Article
Chemistry, Multidisciplinary
Sumit Pal, Antara Reja, Subhajit Bal, Baishakhi Tikader, Dibyendu Das
Summary: In this study, we report the substrate induced generation of a transient catalytic microenvironment from a single amino acid functionalized fatty acid in the presence of cofactor hemin. The catalytic state accessed under non-equilibrium conditions showed accelerated peroxidase activity, leading to substrate degradation and subsequent disassembly. Equilibrated systems could not access the three-dimensional microphases and exhibited significantly lower catalytic activity. Furthermore, the assembled state demonstrated latent catalytic function to hydrolyze a precursor and generate the same substrate, thereby augmenting the lifetime and mechanical properties of the catalytic state through the peroxidase-hydrolase cascade.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Sumit Pal, Antara Reja, Subhajit Bal, Baishakhi Tikader, Dibyendu Das
Summary: This study demonstrates the substrate induced generation of a transient catalytic microenvironment from a single amino acid functionalized fatty acid in the presence of cofactor hemin, leading to accelerated peroxidase activity under non-equilibrium conditions. The assembled state also shows promiscuous catalytic function to hydrolyze a precursor and augment the lifetime and mechanical properties of the catalytic state by exploiting the peroxidase-hydrolase cascade, thus exhibiting protometabolism.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Hao Luo, Eric P. Weeda, Manar Alherech, Colin W. Anson, Steven D. Karlen, Yanbin Cui, Cliff E. Foster, Shannon S. Stahl
Summary: Biomass pretreatment methods can lead to modification, degradation, or low yields of lignin, but catalytic fractionation approaches can effectively separate polymeric sugar and lignin fractions with the help of a catalyst, producing oxygenated aromatics suitable for polymer synthesis and biological funneling to value-added products.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Environmental Sciences
Yang Zhou, Ruizhi Chu, Lulu Fan, Jianqiao Zhao, Weisong Li, Xiaofeng Jiang, Xianliang Meng, Yusai Li, Shi Yu, Yongzhou Wan
Summary: Thermal plasma activation of CH4-CO2 reforming is an efficient and clean technology for utilizing hydrocarbon resources and reducing greenhouse gases. This study investigates the equilibrium state and transformation mechanism of the reaction using experimental, thermodynamic, and kinetic analyses. The results show that the CO2 conversion rate and H2 selectivity decrease with increasing CO2/CH4 ratio, while the CH4 conversion rate and CO selectivity show the opposite trend. Excess CO2 promotes the partial oxidation of CH4, eliminating carbon deposition and achieving higher gas conversion without carbon deposition.
SCIENCE OF THE TOTAL ENVIRONMENT
(2023)
Article
Chemistry, Multidisciplinary
Anna Muhs, Tim Bobrowski, Anna Lielpetere, Wolfgang Schuhmann
Summary: This study presents a new strategy for long-term implantable biosensors, using catalytic enzyme-based biosensors and short potentiometric data acquisition to minimize disturbance to the substrate equilibrium concentration. The biosensor operates under quasi-equilibrium conditions and allows the glucose concentration equilibrium to be quickly restored.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Environmental
R. S. Postma, P. S. F. Mendes, L. Pirro, A. Banerjee, J. W. Thybaut, L. Lefferts
Summary: The interplay between catalytic activation of methane on Fe (c) SiO2 and gas-phase free radical methane coupling under non-oxidative conditions is analyzed by mechanistic modeling and experiments. The model validates the significant contribution of gas-phase reactions responsible for methane conversion and the low-activity induction period in gas-phase methane pyrolysis can be overcome by catalytic activation. Gas-phase reactions determines the selectivity distribution while catalytic reaction only influences the activity of the system.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Wenyao Zhang, Huilong Yan, Qiuwang Wang, Cunlu Zhao
Summary: The study proposes an extended TMS theory applicable to cases with both salinity and temperature gradients, showing good quantitative agreement with experimental data. Results suggest that membrane potential can be enhanced when salinity and temperature gradients are in opposite directions, and can be enhanced or reduced depending on the extent of the TP effect when gradients are in the same direction.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Yu Tang, Yuting Li, Franklin (Feng) Tao
Summary: Scientists worldwide have made significant progress in catalytic transformations of CH4 to chemicals under mild conditions, although challenges remain. Academic research has developed numerous reactions for converting CH4 to oxygenates at relatively low temperatures, but a molecular-level understanding in complex reaction environments under mild conditions is still lacking.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Engineering, Electrical & Electronic
Haowen Zhong, Zhaosheng Teng, Jiangyan Sang, Qiu Tang, Tianyi Deng
Summary: An enhanced bio-impedance demodulation method is proposed in this article to accurately extract impedance from time-domain signals under non-integer period sampling conditions. The proposed method overcomes the limitations of conventional approaches by using a maximum amplitude spectral line to replace hidden spectral values and establishing an optimized bio-impedance demodulation formula that accounts for spectral leakage error. Simulations and experiments on circuits and biological tissues demonstrate the effectiveness of the proposed approach in accurately demodulating impedance at arbitrary frequencies.
