FUEL
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2023
·
IF 7.4
Chunpu Li,Han Zhang,Yuying Zhao,Aiman Li,Zexing Wu,Zhenyu Xiao,Zhenjiang Li,Fusheng Liu,Ying Deng,Lei Wang
Developing non-precious metal catalysts with high catalytic efficiency remains a challenge in the electrocatalytic hydrogen production field. Herein, a defect-rich double-shell CNHC-O-P microsphere is constructed by urea etching and then a step-by-step phosphating process via Co 3 Ni 7 -MOFs as the precursor. During the urea etching process, the organic ligands in MOFs are substituted by CO 3 2– and OH – anions to form basic carbonate double-shell microsphere. Then, the released CO 2 and H 2 O molecule during the calcination process produce a porous and defective oxide double-shell microsphere. Furthermore, more lattice distortions and defects are formed through O and P exchanging during the gas phosphating process. The unique defect-rich and double-shell structure provides a rich and accessible active site for enhanced HER performance. The optimized CNHC-O-P shows the overpotentials of 197 mV, 253 mV, and 245 mV at 10 mA·cm −2 current density in 1 M KOH, 0.5 M H 2 SO 4 , and 1 M PBS solution, separately. This work provides a new method for designing and synthesizing defect-rich and double-shell nanomaterials for energy storage and conversion application.
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CHINESE JOURNAL OF CHEMISTRY
·
2023
·Vol. 42
·期 5
·491-498
·
IF 5.4
Xiangnan Wang,Hongli Zhang,Jiahe Li,Gang Zou
Comprehensive Summary Monitoring of sweat pH plays important roles in physiological health, nutritional balance, psychological stress, and sports performance. However, the combination of functional MOFs with phosphorescent material to acquire the real-time physiological information, as well as the application of dual mode anti-counterfeiting, has seldom been reported. Herein, we developed multifunctional gel films based on MOFs and phosphorescent dyes which responded to H + ions and the related mechanism was studied in detail. Upon exposure to H + , the composite gel film exhibited decreased fluorescent signal but enhanced room temperature phosphorescence (RTP), which could be utilized for sweat pH sensing through a dual-mode. Moreover, multifunctional gel films exhibited a potential application in information encryption and anti-counterfeiting by designing of stimulus responsive multiple patterns. This research provided a new avenue for portable and non-invasive sweat pH monitoring methods while also offering insights into stimulus-responsive multifunctional materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
·
IF 4.2
Haiqin Tang,Qi Chen,Xiang Ke,Hao Wang,Moyan Li,Jing Xie,Jun Luo,Jianshu Li
The development of wet adhesives with robust and reversible adhesion to diverse substrates remains challenging. In nature, sandcastle worm glue exemplifies the successful synergy of vital adhesive components with hydrophobic elements to achieve efficient wet adhesion. Herein, a strategy taking advantage of the structural advantage of urushiol, a natural catechol derivative, is proposed to facilely prepare pH-responsive reversible wet adhesive hydrogels with a commonly used pH-responsive component, 3-(acrylamidophenyl) boronic acid (AAPBA), and a framework monomer, N-2-hydroxyethyl acrylamide (HEAA). In the resulting hydrogel, the catechol groups of urushiol form bonds with the phenyl boric acid groups from AAPBA, enabling responsive wet adhesion. Simultaneously, the hydrophobic long unsaturated alkyl side chains of urushiol (UH) facilitate hydrogel cross-linking and impart moisture-repelling properties upon adhesion. Consequently, the hydrogel demonstrated reliable and universally applicable pH-responsive reversible adhesion. Furthermore, it exhibits remarkable improvements in mechanical properties, including enhanced compressive strength, tensile strength, and elongation at break. This study may present a promising approach to the development of smart and universal wet adhesive hydrogels.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Yuan Li,Miao-Ying Chen,Bang-An Lu,Hao-Ran Wu,Jia-Nan Zhang
Although the Mn-N-C catalyst has low toxicity and high durability, its intense pH-dependent ORR activity is perplexing and prevents its commercial use in PEMFCs. Herein, we have developed a novel understanding of the role of hydrogen peroxide in the pH-dependent activity and stability of Mn-N-C catalysts. Instead of nitrogen protonation, the strong pH effects of ORR activity are caused by the much faster kinetics of the H 2 O 2 reduction reaction in alkaline medium than in acid, due to the lower dissociation energy of the HO-OH bond in alkaline environment. Regarding durability, the deactivation induced by H 2 O 2 demonstrates a strong pH dependence, primarily due to the differing intensities of reactive oxygen species at different pH values. Correspondingly, isopropanol effectively reduces Fenton reagents and increases the acid resistance of Mn-N-C sites. The present research provides a mechanistic understanding of pH effects and paves the way for the creation of more efficient catalysts.
