Tandem Integration of Biological and Electrochemical Catalysis for Efficient Polyester Upcycling under Ambient Conditions.

Excessive production of waste polyethylene terephthalate (PET) poses an ecological challenge, which necessitates developing technologies to extract the values from end-of-life PET. Upcycling has proven effective in addressing the low profitability of current recycling strategies, yet existing upcycling technologies operate under energy-intensive conditions. Here we report a cascade strategy to steer the transformation of PET waste into glycolate in an overall yield of 92.6% under ambient conditions. The cascade approach involves setting up a robust hydrolase with 95.6% PET depolymerization into ethylene glycol (EG) monomer within 12 h, followed by an electrochemical process initiated by a CO-tolerant Pd/Ni(OH)2 catalyst to convert the EG intermediate into glycolate with high Faradaic efficiency of 97.5%. Techno-economic analysis and life cycle assessment indicate that, compared with the widely adopted electrochemical technology that heavily relies on alkaline pretreatment for PET depolymerization, our designed enzymatic-electrochemical approach offers a cost-effective and low-carbon pathway to upgrade PET.

Shape Changes and Interaction Mechanism of Escherichia coli Cells Treated with Sericin and Use of a Sericin-Based Hydrogel for Wound Healing.

UNLABELLED: To verify the interaction mechanism between sericin and Escherichia coli, especially the morphological and structural changes in the bacterial cells, the antimicrobial activity of sericin against E. coli as a model for Gram-negative bacteria was investigated. The antibacterial activity of sericin on E. coli and the interaction mechanism were investigated in this study by analyzing the growth, integrity, and morphology of the bacterial cells following treatment with sericin. The changes in morphology and cellular compositions of bacterial cells treated with sericin were observed by an inverted fluorescence microscope, scanning electron microscopy, and transmission electron microscopy. Changes in electrical conductivity, total sugar concentration of the broth for the bacteria, and protein expression of the bacteria were determined to investigate the permeability of the cell membrane. A sericin-based hydrogel was prepared for an in vivo study of wound dressing. The results showed that the antibacterial activity of the hydrogel increased with the increase in the concentration of sericin from 10 g/liter to 40 g/liter. The introduction of sericin induces membrane blebbing of E. coli cells caused by antibiotic action on the cell membrane. The cytoplasm shrinkage phenomenon was accompanied by blurring of the membrane wall boundaries. When E. coli cells were treated with sericin, release of intracellular components quickly increased. The electrical conductivity assay indicated that the charged ions are reduced after exposure to sericin so that the integrity of the cell membrane is weakened and metabolism is blocked. In addition, sodium dodecyl sulfate-polyacrylamide gel electrophoresis demonstrated that sericin hinders the expression of bacterial protein. Sericin may damage the integrity of the bacterial cell membrane, thereby eventually inhibiting the growth and reproduction of E. coli Compared to sterile gauze, the sericin-based hydrogel promoted fibroblast cell proliferation and accelerated the formation of granulation tissues and neovessels. IMPORTANCE: The specific relationship and interaction mechanism between sericin and E. coli cells were investigated and elucidated. The results show that after 12 h of treatment, sericin molecules induce membrane blebbing of E. coli cells, and the bacteria show decreases in liquidity and permeability of biological membrane, resulting in alterations in the conductivity of the culture medium and the integrity of the outer membrane. The subsequent in vivo results demonstrate that the sericin-poly(N-isopropylacrylamide-N,N'-methylene-bis-acrylamide [NIPAm-MBA]) hydrogel accelerated wound healing compared to that with sterile gauze, which is a beneficial result for future applications in clinical medicine and the textile, food, and coating industries.

Programmable melanoma-targeted radio-immunotherapy via fusogenic liposomes functionalized with multivariate-gated aptamer assemblies.

