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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

pH/redox-responsive release of interleukin-4 from ZIF-8@diselenide block copolymer to regulate inflammation

Congling Yang,Qianying Guo,Xinchun Wang,Hongmei Chen,Huan Tan,Bo Feng,Jie Weng

Multi-responsive drug-delivery systems have been widely explored to enable specific delivery to target sites. Here, interleukin-4 (IL-4), an anti-inflammatory cytokine, is first encapsulated in situ inside a zeolitic imidazolate framework (ZIF-8) to form IL-4@ZIF-8, which is subsequently coated with a diselenide block copolymer to obtain IL-4@ZIF-8@Se-Se-polymer. This delivery system enables redox-responsive release of IL-4 by the diselenide copolymer and a pH-triggered release by ZIF-8. Moreover, IL-4 release is precisely controlled stepwise by the stimuli response, with the dissociation of the diselenide copolymer, and breakdown of the ZIF-8 structure. The targeted release property of the IL-4@ZIF-8@Se-Se-polymer endows the materials with efficient macrophage immune regulation, as systematically demonstrated in vitro. This study provides an effective example of the delivery and on-demand release of IL-4, and may find promising applications in tissue engineering for the management of inflammation.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Sponge-like porous polyvinyl alcohol/chitosan-based hydrogel with integrated cushioning, pH-indicating and antibacterial functions

Yilin Yu,Ning Kong,Zhaoyang Hou,Libo Men,Pei Yang,Zhengjin Wang

Developing a packaging material with integrated cushioning, intelligent and active functions is highly desired but remains challenging in the food industry. Here we show that a sponge-like porous hydrogel with pH-indicating and antibacterial additives can meet this requirement. We use polyvinyl alcohol and chitosan as the primary polymers to construct a hydrogel with hierarchical structures through a freeze-casting method in combination with salting-out treatment. The synergy of aggregated polymer chains and the sponge-like porous structure makes the hydrogel resilient and efficient in energy absorption. It also enables rapid movement of molecules/particles and fast reaction due to the large specific surface area of the pore structures and the large amount of free water in it, leading to a sensitive pH-indicating function. The hydrogel shows an obvious color variation within a wide pH range in 3 min. The silver nanoparticles are fixed in the dense polymer networks , enabling a lasting release of silver ions . The porous structure makes the silver ion reach the protected item in a short time, achieving an antibacterial effect against S. aureus and E. coli with little cytotoxicity. This work paves the way for fabricating multifunctional hydrogels for diverse advanced packaging systems.

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JOURNAL OF HAZARDOUS MATERIALS · 2025 · IF 11.3

Stability and fate of hollow mesoporous silica nanoparticles in aqueous environment: Effects of pH and electrolyte

Zhihui Duan,Qiao Xue,Yuxing Hao,Lizheng Liu,Xian Liu,Wenxiao Pan,Aiqian Zhang,Jianjie Fu

Hollow mesoporous silica nanoparticles (HMSNs) and their carboxyl-functionalized counterparts (C-HMSNs) are promising materials for environmental applications, but their stability in aquatic environments remains poorly understood. This study investigated the aggregation behavior of HMSNs and C-HMSNs under varying pH and electrolyte conditions. Experimental results showed that HMSNs had critical aggragation concentrations (CCC) of 35 mM in NaCl and 2 mM in CaCl 2 , while C-HMSNs exhibited higher CCCs of 52 mM and 3 mM, respectively, indicating greater stability. High concentrations of NaCl and CaCl 2 promoted rapid aggregation of HMSNs and C-HMSNs, with CaCl 2 being more efficient in promoting aggregation. Both HMSNs and C-HMSNs aggregated extensively in acidic environments, while remaining stable in neutral and alkaline environments. Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and molecular dynamics (MD) simulations revealed weakened electrostatic repulsion and reduced total system energy in high ionic strength solutions supporting irreversible aggregation. Simulated environmental conditions showed that HMSNs and C-HMSNs remained stable in rivers, aggregated slightly in groundwater, and aggregated extensively in seawater. These findings provide critical insights into the environmental fate and potential ecological risks of silica nanoparticles, informing future studies on their transport and bioavailability in natural waters.

