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Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction = = Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika.

Record Type:	Language materials, manuscript : Monograph/item
Title/Author:	Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction =/
Reminder of title:	Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika.
Author:	Gebremariam, Goitom K.
Description:	1 online resource (101 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 85-12, Section: B.
Contained By:	Dissertations Abstracts International85-12B.
Subject:	Metals. -
Online resource:	click for full text (PQDT)
ISBN:	9798383013717

Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction = = Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika.
Gebremariam, Goitom K.

Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction =Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika. - 1 online resource (101 pages)

Source: Dissertations Abstracts International, Volume: 85-12, Section: B.

Thesis (Ph.D.)--University of Belgrade (Serbia), 2023.

Includes bibliographical references

Efficient hydrogen production is crucial due to the global energy crisis and environmental concerns, which necessitates identifying catalytic trends for informed choices in hydrogen generation technologies and materials. Hydrogen evolution reaction (HER) volcano plots, initially established for acidic solutions and later adapted for alkaline media, play a crucial role in identifying catalytic trends related to HER. The first part of the thesis focuses on conducting a comprehensive analysis of the HER catalytic trends on nine polycrystalline monometallic surfaces in seven solutions, encompassing a wide pH range from highly acidic to highly alkaline.Using theoretically calculated hydrogen binding energies (HBEs) on clean metallic surfaces and experimentally measured HER overpotentials it is shown, for the first time, that the volcano-like relationships are predominantly preserved across a broad spectrum of pH values, spanning from acidic to neutral and alkaline solutions. This signifies that HBE can be used as a descriptor for the identification of active electrocatalysts in a wide pH range, including pH neutral solutions. Accordingly, Cr was found to have high HER activity in pH-neutral solutions surpassing that of W, Fe, and Co. Furthermore, exposing metallic surfaces to high anodic potentials can lead to either enhanced or suppressed HER, depending on the metal and the electrolyte used. In view of the nontrivial impacts of surface oxidation, its effects might be seen either as a promotion in HER activity or as HER blocking (as in the case of Cr and W). The former case is specifically applicable to Ni and Co in alkaline and pH-neutral solutions, which can be attributed to the enhanced dissociation of water at the metal-oxide interface. This effect is more significant for Ni in NaCl solutions to the extent that, after undergoing oxidation, it becomes more active than Pt. Therefore, this section of the research work reveals that the shape of the volcano curve is largely preserved in the entire pH range, indicating that HBE can be employed to identify powerful catalysts for the HER regardless of pH.Supporting metal catalysts on various supports is another possible design strategy to boost the catalytic activity and stability and improve their utilization. Kinetic Monte Carlo (KMC) simulations were employed in the second part of the thesis work to illustrate that the HER can be enhanced through hydrogen spillover to the support material. This effect happens when the catalysts have a high surface coverage of adsorbed hydrogen atoms under the reaction conditions. Drawing from the insights obtained through KMC, a range of catalysts supported on reduced graphene oxide were synthesized, and their performance in promoting the HER was then compared to their respective pure metal counterparts in alkaline environments. While the support effect is negative for Ag, Au, and Zn, it boosts the HER activity for Pt, Pd, Fe, Co, and Ni. The HER volcano plot, a plot of calculated HBEs vs measured HER activities, is preserved and demonstrates a positive shift in the strong binding region. Thus, this part of the thesis work highlights the potential of metal-support interface engineering in making effective catalysts for HER and provides general guidelines for selecting suitable combinations of catalysts and supports for enhanced electrocatalytic hydrogen production.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2024

Mode of access: World Wide Web

ISBN: 9798383013717Subjects--Topical Terms:

