Article
Chemistry, Physical
Lan Lan, Helen Daly, Rehana Sung, Floriana Tuna, Nathan Skillen, Peter K. J. Robertson, Christopher Hardacre, Xiaolei Fan
Summary: This study investigated the mechanistic details of glucose photoreforming over TiO2 and Pt/m-TiO2 catalysts. The alpha-scission mechanism of glucose oxidation was confirmed by the formation of arabinose and formic acid in the initial oxidation step. The selectivity to sugar products and formic acid differed over Pt/TiO2 and TiO2, with Pt/TiO2 showing lower selectivity to formic acid due to enhanced adsorption/conversion. In situ ATR-IR spectroscopy revealed the presence of molecular formic acid and formate on the surface of both catalysts, suggesting the dominance of formic acid oxidation in glucose photoreforming.
Article
Chemistry, Multidisciplinary
Keri A. Steiniger, Matthew C. Lamb, Tristan H. Lambert
Summary: This study presents a method for C-(sp(3))-C-(sp(3)) cross-coupling of amines. Primary amines are transformed into 1,2-dialkyldiazenes by reacting with O-nosylhydroxylamines in the presence of atmospheric oxygen. The denitrogenation of diazenes using an iridium photocatalyst forms the C-C bond. The substrate scope is broad, allowing for various functional groups, such as heteroaromatics and unprotected alcohols and acids.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Chemical
Sifan Jia, Xin Shu, Hongyan Song, Zhe An, Xu Xiang, Jian Zhang, Yanru Zhu, Jing He
Summary: This study introduces Au/anatase-rutile TiO2 photocatalysts for selective dehydrogenation of ethanol under mild conditions, providing insights into the ethanol photocatalytic mechanism. The investigation reveals that different types of TiO2 in the catalyst dominate the activation of O-H bonds and facilitate the generation of DEE. Au nanoparticles distributed at the TiO2 interface show enhanced electron-hole separation efficiency, leading to improved photocatalytic activity for ethanol selective dehydrogenation. This research is crucial for understanding the reaction mechanism of photocatalytic ethanol conversion.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Physical
Hui Zhang, Jiale Yao, Xinyue Zhang, Chengyu Fu, Yaping Miao, Yani Guo, Zhi Tong, Ningtao Mao
Summary: A ternary component photocatalyst was created by incorporating peptide chains of wool keratin between T i3C2Tx nanosheets and TiO2 nanoparticles. The photocatalytic properties of the composite were evaluated and the calcined composite showed significantly better activity. The composite exhibited adsorption-mediated photocatalytic degradation while the calcined composite showed charge transfer-mediated degradation.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Shaeel Ahmed Althabaiti, Zaheer Khan, Katabathini Narasimharao, Salem Mohamed Bawaked, Soad Zahir Al-Sheheri, Mohamed Mokhtar, Maqsood Ahmad Malik
Summary: An Ag-modified TiO2 nanomaterial was synthesized using a one-pot method. The structure and morphology of the synthesized material were determined using X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The results showed that the addition of metallic Ag nanoparticles decreased the optical band gap and photoluminescence intensity of TiO2, while increasing the Raman peak intensity and absorbance. The Ag-modified TiO2 nanomaterial exhibited higher photocatalytic efficiency than bare TiO2 and Ag metal NPs, attributed to the synergistic effect between Ag metal and TiO2 structures.
Article
Engineering, Environmental
Andreina Garcia, Maibelin Rosales, Minju Thomas, Giovanni Golemme
Summary: Versatile materials for oxidizing As(III) into less hazardous As(V) species have attracted increasing attention. Ti-SBA-15, prepared by coating 7% anatase TiO2 on pre-formed SBA-15, showed efficient adsorption and photo-oxidation of As(III) at different pHs. The presence of TiO2 on SBA-15 promoted reactive oxygen species generation, leading to successful oxidation of As(III). Despite covering only a small percentage of the surface, TiO2 exhibited unprecedented photocatalytic behavior, making it a prominent catalyst for arsenic removal from water.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Chemistry, Physical
Weizi Zhang, Qinfang Li, Haian Xia
Summary: In this work, Ag or Au monometallic nanoparticles and bimetallic Au-Ag nanoparticles supported on TiO2 were prepared. The incorporation of Au NPs into Ag NPs could tune their d-band centers to upshift toward the Fermi Level. The bimetallic catalysts exhibited narrower bandgap energies, better efficiencies in charge separation and transfer, and higher catalytic activities compared to monometallic catalysts.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Chunling Bo, Jing Liu, Yutong Zhang, Huaiqiu Chang, Xinyi Zhang, Xinfeng Liu, Chunying Chen, Lingyu Piao
Summary: This study proposes a photocatalytic system using brookite mesoporous titanium dioxide and methanotrophs to directly convert methane into methanol. The system achieves high activity, selectivity and stability at ambient temperature and pressure, with a methanol production rate of 15,761 μmol g-1 h-1, which is dozens of times higher than previous research. The process achieves nearly 100% selectivity and excellent stability without any cocatalysts, sacrificial agents or inhibitors. The compatibility of semiconductor materials and the contact mode with methanotrophs play a significant role in the process.
