ACS Nano
·
2025
·
IF 16
Wei Liu,Anyang Wang,Jihan Zhang,Shixiang Yu,Maolin Wang,Shuheng Tian,Haoyi Tang,Ziwen Zhao,Xiao Ren,Yuzheng Guo,Ding Ma
Constructing subnanometric electrocatalysts is an efficient method to synergistically accelerate H2O dissociation and H+ reduction for pH-universal hydrogen evolution reaction (HER) for industrial water electrolysis to produce green hydrogen. Here, we construct a subnanometric Pt/α-MoC catalyst, where the α-MoC component can dissociate water effectively, with the rapid proton release kinetics of Pt species on Pt/α-MoC to obtain a good HER performance at high current densities in all-pH electrolytes. Quasi-in situ X-ray photoelectron spectroscopy analyses and density functional theory calculations confirm the highly efficient water dissociation capability of α-MoC and the thermodynamically favorable desorption process of hydrolytically dissociated protons on Pt sites at the high current density. Consequently, Pt/α-MoC requires only a low overpotential of 125 mV to achieve a current density of 1000 mA cm–2. Moreover, a Pt/α-MoC-based proton exchange membrane water electrolysis device exhibits a low cell voltage (1.65 V) and promising stability over 300 h with no performance degradation at an industrial-level current density of 1 A cm–2. Notably, even at a current of 100 A, the cell voltage remains low at 2.15 V, demonstrating Pt/α-MoC’s promising potential as a scalable alternative for industrial hydrogen production. These findings elucidate the synergistic mechanism of α-MoC and atomically dispersed Pt in promoting efficient HER, offering valuable guidance for the design of electrocatalysts in high current density hydrogen.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 21
·9549-9558
·
IF 2.7
Ting-Ting Li,Mengdan Jia,Shuxia Li,Ying Zhang,Xiaomeng Wang,Sheng Chu,Bing-Chiuan Shiu,Ching-Wen Lou,Jia-Horng Lin
Oil spills and industrial wastewater discharge have inflicted severe damage upon the ecological environment and human health. Therefore, the development of an environmentally friendly and pollution-free membrane material for oil–water separation is imperative. This study presents the development of a novel oil–water separation material (PP–PPy–pHR) that is environmentally benign and capable of switching between wetting properties. The material was synthesised by dopamine modification, treatment with a pH-responsive polymer and the use of a high-efficiency photothermal layer composed of self-assembled polypyrrole (PPy), and it not only separates incompatible oil–water mixtures but also efficiently separates oil–water emulsions under different pH conditions. Due to the good photothermal effect of PPy, the evaporation rate of PP–PPy–pHR composite membrane loaded with PPy was 3.95 times higher than that of pure water for oily wastewater. In addition, the PPy–pHR composite membrane exhibited excellent durability and high stability in extremely acidic and alkaline solutions, showing remarkable potential for oil–water separation applications.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shiqiang Liu,Bin Wang,Shihang Jin,Lin Zhang,Zhizhou Yang,Yue Wu,Sheng Gao
Silicone resins, known for their exceptional properties across various industries, are traditionally nonreprocessable due to their permanent cross-linked networks. Herein, we propose a method to turn a disadvantage into an advantage by converting silanol (Si–OH) groups─adverse factors for thermal stability─into dynamic Si–O–Ph bonds, thereby endowing silicone resin with reprocessability. Polysiloxane oligomers with benzoxazine side groups (PBTS) were formed via hydrolysis–condensation reactions between monofunctional benzoxazine-containing siloxane (P-mdes) monomers and triethoxymethylsilane (MTES). The curing behaviors of PBTS are analyzed using DSC and FTIR, confirming the formation of silicone resin-based covalent adaptive networks (CANs) through the introduction of dynamic Si–O–Ph bonds. The resulting silicone resin-based CANs exhibit reprocessability and significantly improved mechanical and thermal properties. The tensile strength of the original silicone resin-based CANs reaches 23.34 MPa, and even after five cycles of reprocessing, the strength remains at 22.98 MPa, demonstrating excellent mechanical retention. The Tg and Td5 of the silicone resin-based CANs reach up to 132 °C, 424 °C, and 425 °C in nitrogen or air atmospheres, respectively. Notably, the reprocessed samples maintain excellent heat resistance and thermal stability even after five reprocessing cycles, with Tg and Td5 values around 130 and 380 °C.
