Article
Chemistry, Applied
Silvio Miguel Parmegiani Marcucci, Gisella Maria Zanin, Pedro Augusto Arroyo
Summary: This study successfully immobilized Burkholderia cepacia lipase by synthesizing SBA 15 with different pore diameters and modifying the silica surfaces with tin. The tin-modified silica SnS23 exhibited the largest pore size and the highest specific activity, indicating a strong interaction between lipases and modified silicas.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Environmental Sciences
Zeinab Ezzeddine, Isabelle Batonneau-Gener, Yannick Pouilloux
Summary: The removal of zinc ions from water was studied using two types of ordered mesoporous silica (SBA-15 and SBA-16). Both materials were modified with APTES and EDTA through post grafting methods. The modified adsorbents were characterized by various analytical techniques, and the structural integrity was maintained. Optimal adsorption conditions and maximum adsorption capacity were determined through experimental tests, and the regenerated adsorbent showed no significant decline in adsorption efficiency.
Article
Engineering, Environmental
Hui Dan, Hongyue Lei, Junyi Luo, Zhongxiang Guo, Yucheng Xiang, Yisheng Chen, Yi Ding
Summary: The effect of pore length, temperature, and amino-functionalization on CO2 adsorption by amino-functionalized SBA-15 (AS) was systematically investigated. It was found that the adsorption capacity and amino efficiency strongly depended on the pore length, amino-functionalization, and adsorption temperature. The short pore SAS exhibited the highest adsorption capacity and amino efficiency due to the high utilization of internal pores. Furthermore, the obtained adsorbents showed good temperature adaptability and reusability.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
Hoang Trung Trinh, Thi Kim Anh Tran, Shuchi Arora, Suchi Mercy George, Jolitta Sheri, Zhixuan Li, Jae-Hun Yang, Parichart Naruphontjirakul, Kantesh Balani, Ajay Karakoti, Ajayan Vinu
Summary: Mesoporous silica-based materials are being studied as bioscaffolds for bone regeneration. Zinc ion incorporation is important for bone regeneration and antimicrobial activity. This study compares the effect of pore size, geometry, and structure on the zinc loading and release of two different mesoporous silica materials. The results show that a 5 wt% zinc loading is sufficient for antibacterial effects and osteogenic differentiation of bone marrow-derived stromal cells.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Nuclear Science & Technology
Shuqiong Liu, Jianqiang Luo, Jianguo Ma, Jianqiang Li, Song Li, Lina Meng, Shujuan Liu
Summary: The novel amine-functionalized magnetic large-pore SBA-15 showed fast adsorption rates for uranium removal, with optimum pH of 6 and good adsorption capacity and kinetics. Compared to the pristine adsorbent, its performance was significantly improved, with spontaneous and endothermic adsorption of uranium. Additionally, it demonstrated excellent recyclability even after four consecutive adsorption-desorption cycles.
JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY
(2021)
Article
Engineering, Environmental
Xinmiao He, Li Chen, Xin Xiao, Yi Gan, Jiaping Yu, Junyi Luo, Hui Dan, Yujie Wang, Yi Ding, Tao Duan
Summary: A new Cu0-SBA-15 adsorbent with high Cu utilization for high capacity adsorption of iodine in gas and solution is reported. The Cu0-SBA-15 composite is fabricated using an improved solvothermal reduction strategy, which confines Cu0 nanoparticles on the surface or pore wall of mesoporous SBA-15, resulting in improved utilization of adsorption sites for iodine. The obtained Cu0-SBA-15 composite shows high adsorption capacities and reaches a record high Cu utilization of 96.93%.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Energy & Fuels
Yang Liu, Junjie Liao, Liping Chang, Weiren Bao
Summary: This paper investigates the adsorption performance of silver-modified mesoporous materials in removing thiophenic compounds. The results show that the adsorption of thiophene by the sorbents involves S-Ag and pi complexation reactions, and the adsorption efficiency is greatly affected by benzene. XPS analysis reveals that silver interacts strongly with the carrier and forms Ag-O-Si bonds as the active centers for thiophenic compounds. The Mulliken charges of sulfur atoms have an impact on the interactions between silver and thiophene sulfur compounds.
