Article
Chemistry, Multidisciplinary
Papri Chakraborty, Sami Malola, Marco Neumaier, Patrick Weis, Hannu Hakkinen, Manfred M. Kappes
Summary: The fragmentation dynamics of ligated coinage metal clusters provides insights into their structural and bonding properties. However, the challenges in methodology have limited the investigation of fragment structures. In this study, we used trapped ion mobility mass spectrometry to determine the geometric structures of the primary fragments of [Ag29L12](3-) and compared them to density functional theory calculations. We also observed a new dissociation channel in the further dissociation of [Ag19L6](-), indicating a competition between retaining electronic stability and increasing steric strain of ligands and staples. These findings have potential implications for studying the catalytic behavior of Ag clusters on supports through soft-landing deposition.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Food Science & Technology
Sha Yan, Xuan Wang, Minghui Sun, Wenqian Wang, Liming Wu, Xiaofeng Xue
Summary: Royal jelly is a popular nutraceutical with unique lipid composition, including phospholipids and trans-10-hydroxy-2-decenoic acid. This study found that the lipid composition of royal jelly is influenced by its botanical origin.
LWT-FOOD SCIENCE AND TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Yao Qian, Xiangyu Guo, Yunfang Wang, Zheng Ouyang, Xiaoxiao Ma
Summary: A mobility-modulated sequential dissociation (MMSD) strategy was developed for mass spectrometry imaging, enabling spatial lipidomics capable of multiplexed MS/MS imaging of 24 structurally distinct lipids. The method revealed a potential biomarker in a human hepatocellular carcinoma tissue.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemical Research Methods
Max L. Feuerstein, Maykel Hernandez-Mesa, Andrea Kiehne, Bruno Le Bizec, Stephan Hann, Gaud Dervilly, Tim Causon
Summary: This study compared the collision cross section (CCS) derived from three different IM-MS technologies for the analysis of steroids and small molecules. The interlaboratory performance was found to be excellent, but differences in ion conformation sampled on different instrument types need further investigation.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Chemistry, Analytical
A. Bianco, I Neefjes, D. Alfaouri, H. Vehkamaki, T. Kurten, L. Ahonen, M. Passananti, J. Kangasluoma
Summary: Mass spectrometry is an effective method for identifying and quantifying environmentally relevant molecules, but it cannot distinguish between isomers. This study combines an experimental set-up using a differential mobility analyser with computational ion mobility calculations to successfully identify isomers. The experimental set-up allows for analysis in both the gas and liquid phase, making it a versatile tool for isomer separation.
Article
Biochemical Research Methods
Taylor M. Domenick, Austin L. Jones, Robin H. J. Kemperman, Richard A. Yost
Summary: To address the poor retention of highly polar metabolites in reversed-phase liquid chromatography (RPLC), a derivatization agent and an internal standard were introduced to improve analyte retention and detection limits. Multiplexed drift-tube ion mobility (IM) was integrated into the LC-MS workflow to enhance method sensitivity and selectivity. The results showed that this method allowed for the quantitation of amino acids in microglial cell extracts.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Analytical
Daniel G. Delafield, Gaoyuan Lu, Cameron J. Kaminsky, Lingjun Li
Summary: Mass spectrometry-based biomolecular analyses have become popular in research settings. Gas phase ion separation techniques provide a fourth dimension of analysis, enabling rapid characterization and high throughput profiling. This review highlights the latest developments and applications of high-end ion-mobility enabled instruments and their advantages for biomolecular research.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Applied
Minna Juvonen, Edwin Bakx, Henk Schols, Maija Tenkanen
Summary: This study investigated the potential of using TWIMS and CID-TWIMS-MS/MS to separate cereal-derived isomeric arabinoxylanoligosaccharides (A)XOS. The triand pentasaccharide isomers were distinguishable by the ATDs of the precursor ions, while CID-TWIMS-MS/MS could effectively separate isomeric fragment ions produced from tetra- and pentasaccharide (A)XOS. The base peak mobility spectrum was also introduced as a practical tool for (A)XOS fingerprinting.
