ACS Omega
·
2026
·Vol. 11
·期 35
·53469-53476
·
IF 5.2
Lu Xin,Yuan Fangfang,Han Xiaojie,Qin Tingting,Wang Qianqian,Li Zengli,Ge Chuanjun,Shi Wenqing,Bai Haijiao,Wang Pei
Desmopressin, a synthetic
analog of vasopressin widely used in
the treatment of diabetes insipidus and bleeding disorders, is a representative
disulfide-containing peptide therapeutic prepared by Fmoc-based solid-phase
peptide synthesis (SPPS). Its unique sequence architecture, particularly
the spatial proximity between the N-terminal mercaptopropionic acid
residue Mpa(1) and the Tyr(2) residue, provides a distinct structural
environment for investigating sequence-dependent side reactions during
peptide manufacturing. The tert- butyl ( t- Bu) protecting group is widely employed for side-chain protection
in Fmoc-based solid-phase peptide synthesis (SPPS). However, under
certain reaction conditions, the highly reactive t- Bu + carbocation generated during acidic deprotection can
participate in nonspecific alkylation, leading to challenging process-related
impurities. In this study, we investigated a unique and highly site-selective
+56 Da impurity observed during side-chain deprotection. High-resolution
MS/MS analysis unambiguously identified this species as a site-selective
product arising from the migration of t- Bu from the
Tyr(2) side chain to the thiol group of Mpa(1). Based on the structural
features of desmopressin, in particular, the spatial proximity between
Tyr(2) and Mpa(1), we propose that the formation of this impurity
most plausibly proceeds via a vicinal-thiol-induced intramolecular
migration mechanism, which competes significantly with the conventional
diffusion-controlled carbocation intermediate intermolecular pathway.
Strengthening the scavenger conditions failed to eliminate this impurity,
further supporting the intramolecular migration mechanism induced
by vicinal thiol. This finding accounts for the observed site selectivity
that cannot be explained by the conventional carbocation intermediate
pathway alone. Guided by these mechanistic insights, we re-evaluated
the necessity of Tyr side-chain protection and proposed a “source-elimination”
strategy. Experimental validation demonstrated that the use of unprotected
Fmoc-Tyr-OH (free phenolic hydroxyl) completely suppressed the formation
of the t- Bu migration impurity and improved the crude
peptide purity to 93.5%. Overall, this study elucidates the formation
mechanism of t- Bu migration impurities and provides
a broadly applicable, mechanism-driven strategy for process optimization
in solid-phase peptide synthesis. While this study focuses on the
desmopressin system, the findings highlight a proximity-driven reactivity
pattern that may be relevant to other thiol-containing peptide sequences.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 34
·18145-18158
·
IF 3.9
He Yiruo,Su Weiyi,Song Jianheng,Liu Qidong,Wang Na,Yu Xiong,Wang Honghai
The
combination of immobilized enzymes and microreactors offers
great advantages in green biomanufacturing. However, improving the
catalytic loading and reusability of immobilized enzymes remains a
challenge. This study developed a magnetically separable immobilized
enzyme system for continuous-flow biocatalysis. Candida antarctica lipase B (CALB) was covalently immobilized onto polydopamine-modified
Fe 3 O 4 nanoparticles to prepare a magnetic nanoimmobilized
enzyme (CALB@PNMNs). Compared to free enzymes, CALB@PNMNs exhibited
enhanced stability in organic solvents and storage stability. CALB@PNMNs
microreactor was constructed, with CALB@PNMNs immobilized on its inner
walls by an external magnetic field. This layer of magnetic particles
allows for the convenient recovery and reuse of the catalyst by removing
the applied magnetic field. After optimizing the immobilization process,
the actual CALB loading per unit area was 0.30 mg/cm 2 ,
and the adsorption yield reached 86.89%. The microreactor was applied
to the transesterification of n -butanol and ethyl
acetate, with the optimal conditions identified as an alcohol–ester
ratio of 1:3, a total flow rate of 10 μL/min, and a reaction
temperature of 60 ° C, yielding an n -butanol
conversion of 63.72%. After short-term continuous operation for 6
h, the microreactor retained 87.63% of the enzyme adsorption capacity
and CALB@PNMNs maintained a n -butanol conversion
above 50% after 8 reuse cycles. This work has established a stable
magnetically controlled immobilized enzyme microreactor (IMER) platform,
offering application potential for continuous-flow bioprocesses.
