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Viscoelastic behaviors for optimizing self-healing of gels with host–guest inclusion complexes 优化含有主客体包合物的凝胶自愈合的粘弹性行为
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-11 DOI: 10.1038/s41428-024-00932-7
Kenji Yamaoka, Ryohei Ikura, Motofumi Osaki, Hidenori Shirakawa, Kazuya Takahashi, Hiroaki Takahashi, Yasumasa Ohashi, Yoshinori Takashima
{"title":"Viscoelastic behaviors for optimizing self-healing of gels with host–guest inclusion complexes","authors":"Kenji Yamaoka, Ryohei Ikura, Motofumi Osaki, Hidenori Shirakawa, Kazuya Takahashi, Hiroaki Takahashi, Yasumasa Ohashi, Yoshinori Takashima","doi":"10.1038/s41428-024-00932-7","DOIUrl":"10.1038/s41428-024-00932-7","url":null,"abstract":"This research showed that the self-healing properties of reversible crosslinked gels with host–guest inclusion complexes depended on the mobility of network chains and the recombination behaviors of reversible complexes, which were affected by changes in the water–glycerol solvent composition. The sticky reptation behaviors of the polymer chains were delayed by the recombination behaviors of reversible bonds. These behavioral characteristics were observed based on a dynamic viscoelasticity. Increasing the glycerol concentration in the mixed solvent decreased the surface tension and increased the mobility of the network chains because the recombination of the complex was slowed by the weak hydrophobic interactions between the host and guest molecules. Consequently, self-healing properties, such as re-adhesion at the cutting surface, were improved by the interdiffusion of polymer chains at the reattached interface. The strong hydrophobic interactions in pure water promoted the formation of complexes within the same cutting surface, thus decreasing the self-healing rates of the mechanical properties. In this study, the solvent was found to be an important parameter for controlling the self-healing properties of reversible crosslinked gels. The competition between the mobility of polymer chains and the recombination behaviors of reversible bonds controlled the self-healing properties of the gels with host–guest inclusion complexes. This study examined how changing the water-glycerol solvent composition affects the self-healing and viscoelastic properties of self-healing gels, which have host-guest inclusion complexes as reversible crosslinks. Increasing glycerol concentration in the mixture solvent reduced hydrophobic interactions between β-cyclodextrin and adamantane, lowering the association constant of host-guest inclusion complexes. The weakened hydrophobic interaction hinders complex recombination and enhances the mobility of the network chains. Consequently, the enhancement of mobility improved the healing ratio because the interfacial diffusion of the chains was promoted at the repair interfaces.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 11","pages":"1031-1039"},"PeriodicalIF":2.3,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00932-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222750","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Post-functionalization of alternating π-conjugated copolymers containing fluorene moieties via anodic chlorination using AlCl3 使用 AlCl3 阳极氯化法对含有芴分子的交替 π 共轭共聚物进行后官能化处理
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-10 DOI: 10.1038/s41428-024-00958-x
Tomoyuki Kurioka, Ikuyoshi Tomita, Shinsuke Inagi
{"title":"Post-functionalization of alternating π-conjugated copolymers containing fluorene moieties via anodic chlorination using AlCl3","authors":"Tomoyuki Kurioka, Ikuyoshi Tomita, Shinsuke Inagi","doi":"10.1038/s41428-024-00958-x","DOIUrl":"10.1038/s41428-024-00958-x","url":null,"abstract":"Fluorene (Fl) derivatives are representative emitting motifs; thus, they are often installed into alternating π-conjugated copolymers (P(Fl-Ar)) as soluble polymeric emitters. Many researchers have focused on modifying the combined arylene units in P(Fl-Ar) derivatives to tune their optoelectronic properties; however, P(Fl-Ar) derivatives that contain fluorene units with functional groups at their sp2 carbons remain limited. Here, we synthesize P(Fl-Ar) derivatives comprising sp2-chlorinated fluorene units via anodic chlorination using aluminum chloride (AlCl3). The introduced chlorine atoms affect the optoelectronic properties of the pristine P(Fl-Ar) derivatives. Compared with the precursor P(Fl-Ar) derivatives, chlorinated P(Fl-Ar) derivatives exhibit longer maximum emission wavelengths. Alternating π-conjugated copolymers containing 9,9-dialkylfluorene (Fl) units have been widely studied, but there are few of these copolymers with sp2-carbon functionalized Fl units. In this study, we expand this limitation by performing the anodic chlorination of alternating π-conjugated copolymers, which are composed of Fl and another arylene (Ar) (P(Fl-Ar)s), using an acetonitrile solution that contains aluminum chloride as an electrolyte. The sp2-carbon at the fluorene ring was successfully chlorinated by anodic chlorination. P(Fl-Ar)s containing sp2-chlorinated fluorene units has different emission properties from the original P(Fl-Ar)s.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1117-1127"},"PeriodicalIF":2.3,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00958-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222751","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fabrication of a peptide–AuNP–TiO2 nanocomposite and its application as a VOC sensor 多肽-AuNP-TiO2 纳米复合材料的制备及其在挥发性有机化合物传感器中的应用