IEEE TRANSACTIONS ON INSTRUMENTATION AND MEASUREMENT
(2023)
Article
Chemistry, Multidisciplinary
Kyeounghak Kim, Sangwook Joo, Rui Huang, Hyung Jun Kim, Guntae Kim, Jeong Woo Han
Summary: This study used density functional theory calculations and in situ X-ray diffraction spectroscopy experiments to investigate the phase transition and ex-solution processes in Co-doped Pr0.5Ba0.5MnO3. The results revealed that the selective formation of oxygen vacancies at the Pr layer plays a key role in the transition to layered perovskite. Additionally, the ex-solved Co nanoparticles exhibited higher catalytic activity for CO oxidation compared to the doped counterpart, offering insights for designing highly-active perovskite-based redox catalysts.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Multidisciplinary Sciences
Hannah L. Rutledge, Brian D. Cook, Hoang P. M. Nguyen, Mark A. Herzik, F. Akif Tezcan
Summary: This study reports cryo-electron microscopy structures of the nitrogenase complex prepared under enzymatic turnover conditions. The research reveals that asymmetry plays a critical role in various aspects of the nitrogenase mechanism.
Article
Multidisciplinary Sciences
Christos S. Karamitros, Kyle Murray, Brent Winemiller, Candice Lamb, Everett M. Stone, Sheena D'Arcy, Kenneth A. Johnson, George Georgiou
Summary: The dynamic motions of enzymes have a significant impact on the reaction pathway. Mutations in enzymes can increase catalytic activity by affecting conformational flexibility and thereby modulating the rate of the chemical step.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Lidai Zhou, Min Zhang, Caixia Liu, Yan Zhang, Huijun Wang, Ziyin Zhang
Summary: This study evaluated the catalytic properties of Ag/CeO2 catalysts prepared by different methods and loadings. The Ag/CeO2-IM catalysts prepared by equal volume impregnation method showed better activity at lower temperatures.
Article
Chemistry, Multidisciplinary
Jiajin Lin, Shuaiqi Zhao, Jin Yang, Wei-Hsiang Huang, Chi-Liang Chen, Tingyu Chen, Yun Zhao, Guangxu Chen, Yongcai Qiu, Lin Gu
Summary: This work reports a PtCo/CoOx/Al2O3 catalyst with PtCo clusters and enriched Pt―O―Co interfaces, which exhibits excellent performance for CO oxidation at low temperatures and humid conditions. The presence of Pt―O―Co interfaces in the catalyst provides a significant number of active sites for oxygen activation and CO2 formation, leading to superior low-temperature activity and long-term stability.
