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Nanoscale · 2024 · IF 5.8

Hydrogen bonding-regulated miscibility of graphene oxide and nonionic water-soluble polymers

Rui Guo,Lidan Wang,Feifan Chen,Kaiwen Li,Yue Gao,Chenwei Shen,Xuan Ye,Senping Liu,Ya Wang,Zeshen Li,Peng Li,Zhen Xu,Yingjun Liu,Chao Gao

The integration of graphene and nonionic water-soluble polymers has generated useful composites with high performances and rich functionalities. These attractive graphene composites are usually synthesized from the aqueous mixture of graphene oxide (GO) precursor and polymers such as synthetic polyvinyl alcohol and natural cellulose. In this widely known preparation method, the miscibility of GO and nonionic water-soluble polymers seems to be intuitive but has been disputed by some observations of gelation and aggregation. Herein, we have re-examined the miscibility of GO and nonionic water-soluble polymers and confirm their general coaggregation caused by hydrogen bonding interaction. Due to the increasing GO concentration, the property of stable miscibility is converted to aggregation by surface adsorption with transient hydrogen bond crosslinking. We have proposed a preheat mixing strategy to prepare a homogenous solution of GO and nonionic water-soluble polymers in any arbitrary ratio. The re-exploited miscibility allows the fabrication of homogeneous composite papers with renewed high performance trend. The hydrogen bonding-regulated miscibility refreshes the understanding on graphene/water-soluble polymeric composites and provides an ecofriendly interaction control method to modulate the assembly of structures and materials.

CAS / MDL: 7631-86-9
研究领域: 材料科学 · 化学
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Materials Chemistry Frontiers · 2021 ·Vol. 6 ·期 1 ·52-62 · IF 6.482

The critical role of inter-component hydrogen bonds in the formation of reversibly interlocked polymer networks

Mei Rui Fu,Yang You,Min Zhi Rong,Ming Qiu Zhang

Recently developed reversibly interlocked polymer networks are made from two pre-formed crosslinked polymers containing reversible covalent bonds via topological rearrangement. Unlike interpenetrating polymer networks, the resultant is rather homogeneous regardless of the miscibility between the parent single networks, and can be repeatedly self-healed and unlocked/re-locked. The present work focuses on revealing the critical role of the hydrogen bonds between the single networks in the construction of the interlocked networks, cooperating with dissociation and re-association of the built-in reversible covalent bonds. Based on the systematic investigations of the small molecules, single networks and interlocked networks, the inter-component hydrogen bonds of the interlocked networks are found to be able to be built-up, which are more stable than the intra-molecular hydrogen bonds of the single networks. They help to pull the chains from different single networks together, preventing the occurrence of phase separation during interlocking and implementing the valuable forced miscibility. Besides, abundant but weak inter-component hydrogen bonds are preferred. The outcomes not only show the hitherto unknown part of the mechanism involved in the formation of the interlocked networks, but also benefit the design of new members of interlocked networks.

研究领域: 聚合物科学 · 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Highly miscible phases in lithium rich manganese-based cathode materials through simple heat treatment control

Zhaojin Li,Jialin Ren,Yifei Wang,Di Zhang,Qiujun Wang,Qujiang Sun,Ranran Li,Fei Yuan,Yufeng Zhu,Bo Wang

Li-rich Mn-based materials composed of C 2/ m and R -3  m mixed phases are considered to be the most promising cathode materials for lithium-ion batteries because of their extremely high specific capacity. However, these materials suffer from serious problems such as metal element leaching, oxygen release, and capacity decay during the cycling process. Realizing high mixing of two phases at the atomic level is an important measure to improve material stability, but there is a lack of methodological guidance. Here, we reported that adopting segmented calcination during the pre-calcination can regulate the forms and concentration of defects, the ratio of C 2/ m phase to R -3  m phase, and the grain size in the materials, thereby achieving effective control over the phase solubility and structural stability in the Li-rich Mn-based materials. With the same pre-calcination time, the sample that pre-sintered for 4 h in the first stage and 1 h in the second stage exhibited the best miscibility, thereby demonstrating excellent electrochemical performance, with a high reversible specific capacity of 230 mAh·g −1 at 0.1C and an incredible capacity retention of 87.7 % after 500 cycles.

研究领域: 材料科学 · 电化学 · 固态化学
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JOURNAL OF PHARMACEUTICAL SCIENCES · 2020 · IF 2.997

Development of Tizanidine Drug-in-Adhesive Patch: Molecular Mechanism of Permeation Enhancer on Regulating Miscibility and Drug Release by Affecting the Status of Ion-Pair in Polymer Matrix

Ting Zhong,Jiuheng Ruan,Chao Liu,Peng Quan,Liang Fang

The objective of this work was to develop a drug-in-adhesive (DIA) patch of TIZ by employing ion-pair and permeation enhancer to increase drug-polymer miscibility and drug release. Special attention was paid on the regulation effect of permeation enhancer on ion-pair status in pressure sensitive adhesives (PSA). Formulation factors including TIZ-fatty acids ion-pair, drug loading and permeation enhancer were investigated by ex-vivo transdermal experiments. Optimized patch was evaluated by pharmacokinetics study. The better polarity similarity and strong hydrogen bonding interactions between TIZ-caproic acid ion-pair (TIZ-C6) and PSA was confirmed by polarity determination, FT-IR, TOPEM of MDSC and theoretical calculation, which determined enhanced miscibility of ion-pair and PSA. The permeation enhancer affected status of ion-pair in PSA by regulating polarity similarity and interaction between ion-pair and PSA, resulting in increased drug-PSA miscibility and drug release, which was characterized by FT-IR, polarity determination, thermal analysis and molecular dynamics simulation. The optimized patch showed high drug-polymer miscibility and drug skin permeability with AUC 0-t of 14641.12 ± 854.45 h ng/mL and C max of 834.55 ± 155.68 ng/mL, which was significantly higher than the control group. In conclusion, DIA patch of TIZ was prepared and it supplied a reference for design of DIA patches with TIZ.

研究领域: 药学 · 药剂学 · 药物递送系统 · 药代动力学 · 材料科学
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