Catalysts
·
2023
·Vol. 13
·期 3
·552
·
IF 3.9
Bingxin Guo,Chengfei Zhao,Yingshuang Zhou,Junjie Guo,Zhongzhe Wei,Jing Wang
Alkali metals, as ideal electron donors, can effectively regulate the valence state distribution of the host metals. Nevertheless, no studies have reported the application of alkali metal promoters in the hydrogen evolution reaction (HER). Here, we designed an efficient and wide pH-universal hydrogen evolution catalyst that utilizes alkali metal to control the valence, size, and dispersion of Ru NPs. The experimental results reveal that the alkali metal additives contribute to the dispersion and stabilization of metallic Ru. More importantly, the interaction between Na and Ru regulates the distribution of Ru valence states and helps to form more active components of Ru0. Additionally, NaCl functioned as an in situ template to assist the construction of a porous carbon skeleton promotes mass transfer and exposes more active sites, further promoting the synergistic effect of Ru and Na. As a result, the optimal Ru0.3/C−800 delivers high efficiency for HER with an overpotential as low as 29 mV in 1.0 M KOH and 83 mV in 0.5 M H2SO4under 10 mA cm−2. Particularly, the catalytic performance of Ru0.3/C−800 even outbalanced that of commercial Pt/C in an alkaline medium. This rational construction strategy opens up new avenues for obtaining superior pH-universal electrocatalysts.Keywords:alkali metal;Ru based;hydrogen evolution reaction;wide-range pH;promotional effect
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Catalysts
·
2023
·Vol. 13
·期 3
·490
·
IF 3.9
Wenrui Zhang,Meilu Hao,Yonghui Wang,Pengfei Sun,Dongjuan Zeng,Xinya Wang,Peng Liang
Layered δ-MnO2catalysts were prepared using the one-step redox method in precursor solutions with five different pH values (pH = 7, 9, 11, 13, and 14). The effects of pH on the physical properties and catalytic activity of the catalyst were investigated through XRD, SEM, TEM, BET, XPS, H2-TPR, and HCHO degradation tests at room temperature. The results showed that the layer spacing, manganese vacancy content, Mn4+/Mn3+ratio, and surface-reactive oxygen species content of MnO2increased with the increase in pH value in the alkaline range. When the catalyst was prepared at pH = 13, the above characteristics of the catalyst reached the optimal value which contributed to the high catalytic activity. Combined with the related characterization results, it was proved that changing the pH can affect the degree of oxidation in the catalyst synthesis process, increase the number of active oxygen and the oxygen mobility of the catalyst, and effectively improve the catalytic activity of the manganese dioxide catalyst for HCHO. This work represents a giant step toward the preparation of an effective catalyst for practical applications of HCHO removal at room temperature at a low concentration and high velocity.Keywords:δ-MnO2;pH;formaldehyde;manganese vacancy;surface-reactive oxygen species
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Heping Wang,Jingping Zhang,Ruijuan Shi,Jiayi Yang,Weidong Song,Qiuhong Bai,Yehua Shen
Fluorescent covalent organic frameworks have been increasingly used as chemical sensors due to their inherent outstanding nature. Here we report two cases of β-ketoenamine typed fluorescent COFs, pyrimidine-cored covalent organic framework (TpApy-COF) and purine-cored covalent organic framework (TpApu-COF). The emission intensities of TpApy-COF and TpApu-COF in aqueous dispersion descend gradually with the ascending of pH value in the range of from 1 to 13. The reversible fluorescence transformation along with the pH change indicates the favorable reusabilities of TpApy-COF and TpApu-COF. The successful assembly of fluorescent liquid glue and fluorescent crayon, as well as their fluorescent turn on and turn off sensing of HCl and NH 3 , suggest positive practicability and processability. The formation and disintegration of extra intramolecular H-bonding during protonation and deprotonation play crucial roles in the reversible fluorescence switching.