Radio-immunotherapy exploits the immunostimulatory features of ionizing radiation (IR) to enhance antitumor effects and offers emerging opportunities for treating invasive tumor indications such as melanoma. However, insufficient dose deposition and immunosuppressive microenvironment (TME) of solid tumors limit its efficacy. Here we report a programmable sequential therapeutic strategy based on multifunctional fusogenic liposomes (Lip@AUR-ACP-aptPD-L1) to overcome the intrinsic radio-immunotherapeutic resistance of solid tumors. Specifically, fusogenic liposomes are loaded with gold-containing Auranofin (AUR) and inserted with multivariate-gated aptamer assemblies (ACP) and PD-L1 aptamers in the lipid membrane, potentiating melanoma-targeted AUR delivery while transferring ACP onto cell surface through selective membrane fusion. AUR amplifies IR-induced immunogenic death of melanoma cells to release antigens and damage-associated molecular patterns such as adenosine triphosphate (ATP) for triggering adaptive antitumor immunity. AUR-sensitized radiotherapy also upregulates matrix metalloproteinase-2 (MMP-2) expression that combined with released ATP to activate ACP through an "and" logic operation-like process (AND-gate), thus triggering the in-situ release of engineered cytosine-phosphate-guanine aptamer-based immunoadjuvants (eCpG) for stimulating dendritic cell-mediated T cell priming. Furthermore, AUR inhibits tumor-intrinsic vascular endothelial growth factor signaling to suppress infiltration of immunosuppressive cells for fostering an anti-tumorigenic TME. This study offers an approach for solid tumor treatment in the clinics.

Structurally dynamic self-healable hydrogel cooperatively inhibits intestinal inflammation and promotes mucosal repair for enhanced ulcerative colitis treatment.

Hydrogels are a class of biocompatible materials with versatile functions that have been increasing explored for the localized treatment of ulcerative colitis (UC), but various mechanical stimuli may cause premature hydrogel breakage and detachment, impeding their further clinical translation. Here we report a multifunctional mechanically-resilient self-healing hydrogel for effective UC treatment, which is synthesized through the host-guest interaction between dopamine/ß-cyclodextrin-modified hyaluronic acid (HA-CD-DA) and amantadine-modified carboxymethyl chitosan (CMCS-AD). The excessive ß-CD cavities allow the incorporation of dexamethasone (DEX), while the porous hydrogel network potentiates the encapsulation of basic fibroblast growth factor (bFGF) and L-alanyl-l-glutamine (ALG). DA moieties in HA components allow firm adhesion of the hydrogel to the ulcerative lesions after in-situ implantation, while the reversible host-guest interaction between CD and AD could enhance the persistence of hydrogel. The hydrogel demonstrated favorable biocompatibility and could continuously release DEX to induce M1-to-M2 repolarization of mucosal macrophages through inhibiting the toll-like receptor 4 (TLR4)-nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB) axis. Furthermore, the co-delivered bFGF and ALG facilitates the regeneration of ulcerative mucosa and restore its barrier functions to ameliorate UC symptoms. The mechanically resilient hydrogel offers an integrative approach for UC therapy in the clinics.

Mussel-Inspired Caries Management Strategy: Constructing a Tribioactive Tooth Surface with Remineralization, Antibiofilm, and Anti-inflammation Activity.

Dental caries is a common chronic oral disease in humans resulting from tooth demineralization caused by acid production of bacterial plaque, which leads to the destruction of enamel and dentin and oral inflammation. However, it is still a challenge that the function of natural active ingredients in currently available oral care products is not comprehensive, especially the lack of remineralization. Here, inspired by the strong biological adhesion ability of mussels and ancient oral disease plant therapy, a multifunctional strategy is proposed to construct a bioactive tooth surface to treat dental caries. It has been demonstrated that the Turkish gall extract (TGE) can inhibit adhesion of cariogenic bacteria Streptococcus mutans and Actinomyces viscosus and destroy biofilms on the tooth surface. Meanwhile, TGE can reduce the expression of inflammatory factors. Notably, the TGE coating can induce the growth of hydroxyapatite (HAP) crystals in vivo and in vitro, recovering the enamel mechanical properties under normal oral conditions. MD simulations interpreted the adsorption mechanism by which the hydroxyl groups in TGE bind to phosphate group (PO43-) on the tooth surface, attracting calcium ions (Ca2+) as nucleation sites for remineralization. This work underlines the importance of TGE coating in remineralization, antibiofilm, and anti-inflammation activity as a promising strategy for dental caries.

Comparative analysis of mussel foot protein 3B co-expressed with tyrosinases provides a potential adhesive biomaterial.

Mussel foot proteins (Mfps), which help mussels attach to various surfaces, are considered to be promising biomaterials due to their outstanding adhesive properties. However, limited production and lack of post-translational modifications of tyrosine residues into 3,4-dihydroxyphenylalanine (Dopa) in bacterial expression systems have hampered their applications. In the present study, for the first time we established the expression of recombinant Mytilus galloprovincialis foot protein type 3 variant B (fp-3B) in Escherichia coli; and achieved its viable production (~51 mg/L). Additionally, the Dopa content and adhesive properties of fp-3B co-expressed using various types of tyrosinases were compared. Consequently, the co-expression of fp-3B construct together with tyrosinase from Verrucomicrobium spinosum (TyrVs) yielded up to 87 mg/L of modified fp-3B; hydroxylation of tyrosine residues accounted for 57.18% by acid-borate difference spectroscopy. The modified fp-3B also showed significant coating and adhesive ability, and its bulk-scale adhesive strength was 2.9-fold higher than that of unmodified fp-3B. Compared with other type 3 mussel foot proteins, the high-yield expression and extensive hydroxylation level of the recombinant protein indicate that fp-3B co-expressed with TyrVs (3B-Vs) has the potential to be widely used as bioglues.

