Cellulose Nanocrystal-Based Gradient Hydrogel Actuators with Controllable Bending Properties.

Stimuli-responsive hydrogel actuators are being increasingly used in microtechnology, but typical bilayer hydrogel actuators have significant drawbacks due to weak adhesive interface between the two layers. In this study, thermoresponsive single-layer hydrogel actuators are produced by generating a gradient distribution of cellulose nanocrystals (CNCs) in a poly(N-isopropylacrylamide) (PNIPAAm) hydrogel network by electrophoresis. Tunable bending properties of the composite hydrogels, such as the thermoresponsive bending speed and angle, are realized by varying the electrophoresis time, applied voltage, and CNC concentration. By varying these conditions, the gradient distribution of the CNCs can be optimized, leading to fast bending and large bending angles of the hydrogels. Bending properties are attributed to the gradient distribution of CNCs causing different deswelling rates across the hydrogel network owing to reinforcing effects. Bending ability is also influenced by differences in the CNC dimensions based on the sources of cellulose, which determine the rigidity of the CNC-rich layer of the polymer composite. It is thus shown that thermoresponsive single-layer gradient hydrogels with tunable bending properties can be realized.

Bio-Inspired Homogeneous Conductive Hydrogel with Flexibility and Adhesiveness for Information Transmission and Sign Language Recognition.

The wearable electronic technique is increasingly becoming an effective approach to overcoming the communication obstacles between signers and non-signers. However, the efficacy of conducting hydrogels currently proposed as flexible sensor devices is hindered by their poor processability and matrix mismatch, which frequently results in adhesion failure at the combined interfaces and deterioration of mechanical and electrochemical performance. Herein, we propose a hydrogel composed of a rigid matrix in which the hydrophobic and aggregated polyaniline was homogeneously embedded, while quaternate-functionalized nucleobase moieties endowed the flexible network with adhesiveness. Accordingly, the resulting hydrogel with chitosan-graft-polyaniline (chi-g-PANI) copolymers exhibited a promising conductivity (4.8 S·m-1) because of the uniformly dispersed polyaniline components and a high strain strength (0.84 MPa) because of the chain entanglement of chitosan after soaking. In addition, the modified adenine molecules not only realized synchronization in improving the stretchability (up to 1303%) and exhibiting a skin-like elastic modulus (≈184 kPa), but also provided a durable interfacial contact with various materials. The hydrogel was further fabricated into a strain-monitoring sensor for information encryption and sign language transmission based on its sensing stability and strain sensitivity of up to 2.77. The developed wearable sign language interpreting system provides an innovative strategy to assist auditory or speech-impaired people in communicating with non-signers using visual-gestural patterns including body movements and facial expressions.

A starch-based, crosslinked blend film with seawater-specific dissolution characteristics.

Existing biodegradable plastics may not be ideal replacements of petroleum-based single-use plastics owing to their slow biodegradation in seawater. To address this issue, a starch-based blend film with different disintegration/dissolution speeds in freshwater and seawater was prepared. Poly(acrylic acid) segments were grafted onto starch; a clear and homogenous film was prepared by blending the grafted starch with poly(vinyl pyrrolidone) (PVP) by solution casting. After drying, the grafted starch was crosslinked with PVP by hydrogen bonds, owing to which the water stability of the film is higher than that of unmodified starch films in fresh water. In seawater, the film dissolves quickly as a result of disruption of the hydrogen bond crosslinks. This technique balances degradability in marine environment and water resistance in everyday environment, provides an alternative route to mitigate marine plastic pollution and could be potentially useful for single-use applications in different fields such as packaging, healthcare, and agriculture.

Donor and Recipient Adipose-Derived Mesenchymal Stem Cell Therapy for Rat Lung Transplantation.

