Article
Chemistry, Physical
Benedikt Soeldner, Kristof Grohe, Peter Neidig, Jelena Auch, Sebastian Blach, Alexander Klein, Suresh K. Vasa, Lars V. Schaefer, Rasmus Linser
Summary: Understanding macromolecular function, interactions, and stability requires detailed assessment of conformational ensembles. Limited by the qualitative or low abundance of solid-state nuclear magnetic resonance internuclear distance information, accurately elucidating the spatial dynamics of solid proteins at physiological temperatures is challenging. However, this study demonstrates unprecedented access to abundant proton-proton internuclear distances, enabling accurate molecular dynamics simulations and providing atomic-level spatial details of conformational dynamics in various biomolecular systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Igor d'Anciaes Almeida Silva, Ettore Bartalucci, Carsten Bolm, Thomas Wiegand
Summary: Recent studies have shown that mechanochemical strategies are beneficial for directed conversions of organic compounds. However, finding new reactions has been challenging due to the lack of mechanistic understanding of mechanochemical reaction events. Spectroscopic techniques play a crucial role in addressing these questions. In this overview, the opportunities and challenges of solid-state nuclear magnetic resonance (NMR) spectroscopy in the field of organic mechanochemistry are discussed. The strengths of solid-state NMR in ex situ structure characterization, differentiating polymorphs, NMR-crystallographic structure-determination protocols, and detecting weak noncovalent interactions in molecular-recognition events using proton-detected solid-state NMR experiments at fast MAS frequencies are highlighted.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Perrine M. R. Wingering, Silvia Hohnstein, Felix Kraemer, Melina E. A. Dilanas, Cristina Ruiz-Martinez, Ignacio Fernandez, Frank Breher
Summary: The synthesis and characterization of rare earth element complexes (Ln=Y, La, Sm, Lu, Ce) of several podant & kappa;N-6-coordinating ligands were conducted. The structural properties of the complexes were studied using X-ray diffraction and advanced NMR methods. To evaluate the donor capabilities of the ligands, cyclic voltammetry, absorption experiments, and Y-89 NMR chemical shift analysis were performed. Quantum chemical calculations were also used to support the experimental findings. Furthermore, coordination competition studies were carried out using H-1 and P-31 NMR spectroscopy to investigate the correlation with donor properties and selectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Chemistry, Multidisciplinary
Boran Tao, Dailin Zhong, Hongda Li, Guofu Wang, Haixin Chang
Summary: Since the breakthrough in 2018, research on halide solid-state electrolytes (SSEs) has gained momentum. Halide SSEs have more balanced properties compared to oxide and sulfide SSEs, making them suitable for all-solid-state batteries (ASSBs). This article provides a comprehensive overview of halide SSEs, including screening principles, structural design theories, substitution strategies, moisture resistance mechanisms, synthesis methods, and application prospects in ASSBs.
Review
Chemistry, Multidisciplinary
Sahil Ahlawat, Kaustubh R. Mote, Nils-Alexander Lakomek, Vipin Agarwal
Summary: In the past two decades, solid-state nuclear magnetic resonance (ssNMR) spectroscopy has evolved from investigating small molecules and industrial polymers to decrypting complex biological systems. This transformation is due to improvements in hardware design, sample preparation, and sensitivity. This review discusses state-of-the-art ssNMR methods and recent developments in signal filtering, proton methodologies, and data acquisition speed in fast magic-angle spinning (MAS) systems.
Article
Chemistry, Physical
Clayton J. Dahlman, Rhys M. Kennard, Piotr Paluch, Naveen R. Venkatesan, Michael L. Chabinyc, G. N. Manjunatha Reddy
Summary: Layered hybrid organic-inorganic perovskites, such as the lead halide Ruddlesden-Popper (RP) series, exhibit tunable optoelectronic properties due to dynamic interactions between the ionic perovskite substructure and organic spacer cations. Solid-state NMR spectroscopy was used to characterize the static and dynamic structures of linear alkylammonium and aromatic spacers in lead iodide RP phases, revealing different site-specific rigidity trends for short and long spacers. The study highlights the interplay between spacer interactions with lead iodide octahedra and van der Waals forces in contributing to a variety of site-specific dynamics and structural distortions at intermediate time scales.
CHEMISTRY OF MATERIALS
(2021)
Article
Polymer Science
Stepan A. Ostanin, Maxim Mokeev, Dmitry Pikhurov, Aleksandr S. Sakhatskii, Vjacheslav V. Zuev
Summary: Aromatic-oxyaliphatic polyurethanes were synthesized with varying mass fractions of components, including fluorinated fragments, and their rigid domains were found to be formed by units containing urethane bonds as well as oxyethylene fragments. The urethane bonds and oxyethylene fragments were incorporated into both rigid and soft phases, showing good agreement with the Cooper and Tobolsky model under specific solubility parameters for different segments.
