研究者詳細 - ジンチェンコ　アナトーリ

Biomass-derived polymers are being increasingly utilized as eco-friendly functional materials in fields ranging from medicine and food to agriculture and environmental engineering. In this report, we developed a novel efficient method for improvement of soil materials based on in situ gelation of a polyion complex formed by biomass-derived carboxymethyl cellulose (CMC) and chitosan (CS). Self-organized network of polymer films and microfibers assembled via electrostatic interactions between oppositely-charged polyions interconnects particles of soil material and imparts the resulted composite with a considerable mechanical strength. Treatment of soil even with a high water content (ca. 30%) by a mixture of CMC and CS at m(CMC + CS)/m(soil) ratio of ca. 1% is sufficient to gain up to 150 kPa compression strength that further increases up to ca. 1 MPa after drying. Similar reinforcement effect by CMC-CS complex was observed for sand, and much higher yield strengths were measured for clay. Mechanical properties of soil materials strengthened by CMC-CS complex depended on structure and stability of CMC-CS polyion network and controlled by the polymerization degrees of macromolecules and the charge ratio between them. Being composed entirely of biomass-derived polymers, the proposed soil treatment system is particularly attractive due to environmental friendliness and sustainability and it can be utilized not only for the soil improvement but also for the construction of functional platforms for soil pollution control and remediation.

DOI： 10.1016/j.jece.2023.111676

Design and Synthesis of Functional Materials by Chemical Recycling of Waste Polyethylene Terephthalate (PET): Opportunities and Challenges 査読有り

Kayee Chan, Anatoly Zinchenko

Journal of Cleaner Production 433 巻頁： 139828 2023年11月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Waste Management

The progressive accumulation of discarded plastic in the environment demands further development of waste management of plastic waste and conversion technologies of such waste to value-added materials. Recently, the conversion of plastic waste to functional materials via chemical recycling has attracted considerable attention. In this report, plastic waste (PET) was utilized for the preparation of a hydrogel-based catalyst via a cross-linking reaction of PET-derived oligo(terephthalamide)s followed by the electroless metallization. The polymeric matrix of PET-derived hydrogel plays multiple roles of (i) an adsorption media for noble metal ions such as Au3+ and Ag+, (ii) a reducing agent of Au3+ and Ag+ ions to Au0 and Ag0, and (iii) a matrix for the controlled growth of Au and Ag nanoparticles (AuNPs and AgNPs). The obtained hybrid hydrogels after metallization contained well-dispersed AuNPs and AgNPs of 6.1 ± 3.7 nm or 6.1 ± 1.4 nm size, respectively. The catalytic activities of the hybrid hydrogels with metal nanoparticles were studied in a model system of p-nitrophenol reduction in an aqueous solution. The hybrid materials of both Au@hydrogel and Ag@hydrogel were catalytically active for the reduction of p-nitrophenol, obeying the first-order kinetics. Importantly, the AuNPs or AgNPs in the hydrogel matrix preserved the original catalytic activity after multiple p-nitrophenol reduction reactions, showing a promising reusability of the catalysts. The proposed here approach aims to broaden the scope of conversion routes of plastic waste to value-added materials as well as to develop new types of polymeric matrices for templating and growth of metal nanoparticles for catalytic applications.

DOI： 10.1016/j.jclepro.2023.139828

Removal of Copper Ions Using a Waste Plastic-Derived Hydrogel Prepared via Microwave-assisted PET Aminolysis 査読有り

Chan Kayee, Kawai Masami, Yamake Mina, Zinchenko Anatoly

Gels 9 巻 ( 11 ) 頁： 874 2023年11月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Nanomaterials

Ubiquitous on Earth DNA and other nucleic acids are being increasingly considered as promising biomass resources. Due to their unique chemical structure, which is different from that of a more common carbohydrate biomass polymers, materials based on nucleic acids may exhibit new attractive characteristics. In this study, fluorescent nanoparticles (biodots) were prepared by a hydrothermal (HT) method from various nucleic acids (DNA, RNA, nucleotides, and nucleosides) to establish the relationship between the structure of precursors and fluorescent properties of biodots and to optimize conditions for preparation of the most fluorescent product. HT treatment of nucleic acids results in decomposition of sugar moieties and depurination/depyrimidation of nucleobases, while their consequent condensation and polymerization gives fluorescent nanoparticles. Fluorescent properties of DNA and RNA biodots are drastically different from biodots synthesized from individual nucleotides. In particular, biodots synthesized from purine-containing nucleotides or nucleosides show up to 50-fold higher fluorescence compared to analogous pyrimidine-derived biodots. The polymeric nature of a precursor disfavors formation of a bright fluorescent product. The reported effect of the structure of the nucleic acid precursor on the fluorescence properties of biodots should help designing and synthesizing brighter fluorescent nanomaterials with broader specification for bioimaging, sensing, and other applications.

