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Article ; Online: Life cycle net energy assessment of sustainable H

Zhang, Xinyi / Schwarze, Michael / Schomäcker, Reinhard / van de Krol, Roel / Abdi, Fatwa F

2023 Volume 14, Issue 1, Page(s) 991

Abstract: Green hydrogen has been identified as a critical enabler in the global transition to sustainable energy and decarbonized society, but it is still not economically competitive compared to fossil-fuel-based hydrogen. To overcome this limitation, we propose ...

Abstract	Green hydrogen has been identified as a critical enabler in the global transition to sustainable energy and decarbonized society, but it is still not economically competitive compared to fossil-fuel-based hydrogen. To overcome this limitation, we propose to couple photoelectrochemical (PEC) water splitting with the hydrogenation of chemicals. Here, we evaluate the potential of co-producing hydrogen and methyl succinic acid (MSA) by coupling the hydrogenation of itaconic acid (IA) inside a PEC water splitting device. A negative net energy balance is predicted to be achieved when the device generates only hydrogen, but energy breakeven can already be achieved when a small ratio (~2%) of the generated hydrogen is used in situ for IA-to-MSA conversion. Moreover, the simulated coupled device produces MSA with much lower cumulative energy demand than conventional hydrogenation. Overall, the coupled hydrogenation concept offers an attractive approach to increase the viability of PEC water splitting while at the same time decarbonizing valuable chemical production.
Language	English
Publishing date	2023-02-22
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-023-36574-1
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Photocatalytic hydrogenation of acetophenone on a titanium dioxide cellulose film

Thiel, Tabea A. / Obata, Keisuke / Abdi, Fatwa F. / van de Krol, Roel / Schomäcker, Reinhard / Schwarze, Michael

RSC advances. 2022 Mar. 01, v. 12, no. 12

2022

Abstract: A previously developed sustainable immobilization concept for photocatalysts based on cellulose as a renewable support material was applied for the photocatalytic hydrogenation of acetophenone (ACP) to 1-phenyl ethanol (PE). Four different TiO₂ ... ...

Abstract	A previously developed sustainable immobilization concept for photocatalysts based on cellulose as a renewable support material was applied for the photocatalytic hydrogenation of acetophenone (ACP) to 1-phenyl ethanol (PE). Four different TiO₂ modifications (P25, P90, PC105, and PC500) were screened for the reaction showing good performance for PC25 and PC500. PC500 was selected for a detailed kinetic study to find the optimal operating conditions, and to obtain a better understanding of the photocatalytic pathway in relation to conventional and transfer hydrogenation. The kinetic data were analyzed using the pseudo-first-order reaction rate law. A complete conversion was obtained for ACP concentrations below 1 mM using a 360 nm filter and argon as the purge gas within 2–3 hours. High oxygen concentrations slow down or prevent the reaction, and wavelengths below 300 nm lead to side-products. By investigating the temperature dependency, an activation energy of 22 kJ mol⁻¹ was determined which is lower than the activation energies for conventional and transfer hydrogenation, because the light activation of the photocatalyst turns the endothermic to an exothermic reaction. PC500 was immobilized onto the cellulose film showing a 37% lower activity that remains almost constant after multiple use.
Keywords	acetophenones ; activation energy ; cellulose ; endothermy ; ethanol ; heat production ; hydrogenation ; oxygen ; photocatalysis ; photocatalysts ; temperature ; titanium dioxide
Language	English
Dates of publication	2022-0301
Size	p. 7055-7065.
Publishing place	The Royal Society of Chemistry
Document type	Article
ISSN	2046-2069
DOI	10.1039/d1ra09294d
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Article ; Online: Photocatalytic hydrogenation of acetophenone on a titanium dioxide cellulose film.

Thiel, Tabea A / Obata, Keisuke / Abdi, Fatwa F / van de Krol, Roel / Schomäcker, Reinhard / Schwarze, Michael

RSC advances

2022 Volume 12, Issue 12, Page(s) 7055–7065

Abstract	A previously developed sustainable immobilization concept for photocatalysts based on cellulose as a renewable support material was applied for the photocatalytic hydrogenation of acetophenone (ACP) to 1-phenyl ethanol (PE). Four different TiO
Language	English
Publishing date	2022-03-01
Publishing country	England
Document type	Journal Article
ISSN	2046-2069
ISSN (online)	2046-2069
DOI	10.1039/d1ra09294d
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Low-bias photoelectrochemical water splitting via mediating trap states and small polaron hopping.

Wu, Hao / Zhang, Lei / Du, Aijun / Irani, Rowshanak / van de Krol, Roel / Abdi, Fatwa F / Ng, Yun Hau

Nature communications

2022 Volume 13, Issue 1, Page(s) 6231

Abstract: Metal oxides are promising for photoelectrochemical (PEC) water splitting due to their robustness and low cost. However, poor charge carrier transport impedes their activity, particularly at low-bias voltage. Here we demonstrate the unusual effectiveness ...

