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Tkachenko, O., Nikolaichuk, A., Fihurka, N. V., Backhaus, A., Zimmerman, J. B., Strömme, M. & Budnyak, T. (2024). Kraft Lignin-Derived Microporous Nitrogen-Doped Carbon Adsorbent for Air and Water Purification. ACS Applied Materials and Interfaces, 16(3), 3427-3441
Open this publication in new window or tab >>Kraft Lignin-Derived Microporous Nitrogen-Doped Carbon Adsorbent for Air and Water Purification
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2024 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 16, no 3, p. 3427-3441Article in journal (Refereed) Published
Abstract [en]

The study presents a streamlined one-step process for producing highly porous, metal-free, N-doped activated carbon (N-AC) for CO2 capture and herbicide removal from simulated industrially polluted and real environmental systems. N-AC was prepared from kraft lignin─a carbon-rich and abundant byproduct of the pulp industry, using nitric acid as the activator and urea as the N-dopant. The reported carbonization process under a nitrogen atmosphere renders a product with a high yield of 30% even at high temperatures up to 800 °C. N-AC exhibited a substantial high N content (4–5%), the presence of aliphatic and phenolic OH groups, and a notable absence of carboxylic groups, as confirmed by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Boehm’s titration. Porosity analysis indicated that micropores constituted the majority of the pore structure, with 86% of pores having diameters less than 0.6 nm. According to BET adsorption analysis, the developed porous structure of N-AC boasted a substantial specific surface area of 1000 m2 g–1. N-AC proved to be a promising adsorbent for air and water purification. Specifically, N-AC exhibited a strong affinity for CO2, with an adsorption capacity of 1.4 mmol g–1 at 0.15 bar and 20 °C, and it demonstrated the highest selectivity over N2 from the simulated flue gas system (27.3 mmol g–1 for 15:85 v/v CO2/N2 at 20 °C) among all previously reported nitrogen-doped AC materials from kraft lignin. Moreover, N-AC displayed excellent reusability and efficient CO2 release, maintaining an adsorption capacity of 3.1 mmol g–1 (at 1 bar and 25 °C) over 10 consecutive adsorption–desorption cycles, confirming N-AC as a useful material for CO2 storage and utilization. The unique cationic nature of N-AC enhanced the adsorption of herbicides in neutral and weakly basic environments, which is relevant for real waters. It exhibited an impressive adsorption capacity for the herbicide 2,4-dichlorophenoxyacetic acid (2,4-D) at 96 ± 6 mg g–1 under pH 6 and 25 °C according to the Langmuir–Freundlich model. Notably, N-AC preserves its high adsorption capacity toward 2,4-D from simulated groundwater and runoff from tomato greenhouse, while performance in real samples from Fyris river in Uppsala, Sweden, causes a decrease of only 4–5%. Owing to the one-step process, high yield, annual abundance of kraft lignin, and use of environmentally friendly activating agents, N-AC has substantial potential for large-scale industrial applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2024
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-521753 (URN)10.1021/acsami.3c15659 (DOI)001150631600001 ()38194630 (PubMedID)
Funder
Swedish Research Council Formas, 2020-02321Uppsala UniversityCarl Tryggers foundation , CTS 21:1701
Available from: 2024-01-27 Created: 2024-01-27 Last updated: 2024-02-21Bibliographically approved
Tammela, P., Iurchenkova, A. A., Wang, Z., Strömme, M., Nyholm, L. & Lindh, J. (2024). Laser irradiation of photothermal precursors – a novel approach to produce carbon materials for supercapacitors. ChemSusChem, 1-11, Article ID e20230.
Open this publication in new window or tab >>Laser irradiation of photothermal precursors – a novel approach to produce carbon materials for supercapacitors
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2024 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, p. 1-11, article id e20230Article in journal (Refereed) Published
Abstract [en]

