document

Promoting Photocatalytic Activity of NH₂-MIL-125(Ti) for H₂ Evolution Reaction through Creation of Ti^III- and Co^I-Based Proton Reduction Sites

Kavun, Vitalii (author), Uslamin, E. (author), van der Linden, B. (author), Canossa, Stefano (author), Goryachev, A. (author), Bos, Emma E. (author), Garcia Santaclara, J. (author), Smolentsev, Grigory (author), Repo, Eveliina (author), van der Veen, M.A. (author)

Titanium-based metal-organic framework, NH2-MIL-125(Ti), has been widely investigated for photocatalytic applications but has low activity in the hydrogen evolution reaction (HER). In this work, we show a one-step low-cost postmodification of NH2-MIL-125(Ti) via impregnation of Co(NO3)2. The resulting Co@NH2-MIL-125(Ti) with embedded single...

journal article 2023

document

Continuous Fatty Acid Decarboxylation using an Immobilized Photodecarboxylase in a Membrane Reactor

Zhou, Jianle (author), Hollmann, F. (author), He, Qi (author), Chen, Wen (author), Ma, Yunjian (author), Wang, Yonghua (author)

The realm of photobiocatalytic alkane biofuel synthesis has burgeoned recently; however, the current dearth of well-established and scalable production methodologies in this domain remains conspicuous. In this investigation, we engineered a modified form of membrane-associated fatty acid photodecarboxylase sourced from Micractinium conductrix...

journal article 2023

document

Exciting Enzymes: Current State and Future Perspective of Photobiocatalysis

Alphand, Véronique (author), van Berkel, Willem J.H. (author), Jurkaš, Valentina (author), Kara, Selin (author), Kourist, Robert (author), Kroutil, Wolfgang (author), Mascia, Francesco (author), Nowaczyk, Marc M. (author), Paul, C.E. (author)

The recent increase of interest in photocatalysis spread to biocatalysis and triggered a rush for the development of light-dependent enzyme-mediated or enzyme-coupled processes. After several years of intense research on photobiocatalysis, it is time to evaluate the state of the field in a structured manner. In this Perspective, we suggest to...

journal article 2023

document

3D-Printed Metal–Organic Framework-Derived Composites for Enhanced Photocatalytic Hydrogen Generation

Hussain, M.Z. (author), Großmann, Paula F. (author), Kohler, Fabian (author), Kratky, Tim (author), Kronthaler, Laura (author), van der Linden, B. (author), Rodewald, Katia (author), Rieger, Bernhard (author), Fischer, Roland A. (author), Xia, Yongde (author)

Direct ink writing technique is used to 3D print Ti-metal–organic framework (MOF) NH₂-MIL-125 mixed with boehmite dispersal. Pt is also deposited onto 3D-printed monolith using atomic layer deposition (ALD) to offer additional catalytic sites. The Ti-MOF-derived powder sample and the pyrolyzed 3D-printed monolith samples are...

journal article 2022

document

Mechanistic insight into the improved photocatalytic degradation of dyes for an ultrathin coating of SiO₂ on TiO₂ (P25) nanoparticles

Benz, D. (author), Van Bui, Hao (author), Hintzen, H.T.J.M. (author), Kreutzer, M.T. (author), van Ommen, J.R. (author)

The photocatalytic mechanism of TiO₂ (P25) nanoparticles coated with SiO₂ (SiO₂:TiO₂) by atomic layer deposition was investigated. The deposition of SiO₂ on TiO₂ not only gives a photocatalytic improvement for the degradation of both Rhodamine B (3.6–fold) and Acid Blue 9 (3...

journal article 2022

document

Intensification of Photobiocatalytic Decarboxylation of Fatty Acids for the Production of Biodiesel

Duong, Hong T. (author), Wu, Y. (author), Sutor, Alexander (author), Burek, Bastien O. (author), Hollmann, F. (author), Bloh, Jonathan Z. (author)

Light-driven biocatalytic processes are notoriously hampered by poor penetration of light into the turbid reaction media. In this study, wirelessly powered light-emitting diodes are found to represent an efficient and scalable approach for process intensification of the photobiosynthetic production of diesel alkanes from renewable fatty acids...