Article
Chemistry, Physical
Feng Shi, Lili Hu, Yun Cui, Jinjun Ren
Summary: Glasses in the xLa(2)O(3)-yAl(2)O(3)-(100 - x - y)NaPO3 system were synthesized and characterized using advanced multinuclei solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy. The study revealed that the depolymerization of the glass Q(2) structure by La2O3 and Al2O3 resulted in the formation of multiple phosphorus species. La coordination number was predominantly nine, with some La atoms transitioning to lower coordination with the addition of Al2O3, and the connection methods between Al/P and La/P were found to be different.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Energy & Fuels
Francesco Panattoni, Jonathan Mitchell, Edmund J. Fordham, Ravinath Kausik, Clare P. Grey, Pieter C. M. M. Magusin
Summary: The study utilized high-field, solid-state NMR methods to analyze kerogen isolates of different maturity levels, finding that the aromatic/aliphatic ratio of kerogen increases with maturity. This increase in ratio is reflected in the H-1 MAS NMR spectra by the intensity ratio of aliphatic-to-aromatic signals, suggesting a decrease in kerogen proton density during maturation.
Review
Biochemistry & Molecular Biology
Vitaly Volkov, Alexander Chernyak, Nikita A. Slesarenko, Irina A. Avilova
Summary: This review focuses on the progress of solvation and mobility studies in solid electrolyte, particularly ion-exchange membranes and composite materials, using NMR techniques. The applications of various NMR techniques are discussed, and comparisons are made between diffusion coefficients and ionic conductivity data. The microscopic mechanism of ionic transfer is also explored.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Analytical
Vincent Moxley-Paquette, Daniel Lane, Katrina Steiner, Katelyn Downey, Peter M. Costa, Daniel H. Lysak, Kiera Ronda, Ronald Soong, Dimitri Zverev, Peter De Castro, Thomas Frei, Juerg Stuessi, Danijela Al Adwan-Stojilkovic, Stephan Graf, Simon Gloor, Daniel Schmidig, Rainer Kuemmerle, Till Kuehn, Falko Busse, Marcel Utz, Andressa Lacerda, Ben Nashman, Larry Albert, Jens Anders, Andre J. Simpson
Summary: Understanding the impact of toxins on invertebrate eggs and egg banks is crucial in environmental research. However, studying these tiny structures using conventional NMR spectroscopy is challenging. This study investigates methods to improve the quality of resonators and enhance the detection limit by enhancing the magnetic susceptibility. Copper-plated aluminum resonators showed the best performance in terms of line shape and SNR. The improved LOD of these resonators allowed for the first H-1-C-13 HMQC of a single intact C-13-labeled Daphnia magna egg, which is important for future screening programs.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Vincent Moxley-Paquette, Daniel Lane, Katrina Steiner, Katelyn Downey, Peter M. Costa, Daniel H. Lysak, Kiera Ronda, Ronald Soong, Dimitri Zverev, Peter De Castro, Thomas Frei, Juerg Stuessi, Danijela Al Adwan-Stojilkovic, Stephan Graf, Simon Gloor, Daniel Schmidig, Rainer Kuemmerle, Till Kuehn, Falko Busse, Marcel Utz, Andressa Lacerda, Ben Nashman, Larry Albert, Jens Anders, Andre J. Simpson
Summary: Understanding the impact of toxins on invertebrate eggs is crucial in environmental research, but studying them using conventional NMR spectroscopy is challenging due to their small size. Microcoil technology has been used to improve the sensitivity of NMR, but the line shape of the resonator needs improvement. This study investigates different approaches to enhance the magnetic susceptibility of the resonator while maintaining the versatility of coil milling. Using copper-plated aluminum resonators resulted in improved line shape and sensitivity, allowing for the first H-1-C-13 HMQC of a single intact C-13-labeled Daphnia magna egg.
ANALYTICAL CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Mokwon Kim, Hyunpyo Lee, Hyuk Jae Kwon, Seong-Min Bak, Cherno Jaye, Daniel A. Fischer, Gabin Yoon, Jung O. Park, Dong-Hwa Seo, Sang Bok Ma, Dongmin Im
Summary: A newly proposed strategy involves designing a highly conductive ruthenium-based composite as a carbon-free cathode to improve the cycle life and capacity of solid-state lithium-oxygen batteries. By utilizing this approach, the batteries achieved a specific capacity of 200 milliampere hour per gram over 665 discharge/charge cycles, showcasing a notable improvement compared to existing cathodes.
