Article
Multidisciplinary Sciences
Cheng Wang, Zirui Qiao, Yulan Tian, Haijun Yang, Huaqiang Cao, Anthony K. Cheetham
Summary: Imines can be synthesized directly from phenylmethanol and ben-zylamine (or aniline) using carbon nanostructures as metal-free catalysts, yielding imines with up to 98% yield and water as the only by-product. The catalytic mechanism involves the reduction of O-2 to O-2(center dot-) by the unpaired electrons in carbon catalysts, triggering the oxidative coupling reaction to form imines, while the holes in the carbon catalysts receive electrons from the amine to restore the spin states. This work provides a new avenue for synthesizing carbon catalysts and has great potential for industrial applications.
Article
Chemistry, Multidisciplinary
Gonzalo de Gonzalo, Caroline E. Paul
Summary: This review discusses recent advances in the application of alcohol dehydrogenases in cascade reactions, collaborating with other enzyme classes, chemocatalysts, or organocatalysts to obtain high value-added products such as chiral diols and amino alcohols. The review also looks towards future developments in chemoenzymatic and organoenzymatic cascades.
CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY
(2021)
Review
Microbiology
Zainab Ahsan, Umme Kalsoom, Haq N. Bhatti, Kiran Aftab, Nasira Khalid, Muhammad Bilal
Summary: Enzyme-assisted catalytic transformation of pollutants is a potential alternative to classical methods due to their ability to react with complex compounds and quick degradation rate. Peroxidases from plants, bacteria, and fungus have gained attention for their capability of detoxifying a wide range of recalcitrant xenobiotics like PAHs and synthetic dyes. They have broad substrate specificity and can transform harmful pollutants into less toxic metabolites.
JOURNAL OF BASIC MICROBIOLOGY
(2021)
Article
Multidisciplinary Sciences
Ankit Thakuri, Mainak Banerjee, Amrita Chatterjee
Summary: In this study, a rapid and convenient method for the synthesis of unsymmetrical azo dyes was developed using microwave-assisted and metal-catalyst-free techniques. The effects of electronic and substituent groups on the reaction were thoroughly understood through competitive reactions.
Article
Chemistry, Multidisciplinary
Yaoyu Liang, Jie Luo, David Milstein
Summary: In this study, a new reaction of acceptorless dehydrogenative coupling of epoxides and amines to form amides catalyzed by ruthenium pincer complexes is reported. This reaction shows high yield and selectivity, and is significant in various academic and industrial fields.
Article
Chemistry, Analytical
Ying Zhou, Hongxia Liao, Yaqin Chai, Ruo Yuan
Summary: Laccase is used as a biocompatible coreactant accelerator to efficiently catalyze the formation of superoxide radical, leading to high-intense ECL emission. A modified strand displacement reaction using hairpin DNA as template is developed to enhance the immobilization of signal probes, resulting in a biosensor with excellent selectivity and sensitivity for microRNA-21 detection. This strategy paves the way for finding more coreaction accelerators with splendid biocompatibility, promoting the application of ternary ECL systems in biological analysis and clinical diagnosis.
Article
Biochemistry & Molecular Biology
Jolanta Polak, Marcin Graz, Kamila Wlizlo, Katarzyna Szalapata, Justyna Kapral-Piotrowska, Roman Paduch, Anna Jarosz-Wilkolazka
Summary: In this study, fungal laccase from Cerrena unicolor was used as a biocatalyst for converting 8-anilino-1-naphthalenesulfonic acid into a green-coloured antibacterial compound with dual functions as an antimicrobial agent and textile dye. The optimized transformation process resulted in a crude product with low cytotoxicity, antibacterial properties, and antioxidant properties. The synthesized green compound was non-allergenic and highly efficient in dyeing wool fibers.
Article
Chemistry, Physical
Giulia R. Gheorghita, Cristina Sora, Sabina Ion, Vasile I. Parvulescu, Madalina Tudorache
Summary: A biocatalytic cascade system using a cocktail of oxidoreductase enzymes was designed for the allylic oxidation of (+)-alpha-pinene into value-added products. The system showed high efficiency under optimal conditions, achieving significant conversion of (+)-alpha-pinene and yield in verbenol. The developed biocatalytic cascade system offers promising perspectives for (+)-alpha-pinene valorization.
Article
Engineering, Environmental
Chuanyu Yan, Abdelhamid Sayari
Summary: One of the most critical challenges in applying amine-based CO2 adsorbents on a large scale is their long-term stability and oxidative degradation. In this study, the oxidation of polyethylenimine (PEI) was investigated using various analysis techniques, and the presence of radical species and their increase in the presence of transition metal catalysts were observed for the first time. Significant amounts of CO2, water, and ammonia were also detected. Surprisingly, although epoxybutane (EB) and polyvinyl alcohol (PVA) improved the oxidation resistance of PEI, they did not reduce the amount of radical species. Theoretical calculations suggested that PEI is more prone to oxidation due to its weaker C-H bonds. The findings provide insights into the oxidation and antioxidation mechanisms of amines and offer clues for further improvement.