Article
Chemistry, Multidisciplinary
Karen E. Butler, Yoshihiko Takinami, Adam Rainczuk, Erin S. Baker, Blaine R. Roberts
Summary: Native mass spectrometry combined with IMS-MS technology can be used to study the tertiary and quaternary structure of proteins, validate other structural determination methods, and provide more comprehensive structural information.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Analytical
Kelly L. Wormwood Moser, Gregory Van Aken, Daniel DeBord, Nathan Galen Hatcher, Laura Maxon, Melissa Sherman, Lihang Yao, Kim Ekroos
Summary: Defects in sphingolipid metabolism serve as a common link in various neurodegenerative disorders, and a better understanding of lipid content presents opportunities for the development of new therapeutic targets and biomarkers.
ANALYTICA CHIMICA ACTA
(2021)
Article
Chemistry, Multidisciplinary
Jan Leipert, Philipp T. Kaulich, Max K. Steinbach, Britta Steer, Konrad Winkels, Christine Blurton, Matthias Leippe, Andreas Tholey
Summary: Researchers have developed a sample preparation method based on protein aggregation and acidic elution, allowing for sensitive protein identification analysis of single nematodes on a digital microfluidics device. Compared to in-tube sample preparation, this method increases proteoform identifications by 46%. Label-free quantification also reveals changes in proteoform abundance that cannot be distinguished by bottom-up proteomics. This workflow facilitates proteoform-focused analysis on limited availability samples.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemical Research Methods
Yanfen Zhang, Yehua Han, Chenglong Dong, Chen Li, Tuo Liang, Guannan Ling, Honggang Nie
Summary: A method for rapid characterization of AAAs in serum was developed using IMS-MS, which was validated and successfully applied to the pharmacokinetics study of AAAs in rats, offering a promising way for fast screening and evaluation with high sensitivity and reliability.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2021)
Article
Multidisciplinary Sciences
Xiaoyu Zhou, Zhuofan Wang, Jingjin Fan, Zheng Ouyang
Summary: Ion mobility is utilized in mass spectrometers for analyzing the structure of biomolecules. Researchers demonstrate that ion mobility analysis in an ion trap with ultra-high fields can achieve resolutions over 10,000 for isomer separation, as shown for disaccharide, phospholipid, and peptide isomers. Elucidating complex structures of biomolecules is crucial in chemistry and life sciences. In the last decade, ion mobility coupled with mass spectrometry has become a unique tool for distinguishing isomers and isoforms of biomolecules. This study presents a concept for ion mobility analysis using an ion trap, enabling ultra-high field isomer separation and achieving resolutions over 10,000. The potential of this technology is demonstrated for analyzing isomers of disaccharides, phospholipids, and peptides with post-translational modifications.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Analytical
Katie M. Kohoutek, Peter de B. Harrington
Summary: Electrospray ionization ion mobility mass spectrometry (ESI-IMS-MS) is a rapidly progressing analytical technique that examines complex compounds in the gas phase. It separates isomers, provides structural information, and quantitatively identifies various compounds in biological samples. ESI-IMS-MS has wide applications in pharmaceutical, environmental, and manufacturing industries.
CRITICAL REVIEWS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Daisy Unsihuay, Ruichuan Yin, Daniela Mesa Sanchez, Manxi Yang, Yingju Li, Xiaofei Sun, Sudhansu K. Dey, Julia Laskin
Summary: The study introduces a novel experimental platform that combines nano-DESI and IM spectrometry for high spatial resolution imaging of molecules in mouse uterine tissues, providing unique molecular descriptors and revealing variations in isomeric composition through isomer-specific imaging.