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-10 DOI: 10.1038/s41428-024-00960-3
Toma Iwakiri, Hikari Suzuki, Shogo Mastubara, Masahiro Higuchi
{"title":"Fabrication of a peptide–AuNP–TiO2 nanocomposite and its application as a VOC sensor","authors":"Toma Iwakiri, Hikari Suzuki, Shogo Mastubara, Masahiro Higuchi","doi":"10.1038/s41428-024-00960-3","DOIUrl":"10.1038/s41428-024-00960-3","url":null,"abstract":"We fabricated a volatile organic compound (VOC) sensor with a peptide–Au nanoparticle (AuNP)–TiO2 nanocomposite in which AuNPs were linked with TiO2-coated conductive peptide nanowires. The conductive peptide nanowires were formed between the AuNPs via self-assembly through the complexation of amphiphilic peptides, LESEHEKLKSKHKSKLKEHESEL, and Co(II). Furthermore, TiO2 mineralization on the surface of the peptide nanowires yielded mixed crystals of rutile and anatase, which exhibited highly effective photolytic activity. In particular, the obtained TiO2 exhibited three times greater photodecomposition activity in the unsintered state toward organic matter than did commercially available TiO2. Next, we constructed a VOC sensor by immobilizing peptide–AuNP–TiO2 nanocomposites on a comb electrode. The electrochemical properties of the nanocomposite changed drastically under light irradiation in the presence of VOCs, indicating transport of the VOC-decomposition-generated photoexcited electrons of TiO2 to AuNPs through conductive peptide nanowires, which prevented electron–hole recombination. The obtained sensor exhibited a sensing range of 2–100 ppm for dichloromethane, which was used as a representative VOC. Therefore, nanocomposites made of AuNPs linked with conductive TiO2 nanotubes may be highly effective for TiO2-driven VOC decomposition. Moreover, we believe that this nanocomposite has high sensitivity for sensing VOCs. The peptide-Au nanoparticle (AuNP)-TiO2 nanocomposite in which AuNPs were connected by TiO2-coated conductive peptide nanowire was acted as effective VOC sensor.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1211-1221"},"PeriodicalIF":2.3,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00960-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stimuli-responsive smart polymers based on functional dyes 基于功能性染料的刺激响应型智能聚合物
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-05 DOI: 10.1038/s41428-024-00951-4
Keiichi Imato, Yousuke Ooyama
{"title":"Stimuli-responsive smart polymers based on functional dyes","authors":"Keiichi Imato, Yousuke Ooyama","doi":"10.1038/s41428-024-00951-4","DOIUrl":"10.1038/s41428-024-00951-4","url":null,"abstract":"Functional dyes exhibit intriguing properties in response to external stimuli related to their optical, electronic, structural, and energetic characteristics and enable unique stimuli-responsive functions in materials by collaborating with polymers, particularly when chemically incorporated into the polymer structures. As well as the structures and properties of functional dyes, polymers, assemblies, and materials, the interactions between these components are important to the functions of materials. In this review, we introduce our recent studies conducted in the past half decade on stimuli-responsive smart polymers and polymeric materials based on functional dyes that are chemically incorporated into the polymer structures, with a special focus on light, force, electric fields, and chemicals including water in a variety of external stimuli. For example, these polymers and materials offer switchable adhesion, mechanical actuation, and chemical sensing. Functional dyes offer fascinating properties in response to external stimuli and enable unique stimuli-responsive functions in materials by chemical incorporation into polymers. In this review, we highlight our recent studies conducted in the last half decade on stimuli-responsive smart polymers and polymeric materials offering, for example, switchable adhesion, mechanical actuation, and chemical sensing based on functional dyes that are chemically incorporated into the structures, with a particular focus on the stimuli of light, force, electric fields, and chemicals including water.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1093-1109"},"PeriodicalIF":2.3,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00951-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222754","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Osteogenic differentiation capabilities of multiarm PEG hydrogels: involvement of gel–gel-phase separation in cell differentiation 多臂 PEG 水凝胶的成骨分化能力:凝胶-凝胶相分离在细胞分化中的作用