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COLLOID AND POLYMER SCIENCE
·
2023
·Vol. 301
·期 5
·455-464
·
IF 2.4
Jong Kwanghyok,Ju Benzhi,Kim Ganghyok,Kim Kwangjin
A novel type of temperature-pH dual-responsive amphiphilic hydrogel, PD(hydroxyethyl starch(HES)-propynyl glycidylether(PGE)-2-dimethylamino ethanethiol (DMAET)-triethoxyvinylsilane (TEVS)) was synthesized and characterized. HES, a hydrophilic polysaccharide, underwent etherification of hydroxyl groups in its glucose units with PGE and then click reaction between carbon–carbon triple bonds in PGE and thiol groups in DMAET thereby possessing a hydrophilic-hydrophobic structure to be used for the preparation of PD, a temperature-pH dual-responsive material, with pH-responsive tertiary amine groups. Next, it further became a dual-responsive hydrogel through the formation of its internal network by TEVS. The hydrogel exhibited its maximum hydroswelling ratio of 2000 and a good transference between its shrinking and swelling. Moreover, during the test experiments to use it as a drug carrier for oral delivery, a doxorubicin (DOX) release was ≤ 15% in acidic conditions in the stomach (pH < 2.0) and ≤ 94% in basic conditions in the small intestine, ensuring that it exhibits relatively good protective and release properties of drugs.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2023
·Vol. 21
·期 1
·1-14
·
IF 10.2
Li Mengyue,Yang Geng,Zheng Yue,Lv Jiazhen,Zhou Wanyi,Zhang Hanxi,You Fengming,Wu Chunhui,Yang Hong,Liu Yiyao
Targeted chemo-phototherapy has received widespread attention in cancer treatment for its advantages in reducing the side effects of chemotherapeutics and improving therapeutic effects. However, safe and efficient targeted-delivery of therapeutic agents remains a major obstacle. Herein, we successfully constructed an AS1411-functionalized triangle DNA origami (TOA) to codeliver chemotherapeutic drug (doxorubicin, DOX) and a photosensitizer (indocyanine green, ICG), denoted as TOADI (DOX/ICG-loaded TOA), for targeted synergistic chemo-phototherapy. In vitro studies show that AS1411 as an aptamer of nucleolin efficiently enhances the nanocarrier’s endocytosis more than 3 times by tumor cells highly expressing nucleolin. Subsequently, TOADI controllably releases the DOX into the nucleus through the photothermal effect of ICG triggered by near-infrared (NIR) laser irradiation, and the acidic environment of lysosomes/endosomes facilitates the release. The downregulated Bcl-2 and upregulated Bax, Cyt c, and cleaved caspase-3 indicate that the synergistic chemo-phototherapeutic effect of TOADI induces the apoptosis of 4T1 cells, causing ~ 80% cell death. In 4T1 tumor-bearing mice, TOADI exhibits 2.5-fold targeted accumulation in tumor region than TODI without AS1411, and 4-fold higher than free ICG, demonstrating its excellent tumor targeting ability in vivo. With the synergetic treatment of DOX and ICG, TOADI shows a significant therapeutic effect of ~ 90% inhibition of tumor growth with negligible systemic toxicity. In addition, TOADI presents outstanding superiority in fluorescence and photothermal imaging. Taken together, this multifunctional DNA origami-based nanosystem with the advantages of specific tumor targeting and controllable drug release provides a new strategy for enhanced cancer therapy.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 6
·1-11
·
IF 5.7
Cheng Yuchi,Zhou Huangmei,Xu Jinming,Zhao Yu,Chen Xihang,Antoine Rodolphe,Ding Meng,Zhang Kun,Zhang Sanjun
Abstract A two-photon excited ratiometric fluorescent pH sensor is reported by combining l -cysteine–protected AuNCs (Cys@AuNCs) with fluorescein isothiocyanate (FITC). Cys@AuNCs were synthesized through a one-step self-reduction route and showed pH-responsive photoluminescence at 650 nm. Benefiting from the opposite pH response of Cys@AuNCs and FITC, the fluorescence ratio (F 515 nm /F 650 nm ) of FITC&Cys@AuNCs provided a large dynamic range of 200-fold for pH measurement in the response interval of pH 5.0–8.0. Based on the excellent two-photon absorption coefficient of Cys@AuNCs, the sensor was expected to achieve sensitive quantitation of pH in living cells under two-photon excitation. In addition, colorimetric biosensing based on enzyme-like metal nanoclusters has attracted wide attention due to their low-cost, simplicity, and practicality. It is crucial to develop high catalytic activity nanozyme from the viewpoint of practical application. The synthesized Cys@AuNCs exhibited excellent photoactivated peroxidase-like activity with high substrate affinity and catalytic reaction rate, promising for rapid colorimetric biosensing of field analysis and the control of catalytic reactions by photostimulation. Graphical Abstract
