Article
Chemistry, Physical
Jie Yang, Shan Ren, Mingming Wang, Zhichao Chen, Lin Chen, Lian Liu
Summary: CeO2/TiO2 catalyst was studied using in situ diffuse reflectance infrared Fourier transform spectroscopy, and it was found that CeO2 particles grew along TiO2 faces and amorphous cerium in the lattice of TiO2. NH4+ could adsorb on the Ti-O-Ce structures or TiO2-CeO2 interface as Bronsted acid sites, and NH4NO3 intermediate dominated the SCR reactions.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Nanoscience & Nanotechnology
Eleonora Romeo, Maria Fernanda Lezana-Muralles, Francesc Illas, Federico Calle-Vallejo
Summary: The electrocatalytic reduction of oxidized nitrogen compounds (NOx) is important for rebalancing the nitrogen cycle. This study explores the use of catalytic matrices to extract features of active transition metal catalysts for NO electroreduction. The matrices reveal that active catalysts stabilize *NHO over *NOH and have undercoordinated sites, indicating their potential in NOx electroreduction.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Rahul D. Kerkar, Arun V. Salker
Summary: The influence of aluminum on copper-manganese composite oxide in the NO-CO redox reaction has been investigated. Aluminum addition resulted in a porous structure and increased the surface acidic/basic character of the catalyst, leading to enhanced catalytic performance. The study highlights the importance of tuning catalytic materials for improving reaction performance.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Rahul D. Kerkar, Arun V. Salker
Summary: This study investigates the influence of aluminum on copper-manganese composite oxide in the NO-CO redox reaction, finding that aluminum fabricated composite oxide exhibits higher conversion and helps establish more acidic/basic sites for enhancing the reaction.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Konstantinos G. Papanikolaou, Michail Stamatakis
Summary: This study investigated the reaction mechanism of two PGM-free Ni/Cu dilute alloys using density functional theory and microkinetic modeling. The addition of trace amounts of Ni on Cu(111) was found to significantly improve catalytic performance, particularly in the catalytic decomposition of N2O. Furthermore, Ni2Cu(111) showed equivalent or even better performance compared to Rh(111) in the NO + CO reaction, contributing to the development of efficient PGM-free catalytic materials for reducing noxious gases.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Energy & Fuels
Bo Xiong, Jing Liu, Yingju Yang, Yuchen Yang, Zhixuan Hua
Summary: In this study, the effect of NO on the electrocatalytic reduction of CO2 over Pd@Cu bimetal catalysts was investigated using density functional theory. It was found that NO is more easily adsorbed on the catalyst surface and reduced to NH3, promoting the CO2RR process.
Article
Chemistry, Multidisciplinary
Chien-Wei Chiang, Kai-Wun Jhang, Jeng-Lung Chen, Liang-Ching Hsu, Wei-Hsiang Huang, Hung-Chi Chen, Ting-Jun Lin, Ci-Yang Sun, Yu-Ning Li
Summary: In this study, a bioinspired {Co(NO)(2)}(10) complex 1 was developed for S-nitrosation of Cys residues. By incorporating a ferrocenyl group, the nitrosation reaction was fine-tuned using the redox ability of Cys residues. Complex 1 was synthesized and characterized, showing its NO translation reactivity. Moreover, complex 1 successfully converted Cys into S-nitrosocysteine (Cys-SNO), as confirmed by UV-Vis, IR, and XAS spectroscopy. This study presents a promising approach for further exploration in the modification of Cys-containing peptides.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Kakuya Ueda, Masashi Tsuji, Junya Ohyama, Atsushi Satsuma
Summary: Cobalt spinel oxides with octahedral (Oh) and tetrahedral (Td) sites show high activity in NO reduction by CO. By studying cobalt spinel oxides with different CoOh/CoTd ratios, it was determined that the octahedral site is responsible for the NO-CO reaction. In-situ XAFS measurements revealed that cobalt spinel oxides with higher CoOh fraction are more easily reduced by CO, leading to higher activity in NO reduction by CO.
