Review
Nanoscience & Nanotechnology
Tianran Sheng, Xun Guan, Chong Liu, Yude Su
Summary: Encapsulating biocatalysts into synthetic host matrixes can enhance their stability and activity, expanding their operational conditions. This review focuses on newly emerged approaches to encapsulating biocatalysts, discussing the advantages and limitations, particularly in encapsulating enzymes in metal-organic frameworks and microbial electrocatalysts on electrodes.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Biochemistry & Molecular Biology
Christoph Diehl, Patrick D. Gerlinger, Nicole Paczia, Tobias J. Erb
Summary: Anaplerosis, a feature of metabolism, has been applied to synthetic in vitro metabolic networks to achieve carbon-positive synthesis of compounds. In this research, anaplerotic strategies were used to access a new-to-nature CO2-fixation pathway and successfully produce 6-deoxyerythronolide B. This work demonstrates the design and customization of anaplerotic modules to enhance and expand synthetic capabilities in complex in vitro reaction networks.
NATURE CHEMICAL BIOLOGY
(2023)
Review
Biochemical Research Methods
Antonin Cros, Gabriela Alfaro-Espinoza, Alberto De Maria, Nicolas T. Wirth, Pablo I. Nikel
Summary: We suggest that deploying synthetic metabolism tailored for biohalogenation presents a unique opportunity for economically attractive and environmentally friendly organohalide production.
CURRENT OPINION IN BIOTECHNOLOGY
(2022)
Article
History & Philosophy Of Science
Milo D. Cornelissen, Henk W. de Regt
Summary: Understanding natural phenomena is important in science, but the concept of scientific understanding has sparked debate in philosophy. This paper examines a case from synthetic chemistry to explore how understanding is achieved in this field. The study reveals that highly idealized models and qualitative concepts are crucial for understanding the synthetic pathway, supporting the notion of non-factivism.
Article
Chemistry, Multidisciplinary
Shuntaro Amano, Massimiliano Esposito, Elisabeth Kreidt, David A. Leigh, Emanuele Penocchio, Benjamin M. W. Roberts
Summary: The framework of information thermodynamics allows us to quantitatively relate information to other thermodynamic parameters and reveals the generation of energy and information flow in the chemical to mechanical process. This is of great significance for understanding the thermodynamic level of molecular motors and has practical implications for machine design.
Article
Chemistry, Multidisciplinary
Alessa Hinzmann, Tobias Betke, Yasuhisa Asano, Harald Groeger
Summary: Nitriles, as a fundamental functional group, pose challenges for efficient and sustainable synthesis. However, a new enzymatic process technology based on aldoxime dehydratase has shown potential in bridging the gap between fine chemicals, pharmaceuticals, and bulk commodity chemicals.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Review
Chemistry, Inorganic & Nuclear
Yi Pan, Zi Han, Shouhui Chen, Kang Wei, Xinlin Wei
Summary: Frequent food safety problems pose a significant threat to people's life and health. Efficient sensing methods are urgently needed for detecting contaminants in food matrix. Metal nanoclusters (MNCs) are promising nanomaterials with superior properties, and can be used to develop effective food safety monitoring technology.
COORDINATION CHEMISTRY REVIEWS
(2023)
Review
Chemistry, Inorganic & Nuclear
Zahra Sharifzadeh, Ali Morsali
Summary: Metal-organic frameworks (MOFs) are widely known and researched in various disciplines due to their specific applications and structural diversity. Amine-functionalized MOFs have gained significant attention, and this review categorizes the synthesis methods and explores the structural changes caused by incorporating amine groups. The review also discusses the excellent applications and the impact of other functional groups on the activity of amine groups in MOFs. Additionally, it presents a comprehensive study on composites derived from amine-MOFs, introducing a new branch of materials for industrial applications. The conclusion discusses the potential opportunities and challenges faced by amine-MOFs, emphasizing the indispensable role of amine functional groups in the design, synthesis, and application of metal-organic structures.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Lukas Friedrich, Gino Cingolani, Ying-Hui Ko, Mariaclara Iaselli, Morena Miciaccia, Maria Grazia Perrone, Konstantin Neukirch, Veronika Bobinger, Daniel Merk, Robert Klaus Hofstetter, Oliver Werz, Andreas Koeberle, Antonio Scilimati, Gisbert Schneider
Summary: The combination of natural products and synthetic molecules provides a new approach for drug discovery based on machine intelligence, creating new molecular designs inspired by bioactive natural products. Experimental results demonstrate that this method can successfully design molecules with specific target activities.
