Article
Chemistry, Physical
Chenbiao Xu, Fei Xu, Xiao Chen, Zhenxing Li, Zhiwen Luan, Xingan Wang, Qing Guo, Xueming Yang
Summary: This study investigates the photoinduced water dissociation and desorption on a R-TiO2(110) surface at different wavelengths, revealing significant increases in the relative yield of H2O oxidation and desorption as the laser wavelength decreases. The results suggest that the energy of charge carriers plays a crucial role in these processes and challenge the widely accepted photocatalysis model of TiO2.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Moritz Eder, Martin Tschurl, Ueli Heiz
Summary: Heterogeneous photocatalytic systems are often described based on electrochemistry, while neglecting the surface chemistry of the photocatalyst. However, studies on alcohol photoreforming reveal that the electrochemical reaction model is not universally applicable. Therefore, the importance of thermal reactions and the need for systematic studies in different environments for a comprehensive understanding of photocatalysis are highlighted.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Manuel Caravaca, Jose Jorge Morales, Jose Abad
Summary: The interaction of nitrogen monoxide with silicon deposited onto a rutile single crystal surface was studied using XPS, UPS, and AES techniques. The results showed oxidation of titanium species and reduction of silicon species, with no detectable adsorbed nitrogen on the surface, suggesting a dissociative adsorption process characterized by a Freundlich isotherm.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Ji Young Hwang, Gun-hee Moon, Bupmo Kim, Takashi Tachikawa, Tetsuro Majima, Seungwoo Hong, Kangwoo Cho, Wooyul Kim, Wonyong Choi
Summary: The generation of mobile free OH radicals on anatase through a reductive conversion of dissolved O2 is crucial in achieving the mineralization of non-adsorbing substrates, while surface trapped holes lead to the generation of surface-bound OH radicals on both anatase and rutile. Understanding the production pathway of OH radicals in photocatalysis will help optimize their generation for efficient photocatalytic oxidation of pollutants.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Fangliang Li, Binli Wang, Xiao Chen, Weiwang Zeng, Rulin Sun, Xinlu Liu, Zefeng Ren, Xueming Yang, Hongjun Fan, Qing Guo
Summary: This study systematically investigated the photochemistry of toluene on a TiO2 catalyst, and found that ultraviolet light can efficiently activate the methyl C-H bond of toluene, forming stable intermediate adsorbed on specific sites until around room temperature. The DFT calculations further revealed that the photocatalytic C-H bond cleavage follows a homolytic manner. These findings provide insights into the photocatalytic functionalization of hydrocarbons on TiO2 catalysts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Philip Petzoldt, Moritz Eder, Sonia Mackewicz, Monika Blum, Tim Kratky, Sebastian Guenther, Martin Tschurl, Ueli Heiz, Barbara A. J. Lechner
Summary: In this study, the effect of O-2 and H-2 on Pt/TiO2(110) catalysts was investigated using synchrotron-based near-ambient pressure X-ray photoelectron spectroscopy. The results showed that the rate of formation of the encapsulating oxide layer on Pt particles varied with different O-2 pressures, and once encapsulation occurred, Pt particles remained embedded in the support.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Philip Petzoldt, Moritz Eder, Sonia Mackewicz, Monika Blum, Tim Kratky, Sebastian Guenther, Martin Tschurl, Ueli Heiz, Barbara A. J. Lechner
Summary: The study shows that O-2 and H-2 have a significant impact on the SMSI state of Pt/TiO2 catalysts, with encapsulating oxide layer forming more rapidly at low O-2 pressures, but less effectively at higher pressures. The oxidation/reduction of Pt particles is reversible, but once encapsulated, they remain embedded in the support.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Xiufeng Lang, Lei Chen, Yan Zhu, Xiaoxu Liu, Hao Guo, Tingting You, Hongsheng Zhang
Summary: Recent experiments have shown that the efficiency of the oxygen evolution reaction (OER) can be greatly improved in fluorinated TiO2 by forming surface hydrogen bonds, but the mechanism is not yet clear. In this study, dual OER pathways on the fluorinated anatase TiO2(101) surface were investigated using first-principles calculations. It was found that dual H-bonding water molecules play a significant role in facilitating proton transfer and hole trapping in both pathways.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Xiao Tong, Scott P. Price, Jeremy C. Robins, Claron Ridge, Hyun You Kim, Paul Kemper, Horia Metiu, Michael T. Bowers, Steven K. Buratto
Summary: In this study, the adsorption behavior of H2O on a TiO2 surface decorated with VO clusters was investigated using UHV-STM and TPD techniques. The results reveal that the preadsorbed VO clusters can induce the adsorption of H2O molecules at room temperature, forming strings of H2O dimers. This adsorption behavior is reversible and unique to the VO-decorated TiO2 surface.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Bing Fu, Zhijiao Wu, Kai Guo, Lingyu Piao
Summary: A simple and environmentally friendly synthetic method was developed to synthesize regulable reductive and oxidative facets of rutile TiO2 single crystals. Sodium fluoride and glycolic acid played crucial roles in this process, serving as effective phase and facet controlling agents.