journal article 2021

document

Surface functionalized N-C-TiO₂/C nanocomposites derived from metal-organic framework in water vapour for enhanced photocatalytic H₂ generation

Hussain, Mian Zahid (author), Yang, Zhuxian (author), van der Linden, B. (author), Huang, Zheng (author), Jia, Quanli (author), Cerrato, Erik (author), Fischer, Roland A. (author), Kapteijn, F. (author), Zhu, Yanqiu (author), Xia, Yongde (author)

Surface-functionalized nitrogen/carbon co-doped polymorphic TiO₂ phase junction nanoparticles uniformly distributed in porous carbon matrix were synthesized by a simple one-step pyrolysis of titanium based metal–organic framework (MOF), NH₂-MIL-125(Ti) at 700 °C under water vapour atmosphere. Introducing water vapour...

journal article 2021

document

3D Printed Scaffolds for Monolithic Aerogel Photocatalysts with Complex Geometries

Schreck, Murielle (author), Kleger, Nicole (author), Matter, Fabian (author), Kwon, Junggou (author), Tervoort, Elena (author), Masania, K. (author), Studart, André R. (author), Niederberger, Markus (author)

Monolithic aerogels composed of crystalline nanoparticles enable photocatalysis in three dimensions, but they suffer from low mechanical stability and it is difficult to produce them with complex geometries. Here, an approach to control the geometry of the photocatalysts to optimize their photocatalytic performance by introducing carefully...

journal article 2021

document

Tuning electron transfer by crystal facet engineering of BiVO₄ for boosting visible-light driven photocatalytic reduction of bromate

Liu, Guoshuai (author), Zhu, Yukun (author), Yan, Qun (author), Wang, Han (author), Wu, Peng (author), Shen, Yaoliang (author), Doekhi-Bennani, Y. (author)

Removal of bromate (BrO₃⁻) has gained increasing attention in drinking water treatment process. Photocatalysis technology is an effective strategy for bromate removal. During the photocatalytic reduction of bromate process, the photo-generated electrons are reductive species toward bromate reduction and photo-generated...

journal article 2021

document

Modifying TiO2 Nanoparticles by Atomic Layer Deposition for Enhanced Photocatalytic Water Purification

Benz, D. (author)

Photocatalysts, contrary to conventional catalysts, utilize light to drive a reaction. By absorption of photons, electrons are excited and reach higher states to initiate a redox reaction. This principle can be broadly used to produce chemicals such as hydrogen via the reduction of water or transform carbon dioxide into solar fuels, i.e.,...

doctoral thesis 2020

document

PEM Electrolysis-Assisted Catalysis Combined with Photocatalytic Oxidation towards Complete Abatement of Nitrogen-Containing Contaminants in Water

Ampurdanés, Jordi (author), Bunea, S. (author), Urakawa, A. (author)

Electrolysis-assisted nitrate (NO₃⁻) reduction is a promising approach for its conversion to harmless N₂ from waste, ground, and drinking water due to the possible process simplicity by in-situ generation of H₂/H/H⁺ by water electrolysis and to the flexibility given by tunable redox...

journal article 2020

document

Multitarget evaluation of the photocatalytic activity of P25-SiO₂ prepared by atomic layer deposition

Martín-Sómer, Miguel (author), Benz, D. (author), van Ommen, J.R. (author), Murugán, Javier (author)

This work presents the evaluation of the photocatalytic activity of P25 TiO₂ particles, coated with SiO₂, using atomic layer deposition (ALD) for the photocatalytic removal of methylene blue, oxidation of methanol and inactivation of Escherichia coli bacteria in water and its comparative evaluation with bare P25 TiO<sub...

journal article 2020

document

Photoenzymatic Production of Next Generation Biofuels from Natural Triglycerides Combining a Hydrolase and a Photodecarboxylase

Ma, Yunjian (author), Zhang, Xizhen (author), Zhang, W. (author), Li, Peilin (author), Li, Yongru (author), Hollmann, F. (author), Wang, Yonghua (author)

A photobiocatalytic cascade transforming natural triglycerides into alkanes/alkenes is proposed. Starting from natural triglycerides, free fatty acids have been obtained using lipases. The free fatty acids were then, in a photoenzymatic step, decarboxylated into the C1-shortened alkanes using a recently described photodecarboxylase from...