Review
Chemistry, Medicinal
Yuxi Fang, Haonan Li, Bao Ji, Keguang Cheng, Bo Wu, Zhanlin Li, Chao Zheng, Huiming Hua, Dahong Li
Summary: Renieramycins, a member of tetrahydroisoquinoline family of marine natural products, show strong antitumor activities with potential for further drug development and innovation. Researches mainly focus on their pharmacological activities and structural modification for enhanced anti-proliferative effects. However, challenges in extraction and separation hinder their development.
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
(2021)
Article
Engineering, Environmental
Efstratios Nikolaivits, George Taxeidis, Christina Gkountela, Stamatina Vouyiouka, Veselin Maslak, Jasmina Nikodinovic-Runic, Evangelos Topakas
Summary: The uncontrolled release of plastics poses a threat to wildlife and human health. Finding novel polymer-degrading enzymes with diverse properties is crucial for plastic-waste upcycling. This study discovered a barely studied psychrophilic enzyme (MoPE) that can degrade various types of plastics.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Plant Sciences
Sergey Kosourov, Maximilian Bohm, Moritz Senger, Gustav Berggren, Karin Stensjo, Fikret Mamedov, Peter Lindblad, Yagut Allahverdiyeva
Summary: Photosynthetic production of molecular hydrogen is a potential source of renewable energy, but current efficiency levels are too low for industrial applications due to physiological, biochemical, and engineering barriers. Researchers have some understanding of the metabolic pathways and enzymes involved in H-2 production in cyanobacteria and green algae, and have made progress in engineering photosynthetic cell factories to overcome major obstacles to efficient and sustainable H-2 production.
PHYSIOLOGIA PLANTARUM
(2021)
Article
Agriculture, Multidisciplinary
Marina S. Robescu, Francesca Annunziata, Valeria Somma, Cinzia Calvio, Carlo F. Morelli, Giovanna Speranza, Lucia Tamborini, Daniela Ubiali, Andrea Pinto, Teodora Bavaro
Summary: In this study, various gamma-glutamyl peptides with biological activities were successfully synthesized using glutamine as the gamma-glutamyl donor and the gamma-glutamyl transferase from Bacillus subtilis (BsGGT) as the catalyst. The synthesis yields of neuroprotective gamma-glutamyl-taurine and antioxidant ophthalmic acid were relatively high, while the purity of the other two kokumi peptides was affected by the presence of byproducts.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2022)
Article
Agriculture, Multidisciplinary
Marina S. Robescu, Francesca Annunziata, Valeria Somma, Cinzia Calvio, Carlo F. Morelli, Giovanna Speranza, Lucia Tamborini, Daniela Ubiali, Andrea Pinto, Teodora Bavaro
Summary: In this study, a variety of gamma-glutamyl peptides were synthesized through an enzymatic transpeptidation reaction, showing potential biological activities. The use of immobilized BsGGT on glyoxylagarose resulted in high protein immobilization yield. The switch from batch to continuous flow synthesis led to increased productivity but not better impurity control.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2022)
Article
Chemistry, Analytical
Juan Huang, Hongfei Gu, Guo Wang, Rufen Wu, Mengru Sun, Zhengbo Chen
Summary: Two nanozymes, ZnCoFe three-atom nanozyme (TAzyme) and Sn single-atom nanozyme (SAzyme)/Ti3C2T (x), are developed for peroxidase-like catalytic reactions. These nanozymes can catalyze the reactions of hydrogen peroxide (H2O2), 4-aminoantipyrine(4-AAP), and phenolic acids to generate colorimetric products, with different phenolic acids resulting in different color variations. An electronic tongue based on these nanozymes is used for distinguishing phenolic acids, achieving good clustering separation of six different phenolic acids at concentrations of 0.1 μM to 1 mM, as validated by linear discriminant analysis (LDA).