Article
Chemistry, Multidisciplinary
ShengQi Xiang, Cecilia Pinto, Marc Baldus
Summary: Membrane proteins play important biological roles by forming complexes in cell membranes. This study focuses on understanding the role of the lipoprotein BamC in the assembly of the beta-barrel assembly machinery (BAM) complex in lipid bilayers. By developing a selective preparation scheme and using proton-detected solid-state NMR methods, the researchers were able to investigate the structure and dynamics of BamC embedded in the entire BAM complex in lipid bilayers. This approach provides insights into the formation and functioning of membrane protein complexes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Linda Cerofolini, Kristian Vasa, Elisa Bianconi, Maria Salobehaj, Giulia Cappelli, Alice Bonciani, Giulia Licciardi, Anna Perez-Rafols, Luis Padilla-Cortes, Sabrina Antonacci, Domenico Rizzo, Enrico Ravera, Caterina Viglianisi, Vito Calderone, Giacomo Parigi, Claudio Luchinat, Antonio Macchiarulo, Stefano Menichetti, Marco Fragai
Summary: Several protein-drug conjugates are currently used in cancer therapy, relying on covalently attached cytotoxic organic compounds or non-covalent interactions. Human transthyretin (TTR) has been identified as a potential carrier protein for cytotoxic drug delivery. This study demonstrates the importance of integrating multiple biophysical and structural techniques, such as microscale thermophoresis, X-ray crystallography, and NMR. Solid-state NMR is particularly valuable in revealing ligand binding effects and their impact on macromolecular complex stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Chemical
Guangying Chen, Guangjie Chen, Maurizio Peruzzini, Rui Zhang, Francesco Barzagli
Summary: The aqueous blends of three different amines were tested as sorbents for CO2 capture processes, showing improved desorption performance and lower energy consumption compared to conventional MEA.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Energy & Fuels
Guangjie Chen, Guangying Chen, Maurizio Peruzzini, Francesco Barzagli, Rui Zhang
Summary: This study evaluated the CO2 capture performance of aqueous blends of benzylamine (BZA) and ethanolamine (MEA). The results showed that blends with a higher relative amount of MEA had higher CO2 loading, and the alkalinity of MEA played a crucial role in achieving higher loading.
Article
Engineering, Environmental
Federico Atzori, Francesco Barzagli, Alberto Varone, Giacomo Cao, Alessandro Concas
Summary: It is well known that CO2 capture and re-use is one of the main challenges to tackle global warming. Aqueous ammonia solutions have shown promising potential as sorbents for CO2 capture, offering higher absorption capacity, lower energy requirements, and greater resistance to degradation compared to conventional alkanolamines. This study investigates the chemical absorption of CO2 in aqueous NH3 solutions and proposes a mathematical model to quantify the capture efficiency dynamics and sorbent composition. The results validate the model's effectiveness in designing and optimizing the capture process, considering the effects of temperature and sorbent concentration.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Rui Zhang, Ruixi Liu, Francesco Barzagli, Meher Geetika Sanku, Chao 'en Li, Min Xiao
Summary: Mixing different amines is a common method for developing better solvents for CO2 capture. The study investigated CO2 absorption in monoethanolamine (MEA), methyldiethanolamine (MDEA), and their mixtures. The speciation profiles and CO2 loading were analyzed using NMR to understand the competition and coordination between MEA and MDEA in the key reactions for CO2 absorption. The calculated CO2 loading agreed well with experimental data.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Thermodynamics
Xinwei He, Hang He, Francesco Barzagli, Mohammad Waleed Amer, Chao'en Li, Rui Zhang
Summary: Blending two or more amines has been recognized as an efficient strategy for CO2 capture. Four new dual-amine aqueous blends based on 2-dimethylamino-2-methyl-1-propanol (2DMA2M1P) mixed with different primary and secondary amines were formulated and evaluated. The blends showed appreciable CO2 capture performance and, importantly, better desorption performance than conventional MEA.
Article
Engineering, Chemical
Suzhou Dai, Yonggao Yin, Yikai Wang, Xuanlin Liu, Maurizio Peruzzini, Francesco Barzagli
Summary: This study experimentally investigated the influence of solvents on the chemical equilibrium of ammonium carbamate (AC). The results confirmed the solvent effect on the equilibrium pressure of AC and established an equilibrium pressure-temperature-concentration relationship of AC solution. These findings provide crucial parameters for the design and operation of low-grade heat management and utilization systems based on AC.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Energy & Fuels
Mohammad W. Amer, Eman M. Khdeir, Leen E. Haimour, Sereen I. Aljariri Alhesan, Francesco Barrzagli, Khitam A. Alzughoul
Summary: The study characterizes the structural features of Jordanian tar sand using various analytical techniques. The tar sand has low volatile matter content and significant nitrogen content. The recovery of bitumen from the tar sand was evaluated using different extraction techniques, with the highest recovery achieved using the non-aqueous solvent extraction method. The extracted bitumen was characterized and found to have high oxygen and sulfur concentrations.