journal article 2020

document

Synthesis of a rationally designed multi-component photocatalyst pt:Sio₂:Tio₂ (p25) with improved activity for dye degradation by atomic layer deposition

Benz, D. (author), Bui, Hao Van (author), Hintzen, H.T.J.M. (author), Kreutzer, M.T. (author), van Ommen, J.R. (author)

Photocatalysts for water purification typically lack efficiency for practical applications. Here we present a multi-component (Pt:SiO₂:TiO₂ (P25)) material that was designed using knowledge of reaction mechanisms of mono-modified catalysts (SiO₂:TiO₂, and Pt:TiO₂ ) combined with the...

journal article 2020

document

Optimizing photon utilization in LED-based photocatalytic reactors

Khodadadian, F. (author)

Photocatalysis involves the absorption of photons by a semiconductor to enhance chemical reactions. Examples of important applications include the degradation of hazardous chemicals, reduction of carbon dioxide to valuable chemicals and (partial) oxidation of hydrocarbons. Despite many successful demonstrations of this technology at lab-scale,...

doctoral thesis 2019

document

Expanding the Spectrum of Light-Driven Peroxygenase Reactions

Willot, S.J. (author), Fernandez Fueyo, E. (author), Tieves, F. (author), Pesic, M. (author), Alcalde, Miguel (author), Arends, I.W.C.E. (author), Park, Chan Beum (author), Hollmann, F. (author)

Peroxygenases require a controlled supply of H₂O₂ to operate efficiently. Here, we propose a photocatalytic system for the reductive activation of ambient O₂ to produce H₂O₂ which uses the energy provided by visible light more efficiently based on the combination of wavelength...

journal article 2019

document

Photoenzymatic Hydroxylation of Ethylbenzene Catalyzed by Unspecific Peroxygenase: Origin of Enzyme Inactivation and the Impact of Light Intensity and Temperature

Burek, Bastien O. (author), de Boer, Sabrina R. (author), Tieves, F. (author), Zhang, W. (author), van Schie, M.M.C.H. (author), Bormann, Sebastian (author), Alcalde, Miguel (author), Holtmann, Dirk (author), Hollmann, F. (author)

Photoenzymatic cascades can be used for selective oxygenation of C−H-Bonds under mild conditions circumventing the hydrogen peroxide mediated peroxygenase inactivation via in situ H₂O₂ generation. Here, we report the “on demand” production of hydrogen peroxide via methanol assisted reduction of molecular oxygen using UV...

journal article 2019

document

Water purification in a solar reactor incorporating TiO₂ coated mesh structures

Elkalliny, A.S.M. (author), Rivandi, Alireza H. (author), Uzun, S. (author), van Ommen, J.R. (author), Nugteren, H.W. (author), Rietveld, L.C. (author), Appel, P.W. (author)

The rate of photocatalytic oxidation of contaminants in drinking water using an immobilized catalyst can be increased by properly designing the catalyst structure. By creating a solar reactor in which meshes coated with TiO₂ were stacked, we demonstrated that degradation of humic acids with four superimposed stainless steel meshes...

journal article 2019

document

Cascading g-C₃N₄ and Peroxygenases for Selective Oxyfunctionalization Reactions

van Schie, M.M.C.H. (author), Zhang, W. (author), Tieves, F. (author), Choi, Da Som (author), Park, Chan Beum (author), Burek, Bastien O. (author), Bloh, Jonathan Z. (author), Arends, I.W.C.E. (author), Paul, C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)

Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H₂O₂ can be addressed via in situ generation of H₂O<sub>2<...

journal article 2019

document

Photocatalytic activity of functionalized nanodiamond-TiO₂ composites towards water pollutants degradation under UV/Vis irradiation

Pastrana-Martínez, Luisa M. (author), Morales-Torres, Sergio (author), Carabineiro, Sónia A.C. (author), Buijnsters, J.G. (author), Figueiredo, José L. (author), Silva, Adrián M.T. (author), Faria, Joaquim L. (author)

Pristine nanodiamonds (NDs) obtained by detonation, or functionalized by different treatments, namely oxidation, hydrogenation and amination, were used to synthesize composites by insertion in TiO₂ matrixes. The different treatments of the NDs lead to materials containing diverse texture properties and surface chemistry...

journal article 2018