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-03 DOI: 10.1038/s41428-024-00955-0
Jinyan Si, Shohei Ishikawa, Shant Nepal, Hiroyuki Okada, Ung-il Chung, Takamasa Sakai, Hironori Hojo
{"title":"Osteogenic differentiation capabilities of multiarm PEG hydrogels: involvement of gel–gel-phase separation in cell differentiation","authors":"Jinyan Si, Shohei Ishikawa, Shant Nepal, Hiroyuki Okada, Ung-il Chung, Takamasa Sakai, Hironori Hojo","doi":"10.1038/s41428-024-00955-0","DOIUrl":"10.1038/s41428-024-00955-0","url":null,"abstract":"The development of bioactive scaffolds is essential for tissue engineering because of the influence of material physicochemical properties on cellular activities. Recently, we discovered that percolation-induced 4-arm polyethylene glycol (PEG) hydrogels achieved gel–gel phase separation (GGPS), which has tissue affinity in vivo. However, whether the 4-arm structure is the optimal configuration for the use of PEG hydrogels as scaffolds remains unclear. In this study, we investigated the effect of an increased branching factor on GGPS. Compared with the 4-arm PEG hydrogel, the 8-arm PEG hydrogel presented a greater degree of GGPS and increased hydrophobicity. We introduced the RGD sequence into PEG hydrogels to directly assess the biological activity of GGPS, with a particular focus on its effects on the activity of bone-forming osteoblasts. Although the 8-arm PEG hydrogel did not enhance cell adhesion, it enhanced osteoblast differentiation compared with the 4-arm PEG hydrogel. Therefore, the 8-arm PEG hydrogel mediated by GGPS shows promise as a scaffold for osteoblast differentiation and holds potential as a foundation for future advancements in bone tissue engineering. The degree of gel-gel phase separation (GGPS) was compared using multi-arm poly(ethylene glycol) (PEG) hydrogels. GGPS can occur at c < c*, with 8-arm PEG exhibiting a stronger turbidity (D) indicating stronger GGPS compared to 4-arm PEG. This indicates that phase-separated PEG can be obtained at low concentrations simply by increasing the number of branches. Furthermore, phase-separated 8-arm PEG showed higher osteogenic differentiation in vitro.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 4","pages":"407-417"},"PeriodicalIF":2.3,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00955-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222758","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-strength, conductive, double-network self-healing antibacterial hydrogel based on the coordination bond and dynamic imine bond 基于配位键和动态亚胺键的高强度、导电、双网络自愈合抗菌水凝胶
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-09-03 DOI: 10.1038/s41428-024-00957-y
Yalei Liu, Junfang Chang, Zhiyong Guo, Sui Wang, Jie Mao
{"title":"High-strength, conductive, double-network self-healing antibacterial hydrogel based on the coordination bond and dynamic imine bond","authors":"Yalei Liu, Junfang Chang, Zhiyong Guo, Sui Wang, Jie Mao","doi":"10.1038/s41428-024-00957-y","DOIUrl":"10.1038/s41428-024-00957-y","url":null,"abstract":"Multifunctional hydrogel materials are being increasingly used in wearable sensing devices and biomedical applications, but the comprehensive performance of hydrogel materials must be further developed. To prepare hydrogels with better self-healing properties, biomacromolecules such as sodium alginate and carboxymethyl chitosan were used as raw materials by combining the dynamic imine bonding network formed by both materials with the coordination bonding network formed by acrylic acid and aluminum ions. The double network structure of the hydrogel provides the hydrogel with excellent self-healing properties (up to 127% recovery of toughness after self-healing) and good mechanical properties with a fracture strain of 3787%. Substances with antimicrobial properties in the hydrogel network inhibited the growth of E. coli and S. aureus. In addition, the hydrogel has good electrical conductivity with a conductivity of 1.41 S/m. This study examined multiple properties of the hydrogel and provides a reference for the application of this material in practical application scenarios. Sodium alginate and carboxymethyl chitosan were used as raw materials, and the dynamic imine bonding network formed by the two was combined with the coordination bonding network formed by acrylic acid and aluminum ions. The dual-network structure of the hydrogel not only gives the hydrogel excellent self-healing properties, but also gives the hydrogel excellent mechanical properties, with a strain at break as high as 3787%. In addition, the hydrogel has the antibacterial property of inhibiting the growth of E. coli and S. aureus and good electrical conductivity.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1197-1209"},"PeriodicalIF":2.3,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222755","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of cross-linking units on the heat resistance and heat insulation properties of polysilsesquioxane-based materials 交联单元对聚硅氧烷基材料耐热性和隔热性能的影响