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Aggregate
·
2023
·Vol. 5
·期 1
·e434
·
IF 18.8
Lianxue Zhang,Jianxiang Huang,Damiano Buratto,Panli Han,Zaixing Yang,Ruhong Zhou
The efficacy of nanoparticle (NP)-based drug delivery technology is hampered by aberrant tumor stromal microenvironments (TSMs) that hinder NP transportation. Therefore, the promotion of NP permeation into deep tumor sites via the regulation of tumor microenvironments is of critical importance. Herein, we propose a potential solution using a dihydralazine (HDZ)-loaded nanoparticle drug delivery system containing a pH-responsive, cyclic RGD peptide-modified prodrug based on doxorubicin (cRGD-Dex-DOX). With a combined experimental and theoretical approach, we find that the designed NP system can recognize the acid tumor environments and precisely release the encapsulated HDZ into tumor tissues. HDZ can notably downregulate the expression levels of hypoxia-inducible factor 1α (HIF1α), α-smooth muscle actin, and fibronectin through the dilation of tumor blood vessels. These changes in the TSMs enhance the enrichment and penetration of NPs and also unexpectedly promote the infiltration of activated T cells into tumors, suggesting that such a system may offer an effective “multifunctional therapy” through both improving the chemotherapeutic effect and enhancing the immune response to tumors. In vivo experiments on 4T1 breast cancer bearing mice indeed validate that this therapy has the most outstanding antitumor effects over all the other tested control regimens, with the lowest side effects as well.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Qing Li,Xinke Yu,Shiqi Zhang,Mengyue Xu,Yunyi Yang,Zhili Wan,Xiaoquan Yang
Supramolecular hydrogels self-assembled from naturally occurring small molecules (e.g., glycyrrhizic acid, GA) are promising materials for controlled bioactive delivery due to their facile fabrication processes, excellent biocompatibility, and versatile stimuli-responsive behaviors. However, most of these natural hydrogels suffer from poor mechanical strength and processability for practical applications. In this work, through adopting a multicomponent gel approach, we developed a novel mechanically robust GA-based hydrogel with an interpenetrating double network (DN) that is composed of a Ca2+-enhanced hydrogen-bond supramolecular GA nanofibril (GN) network and a Ca2+cross-linked natural polysaccharide sodium alginate (ALG) network. Compared to the single GN network (SN) hydrogel, the GN-ALG hybrid hydrogels (GN-ALG-DN) with the hierarchical double-network structure possess excellent mechanical properties and shaping adaptation, encouraging small and large amplitude oscillatory shear (SAOS and LAOS) rheological performances, better thermal stability, higher resistance to large compression deformations, and lower swelling behaviors. Furthermore, the GN-ALG-DN hydrogels exhibit a pH-responsive and sustained release behavior of nutrients (i.e., vitamin B12, VB12), showing a faster VB12 release rate with a higher swelling ratio in an alkaline condition (pH 7.5) than in an acidic condition (pH 2.5). This is ascribed to the fact that the higher dissociation degree of carboxylic groups in GA and ALG molecules in an alkaline environment induces the erosion and looseness of the self-assembled GN network and the ionic-cross-linked ALG network, which can lead to the decomposition of the hybrid hydrogels and thereby increases the release of nutrients. Cytotoxicity tests further demonstrate the excellent biocompatibility of the GN-ALG-DN hydrogels. This study highlights the design of robust shaped and structured supramolecular hydrogels from natural herb small molecules, which can serve as solid, edible, and stimuli-responsive active cargo delivery platforms for food, biomedical, and sustainable applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenxi Wang,Yiming Chen,Chongxin Xiao,Siying Xiao,Chuyi Wang,Qingling Nie,Peipei Xu,Jingbo Chen,Ruiyun You,Guifeng Zhang,Yudong Lu
