Article
Chemistry, Physical
Ren-Jie Li, Kaiyuan Tian, Xirui Li, Anand Raghavendra Gaikaiwari, Zhi Li
Summary: In this study, a group of P450BM3 mutants were developed as unique catalysts for regioselective hydroxylation reactions of aromatic compounds. The mutants showed high regioselectivity and conversion, leading to the production of valuable m-alkylbenzene-1,4-diols. Protein engineering and site-directed mutagenesis were used to reshape the substrate binding pocket and access channel of the P450BM3 monooxygenase. Molecular docking and simulation provided insights into the enhanced regioselectivity and activity of the mutants. The mutants were successfully applied in preparative biohydroxylation reactions for the synthesis of m-alkylbenzene-1,4-diols.
Article
Chemistry, Multidisciplinary
Haonan Shi, Bangyuan Xiong, Ying Chen, Chaojun Lin, Jiajian Gu, Yanpeng Zhu, Jiaobing Wang
Summary: We report the synthesis and characterization of a fan-shaped chiral nanographene 1, which is composed of 6 hexabenzocoronene subunits with 216 conjugated carbon atoms. The synthesized nanographene exhibits strong panchromatic absorption and near-infrared fluorescence emissions. The optical properties were analyzed through DFT calculations.
CHINESE CHEMICAL LETTERS
(2023)
Article
Energy & Fuels
Luna Ramirez, Ivan Moncayo-Riascos, Farid B. Cortes, Camilo A. Franco, Rafael Ribadeneira
Summary: This study evaluated the aggregation behavior of four PA3-type asphaltene molecules dissolved in three different solvents using molecular dynamics simulations. Results showed that molecules with heteroatoms exhibited a stronger tendency to aggregate in n-heptane. The inclusion of heteroatoms increased the polarity and planarity of the molecules, enhancing the aggregation tendency in all solvents, especially in n-heptane.
Article
Environmental Sciences
Wen Chen, Sifu Li, Dingyi Bai, Zongfang Li, Haozhe Liu, Lianyang Bai, Lang Pan
Summary: The excessive use of chemical herbicides has led to the evolution of herbicide-resistant weeds. Cytochrome P450 monooxygenases (P450s) play a vital role in detoxification of herbicide-resistant weeds. A resistant population of Polypogon fugax (R population) was found to be resistant to quizalofop-p-ethyl, pyroxsulam, and several other herbicides. Molecular analysis revealed no target-site gene mutations in the R population. The overexpression of the CYP89A2 gene was found to be responsible for reducing quizalofop-p-ethyl phytotoxicity.
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
(2023)
Article
Chemistry, Multidisciplinary
Sascha Grobe, Christoffel P. S. Badenhorst, Thomas Bayer, Emil Hamnevik, Shuke Wu, Christoph W. Grathwol, Andreas Link, Sven Koban, Henrike Brundiek, Beatrice Grossjohann, Uwe T. Bornscheuer
Summary: In this study, the cytochrome P450 monooxygenase CYP107D1 was engineered for the stereo- and regioselective 7 beta-hydroxylation of lithocholic acid to yield ursodeoxycholic acid. By identifying specificity-determining residues and utilizing a synthetic small library, a nearly perfectly regio- and stereoselective triple mutant was developed, which produces UDCA at significantly higher levels than the initial variant. This biocatalyst offers new possibilities for environmentally friendly synthesis of UDCA from biological waste product.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Dennis Popp, Sven M. Elbert, Chantal Barwig, Julian Petry, Frank Rominger, Michael Mastalerz
Summary: The palladium-catalyzed cyclotrimerization of ortho-silylaryl triflates is a well-established method for synthesizing polycyclic aromatic hydrocarbons with triphenylene cores. In the reaction of pyrene with o-silylaryl triflates, higher homologues with eight- and ten-membered rings were unexpectedly formed along with the trimer, and a protocol was developed to isolate all members of this series. This novel class of PAHs was thoroughly investigated using various techniques, including X-ray diffraction, UV/Vis and fluorescence spectroscopy, and theoretical calculations. A mechanistic proposal for the formation of all higher cyclooligomers was supported by density functional theory (DFT) calculations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Environmental Sciences
Guodong Chai, Dongqi Wang, Jiaqi Shan, Chunbo Jiang, Zhangjie Yang, Enyu Liu, Haiyu Meng, Hui Wang, Zhe Wang, Lu Qin, Jiayao Xi, Yuenan Ma, Huaien Li, Yishi Qian, Jiake Li, Yishan Lin
Summary: Bioretention is an effective management practice for urban stormwater, but the accumulation of high-molecular weight PAHs in bioretention systems and their impact on pollutants removal and microbial ecology are still not fully understood. This study compared the treatment effectiveness, enzyme activity, and microbial community in bioretention systems with different media amendments, and found that the addition of pyrene negatively affected the removal efficiencies of COD and total nitrogen, as well as the microbial diversity.