A wide array of carbon materials finds extensive utility across various industrial applications today. Nonetheless, the production processes for these materials continue to entail elevated temperatures, necessitate the use of inert atmospheres, and often involve the handling of aggressive and toxic chemicals. The prevalent method for large-scale carbon material production, namely the pyrolysis of waste biomass and polymers, typically unfolds within the temperature range of 500–700 °C under a nitrogen (N2) atmosphere. Unfortunately, this approach suffers from significant energy inefficiency due to substantial heat loss over extended processing durations. In this work, we propose an interesting alternative: the carbonization of photothermal nanocellulose/polypyrrole composite films through CO2 laser irradiation in the presence of air. This innovative technique offers a swift and energy-efficient means of preparing carbon materials. The unique interaction between nanocellulose and polypyrrole imparts the film with sufficient stability to retain its structural integrity post-carbonization. This breakthrough opens up new avenues for producing binder-free electrodes using a rapid and straightforward approach. Furthermore, the irradiated film demonstrates specific and areal capacitances of 159 F g−1 and 62 μF cm−2, respectively, when immersed in a 2 M NaOH electrolyte. These values significantly surpass those achieved by current commercial activated carbons. Together, these attributes render CO2-laser carbonization an environmentally sustainable and ecologically friendly method for carbon material production.

Place, publisher, year, edition, pages
Society Publishing, 2024
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-524624 (URN)10.1002/cssc.202301471 (DOI)
Funder
Swedish Energy Agency
Available from: 2024-03-08 Created: 2024-03-08 Last updated: 2024-03-08
Kong, X., Wu, Z., Strömme, M. & Xu, C. (2023). Ambient Aqueous Synthesis of Imine-Linked Covalent Organic Frameworks (COFs) and Fabrication of Freestanding Cellulose Nanofiber@COF Nanopapers. Journal of the American Chemical Society, 146(1), 742-751, Article ID 14.
Open this publication in new window or tab >>Ambient Aqueous Synthesis of Imine-Linked Covalent Organic Frameworks (COFs) and Fabrication of Freestanding Cellulose Nanofiber@COF Nanopapers
2023 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 146, no 1, p. 742-751, article id 14Article in journal (Refereed) Published
Abstract [en]

Covalent organic frameworks (COFs) are usually synthesized under solvothermal conditions that require the use of toxic organic solvents, high reaction temperatures, and complicated procedures. Additionally, their insolubility and infusibility present substantial challenges in the processing of COFs. Herein, we report a facile, green approach for the synthesis of imine-linked COFs in an aqueous solution at room temperature. The key behind the synthesis is the regulation of the reaction rate. The preactivation of aldehyde monomers using acetic acid significantly enhances their reactivity in aqueous solutions. Meanwhile, the still somewhat lower imine formation rate and higher imine breaking rates in aqueous solution, in contrast to conventional solvothermal synthesis, allow for the modulation of the reaction equilibrium and the crystallization of the products. As a result, highly crystalline COFs with large surface areas can be formed in relatively high yields in a few minutes. In total, 16 COFs are successfully synthesized from monomers with different molecular sizes, geometries, pendant groups, and core structures, demonstrating the versatility of this approach. Notably, this method works well on the gram scale synthesis of COFs. Furthermore, the aqueous synthesis facilitates the interfacial growth of COF nanolayers on the surface of cellulose nanofibers (CNFs). The resulting CNF@COF hybrid nanofibers can be easily processed into freestanding nanopapers, demonstrating high efficiency in removing trace amounts of antibiotics from wastewater. This study provides a route to the green synthesis and processing of various COFs, paving the way for practical applications in diverse fields.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Chemistry
Identifiers
urn:nbn:se:uu:diva-518588 (URN)10.1021/jacs.3c10691 (DOI)001140877500001 ()38112524 (PubMedID)
Funder
Swedish Energy Agency
Available from: 2023-12-20 Created: 2023-12-20 Last updated: 2024-01-23Bibliographically approved
Zaar, F., Emanuelsson, R., Gaiser, P., Strömme, M. & Sjödin, M. (2023). Characterization and catalytic prospects of metalloporphyrin-functionalized conducting polymers. Electrochimica Acta, 467, Article ID 143003.
Open this publication in new window or tab >>Characterization and catalytic prospects of metalloporphyrin-functionalized conducting polymers
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2023 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 467, article id 143003Article in journal (Refereed) Published
Abstract [en]