DOI： doi.org/10.3390/gels9110874

Electrochemical extraction of methanol from lignin under mild conditions 査読有り国際共著

Hibino Takashi, Kobayashi Kazuo, Zhou Dongwen, Chen Siyuan, Zinchenko Anatoly, Teranishi Shinya, Miyawaki Aki, Sawada Yoshiharu

Applied Catalysis B: Environmental 341 巻 2023年10月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Applied Catalysis B: Environmental

We report an electrochemical approach to extract methanol from lignin with a maximum efficiency of 95% under mild conditions of ambient pressure and a temperature of 75 °C. Hydroxyl radicals were generated from water over a platinum-sputtered anode and attacked the syringyl and guaiacyl units of the lignin. Methoxy groups in the units were demethylated to methanol with a yield greater than 40% through the formation of hemiketal intermediates. The electro-oxidation was coupled to cathode reactions that generated hydrogen in a helium flow and electric power in an air flow. Another important aspect of this approach is that no extra energy or effort was required to separate methanol from the reaction system. This technology can accelerate the replacement of fossil organic resources with renewable biomass resources.

DOI： 10.1016/j.apcatb.2023.123328

Scopus

Templating of catalytic gold and silver nanoparticles by waste plastic PET-derived hydrogel playing a dual role of a reductant and a matrix 査読有り

Kayee Chan, Anatoly Zinchenko

Waste Management 164 巻頁： 20 - 28 2023年6月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Waste Management

DOI： 10.1016/j.wasman.2023.03.037

Scopus

Reconstituted TAD-size chromatin fibers feature heterogeneous nucleosome clusters 査読有り国際共著

Korolev Nikolay, Zinchenko Anatoly, Soman Aghil, Chen Qinming, Wong Sook Yi, Berezhnoy Nikolay V, Basak Rajib, van der Maarel Johan R. C., van Noort John, Nordenskiold Lars

Scientific Reports 12 巻 ( 1 ) 頁： 15558 2022年9月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Scientific Reports

Large topologically associated domains (TADs) contain irregularly spaced nucleosome clutches, and interactions between such clutches are thought to aid the compaction of these domains. Here, we reconstituted TAD-sized chromatin fibers containing hundreds of nucleosomes on native source human and lambda-phage DNA and compared their mechanical properties at the single-molecule level with shorter ‘601’ arrays with various nucleosome repeat lengths. Fluorescent imaging showed increased compaction upon saturation of the DNA with histones and increasing magnesium concentration. Nucleosome clusters and their structural fluctuations were visualized in confined nanochannels. Force spectroscopy revealed not only similar mechanical properties of the TAD-sized fibers as shorter fibers but also large rupture events, consistent with breaking the interactions between distant clutches of nucleosomes. Though the arrays of native human DNA, lambda-phage and ‘601’ DNA featured minor differences in reconstitution yield and nucleosome stability, the fibers’ global structural and mechanical properties were similar, including the interactions between nucleosome clutches. These single-molecule experiments quantify the mechanical forces that stabilize large TAD-sized chromatin domains consisting of disordered, dynamically interacting nucleosome clutches and their effect on the condensation of large chromatin domains.

DOI： 10.1038/s41598-022-19471-3

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PubMed

Aminolysis-assisted hydrothermal conversion of waste PET plastic to N-doped carbon dots with markedly enhanced fluorescence 査読有り

Kayee Chan, Anatoly Zinchenko

10 巻 ( 3 ) 頁： 107749 2022年6月

Conversion of waste bottle PET to magnetic microparticles adsorbent for dye-simulated wastewater treatment 査読有り

Chan Kayee, Zinchenko Anatoly

Journal of Environmental Chemical Engineering 10 巻 ( 3 ) 頁： 108055 2022年6月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Environmental Chemical Engineering

Mass production and consequent accumulation of plastic wastes in the environment urges the development of technologies for the efficient plastic wastes utilization and valorization to materials and products to support circular economy. Here, we report a novel conversion of PET plastic to a magnetic microparticles adsorbent prepared by co-precipitation of Fe3O4 nanoparticles with oligomeric products of PET aminolysis. The obtained adsorbent represents highly water-dispersible oligo(terephthalamide) particles of several tens μm size embedding magnetic nanoparticles randomly distributed in the organic matrix. The PET-derived magnetic adsorbent was used for the rapid and facile magnetic separation of an anionic dye (Congo Red, CR) from dye simulated water samples. The adsorbent containing plenty of amine groups showed superb adsorption capacity for CR of ca. 780 mg/g which is pH dependent and optimal at pH 6.5. Furthermore, the microparticular, non-aggregative state of the adsorbent coupled with its magnetic functionality provided rapid saturation of the adsorbent with dye by ca. 70% of the equilibrium adsorption capacity within 5 min and possibility of instantaneous removal from solution by a magnet. The proposed here material design addresses simultaneously the problem of plastic wastes utilization and preparation of cost-effective and efficient adsorbents for environmental cleaning purposes.

