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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

pH-driven Zein–peanut protein isolate composite nanoparticles for stabilizing pickering emulsions and enhancing resveratrol delivery

Sufang Chen,Weiwei Cheng,Wenrui Liu,Erna Li,Feng Xiao,Jialiang He,Lili Liu,Suna Han,Baocheng Xu

In this study, zein-peanut isolate protein (PPI) composite nanoparticles were fabricated by pH-driven self-assembly method and their potential applications in Pickering emulsion stabilization and resveratrol encapsulation were systematically explored. The results showed that the particle size, zeta potential, and dispersibility were significantly affected by the Zein:PPI mass ratio. Among them, the composite particles with a mass ratio of Zein:PPI of 1:2 showed the best performance, with an average particle size of approximately 389 nm, a low PDI value (0.32) and a high surface charge (−42 mV), indicating superior colloidal stability. Scanning electron microscopy results showed a porous lamellar structure, and contact angle analysis indicated that the surface wettability of the composite particles increased with increasing PPI ratio. Spectroscopic analyses (UV–vis, fluorescence, circular dichroism and FTIR) revealed significant changes in the protein secondary structure, with a decrease in α-helix and an increase in β-folding, reflecting stronger protein-protein interactions. Molecular docking and molecular dynamics simulations further verified the formation of a stable composite structure between zein and PPI mainly through hydrophobic interactions and hydrogen bonding. The Pickering emulsions stabilized by the composite particles were of the oil-in-water type and exhibited remarkable thermal and long-term storage stability. Meanwhile, they showed good colloidal stability under conditions of a wide pH range and high salt concentration. Rheological tests showed that the emulsions exhibited shear-thinning behavior and predominantly elastic gel properties, reflecting the dense interfacial structure. Furthermore, the composite particles significantly improved the encapsulation efficiency of resveratrol (86.5 %) and enhanced its antioxidant capacity. As a resveratrol-loaded emulsion system, the Pickering emulsion stabilized by Zein-PPI reduced the release rate of free fatty acid (FFA) in in vitro digestion to less than 6 %, and increased the bioaccessibility to more than 40 %. Moreover, the Pickering emulsion stabilized by Zein-PPI was superior to the emulsion stabilized by Zein and PPI in terms of sustained release, anti-ultraviolet stability and simulated gastrointestinal digestion. In summary, zein–PPI composite nanoparticles present a promising platform for the development of stable, lipid-soluble bioactive delivery systems in functional food applications.

CAS / MDL: 3326-32-7 7385-67-3
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Antibacterial starch-cellulose-based films with pH-responsive colorimetric properties for real-time food freshness monitoring

Tianyi Hu,Qun Liu,Zeng Xu,Zhengjiang Zhu,Wuyin Weng,Yucang Zhang

Starch/cellulose-based materials represent one of the most promising classes of biodegradable biomass substrates. However, their susceptibility to microbial contamination and limited function limit their applications in modern intelligent food packaging. In this study, cinnamaldehyde (CA) was employed as an antimicrobial agent, while the food-safe synthetic dyes neutral red (NR) and bromothymol blue (BTB) served as pH-responsive indicators. Using a one-pot strategy, starch granules were simultaneously gelatinized and encapsulated CA, while co-blending with bacterial cellulose nanofibers (CNFs) to yield a uniform film-forming solution. Upon incorporation of NR and BTB into the film solution, the resulting CA/HAS-CNFs-(NR&BTB) film exhibited excellent mechanical performance (tensile strength: 10.20 MPa; elongation at break: 14.76 %) owing to hydrogen bond reorganization between CA/HAS inclusion complexes and CNFs. FTIR and CLSM analyses confirmed the successful encapsulation of CA and uniform dispersion within the matrix. The film demonstrated distinct and reversible color transitions in response to pH variation and effectively tracked shrimp freshness, with a visible change from orange to yellow-green over time during storage. The R, G and B values of the film can be directly obtained through the mobile phone app, and then the GCS value can be calculated to obtain the freshness status of the food. Biodegradation studies under simulated microplastic-contaminated environments revealed that the composite film had favorable environmental compatibility. This work provides a sustainable and intelligent packaging solution with significant potential for real-time food freshness monitoring.