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-08-29 DOI: 10.1038/s41428-024-00953-2
Kosuke Tsutsui, Hiroyuki Koga, Yohei Adachi, Joji Ohshita
{"title":"Effects of cross-linking units on the heat resistance and heat insulation properties of polysilsesquioxane-based materials","authors":"Kosuke Tsutsui, Hiroyuki Koga, Yohei Adachi, Joji Ohshita","doi":"10.1038/s41428-024-00953-2","DOIUrl":"10.1038/s41428-024-00953-2","url":null,"abstract":"Heat insulators are key materials for efficient energy use and reduction of CO2 emissions. Recently, we examined cross-linked polymethylsilsesquioxane (MSQ) for use as the basic structure of heat-resistant insulation materials. In this study, we prepared MSQs with different cross-linking units and examined the effects of their structures on the heat resistance and heat insulation properties. Among those, MSQ linked by diethynylbenzene had sufficiently low thermal diffusivity and moderately high heat resistance. We also showed their structure–thermal property relationships. Although other influencing factors could exist, the rigidity, π‒π interactions, and bulkiness of the cross-linking units were found to predominantly influence the thermal properties. These findings will lead to new molecular designs for polysilsesquioxane (PSQ)-based heat-resistant heat insulators with high performance. Heat insulators are key materials for efficient energy use and reduction of CO2 emissions. Recently, we examined cross-linked polymethylsilsesquioxane (MSQ) for use as the basic structure of heat-resistant insulation materials. In this study, we prepared MSQs with different cross-linking units and examined the effects of their structures on the heat resistance and heat insulation properties. Among those, MSQ linked by diethynylbenzene had sufficiently low thermal diffusivity and moderately high heat resistance.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1231-1235"},"PeriodicalIF":2.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00953-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222756","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular design of reactive polycaprolactone that can be induced into shape-memory materials promotes further functionalization 可诱导形成形状记忆材料的活性聚己内酯的分子设计可促进进一步功能化
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-08-29 DOI: 10.1038/s41428-024-00948-z
Takumi Yoshida, Toru Hoshi, Takao Aoyagi
{"title":"Molecular design of reactive polycaprolactone that can be induced into shape-memory materials promotes further functionalization","authors":"Takumi Yoshida, Toru Hoshi, Takao Aoyagi","doi":"10.1038/s41428-024-00948-z","DOIUrl":"10.1038/s41428-024-00948-z","url":null,"abstract":"In this study, polymers with different copolymerization composition ratios of α-chloro-ε-caprolactone (α-ClCL) and ε-caprolactone (ε-CL) were prepared using α-ClCL, which can polymerize on its own. The copolymers were prepared by using trimethylolpropane as the initiator, and acryloyl groups were added to the polymer ends to form macromonomers capable of cross-linking reactions. The functionalized macromonomers were confirmed to possess shape-memory properties when cross-flinked in film form by heat. The composition of the functional groups in the macromonomer could be adjusted by changing the ratio of α-ClCL to ε-CL used in the copolymerization. In addition, the chloro group introduced by α-ClCL was converted into an azide group. Both the cross-linked film with chloro groups and the film converted to azide groups prepared in this study exhibited shape-memory according to the softening point of the film. Through fluorescence microscopy, it was confirmed that the converted azide groups were modified with alkylated rhodamine B based on the click reaction. Furthermore, azide-assisted films are expected to add various functions through click reactions in the future. In this study, branched polymers with different copolymerization composition ratios of α-chloro-ε-caprolactone (α-ClCL) and ε-caprolactone (ε-CL) were prepared using α-ClCL and trimethylolpropane as the initiator. Furthermore, acryloyl groups were introduced at each chain ends of branched polymer to form macromonomers capable of cross-linking reactions. Films obtained by photo-crosslinking macromonomers with chloro groups showed shape-memory properties. In addition, the chloro group introduced by α-ClCL was converted into an azide group. This film is expected to be applied to various functional surfaces through the click reaction in the future.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1177-1186"},"PeriodicalIF":2.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222757","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Kinetics and thermodynamics analysis of the polybenzimidazole adsorption onto carbon materials using adsorption isotherm measurements 利用吸附等温线测量法对碳材料上的聚苯并咪唑吸附进行动力学和热力学分析
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-08-29 DOI: 10.1038/s41428-024-00950-5