BACKGROUND: Mesenchymal stem cells (MSCs) are beginning to be proven as immunosuppressant in the field of organ transplantation. However, the effects of MSC origin (donor or recipient) on immunosuppression are not clear. Hence, we investigated the effects of recipient and donor adipose-derived MSCs (ADMSCs) on immunosuppression in a rat lung transplantation model. METHODS: Subjects were divided into no treatment, tacrolimus administration, recipient ADMSC administration, donor ADMSC administration, and mixed donor and recipient ADMSC administration groups. ADMSC-administered groups were also treated with tacrolimus. Histologic study, immunofluorescence, immunohistochemistry, enzyme-linked immunosorbent assay, and polymerase chain reaction were used for various analyses. RESULTS: Fluorescently labeled ADMSCs were predominant in the grafted donor lung, but not in the recipient lung, on day 5. On day 7, the pathologic rejection grades of the grafted donor lung were significantly lower in the ADMSC-administered groups (P < .05) and did not differ among these groups. Although serum hepatocyte growth factor and vascular endothelial growth factor levels did not differ among the groups, interleukin 10 level was slightly higher in the ADMSC-administered groups. The numbers of infiltrating regulatory T cells in the grafted lung were significantly higher in the ADMSC-administered groups (P < .05) but did not differ with cell origin. Transcriptional analysis suggested interleukin 6 suppression to be the main overlapping immunosuppressive mechanism, regardless of origin. Therefore, a donor or recipient origin may not influence the immunosuppressive efficacy of ADMSCs in our rat lung transplantation model. CONCLUSIONS: Collectively, the results indicate that allogenic ADMSCs, regardless of their origin, may exert similar immunosuppressive effects in clinical organ transplantation.

Facile Fabrication of Hierarchically Porous Boronic Acid Group-Functionalized Monoliths With Optical Activity for Recognizing Glucose With Different Conformation.

At present, various materials based on helical polymers are nanoparticle or microsphere, which is not ease of use in practical application. Accordingly, facile preparation hierarchically porous monolith based on helical polymer needs to be developed. Herein, hierarchically porous boronic acid group-functionalized monoliths that exhibited optical activity were fabricated with a facile method based on crosslinking and polymerization-induced phase separation (CPIPS). Chiral substituted acetylene and achiral substituted acetylene with a boronic acid group were used as monomers. By regulating the composition of the pre-polymerization solution, the permeability and macropore size of the porous structure could be controlled. The hierarchically porous structure and large surface area were confirmed by scanning electron microscopy and nitrogen gas adsorption/desorption isotherms. In particular, the boronic acid functional group that can interact with a cis-diol group was successfully introduced on the skeleton surface of the monoliths. Further, the main chain of the copolymer that constituted the monoliths exhibited a high cis content and tacticity, and the monoliths showed good optical activity. Thus, the present study established a facile method to synthesize hierarchically porous boronic acid group-functionalized monoliths with optical activity via CPIPS, and the monoliths showed potential in recognition, separation, and adsorption of compound with chirality and cis-diol groups.

Robust Dual-Biomimetic Titanium Dioxide-Cellulose Monolith for Enrichment of Phosphopeptides.

Metal oxide affinity chromatography (MOAC) is considered to be one of the most effective methods for phosphopeptide enrichment. However, most of the materials used in the method are powder; frequent centrifugation is necessitated during the enrichment process, and potential risks of loss of peptides and materials and clogging of the column employed for liquid chromatography-mass spectrometry (LC-MS) arise. Moreover, the reusability of these materials to achieve sustainability was hardly investigated. To overcome these limitations, herein, inorganic titanium dioxide (TiO2) was coated onto the skeletal surface of the organic cellulose monolith (CM) material with a coral-like structure via a sol-gel method. This produced an organic-inorganic hybrid TiO2-CM material, which contained a combination of organic and inorganic substances, making it mimic the mollusk shell in terms of composition. The prepared TiO2-CM material as monolith exhibited excellent mechanical strength and did not break during the enrichment process; thus, the tedious implementation of multiple centrifugation cycles was prevented, thereby streamlining the experimental procedure and avoiding the loss of peptides and materials. Moreover, a large amount of TiO2 was introduced onto the surface of the CM material, and thus, the resultant TiO2-CM material exhibited a large surface area. As a result, the fabricated TiO2-CM material was successfully applied to the enrichment of phosphopeptides obtained from the tryptic digests of a BSA/ß-casein (mass ratio, 500/1) mixture. The results were superior to those achieved for commercial TiO2 beads, confirming that TiO2-CM has excellent selectivity for phosphopeptides and reusability. Furthermore, 9287 unique phosphopeptides derived from the 2661 phosphoproteins were successfully identified from two milligrams of tryptic digests of Hela cell exosomes obtained through five independent replications after enriching using the TiO2-CM material. The results indicated that the material has good application prospects in the analysis of protein phosphorylation. Furthermore, TiO2-CM consists of green and cheap cellulose as the skeleton, and its synthesis process is environment-friendly, simple, and inexpensive.