Flexible wearable sensors can detect analytes continuously, in real time, and non-invasively, and their application in human health monitoring has received great attention. However, traditional sensors suffer from insufficient biocompatibility, wearing discomfort, and low detection sensitivity, so hydrogel is introduced as a sensor patch to improve the contact between skin and sensor, and combined with surface-enhanced Raman spectroscopy (SERS) technology for rapid and sensitive analysis of biomarkers in sweat. Here, a flexible SERS wearable sensor based on a sulfonated cellulose nanocomposite hydrogel (S-CNF-Ag NPs/PAA) was developed. The hydrogel was prepared by photo-crosslinking of sulfonated cellulose silver nanocomposites (S-CNF-Ag NPs) with acrylic acid (AA), which is a quick and easy preparation process. The network structure of hydrogel can retain small molecules and adsorb sweat through hydrophilic groups, which diffuse sweat into the hydrogel and can effectively collect the analyses in sweat. The introduction of cellulose and silver nanoparticles not only provides excellent mechanical and adhesive properties (toughness of ∼3790 kJ/m 3 , interfacial toughness of ∼116.23 J/m 2 ), but also good antimicrobial properties and biocompatibility. The SERS technology enabled the quantitative analysis of metabolites in sweat (the detection limits for urea and uric acid were 63.1 μM and 3.98 μM, respectively) and real-time monitoring of pH. S-CNF-Ag NPs/PAA sensor maintained excellent sensitivity, stability and mechanical properties during the detection process, effectively expanding the application of hydrogels in flexible SERS sensing and human health detection.
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FOOD CHEMISTRY
·
2023
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IF 8.8
Fan Wang,Rongrong Ma,Jingling Zhu,Jinling Zhan,Jun Li,Yaoqi Tian
Steviol glycosides possess Bola-form amphiphilic structure, which can solubilize hydrophobic phytochemicals and exert physical modification to the hydrophilic matrix. However, the effect of steviol glycosides on the starch hydrogel is still unclear. Herein, the physicochemical properties, in vitro digestibility, and release behavior of starch hydrogel in the presence of steviol glycosides were investigated. The results showed that the addition of steviol glycosides promoted the gelatinization and gelation of starch, and endowed the starch hydrogel with softer texture, larger volume, and higher water holding capacity. The hydrophobic curcumin was well integrated into hydrogel by steviol glycosides, providing the gel with improved colour brilliance. The introduction of steviol glycosides hardly affected the digestibility of starch gel, but it promoted the release rate of curcumin. Notably, this release behavior was pH dependent, which tended to target the alkaline intestine. This work provided some theoretical supports for the development of sugar-free starchy foods.
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Journal of Materials Chemistry B
·
2023
·
IF 7
Bin Zhu,Yu Liu,Yanlei Zhao,Xinyu Dou,Linbang Wang,Shuyuan Min,Xiaoguang Liu,Dong Qiu
The ideal skull defect repairing material should have good biocompatibility, mechanical properties, and contribute to osteogenesis. In this study, we designed and fabricated biodegradable, bioactive and mechanically robust porous scaffolds composed completely of biological materials. We used gelatin-chitosan blend as the matrix, sodium phytate instead of toxic glutaraldehyde for cross-linking, and the pH-neutral bioactive glass (PSC) to improve biological activity and mechanical properties. The chitosan-gelatin-30%PSC/sodium phytate composite scaffold avoided the problems of high toxicity in conventional cross-linking agents with glutaraldehyde, the poor mechanical support of pure chitosan or gelatin scaffold, and the mismatch of degradation rate with bone repair, being promising as a new candidate for skull defect repair.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Min Wu,Zhou Xue,Caixia Wang,Tao Wang,Dongcheng Zou,Peng Lu,Xueping Song
Spoilage results in food waste and endangers consumer health, and the smart antibacterial packaging can effectively inhibit bacterial growth and reduce food spoilage . In this study, the smart antibacterial nanocellulose packaging films were developed by adding the pH-stimulated responsive microcapsules into cellulose nanofibril (CNF) film-forming. The microcapsules were synthesized by interfacial polymerization of Pickering emulsion . Carboxylated cellulose nanocrystals as solid particles stabilized the composited oil phase to prepare the oil-in-water Pickering emulsion. The emulsion with the particle concentration of 1.25 wt% and the oil phase mass fraction of 7.5 % processes excellent stability and uniform particle size, was chosen to synthesize microcapsules. The cinnamaldehyde in the film with the addition amount of microcapsules 0.6 g burst released in the first 1 h and then slowly, and the cumulative release at pH 2.0, 4.0, 5.5 and 7.2 was 28.43 μg/cm 2 , 18.84 μg/cm 2 , 16.52 μg/cm 2 and 12.89 μg/cm 2 , respectively. The inhibitory rate of film against both E. coli and L. monocytogenes reached 99 % at pH 4.0. The shelf life of pork packed by the film prolonged to nearly 9 d at room temperature . The developed films have the potential to be used in food packaging.
