Review
Chemistry, Organic
Sayantika Bhakta, Tapas Ghosh
Summary: Nickel-catalyzed cascade reactions have become a valuable tool in the field of organic synthesis, providing comprehensive coverage of different strategies such as photoredox decarboxylative vinylation and asymmetric reductive arylalkynation. These reactions are useful for synthesizing pharmaceutical compounds and bioactive molecules with high selectivity.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yan Xiong, Stanislav Tsitkov, Henry Hess, Oleg Gang, Yifei Zhang
Summary: This study establishes a cascade system using reversible DNA-directed colocalization of enzymes on microspheres to directly evaluate the colocalization effect. In a regime of highly dilute microspheres of particular sizes, the colocalized cascade shows enhanced activity compared to the freely diffusing cascade. The findings provide theoretical support for the rational design of highly efficient multienzyme catalysts.
Article
Chemistry, Physical
Yuwei Li, Li Liu, Hanying Zhao
Summary: By utilizing hydrophobic interaction, multienzyme proteinosomes are fabricated with p-gal, GOx, and HRP on the surfaces in a model system using PDEGMA and bovine serum albumin. The immobilized enzymes show higher bioactivities than the free enzymes, facilitating direct transfer of the product as a substrate from one enzyme molecule to another.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Physical
Sebastian A. Diaz, Priscilla Choo, Eunkeu Oh, Kimihiro Susumu, William P. Klein, Scott A. Walper, David A. Hastman, Teri W. Odom, Igor L. Medintz
Summary: Using nanoparticles as templates can increase the kinetic rates of enzymes, especially in multi-enzyme cascades where enzymes on the same nanoparticle provide advantages such as substrate channeling. The size and curvature of nanoparticles have a significant impact on the kinetics of cascade reactions, with different shaped nanoparticles achieving equivalent enhancements in kinetics.
Article
Chemistry, Multidisciplinary
Wenshu Cong, Li Meng, Yuanjie Pan, Han Wang, Jiahui Zhu, Yuanyu Huang, Qingli Huang
Summary: Population aging is a global issue, and this study presents a novel approach using Pd-based single-atom nanozymes to improve mitochondrial function and attenuate aging. The nanozyme mimics enzyme activities in the mitochondrial respiratory chain and enhances mitochondrial activities and abundance. Additionally, it demonstrates excellent anti-aging and neuroprotective effects through the activation of the mitochondrial unfolded protein response (UPRmt) pathway.
Article
Engineering, Environmental
Hao Yuan, Shuting Yi, Lufan Jia, Sicheng Chen, Ting Guo, Tao Meng
Summary: In this study, a living cell-inspired nanoscale multienzyme complex was designed to enable efficient cascade reactions and enhance the detection sensitivity of biosensors. The systematic study of this nanocomplex can inspire further investigation into the rules of cellular catalytic behaviors.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Sandra Kroell, Teresa Burgahn, Kersten S. Rabe, Matthias Franzreb, Christof M. Niemeyer
Summary: Artificial reconstruction of naturally evolved principles, such as compartmentalization and cascading of multienzyme complexes, offers enormous potential for the development of biocatalytic materials and processes. DNA origami nanostructures (DON) have proven to be an exceptionally powerful tool for studying the fundamental processes in biocatalytic cascades. The results show that microscale compartmentalization strongly influences the productivity of the cascade, while nanoscale enzyme arrangement has no influence but can be modulated by the insertion of a diffusion barrier.
Article
Chemistry, Multidisciplinary
Daniel Kracher, Robert Kourist
Summary: Combining the unparalleled stereoselectivity of enzymes with the efficiency of chemical catalysis offers advantages, but broad applicability has not been achieved yet; challenges such as catalyst stability, solvent preferences, and cross-reactivities need to be addressed; physical separation of individual reaction steps through compartmentalization can overcome incompatibility problems in multistep cascade reactions.
CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY
(2021)
Article
Chemistry, Physical
Xiaoqiang Wang, Jiqiang Li, Lina Li, Lipeng Zhu, Fang Huang
Summary: The fusion enzyme design of UGT76G1 and UGT91C1 enables the production of RM from rebaudioside A, with an enhanced synthesis rate by 1.8-fold using a peptide linker. Overexpression of the fusion enzyme in P. pastoris cells shows higher catalytic efficiency, thermostability, and recyclability compared to separate expression or mixed purified enzymes. This study provides a promising approach for the industrial preparation of RM.
MOLECULAR CATALYSIS
(2023)
Article
Chemistry, Physical
Shih-Chun Wei, Amit Nain, Yu-Feng Lin, Ren-Siang Wu, Pavitra Srivastava, Lung Chang, Yu-Fen Huang, Huan-Tsung Chang, Kuan-Ting Chuang, Chih-Ching Huang
Summary: Bacterial infection in chronic wounds can be effectively treated using light-triggered carbon dot liposomes (CDsomes) to accelerate the healing process by targeting the inflammation and proliferation phase.
Article
Chemistry, Organic
Linpeng Liu, Yanyu Jian, Weigao Hu, Shaohu Zhao, Zhang-Jie Shi, Nicklas Selander, Taigang Zhou
Summary: A method for radical cyclization and ring-opening of oxime esters with diselenides has been developed. Both Ni(0) and Fe(ii) catalysts can be used for the selenylation of olefin-containing and cyclic oxime ester derivatives. Using this method, a variety of functionalized pyrrolines and alkyl nitriles can be synthesized in good yields. Additionally, a mechanism involving iminyl radical and carbon-centered radical intermediates has been proposed.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Richiro Ushimaru, Ikuro Abe
Summary: This review summarizes recent discoveries that have significantly expanded our understanding of unusual nonheme iron enzyme catalysis in natural product biosynthesis.
Article
Chemistry, Organic
Jonathan P. Knowles, Hannah G. Steeds, Maria Schwarz, Francesca Latter, Kevin Booker-Milburn
Summary: This method transforms simple starting materials into complex tetracyclic products with potential medicinal chemistry applications through a sophisticated chemical catalysis process.
Article
Chemistry, Analytical
Lulu Qu, Xuejiao Fang, Tianhua Xie, Hui Xu, Guohai Yang, Weijie Liu
Summary: This study developed a biomimetic nanozyme capable of triggering catalytic cascade reactions for glucose sensing and bactericidal action, successfully applied for real-time glucose sensing. This artificial enzyme captures the complexity and function of natural systems, providing a new effective route for defect engineering in food preservation.
SENSORS AND ACTUATORS B-CHEMICAL
(2022)
Article
Chemistry, Applied
Elisa Vignali, Loredano Pollegioni, Giovanna Di Nardo, Francesca Valetti, Silvia Gazzola, Gianfranco Gilardi, Elena Rosini
Summary: This study reported the first multi-enzymatic, one-pot bioconversion process of vanillin into ccMA, achieving high yield in a lab-scale procedure within 30 hours. This research demonstrates a sustainable alternative for producing high value added products from renewable resources.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Geosciences, Multidisciplinary
C. Furusho-Percot, K. Goergen, C. Hartick, L. Poshyvailo-Strube, S. Kollet
Summary: Climate change increases the frequency and intensity of heat waves, which have multiple adverse effects on ecosystems, human health, societies, and the economy. This study shows that improving hydrological process representation in regional climate models can lead to more accurate simulation of heat wave metrics.