Article
Chemistry, Physical
Long Chen, R. Scott Smith, Bruce D. Kay, Zdenek Dohnalek
Summary: The reaction pathways of glycerol on TiO2(110) involve the production of water, hydrogen, and carbon-containing products, with the C-H bond scission channel identified as the primary pathway for hydrogen evolution. The study also suggests that smaller oxygenates are not suitable models for probing the reaction pathways of larger oxygenates on oxide surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Jessica Kraeuter, Katharina Al-Shamery
Summary: Systematic model investigations have shown that defects, particularly bulk Ti3+ interstitials, play a crucial role in directing reactions of alcohols and aldehydes on rutile Titania. The coadsorption with oxygen can enhance certain reaction paths. In the presence of high defect densities, a stabilisation of acetone on the surface by the formation of a diolate was observed.
Article
Chemistry, Physical
Kasidid Yaemsunthorn, Wiktoria Adamowicz, Marcin Kobielusz, Wojciech Macyk
Summary: The photocatalytic selective reduction of 3-nitrophenol to 3-aminophenol was studied using titanium dioxide in different compositions. Both intrinsic and extrinsic parameters were found to affect the reaction progress, with intrinsic factors related to the chemical, structural, and electronic properties and extrinsic factors related to the reaction conditions. The analysis revealed that the performance of anatase and rutile materials varied due to differences in interfacial electron transfer, charge recombination, reduction driving force, and methanol photooxidation efficiency. The understanding of these factors could lead to the rational design of efficient and selective photocatalysts.
Article
Materials Science, Multidisciplinary
Fatemehsadat Moosavi, Alex Lemarchand, Cyrille Bazin, Maria Konstantakopoulou, Mathieu Fregnaux, Christophe Colbeau-Justin, Touraj Tavakoli Gheinani, Andrei Kanaev, Mehrdad Nikravech
Summary: Nanocomposite TiO2 coatings with mixed anatase-rutile crystalline polymorphs and strong adherence to glass substrates were prepared using a spray-plasma deposition method. The coating exhibited enhanced photocatalytic activity for cefixime antibiotic decomposition under UVA light illumination, and the activity significantly increased after the formation of the rutile phase, suggesting a synergistic effect of the two-component solids.
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
(2022)
Article
Chemistry, Multidisciplinary
Zhi-Wen Wang, Wei-Guang Chen, Da Teng, Jie Zhang, An-Ming Li, Zhao-Han Li, Ya-Nan Tang
Summary: The study shows that external uniaxial strain can significantly reduce the energy barrier for water dissociation on the reduced rutile TiO2(110) surface, especially when the tensile strain is larger than 3%. Additionally, the mechanism of water dissociation changes under certain conditions, indicating the feasibility of engineering water dissociation on this surface using external strain.
