuˇciliˇsteu Splitu Prirodoslovno-matematiˇckifakultet Poslijediplomski sveuˇciliˇsni doktorski studij Biofizika Marjan Krsti´c Uloga metalnih nanoklastera u katalizi za proˇciˇs´cavanje pogonskog plina gorivnih ´celijai spremanje vodika Doktorski rad Split, 2016. Sveuˇciliˇsteu Splitu, Prirodoslovno-matematiˇckifakultet Odjel za fiziku, Poslijediplomski sveuˇciliˇsnidoktorski studij Biofizika "Uloga metalnih nanoklastera u katalizi za proˇciˇs´cavanje pogonskog plina gorivnih ´celijai spremanje vodika" Doktorski rad autora Marjana Krsti´cakao dio obaveza potrebnih da se dobije doktorat znanosti, izraden pod vodstvom mentora prof. dr. dr. h. c. Vlaste Bonaˇci´c-Kouteck´yi prof. dr. sc. Paˇska Zupanovi´caˇ Dobiveni akademski naziv i stupanj: doktor prirodnih znanosti iz polja fizike Povjerenstvo za ocjenu i obranu doktorskog rada u sastavu: 1. prof. dr. sc. Ante Biluˇsi´c,redoviti profesor 2. prof. dr. sc. Franjo Sokoli´c,redoviti profesor 3. dr. sc. Anita Kriˇsko, viˇsiznanstveni suradnik 4. dr. sc. Mile Ivanda, znanstveni savjetnik (zamjenski ˇclan) 1. 2. 3. Potvrduje da je disertacija obranjena dana Voditelj studija: prof. dr. sc. Paˇsko Zupanovi´cˇ Predsjednik Vije´castudija: prof. dr. dr. h. c. Vlasta Bonaˇci´c-Koutecky ACKNOWLEDGMENTS I would like to express my sincere gratitude to all the people who was with me, supported me and helped during the fruitful research time of the last 5 years and preparation of this thesis. First, I am endlessly grateful to the Prof. Vlasta Bonaˇci´c-Kouteck´y,for the continuous support of my Ph.D study and related research, for her motivation, patience and immense knowledge. By accepting me into her research group she showed an infinite faith in me and gave me an opportunity to work on such interesting topics in the field of the nanocluster catalysis. I appreciate all the research related discussions we had, where she motivated me by always asking challenging questions. She steered me in the right direction whenever she thought it was needed but gave me the freedom and showed me the trust to express myself and give my own contribution to the research. I must admit that I am really lucky to be supervised by such intelligent, widely-talented and educated person she is. Furthermore, I have to say special thanks to the thesis co-mentor Prof. Paˇsko Zupanovi´c,ˇ who showed me an incredible world of physics. He was always there for me, believed in me and guide me throughout entire master's education and Ph.D study. All this would not be possible without numerous experimental collaborations. There- fore, I feel a special need to thank to Prof. Thorsten M. Bernhardt, Prof. Sandra M. Lang and Sandra U. F¨ortigfrom University of Ulm for initiating and proposing new challenges as well as stimulating discussions in the research direction of fuel cell feed gas purification. The hydrogen storage research direction would not be such a success without the experi- mental collaboration with Prof. Richard A. J. O'Hair, Athanasios Zavras and Dr. George N. Khairallah from University of Melbourne and Prof. Philippe Dugourd, Dr. Rodolphe Antoine, Dr. Marion Girod, Dr. Luke MacAleese, Prof. J´eromeLemoine, Dr. Steven Daly and Dr. Philippe Maitre from University of Lyon. Without their precious and insightful comments, hard question, encouragement and support it would not be possible to conduct this research, so one sincere thanks goes to all of them. I also thank my fellow coworkers, especially Zeljkaˇ Sanader for the continuous support, help and discussions as well as for all the fun we have had in the last five years working together. Finally, the last but not the least, I must acknowledge gratitude to my parents, sister, brother, other members of family and all my dear friends for providing me with unfailing support and continuous encouragement throughout my work on the research, writing the thesis and my life in general. 