Review
Biotechnology & Applied Microbiology
Prerna J. Yesankar, Ayurshi Patil, Atya Kapley, Asifa Qureshi
Summary: Hydrophobic organic compounds, whether natural or anthropogenic, are a serious threat to life in all spheres, including humans. Microorganisms have evolved metabolic and degradative potential to handle these recalcitrant compounds. Pseudomonas species play a multipotential role in the biodegradation of aromatic hydrocarbons using aromatic ring-hydroxylating dioxygenases (ARHDs). This review focuses on the molecular characterization of ARHDs from Pseudomonas species and their ability to accommodate various low and high molecular weight polycyclic aromatic hydrocarbon (PAH) substrates through flexible catalytic pockets and channels.
WORLD JOURNAL OF MICROBIOLOGY & BIOTECHNOLOGY
(2023)
Article
Environmental Sciences
Lili Wang, Anjie Li
Summary: This study investigates the molecular mechanism of EE2 degradation by AOB and AMO using a combination of experimental and computational simulation methods. The results reveal that ammonia nitrogen is essential for the co-metabolism of EE2 by AOB, and NH3 binds with CuC to induce a conformational change in AMO, enabling EE2 to bind with CuB and undergo biological transformation. These findings provide a theoretical basis and a novel research perspective on the removal of ammonia nitrogen and emerging contaminants in wastewater treatment.
ENVIRONMENTAL RESEARCH
(2023)
Article
Infectious Diseases
Kamal A. Qureshi, Mahrukh Imtiaz, Ibrahim Al Nasr, Waleed S. Koko, Tariq A. Khan, Mariusz Jaremko, Syed Mahmood, M. Qaiser Fatmi
Summary: This study investigated the in vitro and in silico antileishmanial activity of thymoquinone (TQ) against Leishmania major and its cytotoxicity against mice macrophages. Results showed that TQ is a promising antileishmanial drug candidate for the treatment of drug-resistant leishmaniasis.
Article
Environmental Sciences
Li-Ping Tao, Xue Li, Ming-Zhu Zhao, Jing-Ru Shi, Si-Qi Ji, Wen-Yuan Jiang, Qiu-Ju Liang, Yu-Hang Lei, Yi-Yao Zhou, Rong Cheng, Zhe Shi, Wenhai Deng, Jiayin Zhu, Shu-Yun Zhang
Summary: Polycyclic aromatic hydrocarbons (PAHs), particularly chrysene, have toxic effects on the liver by increasing relative liver weight and elevated serum ALT levels; the hepatotoxicity of chrysene is dependent on the aryl hydrocarbon receptor (AhR), while Nrf2 plays a crucial role in protecting against oxidative liver injury induced by chrysene.
Article
Chemistry, Physical
Lea R. Rapp, Sergio M. Marques, Bernd Nebel, Jiri Damborsky, Bernhard Hauer
Summary: The catalytic space of the P450 monooxygenase CYP153A(M.aq) was transformed from a fatty acid hydroxylase to a catalyst capable of omega-hydroxylation of dodecylamine. A rapid screening method called RAPP was established to measure saturation libraries directly from a 96-deepwell plate. Molecular modeling and dynamics simulations revealed significant effects of the mutations on the substrate tunnel architectures.
Article
Environmental Sciences
Daheng Yang, Xiaoqin Chen, Weidong Cao, Cheng Xu, Lin Chang, Guangfeng Long
Summary: Although the association between single PAHs exposure and telomere length has been studied, the relationship between mixed PAHs exposure and telomere length in the general population is still uncertain. This study analyzed 8 PAHs and their correlation with telomere length, finding that mixed PAHs exposure was negatively associated with telomere length. Specifically, 2-napthol and 2-fluorene concentrations showed a significant negative correlation with telomere length. These findings indicate that PAHs may have a negative impact on telomere length in the general population.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2023)
Article
Chemistry, Physical
Nana Ma, Wenhan Fang, Chuanfei Liu, Xiangquan Qin, Xiling Wang, Longyi Jin, Binju Wang, Zhiqi Cong
Summary: By employing a protein engineering strategy, the research group successfully enhanced the peroxidase activity of the modified P450 system and demonstrated excellent oxidation activity towards various substrates. This engineered system achieves the best peroxidase activity reported for any P450 to date and holds significant potential for practical applications.