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 29
·2215116
·
IF 19
Hao Xia,Ze Dong,Qi Tang,Rongjian Ding,Yimeng Bai,Ke Zhou,Lihuang Wu,Lili Hao,Yiyan He,Jun Yang,Hongli Mao,Zhongwei Gu
Excessive inflammation, bacterial infection, and blocked angiogenesis make diabetic wound healing challenging. Multifunctional wound dressings have several advantages in diabetic wound healing. In addition, the pH regulation of the microenvironment is shown to be a key factor that promotes skin regeneration through cellular immune regulation. However, few reports have focused on the development of functional dressings with the ability to regulate the pH microenvironment and promote diabetic wound healing. This study presents a novel approach for regulating the pH microenvironment of diabetic wound sites using a glycopeptide-based hydrogel consisting of modified hyaluronic acid and poly(6-aminocaproic acid). This hydrogel forms a network through Schiff base interactions and metal complexation, which suppresses inflammation and accelerates angiogenesis during wound healing. Hydrogels not only have adequate mechanical properties and self-healing ability but can also support tissue adhesion. They can also promote the secretion of inducible cAMP early repressor, which promotes the polarization of macrophages toward the M2 type. The in vivo results confirm that hydrogel promotes diabetic wound repair and skin regeneration by exerting rapid anti-inflammatory effects and promoting angiogenesis. Therefore, this hydrogel system represents an effective strategy for treating diabetic wounds.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 32
·78229-78242
·
IF 5.8
Chen Jiuyan,Zhang Qiang,Zhu Yuwei,Zhang Mengli,Zhu Yutong,Farooq Usman,Lu Taotao,Qi Zhichong,Chen Weifeng
To date, little information is available regarding the impacts of the widespread anionic surfactants on the adsorption behaviors of antibiotics onto typical iron oxides. Herein, we have investigated the effects of two typical surfactants (sodium dodecyl sulfate (SDS) and sodium dodecylbenzene sulfonate (SDBS)) on the adsorption of two widely used antibiotics (i.e., levofloxacin (LEV) and ciprofloxacin (CIP)) onto ferrihydrite. Results of kinetic experiments showed that the adsorption of antibiotics was well fitted by the pseudo-second-order kinetic models, indicating that the adsorption process might be controlled by chemisorption. The affinity of ferrihydrite toward CIP was greater than that toward LEV, which was ascribed to the higher hydrophobicity of CIP than LEV. Both surfactants enhanced antibiotic adsorption owing to SDS or SDBS molecules as bridge agents between ferrihydrite particles and antibiotics. Interestingly, the extent of the enhanced effects of surfactants on antibiotic adsorption declined as the background solution pH increased from 5.0 to 9.0, which was mainly due to the weaker hydrophobic interactions between antibiotics and the adsorbed surfactants on the iron oxide surfaces as well as the greater electrostatic repulsion between the anionic species of antibiotics and the negatively charged ferrihydrite particles at higher pH. Together, these findings emphasize the importance of widespread surfactants for illustrating the interactions between fluoroquinolone antibiotics and iron oxide minerals in the natural environment.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 31
·e54225
·
IF 3
Fengrong Gong,Lihui Jiang,Yanni Gao,Juan Xu,Ting Wang
Ethinylestradiol (EE) is a potent estrogen widely used to treat diseases such as breast cancer, prostate cancer, and menopausal syndrome. The poor aqueous solubility of EE leads to erratic oral absorption, resulting in suboptimal plasma levels. Developing a formulation to enhance the solubility of EE in the gastrointestinal tract would be beneficial to increase the bioavailability of EE. Thereafter, we prepare diethylenetriamine-β-cyclodextrin/ethinylestradiol (DETA-β-CD/EE) complex, aiming to increase the solubility of EE in water, and design and prepare core-shell composite hydrogel capsules with aldocellulose and hydroxyethyl cellulose as the core and sodium alginate as the shell. The stability, swelling, drug release behavior and biocompatibility of the core-shell hydrogel capsules are carefully investigated. And the results show that the prepared hydrogel capsules have the controlled and sustained release ability of soluble DETA-β-CD/EE, can achieve pH-responding to intestinal fluid, and are non-toxic to normal human cells.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 25