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Holly J. Redman, Ping Huang, Michael Haumann, Mun Hon Cheah, Gustav Berggren
Summary: In this study, a molecular mimic of the [FeFe]-hydrogenase was used to explore sustainable sources of hydrogen. Characterization of the produced species was carried out using various spectroscopy techniques. The results revealed the potential of the compound to generate biologically relevant iron-oxidation states and facilitate H-2 gas formation.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Mariia V. Pavliuk, Marco Lorenzi, Dustin R. Morado, Lars Gedda, Sina Wrede, Sara H. Mejias, Aijie Liu, Moritz Senger, Starla Glover, Katarina Edwards, Gustav Berggren, Haining Tian
Summary: This study introduces the interaction between polymer dots (Pdots) and HydA1 [FeFe]-hydrogenase in a biohybrid assembly, demonstrating efficient charge separation and hydrogen evolution. The attachment of hydrogenase on Pdots leads to a stable biohybrid assembly, enabling continuous hydrogen production for days.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Marco Lorenzi, Mira T. Gamache, Holly J. Redman, Henrik Land, Moritz Senger, Gustav Berggren
Summary: This study explores a whole-cell photocatalytic system based on Escherichia coli cells expressing a highly efficient [FeFe] hydrogenase for hydrogen gas production. The system is driven by the photosensitizer eosin Y and shows protection against oxygen damage. The study also demonstrates the use of factorial experimental design and analysis of variance to identify relevant variables and their interconnectivity.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Afridi Zamader, Bertrand Reuillard, Jacques Pecaut, Laurent Billon, Antoine Bousquet, Gustav Berggren, Vincent Artero
Summary: Surface integration of molecular catalysts inspired by hydrogenase enzymes' active sites offers a promising approach for developing noble metal-free and sustainable H2 production technologies. In this study, a diironhexacarbonyl complex with two pyrene groups per catalytic unit was prepared and electrochemically characterized, allowing for its smooth integration onto multiwalled carbon nanotube-based electrodes through pi-interactions. The grafted catalyst achieved turnover numbers for H2 production of up to 4 +/- 2x10(3) within 20 hours of bulk electrolysis at neutral pH.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Vladimir Pelmenschikov, Chien-Hong Chen, I-Jui Hsu, Ulf-Peter Apfel, Giorgio Caserta, Lars Lauterbach, Tsai-Te Lu, Yu-Ting Tseng, Linda Iffland-Mu''hlhaus, Donato Calabrese, Yu-Che Chang, Konstantin Laun, Chih-Wen Pao, Ilya Sergueev, Yoshitaka Yoda, Wen-Feng Liaw
Summary: Efforts are being made to develop earth-abundant metal catalysts for dehydrogenation/hydrolysis of amine boranes. In this study, complex 3-K-crown was explored as a pre-catalyst for the dehydrogenation of DMAB, and the transformation of 3-K-crown into intermediate A during H-2 generation was supported by experimental and computational results. The substrate-gated transformation of pre-catalyst 3 into intermediate A was also observed in the reaction of complex 4-Na-crown with CO as an alternative synthetic route.
INORGANIC CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Giorgio Caserta, Sven Hartmann, Casey Van Stappen, Chara Karafoulidi-Retsou, Christian Lorent, Stefan Yelin, Matthias Keck, Janna Schoknecht, Ilya Sergueev, Yoshitaka Yoda, Peter Hildebrandt, Christian Limberg, Serena DeBeer, Ingo Zebger, Stefan Frielingsdorf, Oliver Lenz
Summary: In this study, the maturation process of [NiFe]-hydrogenase was investigated using biochemical analysis and various spectroscopic techniques, providing detailed insights into its complex maturation mechanism.
NATURE CHEMICAL BIOLOGY
(2023)
Article
Microbiology
Jovan Dragelj, Chara Karafoulidi-Retsou, Sagie Katz, Oliver Lenz, Ingo Zebger, Giorgio Caserta, Sophie Sacquin-Mora, Maria Andrea Mroginski
Summary: In this study, the conformational and mechanical stability of the large subunit HoxG of the membrane-bound hydrogenase from Cupriavidus necator (CnMBH) was investigated using molecular modelling and molecular dynamics simulations. The simulations revealed that isolated HoxG is stable in aqueous solution and preserves a large portion of its mechanical properties, but loses rigidity around the active site. However, regained rigidity was observed in homodimer models. Furthermore, the simulations showed significant positive charge at the protein surface, especially in solvent-exposed former dimer interfaces.