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TALANTA
·
2024
·
IF 5.6
Hangqian Li,Shu Wang,Shulu Zheng,Tengyue Fang,Huilin Shu,Yi Xu,Xianghui Guo,Eric P. Achterberg,Liyang Zhan,Jian Ma
The development of field-deployable methods and instruments for the measurement of pH and other carbonate parameters is important for the assessment of the marine carbon cycle , ocean acidification and marine carbon dioxide removal techniques. In this study, a high-precision fully automated integrated syringe-pump-based environmental-water analyzer for pH ( i SEA-pH) was developed. The pH is determined spectrophotometrically using purified indicator dye with a high precision (better than ±0.001) and high frequency (3.5 min/sample). For the short-term analysis, the measurement frequency was 18 h −1 , which revealed pH = 7.8148 ± 0.0005 (n = 104) for aged surface seawater (S = 35) from the western Pacific. For long-term analysis, the measurement frequency was 2 h −1 for 4 days, and the results showed that pH = 7.8148 ± 0.0010 (n = 200). Three commonly used pH indicators (meta-cresol purple, thymol blue and phenol red) were purified with improved flash chromatography procedures. The autonomous i SEA-pH can automatically correct for the influence of temperature, salinity and other factors on pH measurements to achieve rapid and accurate on-site measurements, which meet the “climate” goal of the Global Ocean Acidification Observing Network (uncertainty is ±0.003). Three identical i SEA-pH systems were developed and successfully applied in mesocosm experiments and several coastal and open ocean cruises with excellent in field performance.
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CELLULOSE
·
2025
·
IF 4.8
Li Xuanjun,Su Xiaojing,Deng Pingping,Chen Shengye,Chen Zhuohan,Li Kunquan,Wu Wenjian
In recent years, intelligent response membrane materials have aroused considerable interest in controllable oil–water separation. However, challenges such as unstable response repeatability and easy bacterial contamination continue to hinder their effective use. Herein, a superhydrophobic fabric with pH responsiveness and antibacterial property were synthesized by combing (3-mercaptopropyl)trimethoxysilane with AgNPs and pH-responsive polymer on a fabric substrate. The fabric persisted superhydrophobicity with a WCA of 156° under natural conditions, while underwent a controlled transition of surface wettability in acidic environments. Heavy oil–water mixtures and light oil–water mixtures achieved controllable separation both before and after pH response. The fabric exhibited outstanding oil–water separation capability, achieving a separation efficiency of 98.0% and a separation flux of up to 11,025.0 L·m −2 ·h −1 . The pH response and oil–water separation demonstrated excellent repeatability. Specially, the pH responsiveness was maintained for up to 10 cycles, and the oil–water separation remained repeatable for up to 15 cycles. Even when tested under various environmental conditions, the superhydrophobicity was retained. Additionally, the fabric possessed remarkable antibacterial property with an efficiency reaching 90.4%. The preparation of the superhydrophobic fabric serves as a valuable reference for developing multifunctional and stable intelligent materials for oil–water separation. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xinhe Liu,Xin Wang,Dan Zang,Yi Chang,Wei Su,Guangyang Li,Jie Zhang,Pengfei Yang,Xiaoming Ma,Yuming Guo