Article
Environmental Sciences
Yaoyu Tang, Hao Wang, Wu Sun, Dapeng Li, Zhengying Wu, Yifei Feng, Nan Xu
Summary: The removal of phosphate from water is crucial for protecting the ecological environment due to the widespread use of phosphorus fertilizers causing water deterioration. In this study, calcium carbonate-loaded mesoporous SBA-15 nanocomposites with different Ca:Si molar ratios (CaAS-x) were synthesized as effective phosphorus adsorbents. Various characterization techniques were used to examine the structure, morphology, and composition of the nanocomposites. The results showed that increasing the Ca:Si molar ratio improved the phosphate removal capacity, with CaAS-0.55 exhibiting the highest adsorption capacity. The mesoporous CaAS-0.55 nanocomposite demonstrated fast and efficient removal of high concentrations of phosphate in contaminated wastewater.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2023)
Article
Engineering, Environmental
Chaolin Wang, Kunpeng Zhang, Yu Zhao, Jing Bi, Lin Ning, Kun Zhang
Summary: This study proposes an extended simplified local density adsorption (SLD) model and combines it with nuclear magnetic resonance (NMR) tests to predict the adsorption amount and pore size distribution of coal samples. The results are beneficial for the prediction and calculation of coal adsorption amount and pore size distribution.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Engineering, Environmental
Andreina Garcia, Maibelin Rosales, Minju Thomas, Giovanni Golemme
Summary: Versatile materials for oxidizing As(III) into less hazardous As(V) species have attracted increasing attention. Ti-SBA-15, prepared by coating 7% anatase TiO2 on pre-formed SBA-15, showed efficient adsorption and photo-oxidation of As(III) at different pHs. The presence of TiO2 on SBA-15 promoted reactive oxygen species generation, leading to successful oxidation of As(III). Despite covering only a small percentage of the surface, TiO2 exhibited unprecedented photocatalytic behavior, making it a prominent catalyst for arsenic removal from water.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Engineering, Chemical
Tugba Yarbas, Alime Citak
Summary: Pure and boron-containing B-SBA-15 mesoporous materials were synthesized and characterized. The surface properties of the samples were found to be influenced by the boron content and temperature, with higher boron content resulting in more acidic surface.
INTERNATIONAL JOURNAL OF ADHESION AND ADHESIVES
(2022)
Article
Engineering, Chemical
Lady Johana Cardenas, Liliana Giraldo, Juan Carlos Moreno-Pirajan
Summary: This study characterized and investigated the adsorption properties of functionalized SBA-15/PA material, showing that the modified polyaniline silica had higher acid-base values and phenol adsorption capacity.
Article
Chemistry, Physical
Poroshat Taheri, John C. Lang, Jeffrey Kenvin, Peter Kroll
Summary: The study utilized Differential Hysteresis Scanning (DHS) Porosimetry to quantify hierarchical connectivity in amorphous silicon oxycarbide aerogels, revealing a system with monomodal distribution that exhibits uniformity usually only observed in crystalline systems.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Julio Cesar Garcia-Martinez, Gerardo Chavez-Esquivel, Margarita M. Gonzalez-Brambila, Hector H. Leon-Santiesteban, Jose A. Colin-Luna
Summary: Two mesoporous materials, SBA-15 and Zn/SBA-15, were synthesized and tested for quinoline (Q) adsorption in the presence of dibenzothiophene (DBT). The results showed that the SBA-15 adsorbent had a higher removal percentage of Q compared to the Zn/SBA-15 adsorbent, and the Zn incorporation reduced the pore volume and surface area. The highest sulfur removal was observed at a lower temperature for the Zn/SBA-15 adsorbent. Both adsorbents followed the pseudo second-order kinetic model for Q adsorption. The study provides important insights into the application of mesoporous materials for organic pollutant adsorption.
Article
Chemistry, Applied
Kai Zhuang, Minglei Yan, Chunli Qiu, Guangchun He, Quanwen He
Summary: SBA-15 mesoporous particles were successfully prepared using cyclopentanol and cyclohexanol as additives in acid aqueous solution. The morphology of the particles changes from plate-like to rod-shaped with an increase in mass ratio, while still maintaining the typical 2D p6mm mesostructure. This study proposes a six-step growth mechanism for SBA-15 particles using cyclic alcohols as additives, providing valuable insights for their preparation.
MICROPOROUS AND MESOPOROUS MATERIALS
(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
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
Yuqi Zhao, Rongguan Yin, Hanshu Wu, Zongyu Wang, Yue Zhai, Khidong Kim, Changwoo Do, Krzysztof Matyjaszewski, Michael R. Bockstaller
Summary: Van der Waals-driven self-healing in copolymers with lock-and-key architecture has been achieved by synthesizing lock-and-key copolymers with prescribed sequences. The recovery behavior of copolymers with different sequences was evaluated, and copolymers with alternating and statistical sequences showed a 10-fold increase in recovery rate compared to copolymers with a gradient sequence. The results provide strategies for designing and synthesizing engineering polymers with both structural and thermal stability and the ability to recover from structural damage.
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, Physical
Yuqi Zhao, Hanshu Wu, Rongguan Yin, Chenxi Yu, Krzysztof Matyjaszewski, Michael R. Bockstaller
Summary: The effect of sequence structure on the self-healing and shape-memory properties of copolymer-tethered brush particle films was investigated. It was found that statistical copolymer sequence provided the most rapid restoration of mechanical properties and an increase of the high T(g) (MMA) component improved the material's modulus while retaining self-healing ability. The reduction of flow in brush systems was attributed to slow cooperative relaxation due to the complex microstructure.
CHEMISTRY OF MATERIALS
(2023)
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
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.