FRONTIERS IN MICROBIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Armel F. T. Waffo, Christian Lorent, Sagie Katz, Janna Schoknecht, Oliver Lenz, Ingo Zebger, Giorgio Caserta
Summary: This study used cryogenic infrared and electron paramagnetic resonance spectroscopy to decipher the structural basis of the Ni-a-L intermediates in the regulatory [NiFe]-hydrogenase from Cupriavidus necator, revealing the importance of the protein scaffold in fine-tuning proton and electron dynamics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Rhys Grinter, Ashleigh Kropp, Hari Venugopal, Moritz Senger, Jack Badley, Princess R. R. Cabotaje, Ruyu Jia, Zehui Duan, Ping Huang, Sven T. T. Stripp, Christopher K. K. Barlow, Matthew Belousoff, Hannah S. S. Shafaat, Gregory M. M. Cook, Ralf B. B. Schittenhelm, Kylie A. A. Vincent, Syma Khalid, Gustav Berggren, Chris Greening
Summary: Various aerobic bacteria use atmospheric H2 as an energy source. The Mycobacterium smegmatis hydrogenase Huc is an efficient oxygen-insensitive enzyme that can oxidize atmospheric H2 and transfer the derived electrons to the respiratory chain. This understanding provides a mechanistic basis for the important process of atmospheric H2 oxidation and opens up possibilities for catalyst development.
Article
Chemistry, Physical
Princess R. Cabotaje, Kaija Walter, Afridi Zamader, Ping Huang, Felix Ho, Henrik Land, Moritz Senger, Gustav Berggren
Summary: [FeFe] hydrogenases, a type of metalloenzymes, have remarkable catalytic properties and (bio-)technological potential. This study focuses on the Group D hydrogenases, which exhibit relatively low catalytic activity and may have an alternative proton transfer pathway. By analyzing the amino acid residues in Group D hydrogenases, the study provides initial evidence for the existence of this alternative pathway.
Article
Chemistry, Physical
Mira T. Gamache, Rima Charaf, Larissa Kurth, Dawit T. Filmon, Moritz Senger, Nicolas Plumere, Leif Hammarstrom, Gustav Berggren
Summary: In this study, a semi-artificial photocatalytic system using Escherichia coli bacteria as the catalyst for hydrogen gas production was investigated. The addition of a redox mediator greatly improved the efficiency of the system, but also negatively affected the integrity and viability of E. coli cells. Spectroscopic analysis was used to study the influence of photochemistry on the system performance.
Article
Chemistry, Physical
Mira T. Gamache, Larissa Kurth, Dawit T. Filmon, Nicolas Plumere, Gustav Berggren
Summary: This study combines artificial light harvesters with enzyme catalysts to achieve semi-artificial photosynthesis. The researchers found that using Escherichia coli cells as hydrogen evolution catalysts can achieve high hydrogen production efficiency and reduce cytotoxic effects. By optimizing the experimental conditions, the availability of electrons from the electron donor was identified as the primary limiting factor for hydrogen production.
Article
Chemistry, Multidisciplinary
Marco Lorenzi, Joe Gellett, Afridi Zamader, Moritz Senger, Zehui Duan, Patricia Rodriguez-Macia, Gustav Berggren
Summary: Artificial maturation of hydrogenases provides a path to generate semi-synthetic enzymes with novel catalytic properties. This study prepared enzymes containing a synthetic asymmetric mono-cyanide cofactor and investigated their structure and reactivity. The choice of host enzyme was found to have a significant impact on reactivity, and the study showed that synthetic manipulations of the active-site can increase inhibitor tolerance.
Article
Chemistry, Multidisciplinary
Moritz Senger, Tobias Kernmayr, Marco Lorenzi, Holly J. Redman, Gustav Berggren
Summary: This study reveals that small molecules in solution can interfere with mechanistic investigations by affecting the stability of catalytic states and producing off-cycle states. The researchers demonstrate the formation of the hydride state in wild-type [FeFe]-hydrogenases treated with H-2 and discover a new state induced by common low pH buffers, the role of which in catalysis remains unclear.
CHEMICAL COMMUNICATIONS
(2022)
Article
Biochemistry & Molecular Biology
Marco Lorenzi, Pierre Ceccaldi, Patricia Rodriguez-Macia, Holly Jayne Redman, Afridi Zamader, James A. Birrell, Livia S. Meszaros, Gustav Berggren
Summary: Hydrogenases are metalloenzymes that can spontaneously form H-trans-like species under intracellular conditions, and this formation is influenced by both steric factors and proton transfer.
JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY
(2022)