Molecular catalysts are attracting interest as drivers of redox reactions for sustainable applications. Through systematic molecular design, they could be engineered to have high selectivity and activity towards a multitude of catalytic reactions. However, as long as they are used in homogeneous setups, they will suffer from inconvenient energy supply, inefficient charge transport and difficulty in separation from reaction products. To be relevant for industrial applications, molecular catalysts must be bound to solid materials in direct contact with the energy source. In this regard, conducting polymers are particularly interesting, as they provide a straightforward means of both surface immobilization and charge transport. In this work, we synthesize and characterize three different metalloporphyrin-functionalized conducting polymers and apply them to catalysis of the hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR). We show that incorporation of porphyrins into conducting polymers is a reliable immobilization method, that the properties of both the porphyrin units and the polymer backbone are preserved in all systems, and that the polymers provide efficient charge transport to and from the catalytic centers. Nevertheless, we also find that the polymers are negatively affected by intermediates formed during the HER and the ORR. We conclude that the choice of immobilization method has a large impact on the quality of the molecular catalyst, and that the effect of the catalytic cycle on the immobilization matrix must be considered in the molecular design process.

Place, publisher, year, edition, pages
Elsevier BV, 2023
Keywords
Conducting polymers, Porphyrins, Electrocatalysis, Redox chemistry, Reaction kinetics
National Category
Organic Chemistry
Identifiers
urn:nbn:se:uu:diva-514756 (URN)10.1016/j.electacta.2023.143003 (DOI)001075908300001 ()
Funder
Swedish Research Council Formas, 2019-01285
Available from: 2023-10-24 Created: 2023-10-24 Last updated: 2023-10-24Bibliographically approved
Palo-Nieto, C., Blasi Romero, A., Sandström, C., Balgoma, D., Hedeland, M., Strömme, M. & Ferraz, N. (2023). Chemical Modification of cellulose nanofibrils to develop novel ROS-sensitive biomaterials. In: : . Paper presented at Spanish Carbohydrate Meeting (CARB 2023).
Open this publication in new window or tab >>Chemical Modification of cellulose nanofibrils to develop novel ROS-sensitive biomaterials
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2023 (English)Conference paper, Poster (with or without abstract) (Refereed)
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-509811 (URN)
Conference
Spanish Carbohydrate Meeting (CARB 2023)
Available from: 2023-08-23 Created: 2023-08-23 Last updated: 2023-11-20
Katsiotis, C. S., Tikhomirov, E., Strømme, M., Lindh, J. & Welch, K. (2023). Combinatorial 3D printed dosage forms for a two-step and controlled drug release. European Journal of Pharmaceutical Sciences, 187, Article ID 106486.
Open this publication in new window or tab >>Combinatorial 3D printed dosage forms for a two-step and controlled drug release
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2023 (English)In: European Journal of Pharmaceutical Sciences, ISSN 0928-0987, E-ISSN 1879-0720, Vol. 187, article id 106486Article in journal (Refereed) Published
Abstract [en]