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npj Materials Degradation · 2025 ·Vol. 9 ·期 1 ·1-14 · IF 7.6

pH-responsive intrinsic self-healing coating via in-situ confined solid-liquid transition of hydrogel microdomains

Yang Jie,Shen Ting,Wei Jiahong,Chen Chong,Cao Wenkai,Li Weihua

Inspired by pH variation in corrosion microenvironment and the emerging solid-liquid composite strategies, this study presents an innovative self-healing coating based on pH-responsive confined solid-liquid transition behavior, with anti-corrosion functionality as a proof of concept. The coating integrates poly (vinyl alcohol) (PVA) crosslinked with boronic acid (BA) through an in-situ solvent exchange process, forming borate ester-based, pH-responsive PVA-BA (AB) hydrogel microdomains within a poly (3-(trimethoxysilyl) propyl methacrylate) (PTPM) network. The AB/PTPM coating achieves healing within 30 min, based on gel-sol transitions of the AB hydrogel microdomains triggered by different pH conditions (pH = 7 and 11). The hydrophobic PTPM network prevents AB hydrogel microdomains from water intrusion. This design balances the fluidity and stability, providing a solution to enhance the durability of protective coatings. The AB/PTPM coating was applied as a topcoat over an epoxy (EP) primer, and the formed bilayer AB/PTPM@EP coating exhibits excellent anti-corrosion restoration properties after self-healing.

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MATERIALS & DESIGN · 2025 · IF 7.9

pH-Responsive multifunctional drug-loaded covalent organic framework hydrogel dressing for enhanced bacteria-infected wound healing

Zhaojing Lu,Cheng Sun,Pengyu Hu,Jieyan Xu,Fangying Wu,Jian Yu,Rui Cheng,Liqing Gao,Shasha Feng,Tingting Cui

Pathogen-induced delayed wound healing remains a formidable public health challenge. Traditional smart antibiotic delivery systems that spontaneously generate electrical signals to enhance antibacterial efficacy typically require metal electrodes connected to an external power source, thereby limiting their applicability outside of clinical settings. To circumvent this limitation and eliminate the use of antibiotics and external power sources, we synthesized a linarin-loaded covalent organic framework (LN@COF) via condensation and Schiff base reactions. This LN@COF was integrated into a self-healing and highly adhesive hydrogel through free radical polymerization, developing a pH-triggered intelligent drug release dressing for the promotion of wound healing. The LN@COF hydrogel demonstrates pH-responsive LN release under acidic conditions through protonation, indicating effective drug release in acidic extracellular microenvironments. This pH-triggered sustained release system not only mitigates the burst release issue of conventional drug delivery but also exhibits synergistic antibacterial and angiogenic activities during the repair of infected wounds. In vitro assays demonstrated that LN@COF hydrogel possesses significant antibacterial activity and enhances cell proliferation and migration capabilities. In vivo studies revealed that LN@COF hydrogel not only induced epithelialization, collagen deposition, and angiogenesis processes in promoting of wound healing, but also demonstrating excellent biocompatibility. This study provides a novel approach and significant breakthrough in the design and application of intelligent drug release systems for wound dressings.

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Surfaces and Interfaces · 2025 · IF 6.3

pH-Sensitive halloysite nanocontainers encapsulated by silicate-mediated tannic acid networks for the smart epoxy coatings

Xinnian Meng,Jingqi Chen,Zeyang Liu,Yongming Tang

An important issue regarding halloysite nanotubes as inhibitor containers is the stimuli-responsive performance. A novel approach to constructing pH-sensitive halloysite nanocontainers is developed in this study. The silicate-mediated tannic acid complexes (Si-TA) are deposited on the etched halloysite nanotubes (EHNTs) loading Na 2 MoO 4 , endowing the Si-TA/Mo@EHNTs nanocontainers with the high pH-sensitivity. Both the release rate and ratio of the inhibitor increase with increasing pH. The sensitivity of the nanocontainers to the high pH value arises from the rapid hydrolysis of Si-TA encapsulation layers in the basic media. It is evidenced that gallic acid (GA), generated from the hydrolysis of the Si-TA complexes, can further dimerize into ellagic acid (EA) in the basic media. The smart epoxy coatings with the stimuli-responsive performance are prepared by incorporating the Si-TA/Mo@EHNTs nanocontainer, and exhibit better corrosion resistance compared with the epoxy coatings without the nanocontainers as well as directly incorporated with Na 2 MoO 4 . The elevated pH in the cathodic region of corrosion cell trigger the release of MoO 4 2- ions from the nanocontainers, inhibiting the corrosion of the exposed substrates effectively. Furthermore, the EA-Fe(III) depositions could be formed by the combination of the EA compounds from the damage of the encapsulation layers with the Fe 3+ ions, acting as the barrier on the exposed substrates to improve the corrosion resistance of the coating.