Design of Injectable Poly(γ-glutamic acid)/Chondroitin Sulfate Hydrogels with Mineralization Ability.

Biocompatible hydrogels are considered promising agents for application in bone tissue engineering. However, the design of reliable hydrogels with satisfactory injectability, mechanical strength, and a rapid biomineralization rate for bone regeneration remains challenging. Herein, injectable hydrogels are fabricated using hydrazide-modified poly(γ-glutamic acid) and oxidized chondroitin sulfate by combining acylhydrazone bonds and ionic bonding of carboxylic acid groups or sulfate groups with calcium ions (Ca2+). The resulting hydrogels display a fast gelation rate and good self-healing ability due to the acylhydrazone bonds. The introduction of Ca2+ at a moderate concentration enhances the mechanical strength of the hydrogels. The self-healing capacity of hydrogels is improved, with a healing efficiency of 87.5%, because the addition of Ca2+ accelerates the healing process of hydrogels. Moreover, the hydrogels can serve as a robust template for biomineralization. The mineralized hydrogels with increasing Ca2+ concentration exhibit rapid formation and high crystallization of apatite after immersion in simulated body fluid. The hydrogels containing the aldehyde groups possess good bioadhesion to the bone and cartilage tissues. With these superior properties, the developed hydrogels demonstrate potential applicability in bone tissue engineering.

Preparation of pH-Responsive Poly(γ-glutamic acid) Hydrogels by Enzymatic Cross-Linking.

pH-responsive hydrogels are important for oral drug release applications, and they are increasingly demanded to reduce the adverse side effects of drug release and improve drug absorption. In this study, a new type of pH-responsive hydrogel comprised of poly(γ-glutamic acid) modified with tyramine (PGA-Tyr) was developed through enzymatic cross-linking in the presence of horseradish peroxidase (HRP) and hydrogen peroxide (H2O2). The gelation rate, stiffness, swelling behavior, and pore size of the resulting hydrogels were tuned by changing the concentrations of HRP and H2O2 or the degree of substitution (DS) of PGA-Tyr. The pH responsiveness of the hydrogels was evaluated by the swelling ratio in solutions with various pH values, and their pH responsiveness exhibited a good reversibility in pH 2.0 and 7.0 solutions. The degradation rate of the hydrogels in simulated intestinal fluid (SIF) was faster than that in simulated gastric fluid (SGF). Moreover, indomethacin (IM), a hydrophobic drug model, was encapsulated in the hydrogels by rapid in situ gelation, and the pH-dependent drug release of IM-loaded hydrogels was achieved in SGF and SIF. Importantly, when IM was entrapped in pluronic F-127 to form drug micelles, the burst release of the IM-micelle-loaded hydrogels with a high DS of PGA-Tyr was remarkably decreased in SGF, and sustained drug release was presented in SIF. Thus, pH-responsive PGA-based hydrogels have tremendous promise for biomedical applications, especially oral drug delivery.

Superhydrophobic PDMS-pCA@CNWF Composite with UV-Resistant and Self-Cleaning Properties for Oil/Water Separation.

Oil separation is crucial for avoiding environmental pollution originating from industrial wastewater and oil spillage; therefore, it is essential to develop techniques for oil separation. Herein, a new membrane with superhydrophilicity was synthesized by a facile, green, and low-cost method. First, cellulose non-woven fabric (CNWF) was modified by poly (catechin) (pCA), which has good antioxidant and antibacterial activities, to make it unaffected by ultraviolet light and to improve the stability of the structure. Then, hydrolyzed polydimethylsiloxane (PDMS) was coated on the pCA@CNWF surface via chemical bonding to make the composite hydrophobic. This durable superhydrophobic fabric can be used to separate various oil/water mixtures by gravity-driven forces with high separation efficiency (over 98.9%). Additionally, the PDMS-pCA@CNWF possesses the advantages of flexibility, high efficiency, and an outstanding self-cleaning performance, and demonstrates significant potential for applications in various environments, even under various harsh conditions, which make it very promising for the treatment of oil pollution in practical applications.

Stimuli-responsive composite hydrogels with three-dimensional stability prepared using oxidized cellulose nanofibers and chitosan.