Premature drug release in chemotherapy and hypoxic conditions in photodynamic therapy (PDT) are perplexing problems in tumor treatment. Thus, it is of great significance to develop the novel therapeutic system with controllable drug release and effective oxygen generation. Herein, a pH-responsive oxygen self-sufficient smart nanoplatform (named DHCCC), integrating hollow mesoporous silica nanoparticles (HMSNs), chitosan (CS), doxorubicin hydrochloride (DOX), chlorin e6 (Ce6) and catalase (CAT), is fabricated to enhance the tumor therapeutic efficacy efficiently through avoiding premature drug release and mitigating hypoxia of tumor microenvironment (TME). The drug DOX can be efficiently loaded into the HMSNs with large cavity and be controllable released because of the pH responsiveness of CS to the weak acidic TME, thereby elevating the chemotherapy efficacy. Meanwhile, CAT can catalyze the decomposition of endogenous hydrogen peroxide in situ generating oxygen to alleviate the hypoxia and enhance the PDT efficiency considerably. In vitro and in vivo results demonstrate that the combined chemo-photodynamic therapy based on the DHCCC nanoplatform exerts more effective antitumor efficacy than chemotherapy or PDT alone. The current study provides a promising inspiration to construct the pH-responsive oxygen self-sufficient smart nanomedicine with potentials to prevent premature drug leakage and overcome hypoxia for efficient tumor therapy.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Xinyu Jiang,Fengtong Ju,Zhe Wu,Qiuyu Jing,Wenjing Lv,Yongchao Lai,Xiaomei Li
As a molecular-specific and highly sensitive technology, surface-enhanced Raman spectroscopy (SERS) is well-suited to meet the analytical demands of a multidisciplinary range of fields. Nevertheless, the fabrication of SERS substrates that are inexpensive, reproducible, and controllable represents a significant challenge. In this study, a straightforward, reproducible, and controllable strategy was proposed for the fabrication of high-sensitivity SERS substrates based on self-limiting surface reactions. The preparation of the self-confined nanogaps (sCN-Ag) substrate was achieved through the dealloying process of Cu-Ag alloy wires. In this process, the interior nanogaps were self-confined by AgCl produced in situ, thus facilitating the control of "hot spots" on a nanoscale. The sCN-Ag substrate, which can be readily activated by the removal of AgCl with NH₃·H₂O, exhibited high sensitivity, spatial uniformity, and good thermal stability in pH sensing. This self-limiting strategy, which integrates the advantages of controllability, reproducibility, and mass production, is expected to further promote the development and application of SERS.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Yongshuai Jing,Yameng Zhang,Wenjing Cheng,Mingsong Li,Beibei Hu,Yuguang Zheng,Danshen Zhang,Lanfang Wu
The aim of this study was to prepare a drug carrier that could deliver oral insulin to the intestine. A hydrogel beads composed of sodium carboxymethyl cellulose (CMC), Zingiber offtcinale polysaccharide (ZOP) and chitosan (CS) were prepared by ionic gel method as insulin carrier. Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), Scanning electron microscopy (SEM) and thermogravimetric (TGA) showed that the hydrogel was formed by metal ion coordination between ZOP and CMC and Fe 3+ , and CS was coated on the surface of the hydrogel ball in the form of non covalent bond. The results showed that the swelling process of hydrogel spheres has significant pH sensitivity. In addition, the hydrogel beads successfully coated insulin, and the drug loading rate (DL) of (ZOP/CMC-Fe 3+ )@CS could reach 69.43 ± 7.32 mg/g, and the entrapment efficiency (EE) could reach 66.94 ± 7.43 %. In vitro release experiments, the release rate of (CMC/ZOP-Fe 3+ )@CS in simulated gastric fluid (SGF) for 2 h was <20 %, and the cumulative release rate of insulin after 9 h in simulated intestinal fluid (SIF) reached over 90 %. The results showed that the hydrogel beads prepared in this work could be used as a potential carrier for delivering oral insulin.