Review
Chemistry, Multidisciplinary
Rachel Crespo-Otero, Quansong Li, Lluis Blancafort
CHEMISTRY-AN ASIAN JOURNAL
(2019)
Article
Biochemistry & Molecular Biology
Christopher Grieco, Forrest R. Kohl, Yuyuan Zhang, Sangeetha Natarajan, Lluis Blancafort, Bern Kohler
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2019)
Article
Chemistry, Multidisciplinary
Josep Albero, Alfonso Vidal, Annapaola Migani, Patricia Concepcion, Lluis Blancafort, Hermenegildo Garcia
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2019)
Article
Chemistry, Multidisciplinary
Jaume Garcia-Amoros, Benjamin Maerz, Marta Reig, Alba Cuadrado, Lluis Blancafort, Elena Samoylova, Dolores Velasco
CHEMISTRY-A EUROPEAN JOURNAL
(2019)
Article
Chemistry, Physical
Christopher Grieco, Alex T. Hanes, Lluis Blancafort, Bern Kohler
JOURNAL OF PHYSICAL CHEMISTRY A
(2019)
Article
Chemistry, Multidisciplinary
Lucia Viglianti, Ni Xie, Herman H. Y. Sung, Alexander A. Voityuk, Nelson L. C. Leung, Yujie Tu, Clara Baldoli, Ian D. Williams, Ryan T. K. Kwok, Jacky W. Y. Lam, Emanuela Licandro, Lluis Blancafort, Ben Zhong Tang
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Physical
Maria A. Trachsel, Susan Blaser, Simon Lobsiger, Luca Siffert, Hans-Martin Frey, Lluis Blancafort, Samuel Leutwyler
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2020)
Article
Nanoscience & Nanotechnology
Ivan Djordjevic, Gautama Wicaksono, Ivan Solic, Juhi Singh, Tanvi Sushil Kaku, Sierin Lim, Elwin Wei Jian Ang, Lluis Blancafort, Terry W. J. Steele
Summary: Carbene-based macromolecules offer a new approach to biomaterials with stimuli-sensitive properties, using visible light to activate diazirine-to-carbene cross-linking without UVA limitations. Through the use of photocatalysts and light doses, the speed and quality of the transition from liquid to biorubber can be controlled. Experimental results with CaproGlu demonstrate strong adhesion and low toxicity, showing potential for various biomedical applications.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Jun Wang, Lluis Blancafort
Summary: Eumelanin, composed of 5,6-dihydroxyindole (DHI) oligomers, is responsible for photoprotection in living organisms. A preference for oxidized, polycyclic structures has been found, along with stable structures involving quinone oxidation patterns, interfragment double bonds, and zwitterionic resonance structures. Melanin models will need to cover this structural diversity, with some stable oxidized dimers having low absorption energies that may contribute to the biopolymer's absorption spectrum.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Neville J. A. Coughlan, Mark H. Stockett, Christina Kjaer, Eleanor K. Ashworth, Philip C. Bulman Page, Stephen R. Meech, Steen Brondsted Nielsen, Lluis Blancafort, W. Scott Hopkins, James N. Bull
Summary: Incorporation of fluorescent proteins into biochemical systems has revolutionized bioimaging. A study on the red Kaede fluorescent protein chromophore in the gas phase revealed three isomers, highlighting the need for isomer-selective methods in studying biochromophores.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Junkai Liu, Haoke Zhang, Lianrui Hu, Jun Wang, Jacky W. Y. Lam, Lluis Blancafort, Ben Zhong Tang
Summary: This study reveals a new strategy for the luminescence mechanism of tetraphenylethylene, providing a quantitative understanding of the through-space interaction and establishing a theoretical solid-state model, expanding the understanding of molecular behavior.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Xueqing Wang, Lilia Kinziabulatova, Marco Bortoli, Anju Manickoth, Marisa A. Barilla, Haiyan Huang, Lluis Blancafort, Bern Kohler, Jean-Philip Lumb
Summary: Melanins are biopolymers produced from phenols and catechols that provide various functions such as photoprotection, pigmentation, and redox activity. The chemical structures of melanins remain unknown, hindering the design of synthetic materials with specific properties. However, the stabilization of indole-5,6-quinone (IQ) derivatives has allowed the exploration of eumelanin's unique electronic and optical properties, which can contribute to the development of melanin-inspired materials.
Article
Chemistry, Physical
Eleanor K. Ashworth, Min-Hsien Kao, Cate S. Anstoeter, Gerard Riesco-Llach, Lluis Blancafort, Kyril M. Solntsev, Stephen R. Meech, Jan R. R. Verlet, James N. Bull
Summary: This study investigates the photophysical properties of three alkylated derivatives of the chromophore in GFP, using time-resolved photoelectron imaging in the gas phase and femtosecond fluorescence upconversion in water. The results show that the alkylated positions and conformations have an impact on the excited state lifetimes in the gas phase, while the solvent affects the lifetimes in water and ethanol.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Daniel Bosch, Jun Wang, Lluis Blancafort
Summary: This study successfully models the stability and optical absorption of Eumelanin using deep neural networks, addressing the structural challenge of Eumelanin.
Article
Chemistry, Physical
Iker Lamas, Raul Montero, Virginia Martinez-Martinez, Asier Longarte, Lluis Blancafort
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2020)