Abstract	Metal oxides are promising for photoelectrochemical (PEC) water splitting due to their robustness and low cost. However, poor charge carrier transport impedes their activity, particularly at low-bias voltage. Here we demonstrate the unusual effectiveness of phosphorus doping into bismuth vanadate (BiVO
Language	English
Publishing date	2022-10-20
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-022-33905-6
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Article ; Online: Unraveling Electron Dynamics in p-type Indium Phosphide (100): A Time-Resolved Two-Photon Photoemission Study.

Diederich, Jonathan / Velasquez Rojas, Jennifer / Zare Pour, Mohammad Amin / Ruiz Alvarado, Isaac Azahel / Paszuk, Agnieszka / Sciotto, Rachele / Höhn, Christian / Schwarzburg, Klaus / Ostheimer, David / Eichberger, Rainer / Schmidt, Wolf Gero / Hannappel, Thomas / van de Krol, Roel / Friedrich, Dennis

Journal of the American Chemical Society

2024 Volume 146, Issue 13, Page(s) 8949–8960

Abstract: Renewable ("green") hydrogen production through direct photoelectrochemical (PEC) water splitting is a potential key contributor to the sustainable energy mix of the future. We investigate the potential of indium phosphide (InP) as a reference material ... ...

Abstract	Renewable ("green") hydrogen production through direct photoelectrochemical (PEC) water splitting is a potential key contributor to the sustainable energy mix of the future. We investigate the potential of indium phosphide (InP) as a reference material among III-V semiconductors for PEC and photovoltaic (PV) applications. The p(2 × 2)/c(4 × 2)-reconstructed phosphorus-terminated p-doped InP(100) (P-rich p-InP) surface is the focus of our investigation. We employ time-resolved two-photon photoemission (tr-2PPE) spectroscopy to study electronic states near the band gap with an emphasis on normally unoccupied conduction band states that are inaccessible through conventional single-photon emission methods. The study shows the complexity of the p-InP electronic band structure and reveals the presence of at least nine distinct states between the valence band edge and vacuum energy, including a valence band state, a surface defect state pinning the Fermi level, six unoccupied surface resonances within the conduction band, as well as a cluster of states about 1.6 eV above the CBM, identified as a bulk-to-surface transition. Furthermore, we determined the decay constants of five of the conduction band states, enabling us to track electron relaxation through the bulk and surface conduction bands. This comprehensive understanding of the electron dynamics in p-InP(100) lays the foundation for further exploration and surface engineering to enhance the properties and applications of p-InP-based III-V-compounds for,
Language	English
Publishing date	2024-03-19
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.3c12487
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Article: Elucidating the Pulsed Laser Deposition Process of BiVO4 Photoelectrodes for Solar Water Splitting

Kölbach, Moritz / Harbauer, Karsten / Ellmer, Klaus / van de Krol, Roel

Journal of physical chemistry. 2020 Feb. 04, v. 124, no. 8

2020

Abstract: BiVO4 thin films for use as photoelectrodes for solar water splitting are prepared by pulsed laser deposition (PLD), a powerful technique to synthesize compact multinary metal oxide films with high electronic quality. Here, the PLD process of BiVO4 films ...

Abstract	BiVO4 thin films for use as photoelectrodes for solar water splitting are prepared by pulsed laser deposition (PLD), a powerful technique to synthesize compact multinary metal oxide films with high electronic quality. Here, the PLD process of BiVO4 films by ablating a BiVO4 target is systematically elucidated, with a special focus on deviations from an ideal stoichiometric target-to-substrate material transfer. By correlating the V/Bi ratio of the films with their charge carrier transport properties and photoelectrochemical (PEC) performance, AM1.5 sulfite oxidation photocurrents of ∼2.4 mA cm–2 at E = 1.23 V vs reversible hydrogen electrode (RHE) with stoichiometric films are achieved without any deliberate doping or surface modification. In addition, we prepare BiVO4 photoelectrodes for the first time by alternating the ablation of Bi2O3 and V2O5 targets. This approach is found to be an attractive alternative route to control the cation stoichiometry and produces BiVO4 films that generate AM1.5 sulfite oxidation photocurrents of up to 2.6 mA cm–2 at E = 1.23 V vs RHE. Our results provide important insights into the PLD process of ternary oxide semiconductors and help to accelerate the synthesis and investigation of new multinary metal oxide photoelectrodes.
Keywords	bismuth ; cations ; electric current ; electrochemistry ; films (materials) ; hydrogen ; oxidation ; photochemistry ; photoelectrodes ; physical chemistry ; semiconductors ; stoichiometry ; sulfites
Language	English
Dates of publication	2020-0204
Size	p. 4438-4447.
Publishing place	American Chemical Society
Document type	Article
ISSN	1932-7455
DOI	10.1021/acs.jpcc.9b11265
Database	NAL-Catalogue (AGRICOLA)