Different patterns of hypoxia aggravate the toxicity of polystyrene nanoplastics in the mussels Mytilus galloprovincialis: Environmental risk assessment of plastics under global climate change.

Hypoxia, largely triggered by anthropogenic activities and global climate change, exerts widespread and expanding stress on marine ecosystems. As an emerging contaminant, the influence of nanoplastics on marine organisms has also attracted attention in recent years. However, the impact of hypoxia on the risk assessments of nanoplastics is rarely considered. This study investigated the toxicity of PS-NPs (0, 0.5, and 5 mg/L) to the coastal mussels Mytilus galloprovincialis under different patterns of hypoxia (normoxia, constant hypoxia, and fluctuating hypoxia). The results showed that constant hypoxia might reduce the accumulation of PS-NPs in mussels by decreasing the standard metabolic rate. The impairment of PS-NPs on mussel immunity was also exacerbated by constant hypoxia. Fluctuating hypoxia did not affect the accumulation of PS-NPs, but aggravated the oxidative damage caused by PS-NPs. These findings emphasize the importance of environmental factors and their temporal variability in plastic risk assessment.

Natural polyphenol self-assembled pH-responsive nanoparticles loaded into reversible hydrogel to inhibit oral bacterial activity.

Periodontitis is one of the most prevalent chronic inflammatory diseases and Polyphenols isolated from Turkish gall play a major role in the treatment of inflammatory diseases for their antibacterial, anti-inflammatory and antioxidant activities. In this work, Turkish Galls effective constituent (TGEC, T) was prepared into nanoparticles (T-NPs) by principle of oxidative self-polymerization. The pH-sensitive T-NPs was encapsulated into thermosensitive type in-situ hydrogel, and 42.29 ± 1.12% of effective constituent from T-NPs were continuously released within 96 h under the periodontitis environment. In addition, the weakly alkaline oral micro-environment of patients with periodontitis is more conducive to the sustained release of effective constituent, which is 10.83% more than that of healthy periodontal environment. The bacteriostatic test showed that T-NPs had stronger antibacterial activity on oral pathogens than that of TGEC. Compared with TGEC, the minimum inhibitory concentration (MIC) of T-NPs against P. gingivalis and A. viscosus was reduced by 50% and 25%, respectively. Interestingly, T-NPs induced bacteria lysis by promoting the excessive production of ROS without periodontal tissue damage caused by excessive oxidation reaction. In conclusion, a simple method of preparing microspheres with natural polyphenols was developed, which provides beneficial reference for one-step prepared drug carriers from effective components of natural product, likewise the method offers a green and effective solution to synthesis a new adjuvant therapy drugs for treatment of gingivitis associated with periodontal pockets.

Biodegradation and up-cycling of polyurethanes: Progress, challenges, and prospects.

Polyurethanes (PUR) are ranked globally as the 6th most abundant synthetic polymer material. Most PUR materials are specifically designed to ensure long-term durability and high resistance to environmental factors. As the demand for diverse PUR materials is increasing annually in many industrial sectors, a large amount of PUR waste is also being generated, which requires proper disposal. In contrast to other mass-produced plastics such as PE, PP, and PET, PUR is a family of synthetic polymers, which differ considerably in their physical properties due to different building blocks (for example, polyester- or polyether-polyol) used in the synthesis. Despite its xenobiotic properties, PUR has been found to be susceptible to biodegradation by different microorganisms, albeit at very low rate under environmental and laboratory conditions. Discovery and characterization of highly efficient PUR-degrading microbes and enzymes capable of disassembling PUR polymer chains into oligo- and monomeric compounds is of fundamental importance for a circular plastic economy. In this review, the main methods used for screening PUR-degrading microbes and enzymes are summarized and compared in terms of their catalytic mechanisms. Furthermore, recycling and upcycling strategies of waste PUR polymers, including microbial conversion of PUR monomers into value added products, are presented.

Comparison of clinical and radiological outcomes between modified Gallie graft fusion-wiring technique and posterior cervical screw constructs for Type II odontoid fractures.