Article
Biochemistry & Molecular Biology
Xinmiao Liu, Yunjie Xu, Li Sheng
Summary: In this study, the catalytic reduction of NO molecules on an Al-decorated C2N monolayer (Al-C2N) was systematically investigated using density functional theory (DFT) calculations. The results showed that the Al-C2N catalyst is highly selective for NO and the NO reduction reaction preferably undergoes the (NO)2 dimer reduction process. Particularly, the cis-(NO)2 dimer structures were crucial intermediates for NO reduction, while the remaining O-ads species were easily reduced with CO molecules.
Article
Chemistry, Physical
Hong Wen, Hao Sun, Xin Jin, Jing-yao Liu
Summary: The research systematically studied the reduction of NO by CO on transition metal-Pt alloy catalysts using density functional theory calculations and microkinetics simulations. The results showed that Fe-Pt(100), Co-Pt(100), and Ni-Pt(111) are the optimal catalysts for high NO reduction activity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Xianwei Wang, Nobutaka Maeda, Daniel M. Meier, Alfons Baiker
Summary: The catalytic reduction of NO with CO was studied over monometallic Au and bimetallic AuRh nanoparticles supported on potassium titanate (KTN) and TiO2, with KTN showing significant enhancement in catalytic performance. The support material plays a crucial role in promoting the formation of surface species, particularly isocyanide, which is important for producing dinitrogen molecules via reaction with NO.
Article
Multidisciplinary Sciences
Takashi Nomura, Tetsunari Kimura, Yusuke Kanematsu, Daichi Yamada, Keitaro Yamashita, Kunio Hirata, Go Ueno, Hironori Murakami, Tamao Hisano, Raika Yamagiwa, Hanae Takeda, Chai Gopalasingam, Ryota Kousaka, Sachiko Yanagisawa, Osami Shoji, Takashi Kumasaka, Masaki Yamamoto, Yu Takano, Hiroshi Sugimoto, Takehiko Tosha, Minoru Kubo, Yoshitsugu Shiro
Summary: The study investigated the mechanism of NO reductase catalyzing the generation of N2O. Time-resolved techniques and photolabile-caged NO were used to characterize the structure and formation of the intermediate I in NO reductase. Quantum mechanics/molecular mechanics calculations and experimental results revealed the electronic structure characteristics of the intermediate I.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Ping Wang, Xiaoling Mou, Yong Li, Wenjie Shen
Summary: A synthetic strategy for preparing fibrous-like green rusts by using appropriate balancing anions in ethylene glycol was reported. The green rusts can be converted into hematite with fibrous- or plate-like shapes upon thermal activation. The fibrous-like Fe2O3 exhibited higher catalytic activity and structural robustness compared to the plate-like analogue.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Chemistry, Multidisciplinary
Yongjun Ji, Shaomian Liu, Hongdan Zhu, Wenqing Xu, Ruihuan Jiang, Yu Zhang, Jian Yu, Wenxing Chen, Lihua Jia, Jingang Jiang, Tingyu Zhu, Ziyi Zhong, Dingsheng Wang, Guangwen Xu, Fabing Su
Summary: This study reports a highly efficient Ir-based catalyst with only 1% Ir loading for CO-SCR. The catalyst enables complete NO conversion to N2 at 250 degrees C in the presence of 1% O2 and has a wide temperature window (250-400 degrees C). Experimental results and theoretical calculations show that the negatively charged single Ir atoms enhance NO dissociation, while the Ir-W intermetallic nanoparticles accelerate the reduction of N2O and NO2 intermediates by CO.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Konstantin Khivantsev, Ja-Hun Kwak, Nicholas R. Jaegers, Iskra Z. Koleva, Georgi N. Vayssilov, Miroslaw A. Derewinski, Yong Wang, Hristiyan A. Aleksandrov, Janos Szanyi
Summary: In this study, the mechanism of NO reduction using Cu/zeolite catalysts was investigated using spectroscopy, catalysis, and DFT calculations. It was found that nitrosyl ions are the key intermediates and nitrogen gas is produced through the intermediacy of the diazo N2H+ cation. The formation of NH4+ at low temperatures inhibits the catalytic cycle, while at higher temperatures, the cycle can continue.