Article
Chemistry, Multidisciplinary
Giulio Latini, Matteo Signorile, Francesca Rosso, Andrea Fin, Marta D'Amora, Silvia Giordani, Fabrizio Pirri, Valentina Crocella, Silvia Bordiga, Sergio Bocchini
Summary: Choline/amino acid-based ionic liquids were synthesized through ionic metathesis and their CO2 absorption properties were evaluated using various experimental approaches. These ILs demonstrated high molar uptakes and the ability to release CO2 under mild conditions, while also showing non-toxicity and high biocompatibility in zebrafish studies.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Chemistry, Analytical
Daniel Kopp, Kevin Blinn, Haohan Wu, Qinghua Li, Asad J. Mughal, Michael Sender, Bahram Jadidian, Richard E. Riman
Summary: In-situ reaction monitoring using ATR-IR was employed to investigate the carbonation kinetics of wollastonite powder compacts under hydrothermal conditions. The study revealed a rapid reaction onset followed by two distinct slower decaying regimes for carbonate formation.
VIBRATIONAL SPECTROSCOPY
(2022)
Article
Chemistry, Multidisciplinary
Xinhua Windt, Elinor L. Scott, Thorsten Seeger, Oliver Schneider, Akbar Asadi Tashvigh, Johannes H. Bitter
Summary: This study presents a new approach using FTIR spectroscopy to detect the structural changes of feather keratin and its availability for enzymatic hydrolysis induced by the TPH process. The FTIR technique provides rapid information about the changes during TPH and can be used for process control and optimization.
Article
Chemistry, Applied
Sang-Chul Jung, Kyong-Hwan Chung, Jaewook Choi, Young-Kwon Park, Sun-Jae Kim, Byung-Joo Kim, Heon Lee
Summary: This paper proposes a method for mass-producing hydrogen from ammonia water by applying a liquid phase plasma discharge technique and a photocatalyst. By preparing N/Fe/TiO2 photocatalysts and applying them as visible light-sensitive photocatalysts, efficient decomposition of ammonia water and high hydrogen evolution rate were achieved.
Article
Chemistry, Multidisciplinary
Wen -Fang Song, Wei-Qin Yao, Qi-Wen Chen, Diwei Zheng, Zi-Yi Han, Xian-Zheng Zhang
Summary: This study developed a bioorthogonal-mediated bacterial delivery strategy to enhance the colonization of probiotics by modulating bacterial adhesion between probiotics and gut inhabitants, thereby improving the clinical treatment efficacy of oral bacterial therapy.
ACS CENTRAL SCIENCE
(2022)
Article
Chemistry, Physical
Tingcha Wei, Juan Xu, Caixia Kan, Le Zhang, Xingzhong Zhu
Summary: The study focuses on the construction of a g-C3N4/TiO2 heterostructure with tailored Au nanoparticles for efficient charge separation in photocatalysis. The enhanced charge separation leads to excellent photocatalytic activity for pollutant degradation and water splitting, with superoxide radicals identified as playing a crucial role in the catalytic process. Insights into the distinct roles of Au in heterostructure for significantly enhanced charge separation are provided, paving the way for the design of high-efficiency heterostructure photocatalysts with noble metal decoration.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Crystallography
Martina Novotna, Petr Knotek, Tomas Hanzlicek, Petr Kutalek, Ivana Perna, Klara Melanova, Eva Cernoskova, Katerina Kopecka
Summary: This study investigates the photocatalytic activity of three types of industrially produced TiO2 powder incorporated into a geopolymer matrix, along with their pure counterparts, revealing that the geopolymer matrix works well as a supporting material for pure TiO2 powders with better properties. These findings suggest the potential use of these materials in advanced composites for wastewater treatment or air purification, based on their enhanced photocatalytic activity.
