Article
Chemistry, Physical
Lijuan Xiang, Shihan Liu, Lei Zhao, Shisheng Yuan, Xiaotian Li, Nan Li
Summary: A SnS2/MoS2 heterostructure was prepared as a catalyst for electrocatalytic nitrogen reduction reaction (eNRR) by depositing SnS2 nanoparticles onto MoS2 nanosheets. The strong electronic interaction between SnS2 and MoS2 promotes electron redistribution and directed electron transfer, increasing the electron density of Mo sites and electrical conductivity of MoS2. This enhances nitrogen activation, lowers the energy barrier for breaking N-N triple bonds, and accelerates electron transport, resulting in high ammonia yield and Faraday efficiency.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Multidisciplinary
Gaoxin Lin, Qiangjian Ju, Xiaowei Guo, Wei Zhao, Samira Adimi, Jinyu Ye, Qingyuan Bi, Jiacheng Wang, Minghui Yang, Fuqiang Huang
Summary: Manipulating the electronic configuration of electrocatalysts is vital in enhancing metal-nitrogen bonds formation, boosting the nitrogen reduction reaction kinetics, and increasing the efficiency of ammonia synthesis.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Applied
Jian Gao, Kai Zhang, Hao Li, Chen Lang, Lunxiang Zhang
Summary: With the increasing exploration of the marine environment, underwater monitoring equipment like underwater vehicles are being widely used. This paper introduces a superhydrophobic polyurea/TiO2 composite coating with rapid self-healing ability, achieved by sprinkling or spraying modified TiO2 nanoparticles on a brushed polyurea coating. The coating shows enhanced drag reduction efficiency, high water loading capacity, excellent antifouling properties, and chemical durability. This work provides new insights for future applications in drag reduction and pollution prevention of underwater exploration equipment.
PROGRESS IN ORGANIC COATINGS
(2023)
Article
Multidisciplinary Sciences
Mihaela Beregoi, Samuel Beaumont, Alexandru Evanghelidis, Toribio F. Otero, Ionut Enculescu
Summary: This article reports on a non-conventional device based on polypyrrole coated electrospun fibrous microstructures, that can simultaneously act as an artificial muscle and mechanical sensor. By using a simple fabrication algorithm, electroactive aligned ribbon meshes with similar characteristics to natural muscle fibers were produced, which can generate movement and sense changes in load.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Multidisciplinary
Nicolai N. Bach, Verena Josef, Harald Maid, Henry Dube
Summary: Researchers have developed a macrocyclic molecular motor structure that can convert a flexible chain into unidirectional linear motion through active mechanical threading. This offers a new approach for molecular knitting technology.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
Joakim Brorsson, Arsalan Hashemi, Zheyong Fan, Erik Fransson, Fredrik Eriksson, Tapio Ala-Nissila, Arkady Krasheninnikov, Hannu-Pekka Komsa, Paul Erhart
Summary: High-order force constant expansions, combined with GPU-accelerated molecular dynamics simulations, provide an accurate, transferable, and efficient approach for sampling the dynamical properties of materials.
ADVANCED THEORY AND SIMULATIONS
(2022)
Article
Chemistry, Physical
Poe Ei Phyu Win, Dongxue Yu, Wenjuan Song, Xiang Huang, Peng Zhu, Guanyu Liu, Jiong Wang
Summary: By intentionally covering the S edge of 2H-molybdenum disulfide with cobalt phthalocyanine molecules, the catalytic efficiency of the electrochemical N-2 reduction reaction (NRR) in water can be enhanced, resulting in increased ammonia production. These findings provide insights into the mechanism of 2H-molybdenum disulfide-based NRR catalysis and propose an efficient molecular modification strategy to promote NRR in water.
Article
Biochemistry & Molecular Biology
Magnus Hansen-Felby, Steen U. Pedersen, Kim Daasbjerg
Summary: We report the use of AQ center dot(-) as an electron carrier to trigger the catalytic depolymerization of pDTT polymers. The reaction is rapid and catalytic, with as little as a small amount of electrons needed for complete depolymerization. It is driven by thiyl radicals attacking disulfide bonds internally or between chains.