Review
Chemistry, Applied
Rui Zhu, Yang Liu, Yueying Yang, Qing Min, Hua Li, Lixia Chen
Summary: Steroids are a class of drugs with diverse pharmacological properties. Hydroxylation of steroids significantly affects their biological activities and properties. Achieving regio- and stereo-selective hydroxylation on steroids using modern organic synthesis techniques is extremely challenging. However, recent studies have identified and engineered cytochrome P450 monooxygenases that possess the ability to catalyze regio- and stereo-selective oxidations of nonactivated C-H bonds in complex organic molecules.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Physical
Haojie Li, Bingke Yang, Zhen Yao, Xuetao Wang, Kaiming Shen, Mengjie Liu
Summary: This study systematically investigates the influence of metal and nonmetal element doping on the photochemical properties of g-C3N4 for efficient catalytic AB hydrogen production. It provides a design method for high performance bifunctional catalysts of photocatalysis and metal catalysis. The results show that both non-metals (B, P) and metals (Ru, Ni) have efficient regulatory effects on the band structure of g-C3N4, resulting in a reduced band gap and improved hydrogen production. The study offers a theoretical method for the coupling of metal catalysis/photocatalysis ammonia borane to produce hydrogen.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Shrouq Mujahed, Davide Gandolfo, Luigi Vaccaro, Evgueni Kirillov, Dmitri Gelman
Summary: In this study, a high-valent Ru(IV) bifunctional catalyst was successfully applied for the hydrosilylation of various functional groups. The high-valent hydride complexes showed high chemoselectivity and affinity towards reducing polar bonds. The scope, limitations, and plausible mechanism of the reaction were described.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Yongzhen Peng, Kongchen Xia, Qi Wu
Summary: In this study, we report an engineered cyclohexanone monooxygenase that can be used for the asymmetric synthesis of chiral alpha-deuterated carbonyl compounds via enantioselective reductive dehalogenation. The engineered enzyme exhibits good chemoselectivity, stereoselectivity, and d-incorporation, making it a promising method for the synthesis of deuterated drugs.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Qi Yang, Ruixuan Xu, Hongqi Nie, Qilong Yan, Jun Liu, Jiuyu Chen, Yunlan Sun
Summary: The adsorption and decomposition processes of ammonium perchlorate (AP) on pure-Al and Al2O3/Al surfaces were investigated using density functional theory. The results showed that the pure-Al surface is more conducive to the decomposition of AP and the activation of NH3, while the Al2O3/Al surface promotes the disengagement of H and NH3 decomposition.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Yudong Hu, Guochao Xu, Ye Ni
Summary: This study identified a novel phenylalanine dehydrogenase (QtPDH) with high catalytic efficiency and thermal stability, making it a promising biocatalyst for industrial production of bulky aromatic primary amines. QtPDH exhibited a broader substrate specificity and significantly longer half-life compared to BbPDH.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Weiling Zhao, Zhiling Huang, Hui Shen, Xianglong Li, Shaofen Zhao, Bo Xie, Shengjie Xia
Summary: This study investigated the effects of metal doping and crystal plane selection on the CO2 adsorption properties of MgO using density functional theory (DFT) methods. The results showed that the appropriate crystal plane and metal doping can improve the adsorption properties of MgO on CO2. The influence of different crystal planes and metal dopants on CO2 adsorption properties varied significantly. The research provides some references for experimental studies on CO2 adsorption by MgO by combining the dual modification of crystal plane and doped metal.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Jie Zhang, Jinwei Chen, Zongbo Shi, Junyu Zhao, Runsheng Zhuo, Ruilin Wang
Summary: In this study, a double-layered silicalite-1 support with high specific surface area was synthesized, and a magnesium modification strategy was adopted to improve the catalytic activity and stability of the zinc-based catalyst. The modified catalyst showed enhanced propylene selectivity and anti-coking property.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Pei-Sen Gao, Chang-Wang Pan, Cheng Liu, Wen -Tong Chen