DOI： 10.1016/j.jece.2022.108055

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Efficient Stabilization of Soil, Sand, and Clay by a Polymer Network of Biomass-Derived Chitosan and Carboxymethyl Cellulose 査読有り

Anatoly Zinchenko, Takayuki Sakai, Kohki Morikawa, Masaki Nakano

Journal of Environmental Chemical Engineering 10 巻 ( 1 ) 2022年2月

担当区分：筆頭著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Environmental Chemical Engineering

DOI： 10.1016/j.jece.2021.107084

Scopus

DNA-Chitosan Aerogels and Regenerated Hydrogels with Extraordinary Mechanical Properties 査読有り国際共著

Postnova Irina, Sarin Sergey, Zinchenko Anatoly, Shchipunov Yury

ACS Applied Polymer Materials 4 巻 ( 1 ) 頁： 663 - 671 2021年12月

記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：ACS Applied Polymer Materials

It has recently been shown that native ds-DNA and chitosan can coassemble without common phase separation and precipitation, forming a translucent homogeneous hydrogel. This simple approach consists of progressive charging of the polysaccharide through gradual acidification of a solution in the presence of DNA, which slowly strengthens the electrostatic interactions between them, ruling out fast and uncontrolled cooperative association, which is a well-known problem associated with coacervation. Homogeneous hydrogels thus fabricated demonstrated mechanical properties characteristic of quite strong physical hydrogels. Extraordinary mechanical strength and elasticity have been observed in aerogels prepared from an original hydrogel and also in hydrogels, which were restored by the rehydration of aerogels. Aerogels match highly cross-linked synthetic polyurethane foams despite DNA with chitosan being bound only via electrostatic interactions without using a toxic cross-linking agent. Owing to their biocompatibility, biodegradability, and available renewable resources, hydrogels and aerogels might replace typical synthetic polymers. The fabrication of bionanocomposites with luminescent, sensing, and photocatalytic functionalities by entrapping quantum dots, titania nanoparticles, and dyes demonstrates some possible applications.

DOI： 10.1021/acsapm.1c01585

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Conversion of waste bottles' PET to a hydrogel adsorbent via PET aminolysis 査読有り

Kayee Chan, Anatoly Zinchenko

Journal of Environmental Chemical Engineering 9 巻 ( 5 ) 頁： 106129 2021年10月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Journal of Environmental Chemical Engineering

To ensure sustainable use of natural resources and circulation of materials, efficient methods of waste plastic conversion into value chemicals and scenarios for utilization of the latter are increasingly demanded. Here, we propose a method of waste PET bottles conversion to cross-linked hydrogels through PET aminolysis using tri- and tetraamines as a method of plastic waste valorization. Water-soluble oligomeric products of PET aminolysis were cross-linked in water using diglycidyl ether to get mechanically stable hydrogels that show typical polyelectrolyte behavior of polycations. PET-derived hydrogels abundant with amino groups and aromatic moieties were tested as adsorbents for an anionic dye such as Congo Red, and their absorption capacity towards dye was found to be ca. 500 mg/g. Beside demonstrated here application of PET-derived hydrogels for water cleaning from an industrial dye, utilization of such hydrogel materials in fields of environment, agriculture, separation, etc. are also anticipated.

DOI： 10.1016/j.jece.2021.106129

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Metal Ions Sensing by Biodots Prepared from DNA, RNA, and Nucleotides 査読有り国際共著国際誌

Wang Maofei, Tsukamoto Masaki, Sergeyev Vladimir G., Zinchenko Anatoly

Biosensors 11 巻 ( 9 ) 頁： 333 2021年9月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Biosensors

Nucleic acids that exhibit a high affinity toward noble and transition metal ions have attracted growing attention in the fields of metal ion sensing, toxic metal ion removal, and the construction of functional metal nanostructures. In this study, fluorescent nanoparticles (biodots) were synthesized from DNA, RNA, and RNA nucleotides (AMP, GMP, UMP, and CMP) using a hydrothermal (HT) method, in order to study their metal ion sensing characteristics. The fluorescent properties of biodots differ markedly between those prepared from purine and pyrimidine nucle-obases. All biodots demonstrate a high sensitivity to the presence of mercury cations (Hg2+ ), while biodots prepared from DNA, RNA, and guanosine monophosphate (GMP) are also sensitive to Ag+ and Cu2+ ions, but to a lesser extent. The obtained results show that biodots inherit the metal ion recognition properties of nucleobases, while the nucleobase composition of biodot precursors affects metal ion sensitivity and selectivity. A linear response of biodot fluorescence to Hg2+ concentration in solution was observed for AMP and GMP biodots in the range 0–250 µM, which can be used for the analytic detection of mercury ion concentration. A facile paper strip test was also developed that allows visual detection of mercury ions in solutions.

DOI： 10.3390/bios11090333

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PubMed

Fluorescent Nanoparticles Synthesized from DNA, RNA, and Nucleotides 査読有り国際共著

Wang Maofei, Tsukamoto Masaki, Sergeyev Vladimir G., Zinchenko Anatoly

Nanomaterials 11 巻 ( 9 ) 頁： 2265 2021年9月

担当区分：最終著者,　責任著者記述言語：英語掲載種別：研究論文（学術雑誌）出版者・発行元：Nanomaterials

DOI： 10.3390/nano11092265

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PubMed