Bulk Hydroxylation and Effective Water Splitting by Highly Reduced Cerium Oxide: The Role of O Vacancy Coordination

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F18%3A10389434" target="_blank" >RIV/00216208:11320/18:10389434 - isvavai.cz</a>

Výsledek na webu

<a href="https://doi.org/10.1021/acscatal.7b04409" target="_blank" >https://doi.org/10.1021/acscatal.7b04409</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.7b04409" target="_blank" >10.1021/acscatal.7b04409</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Bulk Hydroxylation and Effective Water Splitting by Highly Reduced Cerium Oxide: The Role of O Vacancy Coordination

Popis výsledku v původním jazyce

Reactions of reduced cerium oxide CeOx with water are fundamental processes omnipresent in ceria-based catalysis. Using thin epitaxial films of ordered CeOx, we investigate the influence of oxygen vacancy concentration and coordination on the oxidation of CeOx by water. Upon changing the CeOx stoichiometry from CeO2 to Ce2O3, we observe a transition from a slow surface reaction to a productive H-2-evolving CeOx oxidation with reaction yields exceeding the surface capacity and indicating the participation of bulk OH species. Both the experiments and the ab initio calculations associate the effective oxidation of highly reduced CeOx by water to the next-nearest-neighbor oxygen vacancies present in the bixbyite c-Ce2O3 phase. Next-nearest-neighbor oxygen vacancies allow for the effective incorporation of water in the bulk via formation of OH- groups. Our study illustrates that the coordination of oxygen vacancies in CeOx represents an important parameter to be considered in understanding and improving the reactivity of ceria-based catalysts.

Název v anglickém jazyce

Bulk Hydroxylation and Effective Water Splitting by Highly Reduced Cerium Oxide: The Role of O Vacancy Coordination

Popis výsledku anglicky

Reactions of reduced cerium oxide CeOx with water are fundamental processes omnipresent in ceria-based catalysis. Using thin epitaxial films of ordered CeOx, we investigate the influence of oxygen vacancy concentration and coordination on the oxidation of CeOx by water. Upon changing the CeOx stoichiometry from CeO2 to Ce2O3, we observe a transition from a slow surface reaction to a productive H-2-evolving CeOx oxidation with reaction yields exceeding the surface capacity and indicating the participation of bulk OH species. Both the experiments and the ab initio calculations associate the effective oxidation of highly reduced CeOx by water to the next-nearest-neighbor oxygen vacancies present in the bixbyite c-Ce2O3 phase. Next-nearest-neighbor oxygen vacancies allow for the effective incorporation of water in the bulk via formation of OH- groups. Our study illustrates that the coordination of oxygen vacancies in CeOx represents an important parameter to be considered in understanding and improving the reactivity of ceria-based catalysts.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10305 - Fluids and plasma physics (including surface physics)

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2018

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ACS Catalysis

ISSN

2155-5435

e-ISSN

—

Svazek periodika

8

Číslo periodika v rámci svazku

5

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

4354-4363

Kód UT WoS článku

000431727300068

EID výsledku v databázi Scopus

2-s2.0-85046665112