ANALYTICA CHIMICA ACTA
(2021)
Article
Chemistry, Multidisciplinary
Zoe L. Sinclair, Nicola L. Bell, Jessica. R. R. Bame, De-Liang Long, Leroy Cronin
Summary: Polyoxopalladates (POPs) are a class of self-assembling palladium-oxide clusters that have different sizes, shapes, and compositions. The largest compound in this family, {Pd-84}(Ac), is an ideal molecule for exploring supramolecular behavior in aqueous media. Through molecular visualization and nuclear magnetic resonance studies, it has been found that {Pd-84}(Ac) forms a 1:7 host-guest complex with benzyl viologen (BV2+) in aqueous solution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yupeng Zhao, Dandan Gao, Si Liu, Johannes Biskupek, Ute Kaiser, Rongji Liu, Carsten Streb
Summary: Efficient and stable oxygen evolution reaction (OER) catalysts based on noble-metal-free materials are crucial for energy conversion and storage. This study demonstrated the conversion of polyoxometalate (POM)-doped ZIF-67 into a stable oxygen evolution electrocatalyst through chemical etching, cation exchange, and thermal annealing steps. Characterization techniques confirmed the synthesis of POM-doped ZIF-67 derived carbon-supported metal oxides, which exhibited structural and compositional advantages leading to low overpotential (306 mV at j=10 mA center dot cm(-2)) and long-term stability under harsh OER conditions (1.0 M aqueous KOH).
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Sebastian Knoll, Matthias Haenle, Alexander K. Mengele, Dieter Sorsche, Sven Rau, Carsten Streb
Summary: CLICK-chemistry is used to covalently link organic molecules with azides and alkynes. This study demonstrates the attachment of oligoaromatic organic moieties to Dawson-type polyoxometalates using CLICK-chemistry. The versatility and supramolecular chemistry of these systems are explored, and the charge-transfer behavior is found to depend on the size of the oligoaromatic pi-system.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Daniel J. Kowalski, Catriona M. MacGregor, De-Liang Long, Nicola L. Bell, Leroy Cronin
Summary: Library generation experiments are important in chemistry for discovering new materials, methods, and models, but generating high quality libraries is challenging. This study demonstrates the automation of library generation workflows using coordination chemistry and automated hardware. Directed exploration and diversity analysis of a process space was achieved, leading to unexpected discoveries of new complexes. The engineering of serendipity through the appearance of unexpected ligands highlights the potential of this approach.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Daniel Costabel, Afshin Nabiyan, Avinash Chettri, Franz Jacobi, Magdalena Heiland, Julien Guthmuller, Stephan Kupfer, Maria Waechtler, Benjamin Dietzek-Ivansic, Carsten Streb, Felix H. Schacher, Kalina Peneva
Summary: We present a photocatalytic setup using the organic photosensitizer diiodo-BODIPY, the non-precious-metal-based hydrogen evolution reaction catalyst (NH4)2[Mo3S13], and a polyampholytic unimolecular matrix poly(dehydroalanine)-graft-poly(ethylene glycol) in water. The system exhibits remarkable performance with high turnover numbers (TON > 7300) and turnover frequencies (TOF > 450 h-1), comparable to noble-metal-containing systems. Excited-state absorption spectra confirm the formation of a long-lived triplet state of the photosensitizer in both water and organic media. This system serves as a blueprint for developing noble-metal-free hydrogen evolution reaction in water, allowing for component optimization by modifying the substituent of the photosensitizer and the composition of the catalyst.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Letter
Chemistry, Physical
Yibin Jiang, Abhishek Sharma, Leroy Cronin
Summary: The discrete-dipole approximation (DDA) is widely used for studying the spectral properties of plasmonic nanostructures. However, its high computational cost limits its application in static geometries and makes it impractical for investigating spectral properties during structural transformations. In this study, we developed an efficient method called rank-one decomposition accelerated DDA (RD-DDA) to simulate spectra of dynamically evolving structures. The RD-DDA method can be used to directly investigate the optical properties of nanostructural transformations defined by atomic- or continuum-scale processes, which is crucial for understanding the growth mechanisms of nanoparticles and optimizing their optical properties.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Editorial Material
Chemistry, Multidisciplinary
Carsten Streb
Summary: The atomically precise assembly of metal nanoparticles provides great opportunities for materials chemistry. Ring-shaped polyoxometalates have been used to stabilize Ag-30 nanoparticles with exposed surfaces.