Stimuli-responsive hydrogels have garnered the attention of the hydrogel industry, as they are able to change their physical and chemical properties based on changing external stimuli such as pH, temperature, ionic strength, electromagnetic fields, and light. However, stimuli-responsive hydrogel applications are hindered due to their inevitable swelling and shrinkage. Bacterial cellulose (BC), a natural hydrogel with tightly packed cellulose nanofibers (CNFs) was oxidized into dialdehyde BC (DABC) and was composited with chitosan (CS), a readily available natural polymer, to develop a mechanically adaptive hydrogel composite under different pH conditions. Composites exhibit pH sensitivity by presenting higher mechanical properties under acidic conditions and lower mechanical properties under basic conditions owing to the protonation of amino groups of the chitosan chains. Osmotic pressure is built up under acidic conditions, increasing the mechanical strength of the composites. The good three-dimensional stability of composites enables them to consistently maintain their volume when exposed to acidic or basic conditions.

Optically Transparent and Toughened Poly(methyl methacrylate) Composite Films with Acylated Cellulose Nanofibers.

In this work, nanocomposites of poly(methyl methacrylate) (PMMA) with cellulose nanofiber (CNF) were prepared by a solution casting technique. CNF was modified by propionic anhydride (PA) to form surface-propionylated CNF (CNFp) to improve its compatibility with the PMMA matrix. CNF, CNFp, and acetylated CNF were compared with respect to their influence as fillers in PMMA composite films by ultraviolet-visible transmittance, haze values, tensile strength testing, and water contact angle measurement. It was demonstrated that 1 wt % of CNFp has good compatibility and uniform dispersion in the PMMA matrix, as demonstrated by the formation of a smooth surface composite film with good transparency, enhanced tensile properties, improved toughness, and lower wettability. Therefore, PMMA/CNFp composite films have great potential for use in several applications such as lightweight transparent materials, window substitutes, and see-through packaging.

Effects of Acid-Anhydride-Modified Cellulose Nanofiber on Poly(Lactic Acid) Composite Films.

In this study, we investigated the effect of the addition of cellulose nanofiber (CNF) fillers on the performance of poly(lactic acid) (PLA). Modification of the hydroxyl group of cellulose to the acyl group by acid anhydrides changed the compatibility of the CNF with PLA. CNF was modified by acetic anhydride, propionic anhydride, and butyric anhydride to form surface-modified acetylated CNF (CNFa), propionylated CNF (CNFp), and butyrylated CNF (CNFb), respectively, to improve the compatibility with the PLA matrix. The effects of the different acid anhydrides were compared based on their rates of reaction in the acylation process. PLA with modified cellulose nanofiber fillers formed smoother surfaces with better transparency, mechanical, and wettability properties compared with the PLA/CNF composite film. The effects of CNFa, CNFp, and CNFb on the PLA matrix were compared, and it was found that CNFp was the best filler for PLA.

Injectable poly(γ-glutamic acid)-based biodegradable hydrogels with tunable gelation rate and mechanical strength.

Polypeptide-based hydrogels have potential applications in polymer therapeutics and regenerative medicine. However, designing reliable polypeptide-based hydrogels with a rapid injection time and controllable stiffness for clinical applications remains a challenge. Herein, a class of injectable poly(γ-glutamic acid) (PGA)-based hydrogels were constructed using furfurylamine and tyramine-modified PGA (PGA-Fa-Tyr) and the crosslinker dimaleimide poly(ethylene glycol) (MAL-PEG-MAL), through a facile strategy combining enzymatic crosslinking and Diels-Alder (DA) reaction. The injectable hydrogels could be quickly gelatinized and the gelation time, ranging from 10 to 95 s, could be controlled by varying the hydrogen peroxide (H2O2) concentration. Compared with hydrogels formed by single enzymatic crosslinking, the compressive stress and strain of the injectable hydrogels were remarkably enhanced because of the occurrence of the subsequent DA reaction in the hydrogels, suggesting the DA network imparted an outstanding toughening effect on the hydrogels. Furthermore, the mechanical strength, swelling ratio, pore size, and degradation behavior of the injectable hydrogels could be easily controlled by changing the molar ratios of H2O2/Tyr or furan/maleimide. More importantly, injectable hydrogels encapsulating bovine serum albumin exhibited sustained release behavior. Thus, the developed hydrogels hold great potential for applications in biomedical fields, such as tissue engineering and cell/drug delivery.