Summary: Asymmetric electrocatalysis offers a unique approach to obtain enantioenriched molecules that are difficult to obtain through conventional methods. This study developed a novel bifunctional electrocatalyst, enabling the oxidative kinetic resolution of chiral 1,4-diols and gamma-lactones. The work demonstrates the potential of bifunctional electrocatalysis for asymmetric synthetic methods and its importance in the development of novel electrocatalytic methods.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Qinzhe Lin, Xuanjin Lv, Xianming Zeng, Mengning Zhong, Qiyun Wu, Huilin Ren, Shenpeng Xu, Wentian Chen, Wenting Du, Jun Li
Summary: The catalytic efficiency of engineered IRED M5 was found to be relatively low when tasked with a bulky amine substrate. Rational design led to the mutants M203V and F260A, with F260A exhibiting a substantial improvement in conversion and stereoselectivity. The study revealed the potential molecular mechanisms underlying the effect of F260A and M203V on catalytic performance.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Zhishuai Wang, Fengyun Su, Hailong Cao, Mengzhen Tian, Xiang Li, Haiquan Xie, Xiaoli Jin, Zhengdao Li, Xin Ying Kong
Summary: In this study, the efficiency of photocatalytic CO2 reduction was significantly enhanced by incorporating nickel oxide onto niobium pentoxide. The resulting catalyst showed remarkable methane and carbon monoxide production improvements.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
A. Yu. Sidorenko, Yu. M. Kurban, T. V. Khalimonyuk, I. V. Il'ina, N. S. Li-Zhulanov, O. S. Patrusheva, V. V. Goltsova, M. P. Bei, Zh. V. Ihnatovich, J. Warna, K. P. Volcho, N. F. Salakhutdinov, D. Yu. Murzin, V. E. Agabekov
Summary: This study provides a comprehensive investigation into the catalytic condensation of renewable 3-carene with formaldehyde for the one-step preparation of terpenoid trans-4-hydroxymethyl-2-carene. Various acids and alumino-silicates were found to catalyze the reaction, but the selectivity to the desired product was limited. Phosphoric acid showed the highest selectivity, and an excess of formaldehyde or catalyst loading significantly increased the yield of the target product. Water presence also led to increased selectivity. Additionally, a detailed mechanism for the 3-carene condensation with formaldehyde was proposed and confirmed through kinetic modeling.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Meng-Yu Rong, Jing Nie, Shen Li, Jun-An Ma
Summary: We synthesized a new class of chiral quaternary ammonium salts and used them as catalysts in phase-transfer catalytic asymmetric alkylation. By employing these catalysts, we obtained a series of chiral fluorinated aromatic alpha-amino acid derivatives with high yields and enantioselectivities.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Zhaozhou Wei, Guangtao Wei, Huixian Che, Deyuan Xiong, Linye Zhang, Ruihua Xue, Yalin Tang, Xuanli Lu
Summary: This study demonstrates that small-sized graphite crystallite and highly defective carbon-based catalysts can increase the -SO3H density of the catalysts and modulate their surface electronic properties, leading to improved efficiency in the alpha-pinene hydration reaction. The reduction of graphite crystallite size is considered a critical step in enhancing the selectivity of alpha-terpineol.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Kempanna S. Kanakikodi, Nagendra Kulal, K. S. Subramanya, M. S. Puneethkumar, Bhavana B. Kulkarni, Ganapati Shanbhag, Sanjeev P. Maradur
Summary: An effective and highly selective protocol for synthesizing asymmetric organic carbonates using dimethyl carbonate (DMC) as a reactant and solvent has been developed. The performance of CeO2 nanostructures with different morphologies in the carbonate interchange reaction (CIR) of alcohols was investigated, and the CeO2 nano-catalyst with rod morphology exhibited the highest oxygen vacancy and remarkable enhancement in conversion. The CeO2 characterization data revealed that the exposed active sites, defect density, coordination state of surface atoms, and reducibility of the catalytic materials are the contributing factors to its high catalytic activity. CeO2 can be easily recovered and reused for multiple cycles.
MOLECULAR CATALYSIS
(2024)
Article
Chemistry, Physical
Yanzhao Gao, Xianglei Meng, Shiqi Huang, Hui Wu, Liantao Jiang, Yu Zhou, Yuting Song, Yanyan Diao
Summary: Gamma alumina modified with alkaline earth metal shows improved catalytic performance for hydrogenation reactions. Pd catalysts supported by Al2O3 and Mg-modified Al2O3 were synthesized and their structure, composition, and surface acidity were investigated. The results showed that Pd/MgO-Al2O3-2 catalyst exhibited the best catalytic performance due to its metallic state palladium and weak acid sites.
MOLECULAR CATALYSIS
(2024)