The aim of this study was to compare clinical and radiological outcomes between modified Gallie graft fusion-wiring technique and posterior cervical screw constructs for Type II odontoid fractures, and hope to provide references in decision making and surgical planning for both spinal surgeons and surgically treated patients.This is a retrospective study. By retrieving the medical records from January 2005 to July 2015 in our hospital, 53 Type II odontoid fracture patients were reviewed. According to the instrumentation type, patients were divided into 2 groups: Wiring group and Screw group. Three categorized factors were analyzed statistically: patient characteristics: age, body mass index, preoperative neurological status, duration, complicated injuries; surgical variables: surgery time, blood loss, vertebral artery injury, spinal cord or nerve root injury, major systemic complications, wound infection, pain at the bone donor area, instrumentation failure, revision rate; and radiographic parameters: preoperative and final follow-up data of C0-2 curvature, C2-7 curvature, C2-C7 sagittal vertical axis, C7 slope, fracture classification, separation, and displacement of odontoid fracture, fusion rate. An additional comparison of surgical outcomes was done, including patient satisfaction, visual analog scale score for neck pain, neck stiffness, medical expense.There was no statistically significant difference between the 2 groups in patient characteristics of age, sex, body mass index, preoperative neurological status, duration, and complicated injuries. No statistically significant difference was noted in surgical variables of blood loss, vertebral artery injury, spinal cord or nerve root injury, major systemic complications, wound infection, bone harvested zone pain, instrumentation failure, revision rate. The surgery time was shorter in Wiring group than that in Screw group, with a statistically significant difference. We noted no significant difference between the 2 groups when comparing radiographic parameters of preoperative and final follow-up data of C0-2 curvature, C2-C7 sagittal vertical axis, fracture classification, the separation and displacement of odontoid fracture, and fusion rate. Although we noted no significant difference in preoperative C2-7 curvature and C7 slope, the final follow-up data showed that C2-7 curvature and C7 slope were smaller in Wiring group than that in Screw group. We noted no significant difference in visual analog scale score, neck stiffness, and neurological status at final follow-up. The medical expense was less in Wiring group; the patient satisfaction was lower in the Wiring group than that in the Screw group.The modified Gallie graft fusion-wiring technique provided solid fusion and stabilization for patients with Type II odontoid fractures, Gallie graft fusion-wiring resulted in less surgery time, less medical expense, but lower patient satisfaction when compared with the posterior cervical screw constructs.

Nanoclay cross-linked semi-IPN silk sericin/poly(NIPAm/LMSH) nanocomposite hydrogel: An outstanding antibacterial wound dressing.

High antibacterial and skin-like hydrogels have always been the perfect wound dressing for human to protect wound from infection. Here, based on silk sericin, we design a series of nanoclay lithium magnesium silicate hydrate (LMSH) cross-linked semi-IPN sericin/poly(NIPAm/LMSH) (HSP) nanocomposite hydrogels and demonstrate advantages in serving as antibacterial wound dressing in comparison with gauze. Firstly, the effect of mass ratios of sericin/(sericin+NIPAm) upon pore structure, feasibility of mechanics and gas permeability of HSP nanocomposite hydrogels were evaluated. Then, the relationship between nanocomposite hydrogel and histological/antimicrobial properties was systematically analyzed. It was found that, the introduction of sericin increased internal pore size, leading to obvious transition from honeycomb to layered structure. Furthermore, as mass ratio of sericin/(sericin+NIPAm) is 20%, the wound healing area treated with nanocomposite hydrogels at 6th day reached up to 83%, 3 times of gauze, and almost recovered at 13th day. Especially, antibacterial mechanism can be thought to be the results that the macromolecular sericin embedded in the nanocomposite hydrogel adsorbed bacteria by charge interaction and micromolecular sericin dissociating out from nanocomposite hydrogels can be adsorbed onto bacteria.

[Effects of Choukroun's platelet-rich fibrin on human gingival fibroblasts proliferation, migration and type I collagen secretion].