Endothelial cell adhesion and blood response to hemocompatible peptide 1 (HCP-1), REDV, and RGD peptide sequences with free N-terminal amino groups immobilized on a biomedical expanded polytetrafluorethylene surface.

Blood compatibility generally requires two contradictory characteristics: reduced protein/platelet adhesion and excellent endothelium-related cell affinity. To understand the effect of cell adhesion peptides on blood compatibility, the peptides REDV, RGD, and hemocompatible peptide-1 (HCP-1) were immobilized on an expanded polytetrafluorethylene (ePTFE) surface and evaluated in vitro, in situ, and in vivo. Since the terminal amino groups of functional peptides often have an important effect, a cysteine residue was added to the C terminal and used for immobilization to keep the terminal amino groups free. Maleimide groups were added to carboxylic groups of highly hydrophilic and biologically inert (bioinert) polymer chains grafted onto ePTFE and coupled with cysteine residues. In vitro tests revealed that free N-terminal HCP-1 and RGD-immobilized surfaces improved the adhesion and spread of human umbilical vein endothelial cells (HUVECs), while, unexpectedly, a free N-terminal adjacent to REDV suppressed cell affinity. In situ evaluation with a porcine closed-circuit system for 2 h showed that no platelets adhered to the modified ePTFE sutures due to the bioinert graft chain containing phosphorylcholine groups. Simultaneously, leukocyte-related and endothelium-related cells were observed on RGD-immobilized ePTFE sutures because RGD was recognized by broad types of cells. These cells were not observed on the HCP-1- and REDV-immobilized ePTFE sutures, which may be due to insufficient exposure time. HCP-1-modified ePTFE graft implantation in a porcine femorofemoral (FF) bypass model for 10 days showed that the thrombus layer was clearly mitigated by HCP-1 immobilization. This study suggests that the HCP-1-immobilized ePTFE surface has potential for long-term application by mitigating thrombus and supporting endothelial cell adhesion.

Identification of circulating cells interacted with integrin α4ß1 ligand peptides REDV or HGGVRLY.

Recently, artificial blood vessels modified by integrin α4ß1 ligand, such as REDV, showed endothelialization improvement and antithrombotic properties have been reported. Early endothelialization was affected by the type of circulating cells captured by the peptide in the initial transplantation state, however, it is still not clarified. In this study, we identified in vitro circulating cells bound with the peptides arginine-glutamic acid-aspartic acid-valine (REDV) or histidine-glycine-glycine-valine-arginine-leucine-tyrosine (HGGVRLY). The effect of free C- or N-terminal of HGGVRLY on the type of peptide-binding cells was also studied. The rat circulating cells were isolated from blood and incubated with 5(6)-carboxyfluorescein (5/6-FAM, F) labeled F-REDV (C-terminal free), F-HGGVRLY (C-terminal free), or HGGVRLY-F (N-terminal free). Furthermore, peptide-binding cells were identified by co-staining with various antibodies labeled with PE, PerCP/Cy5.5, or APC. N-terminal free HGGVRLY-F was found to bind to more circulating cells than C-terminal free F-REDV and F-HGGVRLY. The ratio of integrin α4ß1 positive cell bound with F-REDV, F-HGGVRLY, or HGGVRLY-F reached over 90 %, demonstrating that HGGVRLY is also a ligand of integrin α4ß1. Among identified cell types, we found that F-REDV mainly bounds with EPC and BMSC, while F-HGGVRLY with BMSC. HGGVRLY-F bounds with EPC and BMSC, exhibiting a higher EPC binding ratio than F-REDV and F-HGGVRLY.

Synthesis of nanocomposite hydrogel based carboxymethyl starch/polyvinyl alcohol/nanosilver for biomedical materials.

Treatment of infections using wound dressing integrated with multiple functions such as antibacterial activity, non-toxicity, and good mechanical properties has attracted much attention. In this study, carboxymethyl starch/polyvinyl alcohol/citric acid (CMS/PVA/CA) hydrogels containing silver nanoparticles (AgNPs) were prepared. The CMS, PVA and CA were used as polymer matrix and bio-based reducing agents for green synthesis of AgNPs. Silver nitrate (AgNO3) concentrations of 50, 100, and 150 mM were used to obtain nanocomposite hydrogels containing different AgNPs concentrations (AgNPs-50, AgNPs-100 and AgNPs-150, respectively). The minimum inhibitory concentration against E. coli and S. aureus was observed in CMS/PVA/CA hydrogels containing AgNPs-50. Uniform dispersion of AgNPs-100 in the hydrogel provided the highest storage modulus at 56.4 kPa. AgNPs-loaded hydrogels showed low toxicity to human fibroblast cells indicating good biocompatibility. Incorporation of AgNPs demonstrated an enhancement in antibacterial properties and overall mechanical properties, which makes these nanocomposite hydrogels attractive as novel wound dressing materials.