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Article: Influence of Excess Charge on Water Adsorption on the BiVO₄(010) Surface

Wang, Wennie / Favaro, Marco / Chen, Emily / Trotochaud, Lena / Bluhm, Hendrik / Choi, Kyoung-Shin / van de Krol, Roel / Starr, David E. / Galli, Giulia

Journal of the American Chemical Society. 2022 Sept. 08, v. 144, no. 37

2022

Abstract: We present a combined computational and experimental study of the adsorption of water on the Mo-doped BiVO₄(010) surface, revealing how excess electrons influence the dissociation of water and lead to hydroxyl-induced alterations of the surface ... ...

Abstract	We present a combined computational and experimental study of the adsorption of water on the Mo-doped BiVO₄(010) surface, revealing how excess electrons influence the dissociation of water and lead to hydroxyl-induced alterations of the surface electronic structure. By comparing ambient pressure resonant photoemission spectroscopy (AP-ResPES) measurements with the results of first-principles calculations, we show that the dissociation of water on the stoichiometric Mo-doped BiVO₄(010) surface stabilizes the formation of a small electron polaron on the VO₄ tetrahedral site and leads to an enhanced concentration of localized electronic charge at the surface. Our calculations demonstrate that the dissociated water accounts for the enhanced V⁴⁺ signal observed in ambient pressure X-ray photoelectron spectroscopy and the enhanced signal of a small electron polaron inter-band state observed in AP-ResPES measurements. For ternary oxide surfaces, which may contain oxygen vacancies in addition to other electron-donating dopants, our study reveals the importance of defects in altering the surface reactivity toward water and the concomitant water-induced modifications to the electronic structure.
Keywords	X-ray photoelectron spectroscopy ; adsorption ; ambient pressure ; dissociation ; oxygen ; stoichiometry
Language	English
Dates of publication	2022-0908
Size	p. 17173-17185.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.2c07501
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Article: Revealing the relationship between photoelectrochemical performance and interface hole trapping in CuBi

Song, Angang / Levine, Igal / van de Krol, Roel / Dittrich, Thomas / Berglund, Sean P

Chemical science

2020 Volume 11, Issue 41, Page(s) 11195–11204

Abstract: ... p-Type ... ...

Abstract	p-Type CuBi
Language	English
Publishing date	2020-09-14
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/d0sc03030a
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Article ; Online: Solar-driven upgrading of biomass by coupled hydrogenation using in situ (photo)electrochemically generated H

Obata, Keisuke / Schwarze, Michael / Thiel, Tabea A / Zhang, Xinyi / Radhakrishnan, Babu / Ahmet, Ibbi Y / van de Krol, Roel / Schomäcker, Reinhard / Abdi, Fatwa F

Nature communications

2023 Volume 14, Issue 1, Page(s) 6017

Abstract: With the increasing pressure to decarbonize our society, green hydrogen has been identified as a key element in a future fossil fuel-free energy infrastructure. Solar water splitting through photoelectrochemical approaches is an elegant way to produce ... ...

Abstract	With the increasing pressure to decarbonize our society, green hydrogen has been identified as a key element in a future fossil fuel-free energy infrastructure. Solar water splitting through photoelectrochemical approaches is an elegant way to produce green hydrogen, but for low-value products like hydrogen, photoelectrochemical production pathways are difficult to be made economically competitive. A possible solution is to co-produce value-added chemicals. Here, we propose and demonstrate the in situ use of (photo)electrochemically generated H
Language	English
Publishing date	2023-09-27
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-023-41742-4
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Article ; Online: On the Origin of the OER Activity of Ultrathin Manganese Oxide Films.

Plate, Paul / Höhn, Christian / Bloeck, Ulrike / Bogdanoff, Peter / Fiechter, Sebastian / Abdi, Fatwa F / van de Krol, Roel / Bronneberg, Aafke C

ACS applied materials & interfaces

2021 Volume 13, Issue 2, Page(s) 2428–2436

Abstract: There is an urgent need for cheap, stable, and abundant catalyst materials for photoelectrochemical water splitting. Manganese oxide is an interesting candidate as an oxygen evolution reaction (OER) catalyst, but the minimum thickness above which ... ...

Abstract	There is an urgent need for cheap, stable, and abundant catalyst materials for photoelectrochemical water splitting. Manganese oxide is an interesting candidate as an oxygen evolution reaction (OER) catalyst, but the minimum thickness above which MnO
Language	English
Publishing date	2021-01-10
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.0c15977
Database	MEDical Literature Analysis and Retrieval System OnLINE

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