Article
Chemistry, Multidisciplinary
Michal Swierczewski, Thomas Burgi
Summary: Recently, there has been a shift towards using hydrophobic gold and silver nanoparticles as the preferred choice for transferring monolayers onto solid substrates. The interactions between the particles in the absence of polar groups include dispersive attractions from the metal cores, repulsions between ligand shells, and weaker entropic factors. The article explores the evolution of the monolayers, the role of different particle and solution properties, and strategies to enhance their mechanical stability and improve their applicability in the industry.
Article
Materials Science, Multidisciplinary
Maciej Lipok, Patryk Obstarczyk, Sylwia Parzyszek, Yanan Wang, Maciej Baginski, Thomas Buergi, Wiktor Lewandowski, Joanna Olesiak-Banska
Summary: This study proposes a new approach to assemble atomically precise gold nanoclusters into helical nanofilaments using a liquid-crystal template, enabling circularly polarized luminescence. The findings demonstrate that double functionalization and the use of a liquid crystal matrix can successfully assemble ultrasmall particles and tune their optical properties.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Carin R. Lightner, Filip Desmet, Daniel Gisler, Stefan A. Meyer, Ariel Francis Perez Mellor, Hannah Niese, Arnulf Rosspeintner, Robert C. Keitel, Thomas Burgi, Wouter A. Herrebout, Christian Johannessen, David J. Norris
Summary: Spectroscopic techniques can provide information about the chiral structure of molecules, but small errors in optical polarization control can lead to experimental artifacts. This study focuses on Raman optical activity (ROA) as an example and comprehensively investigates chiroptical artifacts. Based on the findings, standard controls are proposed to help researchers better understand, identify, and avoid experimental artifacts.
Article
Chemistry, Multidisciplinary
Ke-Feng Zhang, Nidal Saleh, Michal Swierczewski, Arnulf Rosspeintner, Francesco Zinna, Gennaro Pescitelli, Celine Besnard, Laure Guenee, Thomas Burgi, Jerome Lacour
Summary: A chiral bispyrene macrocycle was synthesized for intermolecular excimer fluorescence upon aggregation using a double hydrothiolation method followed by intramolecular oxidation. High stereoselectivity was achieved for the thiol-ene additions under templated conditions. The structural evolution upon aggregation was monitored by ECD/CPL.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xianwei Wang, Thomas Buergi
Summary: Knowledge of the reaction mechanism is essential for catalyst improvement. Traditionally, mechanistic studies have focused on structure and reaction conditions, neglecting the time dimension. In this study, time-resolved infrared spectroscopy coupled with modulation excitation spectroscopy was used to demonstrate the influence of time on the mechanism of CO oxidation over Au/TiO2. A dual catalytic mechanism was identified, with CO and TiO2 playing key roles at different stages of the reaction. These findings highlight the importance of studying short-time kinetics for mechanistic studies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Abolfazl Ziarati, Jiangtao Zhao, Jafar Afshani, Rania Kazan, Ariel Perez Mellor, Arnulf Rosspeintner, Siobhan McKeown, Thomas Burgi
Summary: Controllable CO2 reduction selectivity can be achieved by tuning the architecture of the photocatalyst. A planar structure (p Au/CN) showed high selectivity for HER with 87%, while a yolk@shell structure (Y@S Au@CN) exhibited high selectivity of carbon products by suppressing the HER to 26%. Further improvement was achieved by surface decorating the yolk@shell structure with Au-25(PET)(18) clusters, resulting in longer charge separation. The optimized Au@CN/Au-c/G Y@S structure achieved high photocatalytic CO2RR selectivity of 88%.
Article
Chemistry, Multidisciplinary
Vera Truttmann, Adea Loxha, Rares Banu, Ernst Pittenauer, Sami Malola, Maria Francisca Matus, Yuchen Wang, Elizabeth A. Ploetz, Guenther Rupprechter, Thomas Burgi, Hannu Hakkinen, Christine Aikens, Noelia Barrabes
Summary: Chiral gold nanoclusters were synthesized using the chiral ligand 2-MeBuSH, leading to the unexpected formation of enantiopure chiral clusters. The chiral activity of Au-144 was found to be stronger than Au-38 or Au-25, as confirmed by experimental evaluation using circular dichroism spectroscopy. The prepared chiral clusters exhibited stability against diastereoisomerization up to temperatures of 80°C. These findings demonstrate the selective preparation of enantiopure, intrinsically chiral, and highly stable thiolate-protected Au nanoclusters, supporting the predicted super chirality in the Au-144 cluster.