Review
Chemistry, Applied
Xin Liu, Timo Jacob, Wang Gao
Summary: This review provides a comprehensive overview of the research on formic acid decomposition and electrooxidation, analyzes the reaction mechanism, and discusses strategies for improving catalyst performance. It also presents a prospect for future studies in formic acid decomposition and electrooxidation.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Electrochemistry
Tanja Geng, Sven J. Zeller, Ludwig A. Kibler, Maximilian U. Ceblin, Timo Jacob
Summary: The electrodeposition of copper onto Au(111) from Deep Eutectic Solvents (DESs) type III has been studied. The article found that the eutectic composition for ChCl/EG DES is 16:84 (ChCl:EG). The study also revealed that the electrolyte composition affects the deposition behavior.
Article
Chemistry, Multidisciplinary
Florian Fiesinger, Daniel Gaissmaier, Matthias van den Borg, Timo Jacob
Summary: Rechargeable magnesium-ion batteries show promise as an alternative to commercial lithium-ion batteries due to their safety, environmental friendliness, and higher volumetric capacity. However, the formation of a passivation layer on metallic magnesium electrodes remains a major challenge.
Article
Biochemistry & Molecular Biology
Marharyta Varatnitskaya, Julia Fasel, Alexandra Mueller, Natalie Lupilov, Yunlong Shi, Kristin Fuchs, Marco Krewing, Christoph Jung, Timo Jacob, Barbara Sitek, Julia E. Bandow, Kate S. Carroll, Eckhard Hofmann, Lars I. Leichert
Summary: This study helps to identify the residues responsible for RidA's chaperone-like function using a combination of LC-MS/MS analysis, chemo-proteomic approach, and mutagenesis study. The enhanced chaperone activity of RidA is associated with the loss of positive charges on the protein surface and increased overall protein hydrophobicity.
Article
Chemistry, Multidisciplinary
Sinwoo Kang, Changbin Im, Ioannis Spanos, Kahyun Ham, Ahyoun Lim, Timo Jacob, Robert Schloegl, Jaeyoung Lee
Summary: In this study, the degradation of NiFe-based oxides in Fe-purified KOH was investigated, and a solution was proposed. Loading TPP on the catalyst/electrolyte interface can alleviate the destabilization of NiFe (oxy)hydroxide and prolong the catalyst's lifetime.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Laura Braunwarth, Christoph Jung, Timo Jacob
Summary: This study uses molecular dynamics simulations to investigate the structure and dynamics of electrode-electrolyte interfaces, focusing on the Pt(111)/water interface. The results reveal changes in water molecule orientation and intermolecular ordering, challenging previous assumptions about their correlation to free charge density. This work contributes to our understanding of electric double layers and electrochemical processes.
Article
Chemistry, Multidisciplinary
Matthias Uhl, Tanja Geng, Philipp A. Schuster, Benjamin W. Schick, Matthias Kruck, Alexander Fuoss, Alexander J. C. Kuehne, Timo Jacob
Summary: By replacing the electrolyte with a deep eutectic solvent and using a polymer as the electrode, an all-organic battery can be achieved. The combination of different solvents and salt concentrations affects the stability and viscosity of the battery. The eutectic mixture with a 1:6 ratio offers the best balance between stability and viscosity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Evelyn Artmann, Lukas Forschner, Konstantin M. Schuettler, Mohammad Al-Shakran, Timo Jacob, Albert K. Engstfeld
Summary: Researchers propose a simple method for the preparation of nanoporous gold films, which can be achieved by high voltage electrolysis or anodic contact glow discharge electrolysis. The structural properties of the resulting films can be controlled by adjusting the electrolysis conditions and the reduction reaction conditions.