Improved exposure of bioactive peptides to the outermost surface of the polylactic acid nanofiber scaffold.

We recently reported a novel method to modify the polylactic acid (PLLA) nanofiber scaffold with IKVAV peptide/oligo (d-lactic acid) (ODLA) heteroconjugates. However, a part of the IKVAV sequence was not exposed to the outermost surface and therefore, cell adhesion was not optimized. In this study, we evaluated two strategies to improve the exposing efficiency of IKVAV. One strategy introduced a hydrophilic diethylene glycol (diEG) segment between IKVAV and ODLA. In the second method, these modified nanofibers were heated to a given temperature and cooled to room temperature in water. The IKVAV peptides at the outermost surface were quantified by the fluorescein isothiocyanate staining method. After being heated above the PLLA glass transition temperature, the exposing efficiency of the IKVAV sequence on the PLLA/ODLA-diEG-IKVAV nanofiber was three times higher than that on the PLLA/ODLA-IKVAV unheated nanofiber. Moreover, nearly 100% of the PC-12 cells seeded onto the PLLA/ODLA-diEG-IKVAV nanofiber and were well distributed, while only 50% of the PC-12 cells seeded onto the PLLA and PLLA/ODLA-IKVAV nanofibers. These strategies markedly enhanced the exposing efficiency of the bioactive peptides; therefore, their use can be applicable to other nanofiber scaffolds.

Superfine Magnetic Resonance Imaging of the Cerebrovasculature Using Self-Assembled Branched Polyethylene Glycol-Gd Contrast Agent.

Magnetic resonance angiography is an attractive method for the visualization of the cerebrovasculature, but small-sized vessels are hard to visualize with the current clinically approved agents. In this study, a polymeric contrast agent for the superfine imaging of the cerebrovasculature is presented. Eight-arm polyethylene glycol with a molecular weight of ≈17 000 Da conjugated with a Gd chelate and fluorescein (F-8-arm PEG-Gd) is used. The relaxivity rate is 9.3 × 10-3 m-1 s-1 , which is threefold higher than that of free Gd chelate. Light scattering analysis reveals that F-8-arm PEG-Gd is formed by self-assembly. When the F-8-arm PEG-Gd is intravenously injected, cerebrovasculature as small as 100 µm in diameter is clearly visualized. However, signals are not enhanced when Gd chelate and Gd chelate-conjugated 8-arm PEG are injected. Furthermore, small vasculature around infarct region in rat stroke model can be visualized. These results suggest that F-8-arm PEG-Gd enhances the MR imaging of cerebrovasculature.

Influence of Molecular Mobility on Contrast Efficiency of Branched Polyethylene Glycol Contrast Agent.

For a water-soluble polyethylene glycol (PEG) magnetic resonance imaging (MRI) contrast agent, it has been demonstrated that the contrast efficiency was increased with increased branched structure of the contrast agent. However, the cause of enhanced contrast efficiency by the branched structure has not been clarified. Hence, we investigate the cause of the contrast agent enhancement by changing the Gd introduction ratio of the eight-arm PEG from 1.97 to 4.07; furthermore, the terminal mobility of the contrast agents with different structures was evaluated using proton nuclear magnetic resonance (1H-NMR) spectroscopy. It was shown that the relaxivity and contrast luminance of the synthesized branched PEG-Gd contrast agents are larger than those of linear PEG-Gd and commercially available contrast agents. Additionally, the change in the Gd introduction ratio did not affect the contrast efficiency. The terminal mobility results measured by NMR show that the linewidth at half height became broader with an increased number of branches, implying that the mobility of branched PEG-Gd is slower than that of linear PEG-Gd. Interestingly, the linewidth at half height of different structures did not change in an organic solvent; this phenomenon appeared specifically in water. It is suggested that the stable branched structure enabled the improvement in the relaxivity and contrast luminance.