GEOPHYSICAL RESEARCH LETTERS
(2022)
Article
Chemistry, Physical
Mathijs Janssen, Taras Verkholyak, Andrij Kuzmak, Svyatoslav Kondrat
Summary: Innovative approaches, such as using supercapacitors, are necessary to meet the increasing global energy demand sustainably. This study focuses on the conversion of waste heat to electricity using supercapacitors and presents an analytically-solvable model to identify optimal conditions. The research reveals that Stirling and Ericsson-like charging cycles yield the most work under different operating limitations, and narrow pores matching the ion size maximize energy storage. Furthermore, moderately ionophilic pores outperform ionophobic and strongly ionophilic pores in heat-to-electricity conversion.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Review
Chemistry, Multidisciplinary
Svyatoslav Kondrat, Guang Feng, Fernando Bresme, Michael Urbakh, Alexei A. Kornyshev
Summary: Room-temperature ionic liquids (RTILs) have diverse applications and exhibit fascinating structural and dynamic phenomena when confined in nanostructures. This review analyzes the physical phenomena, theoretical models, and simulation approaches that study the properties of confined RTILs. The review highlights the importance of molecular simulations in providing microscopic insights and discusses the challenges and applicability of different simulation approaches.
Article
Physics, Multidisciplinary
Tomasz Skora, Mathijs Janssen, Andreas Carlson, Svyatoslav Kondrat
Summary: Macromolecular crowding can have significant impacts on various biophysical processes, including diffusion, gene expression, cell growth, and senescence. However, the effects of crowding on reactions, especially multivalent binding, are not fully understood. In this study, we used scaled particle theory and molecular simulation to investigate the binding of monovalent to divalent biomolecules. Our findings show that crowding can greatly enhance or reduce cooperativity, depending on the sizes of the involved molecular complexes. Furthermore, crowding can enable binding that would not occur otherwise.
PHYSICAL REVIEW LETTERS
(2023)
Article
Multidisciplinary Sciences
Julian Schmitz, Birgit Stute, Sarah Taeuber, Dietrich Kohlheyer, Eric von Lieres, Alexander Gruenberger
Summary: This paper presents an easy-to-implement cell retention concept to prevent cells from leaving microfluidic cultivation chambers, enabling reliable single-cell growth studies.
SCIENTIFIC REPORTS
(2023)
Article
Computer Science, Interdisciplinary Applications
Jan Michael Breuer, Samuel Leweke, Johannes Schmoelder, Gregor Gassner, Eric von Lieres
Summary: We have developed spatial arbitrary order DG methods for three commonly used liquid chromatography models, and implemented them in the open source software CADET, providing efficient implementations publicly for the first time. Validation and benchmarking against the original finite volume CADET code show great performance advantages for DG, depending on the problem size. For a four-component steric mass action GRM model, we achieve a speed-up of an order of magnitude within the typical range of engineering applications. We have also explored the performance of a collocation Legendre-Gauss-Lobatto quadrature DG method in comparison to an exact integration DG method, finding a slight advantage for the collocation DG method in performance benchmarks.
COMPUTERS & CHEMICAL ENGINEERING
(2023)
Article
Computer Science, Interdisciplinary Applications
Jayghosh Subodh Rao, Andreas Puettmann, Siarhei Khirevich, Ulrich Tallarek, Christophe Geuzaine, Marek Behr, Eric von Lieres
Summary: Numerical simulations of chromatography are traditionally performed using reduced-order models, but we present a high-definition model with spatially resolved geometry. The model is solved using a stabilized space-time finite element method on massively parallel high-performance computers. The simulations provide insight into the impact of particle size distribution on velocity and concentration profiles, as well as breakthrough curves. The high-definition data can be used to identify and calibrate reduced-order models for process design and optimization.
