Article
Chemistry, Multidisciplinary
Qiang Chen, Pai Peng, Ganjun Yang, Yanzhi Li, Mengxi Han, Yaozong Tan, Chengxi Zhang, Junwen Chen, Kun Jiang, Lei Liu, Chenliang Ye, Enhui Xing
Summary: In this study, single platinum atoms were selectively encaged in the six-membered rings of sodalite (SOD) cages within Y zeolite using a template-guiding strategy. The Pt@Y-SOD catalyst showed good stability, excellent catalytic selectivity in the semihydrogenation reaction, and resistance to thiophene and carbon monoxide due to the configuration of the encaged single platinum atoms.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Spectroscopy
Sonia Kotowicz, Daiva Tavgeniene, Raminta Beresneviciute, Ernestas Zaleckas, Gintare Krucaite, Agnieszka Katarzyna Pajak, Mateusz Korzec, Jan Grzegorz Malecki, Marek Lipinski, Saulius Grigalevicius, Ewa Schab-Balcerzak
Summary: Fluorene-based low molar weight derivatives were synthesized using Suzuki reactions with key starting materials of 9-benzylidene-2,7-dibromofluorene or 3-(2,7-dibromofluoren-9-ylmethylen)-9-ethylcarbazole and various aryl boronic acids. The compounds exhibited high thermal stability and some showed a high glass transition temperature above 125°C. They also demonstrated electrochemical activity and a energy band gap below 2.97 eV. The investigations were supported by DFT calculations and the photovoltaic ability of the compounds was tested in organic-inorganic solar cells.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2023)
Article
Nanoscience & Nanotechnology
Zizhu Wang, Caiyun Xu, Yuhua Wang, Shenghu Zhou
Summary: This work demonstrates the high selectivity of Pt nanoparticles confined in hollow porous silica nanospheres (Pt@HPSNs) as catalysts for the transfer hydrogenation of phenylacetylene to styrene using ammonia borane. Pt@HPSNs show above 88% styrene selectivity at nearly 100% phenylacetylene conversions, even at high ammonia borane/phenylacetylene ratios and longer reaction time. The enhanced styrene selectivity of Pt@HPSNs is attributed to the electron deficiency of encapsulated Pt nanoparticles, which leads to the fast desorption of styrene and avoids deep hydrogenation.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Jean-Francois Lemineur, Paolo Ciocci, Jean-Marc Noel, Hongxin Ge, Catherine Combellas, Frederic Kanoufi
Summary: Efforts have been made towards designing sustainable and efficient nanocatalysts for the hydrogen evolution reaction, but there is a need for the real-time observation and quantification of gas nanobubble formation. This study utilized interference reflection microscopy coupled with electrochemistry and optical modeling to analyze individual nanobubbles' geometry and growth rate. The results showed that nanobubbles cover Pt nanoparticles and steadily grow on the electrode surface, raising questions about the relationship between nanobubble growth and electrochemical activity.
Article
Chemistry, Physical
Si-Hai Wu, Zhe Zhang, Ren-Hui Zheng, Rong Yang, Lianhui Wang, Jiang-Yang Shao, Zhong-Liang Gong, Yu-Wu Zhong
Summary: Three monoruthenium complexes bearing an N(CH3)-bridged ligand have been synthesized and characterized. The photophysical and electrochemical properties of these complexes have been examined. The emission bands of these complexes are well-separated, with the higher-energy bands having similar emission maxima and the lower-energy bands depending on the electronic nature of the substituents. Computational investigation has been used to analyze the experimental observations.
Article
Chemistry, Physical
Isabela Dancini-Pontes, Rodrigo M. Pontes
Summary: The study investigates the O-Pt bond interaction of a model Pt-3 cluster with molecules of distinct chemical structures, highlighting the contribution of various factors to the interaction process. DFT calculations and statistical tests reveal a correlation between adsorption energy and isolated molecule characteristics, as well as a correlation between activation energy for O-H bond scission and complexation energy. The distortion-interaction model is applied to demonstrate changes in donor-acceptor characteristics along the reaction path for the molecule-Pt-3 system.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2022)
Article
Electrochemistry
Linnea Strandberg, Victor Shokhen, Mathilde Luneau, Goran Lindbergh, Carina Lagergren, Bjorn Wickman
Summary: In this study, the dissolution and oxidation of platinum (Pt) were compared in acidic and alkaline conditions. The results showed a higher mass increase in alkaline conditions, while the dissolution of Pt was similar. Additionally, small yet significant differences were observed in the surface structure of Pt thin films.