Article
Multidisciplinary Sciences
S. Hessam M. Mehr, Dario Caramelli, Leroy Cronin
Summary: Interpreting chemistry experiment outcomes is slow and biased, limiting data collection and progress in the field. A digital Oracle using probability demonstrated its ability to rediscover historically significant reactions and provide a quantitative criterion for discovery using expert chemists' intuition. This paradigm validates and formalizes the experience and intuition of expert chemists, improving the interpretation of high-dimensional data.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Multidisciplinary
Shujun Li, Yubin Ma, Yue Zhao, Rongji Liu, Yupeng Zhao, Xusheng Dai, Nana Ma, Carsten Streb, Xuenian Chen
Summary: The study demonstrates the activation of molecular hydrogen by polyoxometalate (POM)-based heterogeneous compounds functionalized with Platinum particles. The synergism between a hydrogen spillover mechanism and electron-proton transfer by the POM enables the selective catalytic reduction of olefins and nitroarenes with high functional group tolerance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Abhishek Sharma, Daniel Czegel, Michael Lachmann, Christopher P. Kempes, Sara I. Walker, Leroy Cronin
Summary: Scientists propose assembly theory (AT) as a framework that connects physics and biology. In AT, objects are redefined and measured by their possible formation histories. This theory provides a unified language for explaining selection, evolution, and novelty generation.
Article
Multidisciplinary Sciences
Stefan Repp, Moritz Remmers, Alexandra Stefanie Jessica Rein, Dieter Sorsche, Dandan Gao, Montaha Anjass, Mihail Mondeshki, Luca M. Carrella, Eva Rentschler, Carsten Streb
Summary: In this study, a coupled set of light-dependent and light-independent reaction equilibria controlling the mono- and di- metal-functionalization of a prototype molecular vanadium oxide cluster is reported. Mechanistic analyses reveal that coordination of a Mg2+ ion leads to the formation of mono-functionalized compound and release of a placeholder cation. Irradiation with visible light results in one-electron reduction, exchange of the second placeholder cation, and formation/crystallization of the di-metal-functionalized compound. Furthermore, the study demonstrates the feasibility of applying this synthetic concept to other metal cations.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Daniel J. Kowalski, Catriona M. MacGregor, De-Liang Long, Nicola L. Bell, Leroy Cronin
Summary: Library generation experiments are crucial in chemistry for discovering new materials, methods, and models. This study demonstrates the automation of workflows using coordination chemistry for library generation. Validation of key synthetic operations, generation of focused libraries in chemical and process space, and development of a new workflow for prospecting library formation were conducted. The study showcases the directed exploration of process space and the engineering of serendipity for discovering unexpected compounds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Przemyslaw Frei, Philip J. Kitson, Alexander X. Jones, Leroy Cronin
Summary: Performing chemical transformations in a standard way is important for accessibility to high value reagents. This study presents a new concept in reactionware design using 3D printing, allowing the generation of high value compounds. By treating integrated reactor sequences as modular, different synthetic pathways can be selected.
Article
Electrochemistry
Kristine Laws, Marcus Tze-Kiat Ng, Abhishek Sharma, Yibin Jiang, Alexander J. S. Hammer, Leroy Cronin
Summary: This study developed a closed-loop robotic platform driven by a probabilistic algorithm for synthesis and electrochemical characterization. It successfully explored the redox behavior of different polyoxometalates (POMs) precursors and identified 24 complex solutions with significantly different redox activity.
Article
Multidisciplinary Sciences
Abhishek Sharma, Daniel Czegel, Michael Lachmann, Christopher P. Kempes, Sara I. Walker, Leroy Cronin
Summary: Scientists have struggled to reconcile biological evolution with the laws of physics. To understand the emergence of diverse forms without a design blueprint, a new framework called assembly theory (AT) has been proposed. AT redefines the concept of an object and incorporates selection and novelty generation into the physics of complex objects. It provides a powerful interface between physics and biology, revealing new aspects of physics at the chemical scale.
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)