Fused deposition modeling (FDM) and selective laser sintering (SLS) are two of the most employed additive manufacturing (AM) techniques within the pharmaceutical research field. Despite the numerous advantages of different AM methods, their respective drawbacks have yet to be fully addressed, and therefore combinatorial systems are starting to emerge. In the present study, hybrid systems comprising SLS inserts and a two-compartment FDM shell are developed to achieve controlled release of the model drug theophylline. Via the use of SLS a partial amorphization of the drug is demonstrated, which can be advantageous in the case of poorly soluble drugs, and it is shown that sintering parameters can regulate the dosage and release kinetics of the drug from the inserts. Furthermore, via different combinations of inserts within the FDM-printed shell, various drug release patterns, such as a two-step or prolonged release, can be achieved. The study serves as a proof of concept, highlighting the advantages of combining two AM techniques, both to overcome their respective shortcomings and to develop modular and highly tunable drug delivery devices.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Fused deposition modeling, FDM, Selective laser sintering, SLS, Controlled drug release, Hybrid system
National Category
Nano Technology Pharmaceutical Sciences
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-504425 (URN)10.1016/j.ejps.2023.106486 (DOI)001028333700001 ()
Funder
Vinnova, 2019-00029Swedish Research Council, 2019-03729
Available from: 2023-06-13 Created: 2023-06-13 Last updated: 2024-02-23Bibliographically approved
Sjödin, M., Rikard, E., Strietzel, C., Wang, H. & Strömme, M. (2023). Conducting Redox Polymers as Active Materials in Secondary Batteries. In: : . Paper presented at 74th Annual Meeting of the International Society of Electrochamistry.
Open this publication in new window or tab >>Conducting Redox Polymers as Active Materials in Secondary Batteries
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2023 (English)Conference paper, Oral presentation with published abstract (Refereed)
National Category
Other Materials Engineering
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-516846 (URN)
Conference
74th Annual Meeting of the International Society of Electrochamistry
Available from: 2023-11-30 Created: 2023-11-30 Last updated: 2023-11-30
Katsiotis, C. S., Tikhomirov, E., Leliopoulos, C., Strömme, M. & Welch, K. (2023). Development of a simple paste for semi-solid extrusion of different drug formulations containing a drug-loaded mesoporous material.. In: : . Paper presented at ACS Fall, San Francisco.
Open this publication in new window or tab >>Development of a simple paste for semi-solid extrusion of different drug formulations containing a drug-loaded mesoporous material.
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2023 (English)Conference paper, Oral presentation only (Refereed)
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-509949 (URN)
Conference
ACS Fall, San Francisco
Available from: 2023-08-24 Created: 2023-08-24 Last updated: 2023-08-24
Åhlén, M., Zhou, Y., Hedbom, D., Cho, H. S., Strømme, M., Terasaki, O. & Cheung, O. (2023). Efficient SF6 capture and separation in robust gallium- and vanadium-based metal–organic frameworks. Journal of Materials Chemistry A, 11(48), 26435-26441
Open this publication in new window or tab >>Efficient SF6 capture and separation in robust gallium- and vanadium-based metal–organic frameworks
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2023 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 48, p. 26435-26441Article in journal (Refereed) Published
Abstract [en]

Sulfur hexafluoride (SF6) is a highly potent greenhouse gas (GHG) that is mainly emitted from high-voltage electrical applications. The global warming potential (GWP) of the gas is almost 23 000 times that of CO2 and therefore, controlling its emission and recovery is of great importance from both an environmental and economic perspective. Solid adsorbents and adsorption-based technology is a cost-effective and energy-efficient pathway to recapture SF6 from its sources, which usually consist of dilute SF6 in N2. Here, we present a group of four highly porous and robust gallium- or vanadium-based metal–organic frameworks (MOFs) with exceptional SF6 uptake and selectivity. In particular, the novel gallium 1,2,4,5-tetrakis(4-carboxlatephenyl)benzene (TCPB4−) MOF (Ga-TBAPy) possesses 1-dimensional channels of suitable size (5.2 × 8.4 Å and 5.3 × 10 Å) to adsorb up to 2.25 mmol g−1 of SF6 at 10 kPa with an excellent SF6-over-N2 selectivity of 418. Ga-TCPB also exhibits high chemical stability in aqueous and acidic media as well as in organic solvents. 3D electron diffraction (3D ED) patterns combined with high-resolution electron microscopy images were employed to investigate the structure of these water-stable and cyclable MOF SF6 adsorbents. Furthermore, this study demonstrates the possibility of using these highly stable MOFs to capture SF6 from a gas mixture as well as how MOFs can offer an alternative and efficient way to mitigate the global warming contributions from the emission of SF6.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2023
National Category
Nano Technology Other Chemical Engineering
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-517993 (URN)10.1039/d3ta05297d (DOI)001110673700001 ()
Funder
Mistra - The Swedish Foundation for Strategic Environmental Research, 2015/31Swedish Research Council, 2020-04029Swedish Research Council, 2019-03729Swedish Research Council Formas, 2018-00651Swedish Research Council, 2019-00207
Available from: 2023-12-15 Created: 2023-12-15 Last updated: 2023-12-15Bibliographically approved
Palo-Nieto, C., Blasi-Romero, A., Sandström, C., Balgoma, D., Hedeland, M., Strømme, M. & Ferraz, N. (2023). Functionalization of cellulose nanofibrils to develop novel ROS-sensitive biomaterials. Materials Advances, 4(6), 1555-1565
Open this publication in new window or tab >>Functionalization of cellulose nanofibrils to develop novel ROS-sensitive biomaterials
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2023 (English)In: Materials Advances, E-ISSN 2633-5409, Vol. 4, no 6, p. 1555-1565Article in journal (Refereed) Published
Abstract [en]