Review
Optics
Gregory Barbillon
Summary: SHINERS is a novel Raman spectroscopy technique that utilizes plasmonic cores and silica shells to enhance the Raman signal of molecules, making it suitable for catalytic reactions requiring high thermal and chemical stability, with strong surface sensitivity for research at liquid-solid interfaces. Recent studies in the past two years have focused on the applications of this technology in reactions involving CO molecules, surface catalytic reactions, and the detection of molecules and ions.
Article
Chemistry, Multidisciplinary
Nils Heppe, Charlotte Gallenkamp, Stephen Paul, Nicole Segura-Salas, Niklas von Rhein, Bernhard Kaiser, Wolfram Jaegermann, Atefeh Jafari, Ilya Sergueev, Vera Krewald, Ulrike I. Kramm
Summary: In order to achieve a future hydrogen economy, there is a need for non-precious metal catalysts for water splitting reactions that can be used globally. Metal-nitrogen-carbon (MNC) catalysts with active sites consisting of a metal center with fourfold coordination of nitrogen (MN4) have shown promising performance, but their optimization has been hindered by their low structural definition. By studying porphyrin model complexes, insights from well-defined molecules are transferred to MNC systems in order to evaluate the effect of porphyrin substituents on the electronic and electrocatalytic properties of MN4 centers for the hydrogen evolution reaction (HER) in aqueous electrolyte. The choice of substituent was found to impact their utilization on the carbon support and their electrocatalytic performance.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Chemistry, Analytical
Kaimin Wu, Feizhi Kong, Jingjing Zhang, Ying Tang, Yao Chen, Long Chao, Libo Nie, Zhao Huang
Summary: Single-nucleotide polymorphisms (SNPs) are the most common form of genetic variation in the human genome, and are closely related to individual differences. SNP detection with simple preparation and operational procedures, high affinity and specificity, and cost-effectiveness has been a challenge. This review provides an overview on improvements for SNP biosensing based on fluorescent and electrochemical methods, and presents the advantages, disadvantages, and challenges of each method.
Article
Chemistry, Multidisciplinary
Daisuke Saito, Tomasz Galica, Eiji Nishibori, Masaki Yoshida, Atsushi Kobayashi, Masako Kato
Summary: A study on the vapochromic single-crystal-to-single-crystal transformation of a highly luminescent Pt-II complex was reported, revealing the reversible process by the release and reabsorption of water molecules changing the stacked structure of the complex. Additionally, the Pt-II complex showed a similar response to methanol vapor but was inactive towards ethanol vapor.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Andreas Koellisch-Mirbach, Inhee Park, Martina Hegemann, Elke Thome, Helmut Baltruschat
Summary: This study compared the oxygen reduction reaction (ORR) in Ca2+-containing dimethyl sulfoxide (DMSO) at ordered and rough electrode surfaces using various measurement techniques. It found that the formation of peroxide and superoxide differs depending on the surface structure, and the presence of a CaO/CaO2 layer can affect the reaction outcome. Additionally, the reoxidation kinetics of dissolved peroxide were shown to be sluggish, possibly due to ion pairing with Ca2+.