CHEMICAL ENGINEERING JOURNAL
(2024)
Review
Chemistry, Physical
Ivan Bassanini, Erica Elisa Ferrandi, Sergio Riva, Daniela Monti
Summary: Laccases are widely studied multicopper oxidases with great synthetic potential for biocatalyzed organic synthesis. This review focuses on recent and interesting synthetic exploitations of laccases, including alcohol oxidation, Csp(2)-H bonds activation, and domino/cascade synthesis of valuable aromatic (hetero)cycles.
Article
Engineering, Environmental
Jian Peng, Enhui Wu, Xiaoxuan Lou, Qian Deng, Xiaohong Hou, Chongning Lv, Qi Hu
Summary: In this study, a MOF/PVA/Lac composite with excellent enzymatic properties for degrading AQs and removing alizarin green efficiently was synthesized. The degradation product p-toluidine was identified using molecular docking, mass spectrometry, and 2DNMR, confirming the reaction mechanism C-alpha oxidation.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Biotechnology & Applied Microbiology
Ioan Bitcan, Andreea Petrovici, Alessandro Pellis, Szilvia Klebert, Zoltan Karoly, Laura Bereczki, Francisc Peter, Anamaria Todea
Summary: This study screened four commercially available native laccases for glycerol oxidation and identified two highly efficient biocatalysts that were covalently immobilized on functionalized magnetic and polymethacrylate solid supports. The utilization of Ni-Zn or Ni-Zn-Co spinel ferrite microparticles, instead of Fe3O4 magnetic particles commonly used, led to excellent biocatalytic efficiency and stability. The enzymatic preparations demonstrated enhanced storage, pH and thermal stability compared to the native enzymes, and achieved over 50% conversion of glycerol into glyceric acid.
ENZYME AND MICROBIAL TECHNOLOGY
(2023)
Article
Chemistry, Organic
Meixia Liu, Huimin Hu, Runbo Sun, Haoyuan Li, Anjun Ding, Xiaoyong Liu, Zhengjiang Fu, Shengmei Guo, Hu Cai
Summary: We present a nickel-catalyzed reductive cross-coupling method to synthesize phosphinic amides from readily available nitroarenes and phosphine oxides. The reaction employs NiCl2/Xantphos as catalyst, zinc as reductant, and TMSCl as additive, delivering various phosphinic amides in moderate to good yields. Notably, a gram-scale synthesis was successfully achieved, making this method practical for the synthesis of phosphinic amides. Mechanistic insights were also obtained from control experiments.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Biochemistry & Molecular Biology
Dmitry L. Lipilin, Alexander E. Frumkin, Alexey Y. Tyurin, Vitalij V. Levin, Alexander D. Dilman
Summary: This study describes a reaction involving aromatic halides with electron-withdrawing groups and tertiary amines in the presence of an iridium catalyst under blue light irradiation. The products obtained are the result of aromatic substitution of the halide by the dialkylamino fragment. The interaction between aryl radicals and tertiary amines to form zwitterionic radical species is believed to be the main factor contributing to the reaction efficiency.
Article
Environmental Sciences
Marilia Cristina Oliveira Souza, Neus Gonzalez, Marta Herrero, Montse Marques, Joaquim Rovira, Marti Nadal, Fernando Barbosa, Jose Luis Domingo
Summary: This study investigated the concentrations of harmful substances in clothing sold in Brazil and Spain, finding higher levels in Brazil due to the lack of regulation. Some substances exceeded health thresholds. Continuous studies are recommended to determine the co-occurrence of carcinogenic substances.
ENVIRONMENTAL RESEARCH
(2023)
Article
Nanoscience & Nanotechnology
Tiago A. Fernandes, Ines F. M. Costa, Paula Jorge, Ana Catarina Sousa, Vania Andre, Rafaela G. Cabral, Nuno Cerca, Alexander M. Kirillov
Summary: This study presents the preparation, characterization, and antimicrobial properties of novel hybrid biopolymer materials doped with bioactive silver(I) coordination polymers (bioCPs). The bioCP-doped biopolymer films showed remarkable antimicrobial activity against various bacteria, including Staphylococcus aureus, Escherichia coli, and Pseudomonas aeruginosa, and were also effective in inhibiting bacterial biofilm formation.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Correction
Chemistry, Applied
Ana Catarina Sousa, Iolanda Santos, M. F. M. M. Piedade, Ligia O. Martins, M. Paula Robalo
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Physical
Vania Brissos, Patricia T. Borges, Reyes Nunez-Franco, Maria Fatima Lucas, Carlos Frazao, Emanuele Monza, Laura Masgrau, Tiago N. Cordeiro, Ligia O. Martins
Summary: This study characterizes the molecular features of the evolution of a hyperthermostable metallo-oxidase from the multicopper oxidase family into a laccase by combining mutagenesis with structural, kinetic, and in silico analyses. The results show that residue replacements and distal mutations modulate substrate binding and catalysis, and allosterically coupled, long-range dynamic networks favor catalytically competent conformational states.
