HEИндивидуална стипендия2023–2025

PIERCAT · Gap-plasmon electrochemistry coupled with photo-induced enhanced Raman spectroscopy to probe oxygen vacancy dynamics (in-situ) and hot charge carrier kinetics for photoelectrochemical CO2 reduction

„Хоризонт Европа“ — Действия „Мария Склодовска-Кюри“

Период: 2023-06-01 → 2025-05-31
Финансиране от ЕС: 189 687 €
Участници: 1
Схема: HORIZON-TMA-MSCA-PF-EF

Линиите свързват координатора с партньорите.

Накратко на български

Металните оксиди, като цериум(IV) оксид, се анализират, за да се разбере как дефектите в кристалната им решетка влияят върху превръщането на въглеродния диоксид в химикали. Това помага за създаването на по-ефективни катализатори за производство на алтернативни горива и възобновяема енергия.

Този кратък обзор е генериран от изкуствен интелект

Кратко обяснение, генерирано от езиков модел по текста на CORDIS. Оригиналът е по-долу.

Резултати накратко

Gap-plasmon electrochemistry coupled with photo-induced enhanced Raman spectroscopy to probe oxygen vacancy dynamics (in-situ) and hot charge carrier kinetics for photoelectrochemical CO2 reduction

Increasing energy demands and depleting fossil fuel reserves galvanized the efforts to search for alternative renewable energy sources. Photo-electrochemical (PEC) water splitting, carbon dioxide photo-catalytic reduction (CO2 RR), and alcohol oxidation reaction (AOR) for fuel cells are considered alternative pathways to produce high-value-added chemicals and fuels. Such approaches require robust electrode materials and catalysts to drive the redox reactions efficiently. Metal oxides (MOs) have been widely used in this context and have shown great potential for the advancement of these technologies. Many physical and chemical properties of MOs can be controlled by tuning the imperfections in the crystal lattice, of particular interest, oxygen vacancies (VOs). Therefore, the overall aim of the project is to probe the metal oxide (catalyst) interfaces, i.e. to understand the critical role of defect states (for instance, VOs) and their impact on photocatalytic CO2 reduction (CO2 RR). In this context, CeO2 is used as a model metal oxide catalyst; relevant defect dynamics and their influence on catalytic activity have been evaluated by in situ X-ray photoelectron spectroscopy, surface-enhanced Raman spectroscopy and wavelength-dependent photocatalytic CO2 RR measurements. The following specific research objectives (SROs) were set for the project and have been successfully implemented. SRO1: To fabricate the MO thin films with specific design configurations: This objective has been achieved by fabricating the pristine, Au NP, Au/SiO2 NP embedded CeO2 thin films. SRO2: To quantitatively elucidate the defect dynamics in CeO2 and associated charge transfer kinetics: This objective has been implemented fully with the help of state-of-the-art in situ XPS and SERS measurements. SRO3: To reveal the photocatalytic CO2 RR mechanism over pristine, and Au, Au/SiO2 NP embedded CeO2 thin films: The objective resulted a new and measurable findings on how the selectivity of CO2 RR can be impacted by the metal cation reduction under illumination.

Текст от CORDIS, на английски · Данни: CORDIS, © Европейски съюз

Цел на проекта

Photo-electrochemical CO2 reduction (CO2 ER) is a promising technology to mitigate the ever-increasing CO2 levels in the earth's atmosphere as well as to produce chemical feedstocks simultaneously. Though tremendous research has been undertaken in the recent past to enhance the efficiency of CO2ER, still little known about CO2ER reaction pathways, selectivity, and the role of active sites, which impede the largescale implementation at the industrial level. It is well known that the surface structure strongly influences the electrocatalytic activity of electrode materials. Thus, the presence of defects, for instance, oxygen vacancies (VOs) drastically alter the surface physicochemical properties of metal oxide (MO) based electrodes and play a crucial role in defining the overall performance of CO2 ER. Therefore, it is indeed necessary to better understand the VOs formation, healing, and associated reaction kinetics. Here, I introduce photo-induced enhanced Raman spectroscopy (PIERS) coupled with gap-plasmon-assisted electrochemistry as a powerful tool to probe the VOs and associated charge transfer dynamics of MO electro-catalysts. Plasmonic nanogaps are ideal for the extreme localization of light and they generate intense electric fields in confined volumes. Such a small gap volume dramatically enhances the light-matter interaction and enables the creation of single molecule-level spectroscopic probes. Therefore, using the combination of gap-plasmon probe electrochemistry and in-situ PIERS, the current proposal aims to elucidate the underlying reaction mechanism of CO2ER at active sites (VOs). As a result, new strategies may be unveiled to design and tune the active sites on MO electrode surfaces for efficient CO2ER. Therefore, the study is not only limited to CO2ER but also provides significant insights for other important photo-electrocatalytic applications as well, for instance, fuel cells.

Оригинален текст от CORDIS (на английски).

Участници

LUDWIG-MAXIMILIANS-UNIVERSITAET MUENCHEN · PlaneggКоординаторГермания