563369
Metals.
Index Terms--Genre/Form:

554714
Electronic books.

Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction = = Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika.
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245 1 0 $a Investigation of the Influence of Electrolytes and the Role of Reduced Graphene Oxide as a Support for Metal Catalysts on the Catalytic Activity Toward the Hydrogen Evolution Reaction = $b Ispitivanje Uticaja Elektrolita I Uloge Redukovanog Grafen-Oksida Kao Nosaca Metalnih Katalizatora na Kataliticku Aktivnost za Reakciju Izdvajanja Vodonika.
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500 $a Source: Dissertations Abstracts International, Volume: 85-12, Section: B.
500 $a Advisor: Pasti, Igor.
502 $a Thesis (Ph.D.)--University of Belgrade (Serbia), 2023.
504 $a Includes bibliographical references
520 $a Efficient hydrogen production is crucial due to the global energy crisis and environmental concerns, which necessitates identifying catalytic trends for informed choices in hydrogen generation technologies and materials. Hydrogen evolution reaction (HER) volcano plots, initially established for acidic solutions and later adapted for alkaline media, play a crucial role in identifying catalytic trends related to HER. The first part of the thesis focuses on conducting a comprehensive analysis of the HER catalytic trends on nine polycrystalline monometallic surfaces in seven solutions, encompassing a wide pH range from highly acidic to highly alkaline.Using theoretically calculated hydrogen binding energies (HBEs) on clean metallic surfaces and experimentally measured HER overpotentials it is shown, for the first time, that the volcano-like relationships are predominantly preserved across a broad spectrum of pH values, spanning from acidic to neutral and alkaline solutions. This signifies that HBE can be used as a descriptor for the identification of active electrocatalysts in a wide pH range, including pH neutral solutions. Accordingly, Cr was found to have high HER activity in pH-neutral solutions surpassing that of W, Fe, and Co. Furthermore, exposing metallic surfaces to high anodic potentials can lead to either enhanced or suppressed HER, depending on the metal and the electrolyte used. In view of the nontrivial impacts of surface oxidation, its effects might be seen either as a promotion in HER activity or as HER blocking (as in the case of Cr and W). The former case is specifically applicable to Ni and Co in alkaline and pH-neutral solutions, which can be attributed to the enhanced dissociation of water at the metal-oxide interface. This effect is more significant for Ni in NaCl solutions to the extent that, after undergoing oxidation, it becomes more active than Pt. Therefore, this section of the research work reveals that the shape of the volcano curve is largely preserved in the entire pH range, indicating that HBE can be employed to identify powerful catalysts for the HER regardless of pH.Supporting metal catalysts on various supports is another possible design strategy to boost the catalytic activity and stability and improve their utilization. Kinetic Monte Carlo (KMC) simulations were employed in the second part of the thesis work to illustrate that the HER can be enhanced through hydrogen spillover to the support material. This effect happens when the catalysts have a high surface coverage of adsorbed hydrogen atoms under the reaction conditions. Drawing from the insights obtained through KMC, a range of catalysts supported on reduced graphene oxide were synthesized, and their performance in promoting the HER was then compared to their respective pure metal counterparts in alkaline environments. While the support effect is negative for Ag, Au, and Zn, it boosts the HER activity for Pt, Pd, Fe, Co, and Ni. The HER volcano plot, a plot of calculated HBEs vs measured HER activities, is preserved and demonstrates a positive shift in the strong binding region. Thus, this part of the thesis work highlights the potential of metal-support interface engineering in making effective catalysts for HER and provides general guidelines for selecting suitable combinations of catalysts and supports for enhanced electrocatalytic hydrogen production.
520 $a Efikasna proizvodnja vodonika je kljucna zbog globalne energetske krize i zabrinutosti za zivotnu sredinu, sto zahteva identifikaciju katalitickih trendova za informisane izbore u tehnologijama i materijalima za proizvodnju vodonika. Vulkanske krive reakcije izdvajanja vodonika (HER), prvobitno uspostavljene za kisele rastvore, a kasnije prilagodene za alkalne medije, igraju kljucnu ulogu u identifikaciji katalitickih trendova povezanih sa HER. Prvi deo ove doktorske disertacije fokusira se na sprovodenje sveobuhvatne analize HER katalitickih trendova na devet polikristalnih monometalnih povrsina u sedam rastvora, obuhvatajuci sirok pH opseg od visoko kiselih do visoko alkalnih.Koristeci teorijskiizracunate energije vezivanja vodonika (HBE) na cistim metalnim povrsinama i eksperimentalno izmerene HER nadnapone, po prvi put je pokazanoda su relacije vulkanskog tipa pretezno ocuvane u sirokom spektru pH vrednosti, od kiselih do neutralnih i alkalnih rastvora. Ovo znaci da se HBE moze koristiti kao deskriptor za identifikaciju aktivnih elektrokatalizatora u sirokom pH opsegu, ukljucujuci pH neutralne rastvore. Shodno tome, otkriveno je da Cr ima visoku HER aktivnost u pH-neutralnim rastvorima, koja nadmasuje aktivnostV, Fe i Co. Stavise, izlaganje metalnih povrsina visokim anodnim potencijalima moze dovesti do pojacane ili potisnute HER, u zavisnosti od metala i koriscenog elektrolita. S obzirom na netrivijalne uticaje oksidacije povrsine, njeni efekti se mogu posmatrati ili kao promocija HER aktivnosti ili kao HER blokiranje (kao u slucaju Cr i V). Prvi slucaj je posebno primenljiv na Ni i Co u alkalnim i pH-neutralnim rastvorima, sto se moze pripisati pojacanoj disocijaciji vode na granici fazametal-oksid. Ovaj efekat je znacajniji za Ni u rastvorima NaCl, do te mere da posle oksidacije postaje aktivniji od Pt. Stoga, ovaj deo istrazivackog rada otkriva da je oblik vulkanske krive u velikoj meri ocuvan u citavom pH opsegu, sto ukazuje da se HBE moze koristiti za identifikaciju pogodnih katalizatora za HER bez obzira na pH.Postavljanje metalnih katalizatora na razlicite nosace je jos jedna moguca strategija dizajna za povecanje kataliticke aktivnosti i stabilnosti i poboljsanje njihovog koriscenja. Kineticke Monte Karlo (KMC) simulacije su koriscene u drugom delu teze da bi se ilustrovalo da se HER moze pospesitiprelivanjem vodonika na potporni materijal. Ovaj efekat se desava kada katalizatori imaju visoku povrsinsku pokrivenost adsorbovanih atoma vodonika u uslovima reakcije. Na osnovu uvida dobijenih putem KMC- a, sintetisanje niz katalizatora podrzanih na redukovanom grafen-oksidu, a njihov ucinak u promovisanju HER je zatim uporeden sa odgovarajucim cistim metalima u alkalnim sredinama. Dok je efekat nosacanegativan za Ag, Au i Zn, on povecava HER aktivnost za Pt, Pd, Fe, Co i Ni. HER vulkanska kriva, dijagram izracunatih HBE u odnosu na izmerene HER aktivnosti, je ocuvana i pokazuje pozitivan pomak u regionu jakog vezivanja. Stoga, ovaj deo teze naglasava potencijal inzenjeringa granica fazametal-podloga u pripremiefikasnih katalizatora za HER i pruza opste smernice za odabir odgovarajucih kombinacija katalizatora i nosaca za poboljsanu elektrokataliticku proizvodnju vodonika.
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