CAS / MDL: 1310-73-2
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ACS Nano · 2025 · IF 16

Cellulase- and pH-Stimulating Selenium Nanopesticide Enhances Antifungal Efficacy to Anthracnose: Action Mechanism and Environmental Safety

Jingyuan Wang,Xiaoyan Li,Panpan Chen,Rong Li,Jingwei Hu,Xiangwei Wu,Yi Wang,Hui Li

Nanopesticides (NPs) provide a sustainable approach to reducing the use of chemical pesticides and mitigating their environmental risks in agriculture. In the present study, a pH and cellulase dual-stimulating system with the loaded pesticide penthiopyrad (PEN) was developed by incorporating hydroxypropyl cellulose (HPC) on the surfaces of mesoporous nanoselenium (MSe). In the measurement of antifungal efficacy of PEN against Colletorichum orbiculare Arx, compared to the neutral environment, i.e., pH = 7 without cellulase, the cumulative release of PEN from HPC@PEN@MSe NPs increased 5.7 and 4.8 times of the amount released at pH 3 and 5, respectively; at pH 7, the presence of cellulase solution substantially enhanced PEN release by 6.1 times more than that without cellulase. The HPC@PEN@MSe NPs demonstrated 3.2-fold of antifungal efficacy greater than the commercial 20% PEN suspension concentrate (20% PEN SC). This dual-stimulating NPs can induce oxidative stress responses and cell structural damage in pathogens, demonstrating a broad spectrum of antifungal activity. Mechanistic investigations illustrated that HPC@PEN@MSe NPs specifically promote the accumulation of reactive oxygen species, including hydroxyl radicals (•OH), superoxide radicals (•O2–), and singlet oxygen (1O2) in pathogenic cells by regulating gene expressions relevant to oxidative phosphorylation and lipid metabolism pathways, ultimately leading to eradication of pathogens. In vivo, HPC@PEN@MSe NPs sprayed could be transported in plants and specifically activated at the infected leafy, stem, and root tissues of cucumber plants, with the maximum PEN concentration at 0.93 mg/kg detected in the infected leaves at 12 h. The PEN residual concentration still had 0.09 mg/kg after 14 days, which suggests long-lasting activity. Moreover, the results of detached cucumber leaves and pot experiments indicated that HPC@PEN@MSe NPs significantly increased antioxidant enzyme levels, enhanced resistance to anthracnose, and manifested no apparent effects on plant growth. This eco-friendly plant protection strategy developed in this study exhibits apparent potential in practical applications while maintaining ecological sustainability and providing a potential path to address plant health management in modern agriculture.

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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Unravelling pH-dependent formation and deposition mechanisms of Si–Al complex scale in reverse osmosis systems

Hailan Wang,Rui Wang,Ruobin Dai,Zhiwei Wang

Reverse osmosis (RO) is a leading technology for wastewater/water treatment and resource recovery. The formation of Si–Al complex scale significantly impairs the performance of RO systems. Due to the diverse forms of silica and aluminum species, the scaling process involves both homogeneous and heterogeneous mechanisms, presenting substantial challenges in understanding Si–Al scale formation. Herein, we investigated the scaling mechanism of Si–Al complexes in RO systems under acidic, neutral, and alkaline conditions, focusing on Si–Al interactions in solution and their deposition behavior on membrane surfaces. We found that Si–Al interactions in solution did not directly determine their fouling behavior on RO membranes. In acidic conditions, silicic acid and aluminum species (i.e., Al 3+ ) remained stable in solution but underwent heterogenous polymerization on the membrane surface. The electrostatic shielding and the bridging effects of Al 3+ facilitated the formation of a dense and thick Si–Al complex layer. Under neutral and alkaline conditions, the Si–Al complex primarily underwent homogenous polymerization before depositing on the membrane surface, due to the adsorption of silicic acid by polymeric aluminum hydroxide. The electrostatic repulsion between the Si–Al complex and the membrane resulted in minimal scaling. This work offers comprehensive insights into the pH-dependent scaling behavior of Si–Al complexes in RO processes, providing a theoretical foundation for developing effective scaling control strategies.