Wood derived cellulose nanofibrils (CNFs) have emerged as an interesting material for biomedical applications. Functionalization of the nanofibrils with bioactive molecules is a potent tool to tailor CNF materials for specific applications in biomedicine. The present work proposes the functionalization of CNFs with a reactive oxygen species (ROS)-sensitive oligopeptide to develop a novel CNF-based material for the treatment of medical conditions associated with high levels of ROS such as chronic wounds. Oligoproline peptides of two different lengths (5 and 10 proline units) were covalently incorporated onto the CNF surface, several water-based chemical approaches were explored and the reaction conditions to maximize peptide substitution and the degree of fibre crosslinking were optimized. The chemical structure, degree of peptide substitution, degree of fibre crosslinking, surface morphology and ROS-sensitivity of the oligoproline–CNF materials were characterized. Double-crosslinked CNF hydrogels (Ca2+–oligoproline–CNF) were further prepared and the ability of the hydrogels to protect cells from an oxidative environment was investigated in vitro with human dermal fibroblasts, as a first evaluation of the potential of the novel CNF material to be used in chronic wound therapies. Optimization of the reaction conditions resulted in a degree of peptide substitution of 102 ± 10 μmol g−1 CNF irrespective of the oligoproline length and a degree of crosslinking of 55–80% depending on the number of proline units. The results showed that the oligoproline covalently attached to CNFs via carbodiimide chemistry maintained its ability to respond to ROS and that the responsiveness in terms of viscoelastic properties depended on the length of the oligopeptide, with the hydrogel being more responsive when functionalized with 10 proline units compared with 5 proline units. Furthermore, the double crosslinked Ca2+–oligoproline–CNF hydrogels promoted the survival of human dermal fibroblasts exposed to high levels of ROS. This study is the first one to provide an insight into the development of ROS-sensitive materials based on CNFs and opens up possibilities for further investigation on the use of these novel materials in chronic wound care.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2023
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-497259 (URN)10.1039/D2MA01056A (DOI)000939471200001 ()
Funder
Swedish Research Council, 2018-04613Olle Engkvists stiftelse, 191-419
Available from: 2023-02-25 Created: 2023-02-25 Last updated: 2023-05-15Bibliographically approved
Projects
Adhesion optimized bioactive surgical implants with optional drug delivery function [2008-04247_VINNOVA]; Uppsala UniversityMolecular Nanodiagnostics [2010-02580_VR]; Uppsala UniversityNanostructured paper materials for ion exchange and energy storage [2010-05032_VR]; Uppsala UniversityUpsalite; a novel mesoporous magnesium carbonate as stabilizer and solubility enhancer of amorphous compounds [2014-03929_VR]; Uppsala UniversityDiagnosing infectious diseases in low-income countries and regions, having under-developed infrastructures in collaboration with the UN organ FAO/IAEA and its network in Africa with focus on pathogens [2015-03640_VR]; Uppsala UniversityA Resource Efficient Society with sustainable processes for using the waste residue streams from pulp production to produce chemicals for electric energy storage based on reNEWable MATerials (RES-NEWMAT). [P46517-1_Energi]; Uppsala UniversityTailoring mesoporous materials for additive manufacturing of personalized medication (MesMatMed) [2019-03729_VR]; Uppsala UniversitySorption of ions from solutions using bio-based waste stream materials as sorbents [2022-02042_Formas]; Uppsala University
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-5496-9664

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