Protagonists and spectators during photocatalytic solar water splitting with SrTaOxNy oxynitride

Lawley, Craig; Tehrani, Zahra Pourmand; Clark, Adam H.; Safonova, Оlga V.; Döbeli, M.; Strocov, Vladimir N.; Schmidt, Thomas J.; Lippert, Thomas; Nachtegaal, Maarten; Pergolesi, Daniele

doi:10.1039/d1ta05052d

Cited by 11 publications

(19 citation statements)

References 82 publications

(153 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Even using PRCLA with ammonia gas pulses at optimized experimental parameters, achieving the desired N content in the film using conventional oxide substrates can be a major issue. Examples are LTON [ 59 ] and SrTaO 2 N (STON), [ 67 ] while for instance in our experience for BaTaO 2 N the N incorporation seems more facile. In general, the use of oxide substrates (such as SrTiO 3 , LaAlO 3 , Al 2 O 3 , MgO, and others) leads to films with relatively low N content.…”

Section: Oxynitride Thin Films For Solar Water Splittingmentioning

confidence: 96%

“…Examples are LTON [59] and SrTaO 2 N (STON), [67] while for instance in our experience for BaTaO 2 N the N incorporation seems more facile. In general, the use of oxide substrates (such as SrTiO 3 , LaAlO 3 , Al 2 O 3 , MgO, and others) leads to films with relatively low N content.…”

Section: Sample Designmentioning

confidence: 99%

“…The work [ 67 ] to date presents the first operando surface‐sensitive characterization of the oxynitride–liquid interface during the visible light‐driven oxygen evolution reaction. It is worth noticing that only the development of thin film‐based photoelectrodes makes these measurements possible.…”

Section: Oxynitride Thin Films For Neutron Reflectometry and Surface‐...mentioning

confidence: 99%

mentioning

confidence: 99%

See 3 more Smart Citations

Thin‐Film Oxynitride Photocatalysts for Solar Hydrogen Generation: Separating Surface and Bulk Effects Using Synchrotron X‐Ray and Neutron‐Based Techniques

2022

Self Cite

View full text Add to dashboard Cite

The conversion of solar light into hydrogen by photoelectrochemical water splitting is one of the potential strategies that can allow the development of a carbon‐neutral energy cycle. Oxynitride semiconductors are promising materials for this application, although important limitations must still to be addressed. One of the most important issues is physicochemical degradation of the semiconductor, at the interface with water, where the electrochemical reactions occur. In this regard, thin films, with well‐defined and atomically flat surfaces, are invaluable tools for characterizing material properties and degradation mechanisms, while identifying strategies to mitigate detrimental effects. Thin oxynitride films may allow the use of complementary characterizations, not applicable to conventional powder samples. In particular, the study of the solid–liquid interface can benefit enormously from the use of thin films for synchrotron‐based surface‐sensitive X‐Ray scattering methods and neutron reflectometry. These investigation approaches promise to speed up the design and discovery of new materials for the production of solar fuels, while paving the way for similar applications in other research fields. This work aims at reviewing the literature contributions on oxynitride thin films for solar water splitting summarizing what is learnt so far and suggesting experimental strategies to unveil what is still not clear.

show abstract

Section: Oxynitride Thin Films For Solar Water Splittingmentioning

confidence: 96%

Section: Sample Designmentioning

confidence: 99%

Section: Oxynitride Thin Films For Neutron Reflectometry and Surface‐...mentioning

confidence: 99%

mentioning

confidence: 99%

See 2 more Smart Citations

Thin‐Film Oxynitride Photocatalysts for Solar Hydrogen Generation: Separating Surface and Bulk Effects Using Synchrotron X‐Ray and Neutron‐Based Techniques