4 BASIC DOCUMENTATION CARD University of Split Faculty of Science Ph.D. thesis ROLE OF METALLIC NANOCLUSTERS IN CATALYSIS FOR FUEL CELL FEED GAS PURIFICATION AND HYDROGEN STORAGE Marjan Krsti´c Thesis performed at: Center of excellence for science and technology - Integration of Mediterranean region (STIM) at Interdisciplinary center for Advanced science and technology (ICAST), Uni- versity of Split Abstract: Catalytic reactivity of the small transition and coinage metal nanoclusters have been theo- retically studied in context of (1) advancing fuel cell technology by developing cost-effective techniques to improve quality of the feed gas as well as (2) safe storage and release of hy- drogen in its gaseous state at room temperatures and pressures. In order to address the challenge concerning the improvement the quality of fuel cell feed gas reactions of small ruthenium cationic nanoclusters with CO and H2 has been performed. The origin of the selectivity and outstanding activity of small ruthenium nanoparticles in the catalytic CO methanation reaction has been identified. The second aim of this dissertation is to advance materials for hydrogen storage and their release technology. For this purpose a gas-phase study of fragmentation and catalytic activity of ligated coinage metal hydride nanoclusters has been performed. The theoretical findings based on density functional theory (DFT) are strongly supported by experimental results trough international cooperation. Within thesis we demonstrated that powerful combination of density functional theory and experimen- tal investigations can contribute to intelligently developed new materials and procedures to overcome the challenges hampering worldwide application of fuel cells as "green" technology of the future. (100 pages, 25 figures, 1 table, 115 references, 2 appendices, original in English) Thesis deposited in: National and University Library in Zagreb University Library in Split Library of the Faculty of Science, University of Split Keywords: fuel cells, feed gas purification, ruthenium clusters, hydrogen storage and release, coinage metal hydrides, density functional theory Supervisor: Paˇsko Zupanovi´c,Ph.D./Fullˇ professor Supervisor: Vlasta Bonaˇci´c-Kouteck´y,Dr. Dr. h. c./Full professor Reviewers: 1. Ante Biluˇsi´c,Ph.D./Full professor 2. Franjo Sokoli´c,Ph.D./Full professor 3. Anita Kriˇsko, Ph.D. Thesis accepted: 30.11.2016. TEMELJNA DOKUMENTACIJSKA KARTICA Sveuˇciliˇsteu Splitu Prirodoslovno-matematiˇckifakultet Doktorski rad ULOGA MALIH METALNIH NANOKLASTERA U KATALIZI ZA PROCIˇ SˇCAVANJE´ POGONSKOG PLINA GORIVNIH CELIJA´ I SPREMANJE VODIKA Marjan Krsti´c Rad je izraden u: Centru izvrsnosti za znanost i tehnologiju - Integracija Mediteranske regije (STIM) pri Interdiscipliarnom centru za naprednu znanost i tehnologiju (ICAST), Sveuˇciliˇste u Splitu Saˇzetak: Katalitiˇcka reaktivnost malih nanoklastera prijelaznih metala teorijski je istraˇzivana u kon- tekstu (1) unaprjedenja tehnologije gorivnih ˇclanaka razvijaju´cijeftine tehnike poboljˇsanja kvalitete pogonskog plina kao i (2) sigurne pohrane i otpuˇstanja vodika u plinovitom stanju na atmosferskoj temperaturi i tlaku. Da bi rijeˇsiliproblem nedovoljne kvalitete pogonskog plina gorivnih ˇclanaka istraˇzivale su se reakcije malih rutenijevih nanoklastera s CO i H2. Izvor selektivnosti i izvrsne aktivnosti malih rutenijevih ˇcestica u katalitiˇckoj CO metanacijskoj reakciji je identificiran. Drugi cilj ove disertacije ja unaprjedivanje materijala za tehnologiju pohrane i otpuˇstanjavodika. U tu svrhu provela su se istraˇzivanja fragmentacije i katalitiˇcke aktivnosti ligandiranih metalnih hidridnih nanoklastera. Naˇsateorijska istraˇzivanja bazi- rana na teoriji funkcionala gusto´cesu potvrdena eksperimentalnim rezultatima priznatih istraˇzivaˇckihgrupa kroz medunarodnu suradnju. Unutar ove teze demonstrirali smo da mo´cnakombinacija naˇsegteorijskog istraˇzivanja potvrdena eksperimentalnim istraˇzivanjima moˇzedoprinijeti inteligentnom razvoju novih materijala i procedura da bi se nadiˇsliproblemi koji sprjeˇcavaju ˇsirokuprimjenu gorivnih ´celijakao "zelene" tehnologije budu´cnosti. (100 stranica, 25 slika, 1 tablica, 115 literaturnih navoda, 2 priloga, jezik izvornika: engleski jezik) Rad je pohranjen u: Nacionalnoj sveuˇciliˇsnoj knjiˇzniciu Zagrebu Sveuˇciliˇsnoj knjiˇznici u Splitu KnjiˇznicaPrirodoslovno-matematiˇckog fakulteta na Sveuˇciliˇstuu Splitu Kljuˇcnerijeˇci:gorivni ˇclanci, proˇciˇs´cavanje pogonskog plina, rutenijevi klasteri, spremanje i otpuˇstanjevodika, hidridi kovinskih metala, teorija funkcionala gusto´ce Mentor: prof. dr. sc. Paˇsko Zupanovi´c,redovitiˇ profesor Komentor: prof. dr. dr. h. c. Vlasta Bonaˇci´c-Kouteck´y,redoviti profesor Ocjenjivaˇci: 1. prof. dr. sc. Ante Biluˇsi´c,redoviti profesor 2. prof. dr. sc. Franjo Sokoli´c,redoviti profesor 3. dr. sc. Anita Kriˇsko, viˇsiznanstveni suradnik Rad
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