Article
Chemistry, Multidisciplinary
Daniele Rosa-Gastaldo, Marion Pupier, Giorgi Meshvildishvili, Jasmine Viger-Gravel, Thomas Burgi
Summary: Ligand and metal exchange reactions are important for shaping the properties of metal nanoclusters, and understanding the dynamics of the ligand monolayer is crucial for functionalization. Through experiments and simulations, we determined the activation parameters for an intracluster ligand rearrangement in specific clusters, revealing that the process does not involve metal-sulfur bond breaking and follows a first-order rate law, different from collisional ligand exchange.
Article
Chemistry, Multidisciplinary
Jiangtao Zhao, Abolfazl Ziarati, Arnulf Rosspeintner, Yanan Wang, Thomas Buergi
Summary: The conversion of hydrophobic Au25PET18 nanoclusters to Au25SR19 nanoclusters was achieved through ligand exchange reactions with thiolated terpyridine-metal complexes. The preference for ligand addition or exchange was found to be metal dependent. The photophysical properties of the resulting Au25SR19 nanoclusters were significantly different from those of Au25PET18.
Article
Chemistry, Multidisciplinary
Xianwei Wang, Jiangtao Zhao, Henrik Eliasson, Rolf Erni, Abolfazl Ziarati, Siobhan Mckeown Walker, Thomas Burgi
Summary: Depositing Au-25 nanoclusters onto a manganese oxide support produces a stable and highly active catalyst. By optimizing the pretreatment temperature, the performance of the Au-25/MnO2 catalyst in low-temperature CO oxidation can be significantly enhanced.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Green & Sustainable Science & Technology
Yuming Wang, Yi Li, Longfei Wang, Wenlong Zhang, Thomas Burgi
Summary: This study investigates the collaborative enhancement of photocatalytic properties by graphitic carbon nitrides (g-C3N4) and microorganisms, and its potential for environmental depollution. The research explores the electronic interactions and roles of bio-substances in this process. The study finds that nano-photocatalysts are adsorbed onto bio-aggregates and surface hydrophilicity plays a role in the toxicity of photocatalysts in dark environments. The research also reveals hetero-junctions between photocatalysts and bio-substances and demonstrates effective nitrobenzene degradation. The findings suggest that bio-activities can stimulate material modification and the integration of inorganic and organic systems in a sustainable manner.
Article
Chemistry, Multidisciplinary
Jiangtao Zhao, Abolfazl Ziarati, Arnulf Rosspeintner, Thomas Burgi
Summary: In this study, a new hybrid material is obtained by anchoring thiol functionalized terpyridine metal complexes on Au nanoclusters. This material exhibits high activity and selectivity in the process of photosensitizing CO2 reduction, along with excellent long-term stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Anton Kudashev, Stefania Vergura, Marco Zuccarello, Thomas Burgi, Olivier Baudoin
Summary: The divergent synthesis of two indane polyketides of the indidene family has been reported. The study demonstrates the construction of the indane intermediate and the installation of the aroyl moiety using palladium-catalyzed and nickel-catalyzed reactions. The structures of indidenes B and C have been revised based on these investigations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Krishnadas Kumaranchira Ramankutty, Thomas Buergi
Summary: The properties of nanoscale matter are highly dependent on size and shape, requiring atomic precision synthesis and separation to achieve the envisioned idea of 'maneuvering things atom by atom' by Richard Feynman. Analytical separation techniques have played a key role in understanding the size- and shape-dependent properties of nanomaterials, contributing tremendously to the progression of nanomaterials science. Limitations, challenges, and future perspectives of these techniques are also discussed in the context of nanomaterials research.
Article
Chemistry, Physical
Krishnadas Kumaranchira Ramankutty, Huayan Yang, Ani Baghdasaryan, Jeremie Teyssier, Valentin Paul Nicu, Thomas Buergi
Summary: We study distinct molecule-like and lattice vibrational properties of atomically precise, ligand-protected metal clusters using low-temperature Raman spectroscopy. Our results show the fingerprint Raman spectra of different metal clusters and how these spectra change with variations in metal atoms and/or ligands. This highlights the importance of low-frequency Raman spectroscopy in understanding the vibrational dynamics of other materials.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)