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Materials Today Advances · 2025 · IF 8

A pH-triggered antioxidative stem cell spheroid platform restores paracrine signaling to enhance osteoporotic bone regeneration

Lina Huang,Chao Lin,Hanyi Hua,Zehao Chen,Yong Xu,Kezhen Zhou,Xiaoming Liu,Yifan Li,Jiangming Yu,Xiaojian Ye,Xiaoxiao Li,Shuai Jiang

In osteoporotic bone defects, bone marrow mesenchymal stem cells (BMSCs) play a pivotal role in tissue regeneration by orchestrating the local microenvironment through both differentiation and paracrine signaling. However, persistent pathological stimuli such as oxidative stress significantly impair their functionality, while limited cell survival and homing efficiency at the defect site remain major obstacles hindering therapeutic efficacy. To overcome these issues, we designed a stem cell delivery system using microfluidic techniques, in which microspheres were modified with resveratrol. This system leveraged a sustained-release liposomal formulation of resveratrol to enhance the antioxidant resilience of BMSCs. Simultaneously, the platform created a three-dimensional porous microenvironment using pH-responsive microspheres, which supported the maintenance of paracrine activity and promoted osteogenic differentiation of transplanted cells, thereby accelerating bone regeneration. In vitro experiments demonstrated that this system significantly enhanced mineralized nodule formation, accompanied by marked upregulation of osteogenesis-related genes and proteins including RUNX2, COL-1, and SP7. Furthermore, BMSCs exhibited increased secretion of key paracrine factors such as VEGFA, thereby improving proangiogenic support to endothelial cells. In vivo study, we employed an osteoporotic rat model with femoral bone defects, micro-CT imaging and multimodal histological analyses confirmed that the proposed platform markedly facilitated new bone formation and structural tissue reconstruction. Collectively, this study proposes a synergistic strategy for osteoporotic bone repair, providing a new approach to cell therapy design.

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Chemical Engineering Journal Advances · 2025 · IF 7.1

UV-driven trace Cu(II)/peroxymonosulfate for efficient degradation of phosphonate: Mechanism and broad pH adaptability

Tianhong Wang,Jiahui Xu,Anhong Cai,Jibo Xiao,Peng Wang,Min Zhao,Xianfeng Huang

Organic phosphonates detected frequently in water bodies pose severely environmental risks, and the cleavage of their C-P bonds to converse orthophosphate (PO 4 3- ) serves as a prerequisite step for achieving deep phosphorus elimination. Although the in situ generation of Cu(III) via Cu(II)/oxidant system for selective phosphonates degradation has been studied, the oxidation efficiency is constrained by sluggish Cu(II)/Cu(I) reduction, especially under acidic conditions. In this study, the introduction of UV irradiation accelerated the Cu(I)/Cu(II)/Cu(III) cycle in Cu(II)/peroxymonosulfate (PMS) process, enabling efficient and selective oxidation of 1,1-diphosphonic acid (HEDP, a typical phosphonate) into PO 4 3- across a wide pH range. UV-driven trace Cu(II)/PMS system can convert 90% of HEDP into PO 4 3- within 10 min at the pH range of 4-10, which was significantly higher than the conversion efficiency of HEDP by UV/PMS, Cu(II)/PMS and UV/Cu(II)/H 2 O 2 processes. The decomposition of HEDP was enhanced with increasing Cu(II) and PMS concentrations. Notably, mechanistic investigation revealed that Cu(III)-induced intramolecular electron transfer was the key contributor during the UV/Cu(II)/PMS-driven decomposition of HEDP into PO 4 3- . The experimental results of competitive ligands clearly suggested that the high selectivity of HEDP oxidation by UV/Cu(II)/PMS was closely related to the complexation of Cu(II) with HEDP. Additionally, although natural organic matter and inorganic anions to some extent affected HEDP degradation, UV-driven trace Cu(II)/PMS system still exhibited satisfactory results in treating HEDP in actual wastewater. This study proposes a strategy for efficient phosphonate removal under varying pH conditions, which provides new insights for practical wastewater treatment applications.