Article
Chemistry, Multidisciplinary
Florian Fiesinger, Daniel Gaissmaier, Matthias van den Borg, Julian Bessner, Adri C. T. van Duin, Timo Jacob
Summary: One of the key challenges in the development of magnesium-ion batteries (MIB) is the formation of a passivating boundary layer at the magnesium anode. A Mg/O ReaxFF parameter set was developed to accurately model the degradation process of the magnesium anode by O-2 impurities. It was found that O-2 immediately dissociates upon first contact with the magnesium anode, leading to high temperatures and further oxidation. The trained force field can be used to study reactions in Mg-air batteries and the oxidation of magnesium metal in general.
Article
Electrochemistry
Daniel Rutz, Ingolf Bauer, Felix Brauchle, Timo Jacob
Summary: In this study, user-defined reference electrodes based on LFP were fabricated using an ultrashort pulse laser. The results showed that these electrodes have minimal impact on the cell capacity and can provide reproducible voltage output at low to moderate C-rates. They also do not affect the cell expansion during cycling.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Julia Bord, Bjoern Kirchhoff, Matthias Baldofski, Christoph Jung, Timo Jacob
Summary: Density functional theory (DFT) is utilized to investigate the electronic structure of platinum clusters on different graphene substrates. The size and defects of both the clusters and the graphene substrates are examined. The results reveal that larger vacancies lead to stronger binding of Pt clusters, while defect-free graphene shows more exothermic formation energy with increasing cluster size. Oxygen-free graphene supports are crucial for successful attachment of Pt, and cluster stability depends on the number and ratio of Pt-C, Pt-Pt, and Pt-O bonds rather than the cluster geometry.
Article
Chemistry, Physical
Hongyuan Yang, Pramod V. Menezes, Guoliang Dai, Gonela Vijaykumar, Ziliang Chen, Mohammad Al-Shakran, Timo Jacob, Matthias Driess, Prashanth W. Menezes
Summary: Developing bifunctional electrodes for oxidation catalysis is highly desirable for hydrogen and value-added chemicals production. Here, we directly activate the nickel foam through the incorporation of elemental P (P-NF) using a facile, controllable, and ultrafast in-liquid plasma electrolysis approach. The practical bifunctionality of P-NF is additionally verified with selective oxygenation of organics forming value-added chemicals.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Changbin Im, Bjorn Kirchhoff, Igor Krivtsov, Dariusz Mitoraj, Radim Beranek, Timo Jacob
Summary: Computational investigation of PCN materials can lead to better understanding and optimization strategies. Thermochemical calculations predict stable structural motifs and show that condensed PCN domains in a less condensed framework can have desirable optical properties.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Lukas Forschner, Evelyn Artmann, Timo Jacob, Albert K. Engstfeld
Summary: Applying an external potential difference between two electrodes leads to a voltage drop in an ion conducting electrolyte. The electrolyte potential is relevant in electrochemistry and various applications such as bipolar electrochemistry, ohmic microscopy, or contact glow discharge electrolysis. This study focuses on the electrolyte potential during high voltage electrolysis in an electrolysis cell using reversible hydrogen electrodes as reference electrodes. A computational COMSOL model is used to support the experimental findings, and the influence of cell geometry on the electrolyte potentials is evaluated. The amount of oxide formed during high voltage electrolysis is found to be related to the current rather than the applied voltage, based on the knowledge of potential distribution.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Chemistry, Physical
Bjoern Kirchhoff, Christoph Jung, Daniel Gaissmaier, Laura Braunwarth, Donato Fantauzzi, Timo Jacob
Summary: Nanoparticles (NPs) as heterogeneous catalysts have large active surface area and size-dependent catalytic properties. The ability to computationally predict the most favorable NP structures for catalytic reactions is important for material optimization. However, simulations of NP model systems present unique challenges to computational scientists and require different data analysis strategies compared to simulations of single crystal surface models. This work aims to review analytical methods and data analysis strategies for extracting thermodynamic trends from NP simulations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)