·2302007
·
IF 29.4
Zongpeng Wang,Zhiping Lin,Yinglan Wang,Shijie Shen,Qinghua Zhang,Jiacheng Wang,Wenwu Zhong
Nontrivial topological surface states (TSSs), which possess extraordinary carrier mobility and are protected by the bulk symmetry, have emerged as an innovative platform to search for efficient electrocatalysts toward hydrogen evolution reaction (HER). Here, a Sn-based nontrivial metal Ru 3 Sn 7 is prepared using electrical arc melting method. The results indicate that the (001) crystal family of Ru 3 Sn 7 possesses nontrivial TSSs with linear dispersion relation and large nontrivial energy window. Experimental and theoretical results demonstrate that nontrivial TSSs of Ru 3 Sn 7 can significantly boost charge transfer kinetics and optimize adsorption of hydrogen intermediates due to bulk symmetry-protected band structures. As expected, nontrivial Ru 3 Sn 7 exhibits superior HER activity to Ru, Pt/C, and trivial counterparts (e.g., Ru 2 Sn 3 , IrSn 2 , and Rh 3 Sn 2 ) with higher ratios of noble metals. Furthermore, the wide pH-range activity of topologically nontrivial Ru 3 Sn 7 implies the robustness of its TSSs against pH variation during the HER. These findings provide a promising approach to the rational design of topologically nontrivial metals as highly efficient electrocatalysts.
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Materials
·
2022
·Vol. 15
·期 24
·8787
·
IF 3.748
Xuemei Hou,Huijing Zhao,Ke-Qin Zhang,Kai Meng
In recent years, there has been an increase in demand for pH color-changing materials. These materials can visually communicate signals to people by connecting pH changes with color information. Embedding pH indicators into fibers to create flexible color-changing materials is an effective way to develop daily wearable products. For the stability of the indicator and the indirect contact of the indicator with the human body, it is usually necessary to encapsulate it in capsules. In this study, different pH indicators (Thymol Blue-TB, Bromocresol Green-BCG, and Bromocresol Purple-BCP) were mixed into a wide-domain pH color-changing indicator and encapsulated with ethyl cellulose (EC) by the flash nanoprecipitation (FNP) method using a new-type droplet-shaped confined impinging jet mixer. The effects of flow rate, core-to-wall ratio, and mixed solution concentration on the formation of the nanocapsules were investigated. In addition, the morphology, particle size, size distribution, dispersion stability, and encapsulation efficiency were systematically studied. At a core-to-wall ratio of 1:2, a mixed solution with a concentration of 6 mg/mL and a feed flow rate of 40 mL/min produced nanocapsules with an average particle size of 141.83 ± 0.98 nm and a PDI of 0.125 ± 0.01. Furthermore, a zeta potential with a range of −31.83 ± 0.23 mV and an encapsulation efficiency of 75.20 ± 1.72% were observed at 1:2 core-to-wall ratios. It was concluded that the color of the nanocapsules continuously changed from yellow to green and green to blue when the pH range was increased from 3 to 10. The color-changing nanocapsules were then embedded into sodium alginate hydrogel fibers, resulting in the same color-changing trend (pH 3–10) as that obtained for the nanocapsules. This study can be useful for the pH monitoring of various body fluids, such as wound exudate, urine, and sweat.Keywords:pH color-changing;nanocapsules;flash nanoprecipitation;pH indicator
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Yongyan Yang,Gangying Feng,Jingfei Wang,Ruiting Zhang,Shuangling Zhong,Jia Wang,Xuejun Cui
In this study, a supramolecular hydrogel was fabricated with orotic acid (OA) modified chitosan (OACS) and 2,6-diaminopurine (DAP). The obtained OACS-DAP supramolecular hydrogels have dual responsiveness to temperature and pH. Phase transition experiments indicate this is a temperature-dependent thermoreversible supramolecular hydrogel. Rheological experiments proved the formation of the supramolecular hydrogel and its thixotropic properties. FTIR spectra confirmed that hydrogen bonds and π-π interactions are the main driving forces for OACS and DAP to form hydrogels through intermolecular self-assembly. XRD pattern confirmed the amorphous morphology of OACS-DAP hydrogels. The hydrogel has excellent electrical conductivity with a conductivity of 9.48 μ S·cm −1 . And can achieve the precise release of gastrointestinal drugs. OACS-DAP hydrogel is expected to have better applications in the field of gastrointestinal drug release.
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