Article
Chemistry, Physical
Christoph J. Bondue, Zhiqin Liang, Marc T. M. Koper
Summary: This study investigates the poisoning reaction at platinum electrodes during the electrocatalytic hydrogenation of acetone. It was found that acetone adsorbs molecularly intact on most sites but dissociatively on Pt(100) terraces, leading to poisoning. The dissociative adsorption is limited to Pt(100) terraces, indicating a certain minimum ensemble number of freely available Pt atoms is needed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Jie Wei, Si-Na Qin, Ji Yang, Han-Long Ya, Wei-Hsiang Huang, Hua Zhang, Bing Joe Hwang, Zhong-Qun Tian, Jian-Feng Li
Summary: The development of shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) has allowed for the characterization and in situ monitoring of Pd single-atom catalysts (SACs), revealing their unique catalytic properties and evolution processes. This new spectroscopic tool provides molecular insights into SACs and is particularly useful for studying solid-liquid interfaces.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Xiaoli Jiang, Lei Tang, Lei Dong, Xuedi Sheng, Wenfei Zhang, Zhen Liu, Jianhua Shen, Hongliang Jiang, Chunzhong Li
Summary: In this study, density functional theory (DFT) simulations were used to investigate the site isolation strategy in electrocatalytic selective hydrogenation of acetylene. The results showed that isolated Cu metal sites have higher energy barriers on overhydrogenation and C-C coupling reactions. Based on this, Cu single-atom catalysts highly dispersed on nitrogen-doped carbon matrix were developed and demonstrated high ethylene selectivity under high concentrations of acetylene. The superior performance was attributed to the weak adsorption of ethylene intermediates and highly energy barriers on C-C coupling at isolated sites, as confirmed by both DFT calculations and experimental results. This study provides a comprehensive understanding of the isolated sites inhibiting the side reactions in electrocatalytic acetylene semihydrogenation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
L. Baker, M. P. Renshaw, M. D. Mantle, A. J. Sederman, A. J. Wain, L. F. Gladden
APPLIED CATALYSIS A-GENERAL
(2018)
Article
Chemistry, Physical
Naresh Kumar, Sam Kalirai, Andrew J. Wain, Bert M. Weckhuysen
Article
Electrochemistry
Alex G. M. Litherland, Lee M. Spurway, Sergey N. Gordeev, Barak D. B. Aaronson, Andrew J. Wain, Michael A. O'Connell, Heidi Piili, Mikko Hovilehto, Ville-Pekka Matilainen, Anne Vuorema, Frank Marken
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
(2018)
Article
Chemistry, Multidisciplinary
Naresh Kumar, Weitao Su, Martin Vesely, Bert M. Weckhuysen, Andrew J. Pollard, Andrew J. Wain
Article
Chemistry, Physical
Andrew J. Wain, Michael A. O'Connell, Gary A. Attard
Article
Chemistry, Multidisciplinary
Matej Velicky, Gavin E. Donnelly, William R. Hendren, Stephen McFarland, Declan Scullion, William J. I. DeBenedetti, Gabriela Calinao Correa, Yimo Han, Andrew J. Wain, Melissa A. Hines, David A. Muller, Kostya S. Novoselov, Hector D. Abruna, Robert M. Bowman, Elton J. G. Santos, Fumin Huang
Article
Chemistry, Physical
Naresh Kumar, Caterina S. Wondergem, Andrew J. Wain, Bert M. Weckhuysen
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2019)
Article
Biochemical Research Methods
Naresh Kumar, Bert M. Weckhuysen, Andrew J. Wain, Andrew J. Pollard
Article
Chemistry, Analytical
Edmund J. F. Dickinson, Andrew J. Wain
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2020)
Article
Nanoscience & Nanotechnology
Douglas W. G. Stewart, Keith Scott, Andrew J. Wain, Timothy E. Rosser, Edward Brightman, Donald Macphee, Mohamed Mamlouk
ACS APPLIED MATERIALS & INTERFACES
(2020)
Article
Chemistry, Physical
Maria Chiara Spadaro, Jo J. L. Humphrey, Rongsheng Cai, Lidia Martinez, Sarah J. Haigh, Yves Huttel, Steve J. Spencer, Andrew J. Wain, Richard Palmer
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Electrochemistry
Timothy E. Rosser, Edmund J. F. Dickinson, Rinaldo Raccichini, Katherine Hunter, Andrew D. Searle, Christopher M. Kavanagh, Peter J. Curran, Gareth Hinds, Juyeon Park, Andrew J. Wain
Summary: Operando Raman spectroscopy is a well-established technique for monitoring chemical changes in alkali-ion cells, but its application to commercial electrodes has been limited by cell design constraints. An improved configuration is introduced for reliable operando Raman spectroscopy on commercial battery electrodes, along with a general methodological framework for validation.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Timothy E. Rosser, Juliana P. S. Sousa, Yasmine Ziouani, Oleksandr Bondarchuk, Dmitri Y. Petrovykh, Xian-Kui Wei, Jo J. L. Humphrey, Marc Heggen, Yury V. Kolen'ko, Andrew J. Wain
CATALYSIS SCIENCE & TECHNOLOGY
(2020)
Article
Chemistry, Multidisciplinary
Jo J. L. Humphrey, Rasmus Kronberg, Rongsheng Cai, Kari Laasonen, Richard E. Palmer, Andrew J. Wain