Article
Chemistry, Physical
Shixiong Min, Huaiyu Chang, Huanhuan Tao, Fang Wang
Summary: A highly defective, self-supported porous carbon membrane (HDPCM) electrode was developed by CO2-assisted thermal etching of carbonized wood. The as-fabricated HDPCM is heteroatom-free and exhibits abundant intrinsic carbon defects, resulting in enhanced CO2 adsorption and activation capability. It showed high efficiency for electrocatalytic CO2-to-CO conversion, with a FECO of 81.1% and a j(CO) of -3.88 mA cm(-2) at -0.66 V versus RHE. After hydrophobic treatment, the HDPCM could be directly used as an integrated gas-diffusion electrode (GDE) in the flow cell, achieving a much enhanced and relatively stable j(CO) (-50 mA cm(-2) at -0.76 V vs. RHE). This work not only provides an effective strategy for creating intrinsic defects on carbon-based electrocatalysts but also offers new insights into the development of integrated metal-free carbon-based GDEs for large-scale CO2 electroreduction.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Ceramics
Lei Li, Xiaochi Chen, Xiaoli Wu, Xuqiang Liu, Guang Zeng, Guixia Yang, Yuan Jian
Summary: This study investigates the effects of uniaxial tensile strain on one-electron trapping behaviors in amorphous silica (a-SiO2) by using first-principle calculations and molecular dynamic calculations. The results show that a SiO4 unit with a wide O-Si-O angle (≥132.0 degrees) and a long Si-O bond (≥1.660) can act as a novel intrinsic electron trap.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2023)
Article
Chemistry, Multidisciplinary
Javier Echavarren, Malcolm A. Y. Gall, Adrian Haertsch, David A. Leigh, Justin T. J. Spence, Daniel J. Tetlow, Chong Tian
Summary: This study reports the preparation of a decapeptide through the parallel operation of two rotaxane-based molecular machines, involving simultaneous operation of two molecular peptide synthesizers, selective residue activation, ligation, and product release. The design of the machines enables the synthesis of a product that exceeds the capabilities of individual small-molecule machines, reminiscent of the ligation and post-translational modification of proteins in biology.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Ruoqi Liu, Ting Guo, Hao Fei, Zhuangzhi Wu, Dezhi Wang, Fangyang Liu
Summary: In this study, different active sites of MoS2 were found to exhibit different catalytic selectivity for nitrogen reduction and hydrogen evolution reactions through DFT calculations. A new synergistic mechanism was proposed and a self-sacrificial strategy using g-C3N4 as templates was developed to synthesize 1T-MoS2 with an ultrahigh 1T content. This work provides a promising new direction for synchronizing selectivity and activity in multistep catalytic reactions.
Article
Chemistry, Physical
Hao Ma, Zhengjie Wang, Wen Zhao, Hao Ren, Houyu Zhu, Yuhua Chi, Wenyue Guo
Summary: In this study, a type-II band alignment was achieved in Janus-MoSSe/WS(2) heterostructure, improving charge separation efficiency. The intrinsic self-built electric field of Janus-MoSSe can effectively weaken the hindrance effect of E-hetero for charge transfer, providing a new paradigm for heterostructure engineering.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Review
Chemistry, Multidisciplinary
Zhi-Wen Yang, Jin-Mei Chen, Li-Qi Qiu, Wen-Jun Xie, Liang-Nian He
Summary: This review summarizes the molecular engineering of several N-based metal complexes and provides general modification strategies for designing novel molecular catalysts with high intrinsic activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Nanoscience & Nanotechnology
Guohua Yang, Lei Zhao, Guoqing Huang, Zhipeng Liu, Shuyi Yu, Kaiwen Wang, Shisheng Yuan, Qiwei Sun, Xiaotian Li, Nan Li
Summary: In this study, a CoS2/MoS2 nanocomposite was fabricated and used as a catalyst for the N-2 reduction reaction. By modulating the interfacial charge distribution and promoting N-2 absorption, the catalyst exhibited excellent NRR performance.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Kriti Kapil, Grzegorz Szczepaniak, Michael R. R. Martinez, Hironobu Murata, Arman Moini Jazani, Jaepil Jeong, Subha R. R. Das, Krzysztof Matyjaszewski
Summary: In this study, hyperbranched polymethacrylates were synthesized by green-light-induced atom transfer radical polymerization (ATRP) under biologically relevant conditions. By using a water-soluble SBA inibramer as a inducer during the copolymerization of methacrylate monomers, well-defined branched polymethacrylates can be obtained in less than 30 minutes with predetermined molecular weights, tunable degree of branching, and low dispersity values (1.14 <= D <= 1.33). Moreover, SBA inibramer enables the synthesis of bioconjugates with a well-controlled branched architecture.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Jing Lyu, Yinghao Li, Zishan Li, Piotr Polanowski, Jeremiasz K. Jeszka, Krzysztof Matyjaszewski, Wenxin Wang