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MICROPOROUS AND MESOPOROUS MATERIALS · 2025 · IF 4.7

Engineering Bipedal Janus Nanocarriers: Dual-Targeting and pH/Microwave-Responsive Drug Delivery System for Cancer Therapy

Rong Wang,Xiaodan Kong

The development of intelligent platforms capable of precisely targeting cancer cells while minimizing toxic side effects on normal tissues remains a significant challenge in medical applications. This study proposes a structurally innovative bipedal Janus nanocarrier (Fe 3 O 4 @TiO 2 &dmSiO 2 /FA) for intelligent drug delivery. The architecture integrates magnetic-responsive and microwave (MW)-responsive Fe 3 O 4 @TiO 2 (core@shell) components with anisotropic growth bipedal mesoporous silica (dmSiO 2 ), the latter being modified with folic acid (FA) targeting ligands. This design achieves dual-mode tumor targeting by concurrently enabling FA-mediated active recognition and magnetic field-guided navigation. The system demonstrates drug release behavior orchestrated through the synergistic interplay between endogenous tumor microenvironmental stimuli (pH 5.3) and exogenous MW irradiation. MTT assays revealed that doxorubicin-loaded nanocarriers exhibit significant cytotoxicity under MW exposure, achieving over 80% proliferation inhibition in multiple cancer cell lines. These results position this nanocarrier as a promising candidate for effective cancer therapy.

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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2025 · IF 6.2

pH-Responsive Sustained-Release Hydrogel Microspheres for the Protection, Delivery and Release of Oral Polysaccharide Iron

Huabin Liao,Feina Gu,Ya Wen,Weichun Pan,Fuge Niu

Oral administration of polysaccharide-iron complexes (UCP-Fe(III)) is limited by their degradation in the gastric environment, which reduces bioavailability. We developed core–shell sodium alginate/chitosan hydrogel microsphere for pH-responsive UCP-Fe(III) delivery. High sodium alginate (SA) concentrations increased viscosity and storage modulus, enhancing mechanical stability. The encapsulation efficiency of UCP-Fe(III) reached 94.41% using 2.0% SA. Noncovalent interactions between UCP-Fe(III) and SA contributed to enhanced hardness and chewiness of the microspheres, while higher SA concentrations promoted a denser cross-linked network. The hydrogel microspheres showed low swelling in simulated gastric fluid (SGF, pH 2.0; swelling ratio: 467.33–588.50%) but rapid swelling in simulated intestinal fluid (SIF, pH 7.4; swelling ratio: 800–962.17%), indicating significant pH responsiveness. They effectively prevented premature release (only 12.14–23.48% in SGF after 2 h) while enabling sustained release (87.60–95.16% in SIF after 6 h). This study provides a new strategy for developing oral iron supplements with pH-responsive sustained-release properties.

CAS / MDL: 9005-38-3
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

4D-Printed Microrobots with Synergistic Integration of Magnetic Actuation, Diffractive Optical Sensing, and pH-Adaptive Morphing

Jingang Wang,Jianchen Zheng,Chengzhi Zhang,Ya Duan,Yuzhao Zhang,Hongji Guo,Ye Qiu,Xiaoduo Wang,Lianqing Liu,Haibo Yu