INTERNATIONAL JOURNAL OF COAL PREPARATION AND UTILIZATION
(2023)
Article
Chemistry, Multidisciplinary
Rui Zhang, Yufan Li, Yiming Zhang, Ting Li, Luning Yang, Chao'en Li, Francesco Barzagli, Zhien Zhang
Summary: Recently, low-cost environmentally friendly sepiolite clay has been evaluated as a support for metal oxide catalysts to enhance the desorption of CO2. The study shows that the catalytic performance of Fe2O3-SEP is stable and efficient, and the high mesoporous specific surface area and acid sites contribute to its activity. This work highlights the potential of SEP as a low-cost and competitive catalyst carrier for CO2 capture.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Review
Engineering, Chemical
Yufan Li, Francesco Barzagli, Peng Liu, Xiaoan Zhang, Zhao Yang, Min Xiao, Yangqiang Huang, Xiao Luo, Chao'en Li, He'an Luo, Rui Zhang
Summary: Stainless steel is commonly used for high-pressure hydrogen storage, but hydrogen can cause embrittlement, reducing the lifetime and hindering the development of the hydrogen industry. Adding hydrogen permeation barrier coatings to stainless steel surface is an effective way to delay or prevent hydrogen permeation. This review investigates the mechanism and working principle of hydrogen permeation, classifies hydrogen barrier coatings, analyzes their influence factors and defects, and summarizes preparation techniques and evaluation methods. Polymer composites strengthened by graphene and other materials are considered more competitive.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Engineering, Chemical
Rui Zhang, Yufan Li, Xinwei He, Yingjie Niu, Chao 'en Li, Mohammad Waleed Amer, Francesco Barzagli
Summary: Mixing different amines is a smart strategy for developing efficient aqueous solutions for CO2 capture, and adding a third amine can further enhance the performance of dual-amine blends. In this study, three new aqueous solutions containing 2DMA2M1P, MEA, and AMP were formulated and their CO2 capture performance was evaluated. The trio-amine blends exhibited superior CO2 equilibrium solubility and desorption performance compared to the benchmark MEA and dual-amine mixtures.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Umair H. Bhatti, Masood S. Alivand, Francesco Barzagli, Meher Geetika Sanku, Jorge Gascon, Kathryn A. Mumford
Summary: Catalyst-facilitated amine regeneration provides an energy-efficient and economically feasible CO2 capture process. Glucose-derived carbon sphere nanocatalysts with isethionic acid functionalization were developed to optimize the CO2 desorption rate of CO2-loaded monoethanolamine solutions. The synthesized catalysts accelerated the CO2 desorption rate by up to 108% and reduced the heat duty by approximately 10.8% compared to traditional uncatalyzed regeneration. These catalysts can be separated easily, stable in cyclic uses, and suitable for industrial-scale applications. Regenerating solvents with catalysts at 86°C allows the use of low-grade industrial waste heat, enabling efficient CO2 capture facilities to be installed at various industrial sites for achieving net zero emissions by 2050.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Energy & Fuels
Rui Zhang, Haonan Liu, Ruixi Liu, Yingjie Niu, Luning Yang, Francesco Barzagli, Chao'en Li, Min Xiao
Summary: This study investigates the CO2 absorption performance of amine blends and elucidates the reaction mechanisms and species formed during CO2 capture using experimental methods and 13C NMR spectroscopy. An excess property model is introduced to accurately predict CO2 equilibrium solubility.
GAS SCIENCE AND ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
F. Telesio, F. Mezzadri, M. Serrano-Ruiz, M. Peruzzini, F. Bisio, S. Heun, F. Fabbri
Summary: This study demonstrated the transportation of visible light in nanometric niobium stripes coupled with a dielectric polymeric layer and utilizing the remotely-excited/detected Raman signal of black phosphorus as a probe. The light transport mechanism is attributed to the generation of surface plasmon polaritons at the Nb/polymer interface.
MATERIALS FOR QUANTUM TECHNOLOGY
(2022)
Article
Energy & Fuels
Guangjie Chen, Guangying Chen, Maurizio Peruzzini, Francesco Barzagli, Rui Zhang
Summary: In this study, the CO2 capture performance of aqueous blends of ethanolamine (MEA) and benzylamine (BZA) was evaluated, and the species present during the CO2 absorption process were identified and quantified through 13C NMR. The results showed that a higher relative amount of MEA in the blend is advantageous for achieving higher CO2 loading, and the CO2 absorption heat of the mixtures is comparable to that of individual amines.
Article
Green & Sustainable Science & Technology
Francesco Barzagli, Maurizio Peruzzini, Rui Zhang
Summary: Five different diamines were investigated as liquid sorbents for direct capture of CO2 from air. The capture performance and carbonated species formed in solution were evaluated, and compared to conventional alkanolamine solutions.
CARBON CAPTURE SCIENCE & TECHNOLOGY
(2022)