Summary: This article presents a minireview on the most important modelling techniques and their applications in free radical polymerization (FRP) and reversible-deactivation radical polymerization (RDRP) of multivinyl monomers (MVMs). The combination of experiments and modelling can provide valuable assets for polymer researchers, inspiring new thinking for future MVMs experiment optimization and product design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Polymer Science
Mingkang Sun, Grzegorz Szczepaniak, Sajjad Dadashi-Silab, Ting-Chih Lin, Tomasz Kowalewski, Krzysztof Matyjaszewski
Summary: Cu-catalyzed atom transfer radical polymerization is a powerful method for preparing well-defined (co)polymers. This minireview summarizes the development of cocatalysts for regenerating Cu-I complex activators during polymerizations. Recent developments of photochemical cocatalysts and methods to study their properties and roles are also discussed.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Julian Sobieski, Illia Ruzhylo, Grzegorz Szczepaniak, Adam Gorczynski, Krzysztof Matyjaszewski, Eric Manoury, Rinaldo Poli
Summary: Simple synthetic routes for the regioselective deuteration of tris[2-(dimethylamino)ethyl]amine (Me6TREN) variants are described. Formation of imine with formaldehyde-d(2) from tris(2-aminoethyl)amine (TREN) and subsequent reduction with NaBD4 resulted in N[CH2CH2N(CD3)(2)](3) or d(18)-Me6TREN in 79% yield. A trisubstitution protocol from 2-bromo-N,N-dimethylacetamide and ammonium carbonate, followed by reduction of the N(CH2CONMe2)(3) intermediate with lithium aluminum deuteride, afforded N[CH2CD2N(CH3)(2)](3) or (d(6)-arm)-Me6TREN in three steps and 52% overall yield. A similar protocol using 2-bromo-N,N-dimethyl-d(2)-acetamide, obtained from d(4)-acetic acid in two steps, and reduction of the N(CD2CONMe2)(3) intermediate with lithium aluminum hydride, resulted in N[CD2CH2N(CH3)(2)](3) or (d(6)-cap)-Me6TREN in four steps and 13% overall yield.
Article
Polymer Science
Dirk J. Schild, Juliana Bem, Grzegorz Szczepaniak, Arman Moini Jazani, Krzysztof Matyjaszewski
Summary: We report a photoinduced initiators for continuous activator regeneration atom transfer radical polymerization (PICAR ATRP) using sodium pyruvate and blue light (λ(max) = 456 nm). Water-soluble oligo(ethylene oxide) methyl ether methacrylate (OEOMA(500)) was polymerized under biologically relevant conditions. Well-defined polymers with high molecular weights and low dispersity were synthesized in less than 60 min using Cu/Fe dual catalysis and without deoxygenation.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Chuao Ma, Jun Wei, Yuqiang Zhang, Xingchao Chen, Chan Liu, Shen Diao, Yuan Gao, Krzysztof Matyjaszewski, Hongliang Liu
Summary: Currently, there is a significant challenge in meeting the increasing demands for conductive ionogels with complex shapes and high processability for next-generation flexible electronics. In this study, highly processable ionogels with mechanical robustness are designed by self-assembly of a common triblock copolymer into a precursor in functional mixed ionic liquids. The viscosity of the self-assembled precursor can be adjusted, making it compatible with various fabrication technologies. By using 3D printing, an auxetic-structured ionogel is easily generated, showing improved sensitivity for monitoring small deformations. This research establishes a new approach for versatile and programmable fabrication of high-performance ionogels, focusing on designing functional mixed ionic liquids rather than synthesizing new polymers.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Yilin Zhang, Michael R. Martinez, Hui Sun, Mingkang Sun, Rongguan Yin, Jiajun Yan, Benedetto Marelli, Juan Pablo Giraldo, Krzysztof Matyjaszewski, Robert D. Tilton, Gregory V. Lowry
Summary: The understanding of how agrochemical nanocarrier properties affect their uptake and translocation in plants is incomplete. Our study found that anionic nanocarriers were transported at a higher rate than cationic nanocarriers in tomato, while only anionic nanocarriers were transported in wheat. These findings provide design parameters for efficient and targeted agrochemical delivery.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Polymer Science
Kriti Kapil, Shirley Xu, Inseon Lee, Hironobu Murata, Seok-Joon Kwon, Jonathan S. Dordick, Krzysztof Matyjaszewski
Summary: Well-defined multifunctional copolymers with rhodamine B dye were synthesized by ATRP, enabling efficient and specific bioimaging of Staphylococcus aureus. The combination of multifunctional polymeric dyes and strain-specific Ab or CBD showed enhanced fluorescence and target selectivity, making them potential biosensors for the detection of target DNA, protein, or bacteria.