CAS / MDL: 68-12-2
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

The electro-Fenton/sulfite process with Fe-Mn bimetallic catalyst for diclofenac degradation at neutral pH

Ge Song,Yang Zheng,Minghua Zhou

The application of bimetallic catalysts in heterogeneous electro-Fenton (Hetero-EF) is limited due to its poor performance over a wide pH range. In this work, the Hetero-EF/sulfite process was constructed with FeMn@C as the catalyst to improve the degradation of pollutants under neutral pH. The removal efficiency of diclofenac (DCF) (97.8%) was significantly higher than that of Hetero-EF (15.0%) at pH 7, in which the degradation rate constant k was increased by 19.75 times. The existence and transformation process of various active species ( • OH, SO 4 •- , O 2 •- , and 1 O 2 ) in the process were verified by capture experiments and electron paramagnetic resonance (EPR) test. The possible DCF degradation pathway was also proposed. The introduction of sulfite could reduce Fe 3+ and Mn 3+ , promote the Fe(II)/Fe(III) and Mn(II)/Mn(III) cycles, strengthen the generation of active species, and thus promote the degradation of pollutants. The removal efficiency was still maintained 76.6% after five cycles. The Hetero-EF/sulfite process is a simple, feasible, and efficient method to degrade pollutants, which has a broad application prospect.

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Gels · 2024 ·Vol. 10 ·期 12 ·840 · IF 5

The Influence of Protein Components on Quinoa Protein–Xanthan Gum Complex Gels at Different pH Levels

Xinxia Zhang,Yafeng Ding,Jiangtao Zhou,Qianqian Xu,Ting Li,Li Wang

The study aimed to prepare complex gels of sonicated quinoa protein (QP) and polysaccharides, comparing the effects of different protein components and pH on gel properties. FTIR analysis demonstrated that the β-structure in protein at pH 7.0 was enhanced by ultrasonic treatment, which could promote the formation of a gel network. Moreover, XG-AG (gel prepared by xanthan gum and albumin) and XG-GG (gel prepared by xanthan gum and globulin) exhibited higher levels of disulfide bonds and free sulfhydryl groups in the gel, requiring more energy to break the intermolecular sulfide bonds during heating. Under the same heating conditions, the rheological properties and gel strength of XG-UQPG (gel prepared by xanthan gum and ultrasonically treated QP) were superior to those of XG-UGG (gel prepared by xanthan gum and ultrasonically treated globulin) and XG-UAG (gel prepared by xanthan gum and ultrasonically treated albumin). Additionally, XG-UGG (pH 7.0) demonstrated the highest water holding capacity (WHC) and oil holding capacity (OHC). This was attributed to the disulfide bonds created in the proteins by the ultrasound treatment, encouraging them to interact to form more uniform holes in gel that can hold more water/oil molecules. Conversely, at pH 4.5, the WHCs of the gels were reduced due to the presence of rougher protein structures. These findings shed light on the impact of protein composition on gel properties and offer insights into enhancing the quality of quinoa protein gel.