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LANGMUIR
·
2025
·
IF 3.9
Lijuan Zhu,Chun Feng,Pengao Yu,Yuchi Guo,Zongxue Yu,Xiaofeng Bai,Yuji Li
This article prepared a multifunctional anticorrosion superhydrophobic dual-layer coating with pH-response behavior. By modification of ZIF-8 with low surface energy substance stearic acid, and then loading the corrosion inhibitor 2-amino-5-mercapto-1,3,4-thiadiazole (AMT), a superhydrophobic nanocontainer encapsulating the corrosion inhibitor was prepared. The first layer of the smart coating was applied by using a brushing technique, while the second layer of the superhydrophobic coating was achieved through a spraying method. This composite coating exhibits both pH-responsive behavior and superhydrophobic properties. An electrochemical impedance spectroscopy test was conducted by immersing the composite coating in a 3.5 wt % NaCl solution. The results indicated that the dual-layer superhydrophobic anticorrosion composite coating, designated as ZST/EP-S, maintained the highest low-frequency impedance value after 40 days of immersion, which was 4 orders of magnitude greater than that of pure EP and 1 order of magnitude higher than the smart anticorrosion coating ZST/EP. This demonstrates a significant enhancement in corrosion resistance for the dual-layer superhydrophobic anticorrosion composite coating. Scratch test and UV–vis light experiments verified the successful release of corrosion inhibitor AMT.
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Advanced Energy Materials
·
2018
·Vol. 8
·期 18
·1703489
·
IF 21.875
Fulin Yang,Yuanmeng Zhao,Yeshuang Du,Yongting Chen,Gongzhen Cheng,Shengli Chen,Wei Luo
The search for Pt-free electrocatalysts exceeding pH-universal hydrogen evolution reaction (HER) activities when compared to the state-of-the-art commercial Pt/C is highly desirable for the development of renewable energy conversion systems but still remains a huge challenge. Here a colloidal synthesis of monodisperse Rh 2 P nanoparticles with an average size of 2.8 nm and their superior catalytic activities for pH-universal HER are reported. Significantly, the Rh 2 P catalyst displays remarkable HER performance with overpotentials of 14, 30, and 38 mV to achieve 10 mA cm −2 in 0.5 m H 2 SO 4 , 1.0 m KOH, and 1.0 m phosphate-buffered saline, respectively, exceeding almost all the documented electrocatalysts, including the commercial 20 wt% Pt/C. Density functional theory calculations reveal that the introduction of P into Rh can weaken the H adsorption strength of Rh 2 P to nearly zero, beneficial for boosting HER performance.
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Food Bioscience
·
2025
·
IF 5.9
Yu Li,Jiaxuan Li,Wentao Su,A.M. Abd El-Aty,Yukun Song,Mingqian Tan
Microbial contamination significantly accelerates food spoilage and poses serious risks to public health, thereby necessitating the urgent development of eco-friendly antimicrobial materials to ensure food safety and mitigate health hazards. In this study, a curcumin-zinc complex (Cur-Zn) was synthesized through a hydrothermal method under alkaline conditions, resulting in a metal-polyphenol composite targeted for antibacterial applications. The optimized Cur-Zn (at pH 8, 80 °C) exhibited a spherical nanostructure (30-40 nm) with a substantial Zn 2+ content of 13.56% (m/m) and exceptional aqueous dispersibility. Cur-Zn demonstrated the pH-responsive release kinetics of curcumin, adhering to a first-order model in acidic environments, and exhibited superior antioxidant capacity compared with that of the physically mixed components. Notably, Cur-Zn effectively inhibited the growth of E. coli and S. aureus by disrupting bacterial membranes while concurrently reducing intracellular reactive oxygen species (ROS) levels under oxidative stress at safe dosages. This investigation underscores the dual antioxidative and antibacterial functions of Cur-Zn and its pH-triggered release mechanisms, thereby presenting a green strategy for the design of metal-phenolic antimicrobial agents.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Meili Yang,Liu Yang,Huixin Yu,Xin Zhang,Zhong Zhang,Mao-Sen Yuan
Based on the ESIPT effect, a fluorescence probe HBT-TBD was successfully synthesized, with HBT as the luminescent group and a Si-O bond as the F - recognition site. HBT-TBD is a typical ratiometric fluorescence probe, and can realize the naked-eye monitoring of F - quickly and sensitively. HBT-TBD exhibits different fluorescence colour at various pH, providing a promising approach for developing a new type of acid-base indicator.
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