Soft microrobots exhibit distinct advantages in biomedical applications, with their exceptional maneuverability in confined spaces and environmental adaptability offering innovative solutions for targeted theranostics. However, current systems are inherently constrained by the physical separation of sensing and actuation modules, leading to inadequate integration and operational efficiency that hinder practical implementation. To overcome this challenge, a micro-nano 4D printing design paradigm is proposed. Through spatial programming of multi-responsive materials and biomimetic microstructural engineering, a microrobotic system is fabricated with synergistic perception-actuation capabilities. By integrating gradient magnetic field-responsive composites and pH-sensitive hydrogels, a 150-µm-scale biomimetic fish-shaped microrobot is developed, innovatively integrating three functionalities: magnetic-actuation, pH-triggered joint actuation, and diffractive optical sensing. Specifically, its tail joint enables adaptive modulation of doxorubicin release kinetics via pH-mediated mechanical deformation, while the head-mounted diffractive spectral sensor provides dynamic optical feedback of pathological microenvironment pH (5.0–6.5). Proof-of-concept experiments demonstrate the system's precise drug release control and environmental monitoring capabilities in gastric cancer cell therapy. This work provides a 4D printing design approach for next-generation intelligent therapeutic microrobots capable of environmental perception, intelligent response, and precise execution.

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Advanced Science · 2025 · IF 14.1

Physiological pH Transition-Driven Protein Corona Dynamics Regulate Cellular Uptake and Inflammatory Responses of Silica Nanoparticles

Yuting Ge,Fangqin Fu,Yu Gao,Tianchang He,Volker Mailänder,Daniel Crespy,Katharina Landfester,Shuai Jiang

Protein corona alters the biological identities and interactions of nanoparticles with cells, needing to be thoroughly scrutinized before in vivo applications. Importantly, protein corona is evolving as nanoparticles cross different microenvironments, leading to unpredictable biological behaviors. Unveiling how physiological conditions change, especially pH changes associated with tumor-targeted delivery, affect protein corona composition and subsequent bio-interactions, is thus essential for understanding the bio-fate and therapeutic efficacy of nanomedicines. This study investigates how physiological pH transitions influence protein corona dynamics on silica nanoparticles, cellular uptake, and inflammatory responses. Incubating nanoparticle-protein corona complexes at different pH values reveals that acidic pH increases protein adsorption and induces structural changes of adsorbed proteins, enhancing uptake by macrophages (RAW264.7 and dTHP-1) and tumor cells (A549) due to reduced electrostatic repulsion and enhanced membrane interactions. Despite increased uptake at acidic pHs, inflammatory responses of dTHP-1 cells are reduced as indicated by lower levels of reactive oxygen species and pro-inflammatory cytokines (e.g., IL-1 β , TNF- α , and IL-6). This is consistent with altered protein corona composition, featuring decreased levels of complement protein C3 and immunoglobulins, and increased regulatory proteins (e.g., C4BPA). These findings highlight the crucial role of microenvironmental pH in modulating protein corona fingerprints and in vivo behaviors of nanomedicines.

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Gels · 2025 ·Vol. 11 ·期 9 ·700 · IF 5.3

Amidated Pectin/Nanocellulose Hybrid Cryogel System with a pH-Responsive Release Profile for Small Intestinal Delivery

Shuhan Feng,Patrick Laurén,Jacopo Zini,Zahra Gounani,Jinfeng Bi,Jianyong Yi,Timo Laaksonen

Cellulose nanofibers and pectin are promising candidates for polysaccharide-based gel carriers. However, their integration into a structurally modified hybrid gel system has not been extensively investigated. In this study, hybrid cryogels with a pH-responsive release profile favoring small intestinal delivery were prepared by freeze-drying various ratios of anionic nanofibrillar cellulose (aNFC) and amidated pectin (AP). Under acidic conditions, carboxylate protonation reduced intermolecular electrostatic repulsion, promoting the formation of the aNFC/AP hybrid gel network. Increasing the AP content enhanced the mechanical strength of the hydrogels and resulted in larger pore sizes after freeze-drying. The hybrid cryogels prolonged the release of a model drug for up to 20–30 min at pH 3.0, while exhibiting rapid release within 1–2 min when the pH exceeded 6.5, due to gel network collapse. The release behavior was governed by both the porous morphology and the crosslinking density of the cryogel scaffolds. These findings demonstrate that aNFC/AP hybrid cryogels possess a well-defined pH-responsive functional window (pH 6.5–7.0) and hold strong potential as oral drug delivery systems targeting the small intestine.

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