2022

Self Cite

View full text Add to dashboard Cite

show abstract

“…Still, PSD applied to MES data results in a special kind of difference spectrum between excited and non-excited states (Gremlich & Yan, 2000), thus allowing qualitative analysis. In electrocatalysis research, MES experiments and PSD analysis have been used to catch the dynamic changes in adsorption species and surface structure (Czioska et al, 2021;Lawley et al, 2022;Ebner et al, 2022), which proved the great potential of this method. However, if the quantitative relationship between PSD demodulated XAS and the diffXAS could be elucidated, PSD analysis can give more quantitative results.…”

Section: Introductionmentioning

confidence: 99%

Approach to electrochemical modulating differential extended X-ray absorption fine structure

Zhang

Shou

et al. 2022

J Synchrotron Radiat

View full text Add to dashboard Cite

The differential XAFS technique holds promise for detecting surface changes, which benefits many chemical applications. Phase-sensitive detection (PSD) analysis based on modulated excitation spectroscopy experiments is expected to obtain a high-quality difference spectrum, while the mathematical relationship and experiment parameters remain to be discussed. In this article, an approach to obtaining the difference spectrum from the PSD demodulated spectrum is described and its applicability in different experiment settings is discussed. The results indicate that the demodulated spectrum is almost equal to the difference spectrum when the modulating period is 20 times larger than the relaxation time constant. This approach was subsequently applied to an electrochemical modulation experiment and the demodulated spectrum was analyzed. A reversible lattice shrinking is observed via the fitting of demodulated spectra, which is proportional to the charge amount on the electrode. This approach could be used to quantitatively analyze the modulated excitation XAS data and holds promise for a wide range of electrochemical studies.

show abstract

Semi Transparent Three-Dimensional Macroporous Quaternary Oxynitride Photoanodes for Photoelectrochemical Water Oxidation

Chen

Piętak

et al. 2022

Chem. Mater.

View full text Add to dashboard Cite

Semi transparent three-dimensional macroporous (3DM) photoanodes based on quaternary oxynitrides have the potential to simultaneously realize superior light harvesting and efficient charge transfer in a tandem photoelectrochemical (PEC) cell. A 3DM CaTaO 2 N photoanode was prepared for the first time on a GaN/Al 2 O 3 substrate via a chemical route, and it exhibits a high transmittance of >60% in the wide solar spectrum and a photoresponse onset at −0.3 V versus the reversible hydrogen electrode (V RHE ) under simulated solar illumination. In particular, a plateau photocurrent density of 0.21 mA cm −2 was achieved at a low potential of 0.4 V RHE , which was 1.6-fold and more than 50fold higher than a two-dimensional macroporous (2DM) CaTaO 2 N/GaN/Al 2 O 3 photoanode and a conventional particlebased CaTaO 2 N/GaN/Al 2 O 3 photoanode, respectively. The bicontinuous, interconnected pore structure within this 3DM film can improve charge carrier separation and collection by reducing the average diffusion distance for minority carriers toward the electrolyte. Optical measurements and simulations verified the enhanced sunlight harvesting in the 3DM photoanode, which was ascribed to the concentrated distribution of the electric field and multiple scattering. This study provides guidance for future synthesis of highly efficient semitransparent 3DM quaternary oxynitride-based photoanodes for a tandem PEC device.

show abstract

Protagonists and spectators during photocatalytic solar water splitting with SrTaO_xN_y oxynitride

Abstract: Oxynitrides have been shown to be promising visible light water splitting photocatalysts, but rapidly degrade under operating conditions. With a custom designed photoelectrochemical cell, we perform operando grazing incidence X-ray...

Cited by 11 publications

References 82 publications

Thin‐Film Oxynitride Photocatalysts for Solar Hydrogen Generation: Separating Surface and Bulk Effects Using Synchrotron X‐Ray and Neutron‐Based Techniques

Thin‐Film Oxynitride Photocatalysts for Solar Hydrogen Generation: Separating Surface and Bulk Effects Using Synchrotron X‐Ray and Neutron‐Based Techniques

Approach to electrochemical modulating differential extended X-ray absorption fine structure

Semi Transparent Three-Dimensional Macroporous Quaternary Oxynitride Photoanodes for Photoelectrochemical Water Oxidation

Contact Info

Product

Resources

About