CAS / MDL: 69-78-3 7758-02-3
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ACS ES&T Water · 2025 · IF 4.3

The pH Dependence of O3/Mn(II) Synergy for the Reactive Species Evolution and Micropollutant Degradation

Wen-Long Wang,Peng-Hui Liu,Jung-Hyun Son,Hang Su,Min-Yong Lee,Hong-Ying Hu,Qian-Yuan Wu,Uwe Hübner

The combination of ozonation and Mn(II) (O3/Mn(II)) is expected to synergistically eliminate recalcitrant organic micropollutants in water. However, the decay of O3, formation of •OH and reactive manganese species (RMnSs), and synergism in micropollutant degradation have not been comprehensively understood. Herein, the synergism of O3 and Mn(II) was observed to be pH-dependent. Compared to ozonation alone, O3/Mn(II) preferentially formed Mn(V and VI) and slightly increased •OH yield (from 0.22 to 0.30) at acidic pH 4–5, while it preferentially formed Mn(VII) and significantly increased OH yield (from 0.52 to 0.74) at circumneutral pH 6–7. Thereafter, O3/Mn(II) prominently increased RMnS exposure at acidic pH, while it dramatically diminished O3-exposurse to increase •OH exposure at circumneutral pH. As a result, O3/Mn(II) outperformed ozonation alone for the degradation of various O3-resistant micropollutants (3.7–7.9 times faster). For example, the RMnSs (82.7% contribution) and •OH (84.2% contribution) were the dominant contributors to the degradation of the isothiazolinone biocide (5-chloro-2-methyl-4-isothiazolin-3-one) at acidic and circumneutral pH, respectively. Mn(II) can enhance the removal of O3-resistant micropollutants in relatively clean waters (e.g., tap water), but its effectiveness was limited in more contaminated waters (e.g., WWTP effluent). These findings support the practice and pH optimization of the O3/Mn(II) in various water types.

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FOOD HYDROCOLLOIDS · 2025 · IF 12.4

A pH responsive fluorescent/visible light-emitting film for real time visual monitoring of food freshness

Chang Liu,Ning Li,Linjie Luo,Xu Li,Zhiming Liu

A dual-layer pH-responsive fluorescent film was developed using hydroxypropyl methylcellulose (HPMC), zinc alginate (ZA), fluorescein isothiocyanate (FITC), and dragon fruit peel extract (DE) for real-time food freshness monitoring. The outer protective layer served as a hydrophobic barrier to reduce moisture interference, while the inner indicator layer acted as a pH-sensitive interface, integrating FITC's fluorescence and DE's visible color change for dual-mode sensing. The film exhibited good thermal stability, antimicrobial activity, and improved hydrophobicity. Optical responses were evaluated across a wide pH range (2.0–12.0), showing stable visible color under ambient light and enhanced fluorescence under 365 nm UV. Upon exposure to ammonia vapor, fluorescence intensity increased linearly from 0 to 1000 ppm (R 2  = 0.9895; LOD = 6.73 ppm), while visible color changes became evident at 500–5000 ppm, with R/B and R/G ratios exhibiting strong linearity (R 2  = 0.96176 and 0.96747; LODs = 1126 ppm and 958 ppm, respectively). Application trials with pork revealed distinct color changes after 4 days at 25 °C or 2 days at 5 °C. These results confirm the film's effectiveness for dual-mode, non-destructive, and real-time monitoring of pork freshness.

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JOURNAL OF MOLECULAR LIQUIDS · 2025 · IF 5.2

Reversible pH-responsive Pickering emulsions stabilized by amine oxide-functionalized nanoparticles: interfacial regulation and stabilization mechanisms