Article
Chemistry, Multidisciplinary
Francesca Lorandi, Marco Fantin, Hossein Jafari, Adam Gorczynski, Grzegorz Szczepaniak, Sajjad Dadashi-Silab, Abdirisak A. Isse, Krzysztof Matyjaszewski
Summary: Linear free energy relationships (LFERs) were used to establish the reductive cleavage of the C(sp(3))-X bond in alkyl halides (RX) by Cu complexes. The activation rate constant, k(act), for 107 Cu complex/RX couples in 5 different solvents were effectively interpolated by an equation. The set of descriptors determined the fundamental properties of Cu complexes and RX, which need to be considered when designing atom transfer radical reactions. A multivariate linear regression (MLR) approach was adopted to develop an objective model that surpassed the predictive capability of the LFER equation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaolei Hu, Grzegorz Szczepaniak, Anna Lewandowska-Andralojc, Jaepil Jeong, Bingda Li, Hironobu Murata, Rongguan Yin, Arman Moini Jazani, Subha R. Das, Krzysztof Matyjaszewski
Summary: This article introduces the first example of fully oxygen-tolerant red/NIR-light-mediated photoinduced atom transfer radical polymerization under biologically relevant conditions, using commercially available methylene blue as the catalyst. The method exhibits excellent oxygen tolerance and enables high-throughput synthesis of well-defined polymers and DNA-polymer bioconjugates in a short time.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Kostas Parkatzidis, Nghia P. Truong, Krzysztof Matyjaszewski, Athina Anastasaki
Summary: This paper introduces a photocatalytic ATRP depolymerization method, which significantly reduces the reaction temperature while enabling temporal regulation and high monomer recovery through the use of low-toxicity catalysts and visible light irradiation. The depolymerization rate can be modulated by simply turning the light on and off, and the method is compatible with various polymers and light sources while preserving the end-group fidelity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jaepil Jeong, Xiaolei Hu, Hironobu Murata, Grzegorz Szczepaniak, Marta Rachwalak, Anna Kietrys, Subha R. R. Das, Krzysztof Matyjaszewski
Summary: Combining synthetic polymers with RNA allows for creating RNA-based materials with unique functions. By developing an acylation reagent, we achieved the direct incorporation of an atom transfer radical polymerization (ATRP) initiator into both synthetic oligoribonucleotides and natural biomass RNA. This approach enables the grafting of polymer chains from RNA and the synthesis of RNA-polymer hybrids with narrow molecular weight distributions, including RNA bottlebrushes, hydrogels, and stimuli-responsive materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Polymer Science
Martin Cvek, Arman Moini Jazani, Julian Sobieski, Thaiskang Jamatia, Krzysztof Matyjaszewski
Summary: ZnO nanocrystals were successfully synthesized and used as a heterogeneous co-catalyst in mechano- and photoATRP. The photoATRP with ZnO exhibited faster reaction kinetics compared to mechanoATRP and did not require excess ligand. This study demonstrated the versatility and robustness of ZnO-cocatalyzed photoATRP for various monomers.
Article
Polymer Science
Gianluca Gazzola, Irene Filipucci, Andrea Rossa, Krzysztof Matyjaszewski, Francesca Lorandi, Edmondo M. M. Benetti
Summary: Achieving tolerance toward oxygen is essential for the upscalable and technologically relevant processes of fabricating polymer brush-coatings. By judiciously tuning the reaction mixtures and polymerization setup, the compatibility of surface-initiated photoinduced atom transfer radical polymerization (SI-photoATRP) technique can be maximized. Through precise variation of reaction conditions, key parameters like the concentration of Cu-based catalyst and free alkyl halide initiator can be optimized to efficiently consume oxygen and yield uniform and thick brushes, even in more exposed polymerization mixtures.
Article
Chemistry, Multidisciplinary
So Young An, Xinsheng Wu, Yuqi Zhao, Tong Liu, Rongguan Yin, Jung Hyun Ahn, Lynn M. Walker, Jay F. Whitacre, Krzysztof Matyjaszewski
Summary: This study synthesized bottlebrush polymers with poly(ethylene oxide) (PEO) side chains by ring-opening metathesis polymerization. These polymers can act as solid polymer electrolytes with impressive ionic conductivity and excellent electrochemical performance. The new design paradigm provides a new avenue for developing stable and conductive polymer electrolytes for lithium-metal batteries.