Article
Chemistry, Physical
Lingsong Wang, Huanshun Yin, Suo Wang, Jun Wang, Shiyun Ai
Summary: Bi/BiOCl/Bi2O2CO3 heterojunction with enhanced photocatalytic activity was prepared via one-step hydrothermal process under the synergistic catalysis of Ni2+, showing promising application potential in environmental remediation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Review
Biochemistry & Molecular Biology
Annalisa Tassoni, Tullia Tedeschi, Chiara Zurlini, Ilaria Maria Cigognini, Janos-Istvan Petrusan, Oscar Rodriguez, Simona Neri, Annamaria Celli, Laura Sisti, Patrizia Cinelli, Francesca Signori, Georgios Tsatsos, Marika Bondi, Stefanie Verstringe, Geert Bruggerman, Philippe F. X. Corvini
Article
Chemistry, Multidisciplinary
Sushmitha Chandrabhas, Subhabrata Maiti, Ilaria Fortunati, Camilla Ferrante, Luca Gabrielli, Leonard J. Prins
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Review
Chemistry, Multidisciplinary
Krishnendu Das, Luca Gabrielli, Leonard J. Prins
Summary: Life is a non-equilibrium state of matter sustained by energy expenditure, mostly utilizing chemical energy stored in molecules. Understanding the transfer of chemical energy to biochemical processes is crucial for developing artificial systems with life-like processes. Strategies for controlling the structural organization of organic molecules have been identified based on distinguishable physical-organic foundations, with examples from biology and chemistry illustrating their practical implementation and unique opportunities.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Serena Gentile, Erica Del Grosso, Passa E. Pungchai, Elisa Franco, Leonard J. Prins, Francesco Ricci
Summary: The study demonstrates a strategy to allow for the spontaneous reconfiguration of self-assembled DNA polymers using RNA as chemical fuel. By designing orthogonally addressable DNA building blocks, the researchers can temporarily deactivate and reactivate the building blocks to control the final composition of the polymer. This approach suggests a novel route towards developing biomolecular materials that support autonomous spatial reorganization of multiple components through engineered chemical reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Rui Chen, Krishnendu Das, Maria A. Cardona, Luca Gabrielli, Leonard J. Prins
Summary: Cellular functions are regulated through local activation of chemical processes in a complex matrix. Synthetic macroscopic systems with similar capacity allow fundamental studies on the relationship between local molecular events and macroscopic functional properties. This study demonstrates the spontaneous formation of an inhomogeneous hydrogel matrix upon local injection of ATP, leading to the self-assembly of nanoreactors and local upregulation of a chemical reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Erica Del Grosso, Patrick Irmisch, Serena Gentile, Leonard J. Prins, Ralf Seidel, Francesco Ricci
Summary: This study presents a general approach to achieve dissipative control over toehold-mediated strand-displacement, a widely used reaction in DNA nanotechnology. By re-engineering the classic reaction, the high-energy invader strand is converted into a low-energy waste product, allowing the system to spontaneously return to its original state over time. This method enables unique temporal activation of DNA systems and is reversible and highly controllable.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Erica Del Grosso, Elisa Franco, Leonard J. Prins, Francesco Ricci
Summary: DNA nanotechnology is a powerful tool for designing and controlling molecular systems. Dissipative DNA nanotechnology aims to build life-like systems by combining programmable reactions with energy-dissipating processes.
Article
Chemistry, Multidisciplinary
Yingjuan Cao, Luca Gabrielli, Diego Frezzato, Leonard J. Prins
Summary: This study demonstrates the formation of macroscopic ATP concentration gradients in agarose gel and shows that these gradients can be sustained by consuming chemical fuel. Controlled activation of ATP-producing and ATP-consuming reactions through the injection of enzymes allows for the formation of complex fluorescence patterns that change over time as a function of ATP concentrations in the system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Krishnendu Das, Haridas Kar, Rui Chen, Ilaria Fortunati, Camilla Ferrante, Paolo Scrimin, Luca Gabrielli, Leonard J. Prins
Summary: This article describes a self-assembly of surfactant-based structures that rely on a combination of a thermodynamically controlled and a dissipative pathway for their formation. Adenosine triphosphate (ATP) acts as a high-affinity template and triggers the formation of assemblies at low surfactant concentrations. The presence of these assemblies allows for the activation of a dissipative self-assembly process by a weak-affinity substrate. The induced recruitment of additional surfactants by the substrate leads to the spontaneous formation of catalytic hotspots in the ATP-stabilized assemblies, resulting in substrate cleavage. Catalysis can be observed at a surfactant concentration where low catalytic activity is observed in the absence of ATP.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Organic
Flavio della Sala, Elisa Ceresara, Fabrizio Micheli, Stefano Fontana, Leonard J. Prins, Paolo Scrimin
Summary: Cationic, monolayer-protected gold nanoparticles with a multivalent charged surface and a hydrophobic monolayer can effectively bind to phosphatidylinositol (3,4,5)-trisphosphate, a relevant biomarker, with a dissociation constant in the picomolar range. This suggests that these gold nanoparticles can be used for the selective extraction of this molecule from biological fluids.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tommaso Marchetti, Diego Frezzato, Luca Gabrielli, Leonard J. Prins
Summary: An energy ratchet mechanism is used to synthesize a molecule by accelerating the hydrazone-bond formation in the presence of ATP. The hydrolysis of ATP creates a kinetically stable state with a higher concentration of hydrazone compared to the thermodynamic equilibrium. This kinetic state shows enhanced catalytic activity in the hydrolysis of an RNA-model compound.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Maria A. Cardona, Rui Chen, Subhabrata Maiti, Ilaria Fortunati, Camilla Ferrante, Luca Gabrielli, Krishnendu Das, Leonard J. Prins
CHEMICAL COMMUNICATIONS
(2020)