Article
Biochemistry & Molecular Biology
Mario De Simone, Laura Alvigini, Lur Alonso-Cotchico, Vania Brissos, Jonatan Caroli, Maria Fatima Lucas, Emanuele Monza, Eduardo Pinho Melo, Andrea Mattevi, Ligia O. Martins
Summary: This study presents a new variant of the dioxygenase NOV1 that exhibits improved activity and stability compared to the wild type. The replacement of S283F in the variant leads to increased turnover rate and catalytic efficiency. The variant also demonstrates enhanced stabilization of the iron cofactor in the active site. Importantly, the variant is capable of catalyzing the conversion of isoeugenol to vanillin with high molar conversion yields within 24 hours.
Article
Chemistry, Medicinal
Tania S. Morais, Fernanda Marques, Paulo J. Amorim Madeira, Maria Paula Robalo, Maria Helena Garcia
Summary: New water-soluble Ru(II) organometallic complexes with potential anticancer activity were synthesized and characterized. These complexes showed promising antiproliferative potential on breast adenocarcinoma, ovarian carcinoma, and colorectal adenocarcinoma cell lines. Additionally, their interaction with human serum albumin was evaluated, highlighting their ability to strongly quench the intrinsic fluorescence of albumin.
Article
Biochemistry & Molecular Biology
Rafaela G. Cabral, Goncalo Viegas, Rita Pacheco, Ana Catarina Sousa, Maria Paula Robalo
Summary: This study describes the sustainable synthesis, characterization, and evaluation of the electrochemical and biological properties of different substituted derivatives of 1,4- and 1,2-naphthoquinones (NQ). The synthesis of the derivatives was optimized using a microwave-assisted protocol, providing a more sustainable approach. The compounds were found to have potential anti-cancer activity against HepG2 cell lines and inhibitory action against AChE enzymes. Docking studies showed different binding interactions for the derivatives.
Article
Biochemical Research Methods
Diogo Silva, Ana Catarina Sousa, M. Paula Robalo, Ligia O. Martins
Summary: Lignin is the largest renewable source of aromatic compounds and has immense potential in biorefineries. The engineered PpDyP variant 6E10 showed significantly higher oxidation rates for lignin-phenolic derivatives compared to other enzymes. The reaction products have potential applications in medicinal chemistry, food additives, and polymers.
Article
Chemistry, Physical
Magali F. Scocozza, Francisco Vieyra, Fernando Battaglini, Ligia O. O. Martins, Daniel H. H. Murgida
Summary: In this study, it was found that the performance of DyP enzyme from Bacillus subtilis can be greatly enhanced by electrochemical activation in the absence of externally added H2O2. The enzyme shows higher specific activities towards different substrates and broader pH activity profiles under these conditions.
Article
Biochemistry & Molecular Biology
Paulo Durao, Peter Kis, Ivo M. Chelo, M. Rita Ventura, Ligia O. Martins
Summary: An environmentally friendly two-step process has been developed to effectively transform the antibiotic rifampicin into non-antimicrobial compounds. The process involves an enzymatic oxidation step by the bacterial CotA-laccase and a hydrogen peroxide bleaching step. NMR identified rifampicin quinone as the main product of the enzymatic oxidation. Growth and bioassays confirmed that the final degradation products (FP) are non-antimicrobial and non-toxic to eukaryotic organisms, and susceptible bacteria is strongly favored in the presence of FP.
Article
Biochemistry & Molecular Biology
Patricia T. Borges, Diogo Silva, Tomas F. D. Silva, Vania Brissos, Marina Canellas, Maria Fatima Lucas, Laura Masgrau, Eduardo P. Melo, Miguel Machuqueiro, Carlos Frazao, Ligia O. Martins
Summary: In this study, the molecular basis and pH-dependent conformational plasticity of DyP-type peroxidases (DyPs) were revealed through high-resolution structural analysis. Variant 6E10 displayed higher catalytic efficiency but poorer protein stability compared to wild-type and 29E4 variants. The findings contribute to the understanding and improvement of the catalytic properties of DyPs for future biotechnological applications.
COMPUTATIONAL AND STRUCTURAL BIOTECHNOLOGY JOURNAL
(2022)
Article
Engineering, Chemical
Jose P. Coelho, Maria Paula Robalo, Ines S. Fernandes, Roumiana P. Stateva
Summary: This study presents an optimization strategy for the recovery of oil from Japonica Luna rice bran using supercritical carbon dioxide (scCO(2)). The study utilized design of experiments (DoE) and central composite design (CCD) to determine the significant variables and create quadratic surfaces for optimization. The results showed that pressure, temperature, and scCO(2) flow rate of 34.35 MPa, 339.5 K, and 1.8 x 10(-3) kg/min, respectively, optimized the yield, total polyphenols content (TPC), and total flavonoids content (TFC).