A. B. M. Nazmul Islam, Nana Kayo, Yuki Motoishi, Ryo Hamano, Naoki Tanaka, Koichiro Kato, Tsuyohiko Fujigaya
{"title":"Kinetics and thermodynamics analysis of the polybenzimidazole adsorption onto carbon materials using adsorption isotherm measurements","authors":"A. B. M. Nazmul Islam, Nana Kayo, Yuki Motoishi, Ryo Hamano, Naoki Tanaka, Koichiro Kato, Tsuyohiko Fujigaya","doi":"10.1038/s41428-024-00950-5","DOIUrl":"10.1038/s41428-024-00950-5","url":null,"abstract":"The surface modification of carbon materials is an effective method for enhancing the properties of carbon-based functional materials; particularly, the use of a polymer coating is advantageous owing to its intactness and simplicity. Polybenzimidazole (PBI) has been used to modify carbon surfaces, yet its adsorption behavior has not been thoroughly examined. In this study, the adsorption kinetics and thermodynamics of PBI adsorption on various types of carbon black with different surface morphologies and chemical compositions were analyzed via isotherm measurements. To determine the effects of the polymer, its adsorption behavior was compared to that of the PBI monomer (1,3-bis(1H-benzo[d]imidazol-2-yl)benzene (referred to as the PBI-unit)). The surface adsorption of PBI was slower than that of the PBI-unit; however, PBI exhibited a greater adsorption capacity. The PBI adsorption is an entropy-driven process, whereas PBI-unit adsorption is enthalpy-driven. The adsorption of PBI was more thermodynamically favorable on carbon surfaces with higher crystallinity (lower oxygenation) owing to the easier detachment of solvent molecules from the carbon surface, leading to a higher adsorption constant. Physical modification of carbon materials using polymers is a useful technique for altering surface properties. The adsorption phenomenon of polybenzimidazole (PBI) in organic solvents onto different carbon materials with different surface morphologies and chemical compositions was examined to assess the key parameter controlling the adsorption phenomena. Adsorption isotherm measurements revealed that the adsorption of PBI was irreversible and thermodynamically favourable when interaction between solvent-carbon or PBI-solvent is low. PBI did not diffuse into micropore and the coverage ratio of the PBI onto mesopore and macropore surface was around 60%.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1153-1163"},"PeriodicalIF":2.3,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-024-00950-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222759","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ion-conductive properties and lithium battery performance of composite polymer electrolytes filled with lignin derivatives 填充木质素衍生物的复合聚合物电解质的离子导电特性和锂电池性能
IF 2.3 4区 化学
Polymer Journal Pub Date : 2024-08-28 DOI: 10.1038/s41428-024-00941-6
Zitong Liu, Takumi Karasawa, Wei Tan, Hikaru Minegishi, Yasuyuki Matsushita, Kazuhiro Shikinaka, Yuichiro Otsuka, Yoichi Tominaga
{"title":"Ion-conductive properties and lithium battery performance of composite polymer electrolytes filled with lignin derivatives","authors":"Zitong Liu, Takumi Karasawa, Wei Tan, Hikaru Minegishi, Yasuyuki Matsushita, Kazuhiro Shikinaka, Yuichiro Otsuka, Yoichi Tominaga","doi":"10.1038/s41428-024-00941-6","DOIUrl":"10.1038/s41428-024-00941-6","url":null,"abstract":"Lignin is the most abundant aromatic material in the Earth’s terrestrial ecosystems. However, very few studies have been conducted on the potential application of lignin derivatives as fillers for electrolytes in lithium batteries to determine cell performance. Herein, a novel electrochemically stable composite polymer electrolyte (CPE) containing a lignin derivative and dilignol was exploited for battery application for the first time. The lignin derivatives improved both the ionic conductivity and mechanical performance of the polymer-based electrolytes. The resulting alterations in the coordination number led to enhanced Li+ mobility and consequently, increased conductivity. Notably, the LiFePO4/Li cell had good stability and recovery capacity, and the Coulombic efficiency was approximately 100%, with a capacity of more than 150 mAh g−1. A novel electrochemically stable composite polymer electrolyte (CPE) containing a lignin derivative and dilignol was exploited for battery application for the first time. The lignin derivatives improved both the ionic conductivity and mechanical performance of the polymer-based electrolytes. Notably, the LiFePO4/Li cell had improved stability and recovery capacity, and the Coulombic efficiency was approximately 100%, with a capacity of more than 150 mAh g−1. The resulting alterations in the coordination number led to enhanced Li+ mobility and consequently, increased conductivity and cell capacity.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"56 12","pages":"1165-1175"},"PeriodicalIF":2.3,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142222760","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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