COMPUTERS & CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Physical
Edyta Slyk, Tomasz Skora, Svyatoslav Kondrat
Summary: Immunoglobulin G (IgG) is the most common type of antibody found in blood and extracellular fluids. This study develops a coarse-grained model of IgG and uses simulations to investigate the effects of macromolecular crowding on IgG's flexibility and binding kinetics. The results show that crowding slightly affects IgG's flexibility but has different effects on the diffusion and binding kinetics compared to smaller molecules.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Physics, Multidisciplinary
Jie Yang, Svyatoslav Kondrat, Cheng Lian, Honglai Liu, Alexander Schlaich, Christian Holm
Summary: In this study, the influence of solvent on the structure and ionic screening of electrolytes under slit confinement and in contact with a reservoir was investigated using classical density functional theory. It was found that spatially resolving solvent molecules is essential for understanding the ion structure, excess ion adsorption, and pressure exerted on the walls. While there were only moderate differences observed in the pressure oscillations and decay lengths based on the ion diameter and Debye length, the crossover to the hard-core-dominated regime depended sensitively on the relative permittivity, ion concentration, and other factors.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Physical
Henrik Jaeger, Alexander Schlaich, Jie Yang, Cheng Lian, Svyatoslav Kondrat, Christian Holm
Summary: The emergence of anomalously large screening lengths at high ion concentrations in room-temperature ionic liquids and concentrated electrolytes, known as underscreening, challenges classical theories and our understanding of electrostatic correlations. Despite extensive experimental, analytical, and simulation efforts, the origin of this long-range screening remains elusive.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Physical
Ganji Seeta Rama Raju, Svyatoslav Kondrat, Nilesh R. Chodankar, Seung-Kyu Hwang, Jeong Han Lee, Teng Long, Eluri Pavitra, Swati J. Patil, Kugalur Shanmugam Ranjith, M. V. Basaveswara Rao, Peng Wu, Kwang Chul Roh, Yun Suk Huh, Young-Kyu Han
Summary: Hierarchically-porous activated carbons derived from Miscanthus sinensis exhibit high specific capacitance and fast charging in KOH electrolyte. By adding K3Fe(CN)6 redox species to the electrolyte, the capacitance of the SHAC electrode increases significantly in a hybrid electrolyte.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Anna Seltmann, Taras Verkholyak, Dariusz Golowicz, Emmanuel Pamete, Andrij Kuzmak, Volker Presser, Svyatoslav Kondrat
Summary: Ionic liquid mixtures show promise as electrolytes for supercapacitors, particularly under negative potential differences. However, for two-electrode cells, they are only beneficial at low and intermediate voltages, while neat ionic liquids perform better at higher voltages. We also discovered subtle correlations between ion distribution and pore accessibility, and suggested approaches to increase energy density.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Environmental Sciences
Liubov Poshyvailo-Strube, Rolf Mueller, Stephan Fueglistaler, Michaela Hegglin, Johannes C. Laube, C. Michael Volk, Felix Ploeger
Summary: The stratospheric meridional overturning circulation plays a crucial role in controlling the composition and climate of the stratosphere. This study explores how the mean age of air trends can be estimated using a combination of stratospheric water vapor (H2O) and methane (CH4) data. The results reveal the uncertainties in these estimations and offer practical advice for obtaining more reliable results.
ATMOSPHERIC CHEMISTRY AND PHYSICS
(2022)
Article
Chemistry, Physical
Edyta Slyk, Tomasz Skora, Svyatoslav Kondrat
Summary: The softness and shape of macromolecules in a macromolecularly crowded environment play crucial roles in determining diffusion. Soft crowders generally slow down diffusion less effectively than hard crowders, but elongated macromolecules may diffuse even faster in hard crowders.
Article
Chemistry, Physical
Tangming Mo, Liang Zeng, Zhenxiang Wang, Svyatoslav Kondrat, Guang Feng
Summary: Asymmetric behaviors of capacitance and charging dynamics in nanoporous supercapacitors play a crucial role in the optimal design of supercapacitors. Molecular dynamics simulations reveal the asymmetric features of porous supercapacitors and their effects on capacitance and charging dynamics. The response of ions to an applied cell voltage influences the capacitance and charging dynamics, and symmetrizing this response can enhance the power density of supercapacitors.
GREEN ENERGY & ENVIRONMENT
(2022)