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MOLECULES
·
2023
·Vol. 28
·期 19
·6769
·
IF 4.6
Song Zhang,Miao Yu,Guoqiang Zhang,Guanmei He,Yunxu Ji,Juan Dong,Huayan Zheng,Lu Qian
Chitin is one of the most common polysaccharides and is abundant in the cell walls of fungi and the shells of insects and aquatic organisms as a skeleton. The mechanism of how chitin responds to pH is essential to the precise control of brewing and the design of smart chitin materials. However, this molecular mechanism remains a mystery. Results from single-molecule studies, including single-molecule force spectroscopy (SMFS), AFM imaging, and molecular dynamic (MD) simulations, have shown that the mechanical and conformational behaviors of chitin molecules show surprising pH responsiveness. This can be compared with how, in natural aqueous solutions, chitin tends to form a more relaxed spreading conformation and show considerable elasticity under low stretching forces in acidic conditions. However, its molecular chain collapses into a rigid globule in alkaline solutions. The results show that the chain state of chitin can be regulated by the proportions of inter- and intramolecular H-bonds, which are determined via the number of water bridges on the chain under different pH values. This basic study may be helpful for understanding the cellular activities of fungi under pH stress and the design of chitin-based drug carriers.Keywords:chitin;single-molecule force spectroscopy;molecular dynamic simulations;non-covalent interactions;elasticity
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Biomaterials Science
·
2023
·
IF 6.6
Muse Ji,Hongbing Liu,Hanxun Wang,Xinxin Liang,Mingli Wei,Dongmei Shi,Jingxin Gou,Tian Yin,Haibing He,Xing Tang,Yu Zhang
Chemodynamic therapy (CDT) is an emerging oncological treatment that can kill tumor cells by generating lethal hydroxyl radical (•OH) via Fenton or Fenton-like reaction inside tumors. However, the overexpression of glutathione (GSH) and low reaction efficiency in the tumor microenvironment (TME) limited the therapeutic efficacy of CDTs. Herein, CDT agents (Cu2+) and chemotherapeutic agent (Axitinib, AXB) were employed to fabricate a novel pH-activatable metal ion-drug coordinated nanoparticles (Cu-AXB NPs) for enhancing the treatment of tumors. The obtained nanoparticles exhibited ultrahigh drug loading capacity of 87.55% and had an average size of 180 nm. Moreover, the characteristics of excellent plasma stability and pH-responsive drug release contribute to the long circulation in the blood and targeted therapy at the weakly acidic tumor site. The released AXB could play a chemotherapeutic role in killing tumor cells and Cu2+ ion could be reduced to Cu+ by GSH, further generating toxic •OH with hydrogen peroxide (H2O2) for CDT through Fenton-like reaction. Cu-AXB NPs could also efficiently break copper metabolic balances and increase the intracellular Cu content, thus amplifying CDT. In vitro research results of cytotoxicity and apoptosis confirmed the optimal tumor cell killing efficacy of the Cu-AXB NPs, which was attributed to the synergistic effect of CDT with chemotherapy. What is more, Cu-AXB NPs exhibited good tumor targeting and potent tumor inhibition effect (77.53% inhibition), while exhibiting good biocompatibility in tumor bearing mice. In conclusion, this work provided a promising strategy for safe and efficient cancer therapy through the combination of CDT with chemotherapy.
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