OBJECTIVE: To investigate the effect of platelet-rich fibrin (PRF) on human gingival fibroblasts (HGF) biological behavior such as proliferation, migration and collagen-I expression. METHODS: Human healthy gingival tissues were cultured according to the explant technique to obtain primary cultures. PRF was prepared by means of Choukroun's. HGF were co-cultured with PRF membrane originating from the same donor as the explants, divided into three groups, PRF1 group, PRF2 group and blank control group. Methyl thiazolyl tetrazolium (MTT) assay was used for cytotoxicity and cell proliferation study, and enzyme-linked immunosorbent assay (ELISA) for collagen-I (COL-I) secretion study at the 1st, 3rd, 5th day respectively. Eluates from PRF membrane was prepared, and divided into three groups, PRF1 group, PRF2 group and blank control group. Transwell chamber was utilized to determine the effect of PRF membrane eluate on cell migration. RESULTS: The A values of HGF in culture of the PRF1 (0.615 ± 0.036, 0.686 ± 0.006, 0.693 ± 0.004) and PRF2 groups (0.653 ± 0.023, 0.766 ± 0.034, 0.775 ± 0.053) were significantly higher than those of the control cultures (0.514 ± 0.020, 0.544 ± 0.006, 0.545 ± 0.009) (P < 0.01), but the difference between PRF1 and PRF2 group was not significant (P > 0.05). In each group at different time points, the HGF proliferation effect was significantly enhanced with time (P < 0.01). Cell migration test showed that the migration numbers of HGF in PRF1 and PRF2 groups (85.67 ± 2.94, 85.83 ± 1.47) were significantly higher than those of the control group (54.17 ± 2.48) (P < 0.01), but the difference between the two experimental groups was not significant (P > 0.05). COL-I secretion test exhibited that the A values of COL-I in PRF1 (0.184 ± 0.004, 0.200 ± 0.004, 0.204 ± 0.009) and PRF2 group (0.213 ± 0.008, 0.226 ± 0.005, 0.229 ± 0.006) were significantly higher than the A values of the control group (0.174 ± 0.002, 0.184 ± 0.002, 0.186 ± 0.003) (P < 0.01), but the difference between the two experimental groups was not significant (P > 0.05). In each group, the secretion level of COL-I increased significantly with time (P < 0.01). CONCLUSIONS: PRF could exert a positive effect on HGF biological behaviour and had clinical application potential in the treatment of gingival recession and in the periodontal tissue engineering when combined with seed cell HGF.

Implantable polyimide cable for multichannel high-data-rate neural recording microsystems.

To avoid or minimize postimplantation injury as a result of brain micromotion relative to the skull, a flexible multichannel polyimide (PI) cable was designed and microfabricated for data and power transmission between an intracranial IC recording from a neural probe array and an extracranial IC exchanging power and data wirelessly with an external unit. Surface characteristics, electrical properties, and cytocompatibility of the PI ribbon cable were investigated in this study. Scanning electron microscopic examination and atomic force microscopy analyses showed that the surface of the PI ribbon cable became significantly rougher due to the reactive oxygen ion etching process to open bonding pads. The enhanced surface roughness was also responsible for the increase in wettability and water absorption rate. However, water permeability measurement revealed that the micromachining fabrication process did not meaningfully affect the acceptable water vapor transmission rate of PI. Moreover, electrical properties, such as insertion loss, isolation between channels and data transmission capacity, were assessed for each channel of the PI ribbon cable on the basis of scattering parameter (S-parameter) measurement. Finally, 3-(4, 5-dimethylthiazol-2-yl)-2, 5-diphenyltetrazolium bromide assay and live/dead intracellular staining tests were carried out to evaluate cell behaviors on the PI ribbon cable, indicating that the PI ribbon cable did not have acute cytotoxicity and appeared to be as cytocompatible as blank PI foils.

[Measurement of exhaled nitric oxide in healthy Chinese].

OBJECTIVE: To obtain the normal values of nitric oxide (NO) exhaled through nose and mouth in healthy Chinese adults by measuring exhaled NO and analyzing the influencing factors. METHODS: Eighty healthy Chinese adults were recruited, including 20 males and 60 females. The age ranged from 18 to 44 years old. Chemiluminescence analyzer (NIOX) was used to obtain the values of exhaled NO through nose and mouth. The relativity between NO and gender, age, height, body mass index, time, ambient NO were analyzed with Multiple linear regression and correlation. RESULTS: Exhaled NO values were (17+/-8)x10(-9) and correlated significantly with height. Regression equation: Y (exhaled nitric oxide)=-58.524+0.457X (height, cm), t=-2.985, P<0.01. Transnasal NO values were (819+/-211)x10(-9) and correlated significantly with age and gender. Regression equation: Y (nasal nitric oxide)=760.245+9.417X1(age)-111.222X2(gender), t=5.188, P<0.01. CONCLUSIONS: Exhaled NO normal values were 17x10(-9) and Transnasal NO normal values were 819x10(-9). Exhaled NO correlated positively with height. Transnasal NO correlated positively with age and negatively with gender.