Haihua Pei,Yuhui Wu,Jianwei Zhao,Jian Zhang,Yang Liu,Zhanlei Ma,Guicai Zhang

This study introduces a novel pH-responsive Pickering emulsion system stabilized by lauramidopropyl amine oxide (LAO)-functionalized SiO₂ nanoparticles, demonstrating reversible stabilization controlled by LAO's protonation state. At pH 7, the protonated cationic LAO electrostatically adsorbs onto nano-SiO₂ surfaces, imparting optimal amphiphilicity (θ = 87.6°). The resulting interfacial stabilization is attributable to three synergistic mechanisms: (1) enhanced electrostatic nanoparticle adhesion, (2) hydrophobic shielding by oriented lauryl chains, and (3) mechanical reinforcement via nanoparticle aggregation at the interface. When the pH is increased to 10, LAO deprotonation induces complete demulsification due to interfacial film disintegration. Zeta potential measurements, interfacial rheology, and confocal laser scanning microscopy (CLSM) have been employed to confirm the system's fully reversible pH response (7 ↔ 10) over multiple cycles, with >80 % efficiency retention even at ultralow LAO concentrations (0.1 mM). The system's exceptional recyclability and rapid pH response, in conjunction with minimal surfactant requirements, establish it as a sustainable platform for applications such as enhanced oil recovery. Furthermore, it serves as a fundamental framework for designing smart, stimulus-responsive materials with tunable stability and reversible properties.

CAS / MDL: 1330-20-7
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Dual-signal assay integrating colorimetric and pH biosensing pathways for simultaneous detection of multiple pathogenic bacteria

Jin Wen,Zhaoyang Fang,Shuyao Chen,Wanyi Xu,Yongjun Liu,Hongwen Wu,Hongliang Tan

The increasing prevalence of multi-pathogen contamination highlights the critical need for advanced diagnostic technologies capable of accurately detecting multiple pathogens simultaneously. In this study, we developed a dual-signal assay that synergistically integrates colorimetric and pH biosensing pathways to detect multiple pathogenic bacteria simultaneously. This assay employs the unique properties of rhodamine B (RhB) and urease to create two distinct and independent signaling transduction pathways: RhB provides a characteristic colorimetric absorbance, while urease catalyzes the hydrolysis of urea, generating a pH-modulating signal. The spatiotemporal separation between RhB absorbance and the pH signal can effectively eliminate crosstalk interference, ensuring exceptional accuracy and reliability. Implemented through a dual-recognition strategy, the assay uses Fe 3 O 4 -functionalized phenylboronic acid nanoparticles to capture a wide range of bacteria. Pathogen-specific probes, featuring immunoglobulin G- and aptamer-conjugated ZIF-90 composites encapsulating either RhB or urease, enable precise bacterial identification. The assay exhibits remarkable sensitivity, with detection limits as low as 6 CFU/mL for Staphylococcus aureus and 8 CFU/mL for Escherichia coli . Moreover, it demonstrates excellent accuracy in actual samples, with recovery rates exceeding 97.75 % and a relative standard deviation below 4.99 %. We believe that this study can offer a new insight into the development of multiplex assays for simultaneous multi-target detection.

CAS / MDL: 81-88-9
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Fabrication of pH-sensitive cellulose colorimetric papers for rapid detection of water content in transformer oil

Kai Xu,Xuefeng Zhang,Ming Zhang,Lanhe Zhang,Zicheng Chen

The combination of highly hydrophilic plant fiber and water molecule sensitive material can effectively detect the water content in transformer oil. In this study, two types of rapid response cellulose colorimetric papers (Rp and Bp) were fabricated through a simple impregnation method, with cellulosic fiber serving as the substrate, cresol red/thymol blue as the color developer, boric acid as the pH regulator, and silica aerosol as the filler. Rp and Bp were tested and analyzed using various characterization methods, and their performance in detecting bound water content in transformer oil was investigated. The results indicate that Rp changes from magenta to light yellow and Bp changes from lavender to light yellow with the increase of water content of transformer oil. The water content detection accuracy of both is 92 % and 95 %, respectively. The rapid color change of them is due to boric acid's acidity triggering molecular structure changes in the color developers. After six cycles of use, Rp and Bp still exhibited excellent color-changing properties. Therefore, colorimetric papers have the attributes of rapidity, high efficiency, low cost, and desired accuracy, providing an alternative approach for evaluating transformer oil's water content and showing promising application potential.

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