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DENTAL MATERIALS
·
2026
·
IF 6.3
Changyu Shao,Tong Shi,Dayu Wang,Chang Liu,Zhenhang Tang,Yuanyu Zhou,Haihua Pan,Zhijian Xie,Ruikang Tang,Zhuo Chen
Chondroitin sulfate mediates the amorphous calcium phosphate ordered assembly. • Chondroitin sulfate directs the oriented crystallization of the hydroxyapatite. • Biomimetic restores the enamel hierarchical structure and mechanical properties. • Hydrogel mineralization system demonstrates significant efficacy for enamel repair. Objectives This study aims to develop a biomimetic mineralization strategy using chondroitin sulfate (CS) to reconstruct the intricate hierarchical structure of enamel and restore its mechanical properties. Methods Demineralized enamel was remineralized in a CS-containing artificial saliva (AS). The crystallization of hydroxyapatite (HAP) in AS was investigated using transmission electron microscopy (TEM) and atomic force microscopy (AFM)-infrared spectroscopy. Enamel repair efficacy was systematically evaluated via scanning electron microscopy (SEM) and AFM to characterize the microstructure and repair thickness, while nanoindentation was employed to quantify the mechanical properties. In addition, acid resistance was evaluated using a 50 mM HCl solution. Furthermore, an AS-hydrogel mineralization system was developed to evaluate its efficacy in restoring demineralized enamel under biologically relevant conditions. Results The results demonstrate that CS-modified ACP successfully assembles into chain-like precursors via anisotropic forces, which simultaneously regulate the oriented crystallization of HAP. This strategy resulted in a newly formed mineralized layer that effectively reconstructs the hierarchical architecture and recovers mechanical properties, including hardness, elastic modulus, and coefficient of friction, to near-native levels. In addition, the repaired enamel exhibits an acid resistance level comparable to that of native enamel. Significance This study establishes a new, mechanism-driven strategy for enamel remineralisation that is mediated by CS, and a corresponding hydrogel mineralization system, which can be translated into practice, offering a promising approach to future clinical enamel restoration. Download: Download high-res image (411KB) Download: Download full-size image
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ELECTROANALYSIS
·
2026
·Vol. 38
·期 4
·e70149
·
IF 2.6
Haixu Wang,Xiaonan Qi,Shunli Zhou,Rongsong Cao,Xi Yang,Le Li,Zhen Sun
Gallic acid (GA) is a natural polyphenol known for its significant biological activity and widespread presence in food, medicine, and various other fields. The accurate and rapid detection of GA is crucial for ensuring food quality control and conducting pharmaceutical analyses. In this study, we successfully developed a novel electrochemical sensor based on a ZIF-67/pomelo carbon (ZIF-67/PC) composite through a simple and environmentally friendly synthetic route. The results indicated that the glassy carbon electrode (GCE) modified with ZIF-67/PC exhibited remarkable electrocatalytic activity towards GA oxidation. The pore-like structure of ZIF-67/PC accelerates the diffusion of GA, the carbon matrix enhances electron transfer, and the Co-N-C sites catalyze the oxidation of GA, thereby achieving excellent detection performance. Under optimal conditions, the sensor demonstrated an extensive linear response range of 8–1000 μM for GA, accompanied by a low detection limit of 0.25 μM (S/N = 3). Furthermore, this sensor displayed excellent selectivity as well as good stability-retaining 91.27% current after 15 days and satisfactory reproducibility with a relative standard deviation below 2%. When applied to detect GA in green tea samples, recovery rates ranged from 95.2% to 102.1%, underscoring its practical application potential. This work presents a viable strategy for developing low-cost yet high-performance electrochemical sensors by integrating metal–organic frameworks with biomass-derived carbon materials.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Chengdong Ma,Hongrui Zhang,Weigui Xie,Wangyu Liu
Phosphoric acid-based ion-conductive hydrogels face a long-standing challenge of balancing toughness, low hysteresis, and high conductivity, which are key requirements for advanced flexible sensing materials. In this work, a tough and low-hysteresis acrylamide-phosphoric acid (AP) hydrogel is proposed, using an ultralow-initiator-concentration (0.005 wt % relative to the monomer mass) polymerization method. Swelling, SAXS, and SEM experiments confirm the uniform chains, and FT-IR experiments demonstrate a strong hydrogen-bonding network of our ultralow-initiator-concentration-polymerized AP hydrogel. Uniaxial tensile tests show that the toughness and hysteresis of the AP hydrogel are inversely associated with the initiator concentration. Consequently, the ultralow-initiator-concentration-enabled AP hydrogel presents a tensile strength of 2.1 MPa, a toughness of 8.9 MJ m–3, and an ultralow hysteresis of 1.35% under 100% strain. Benefiting from the excellent electromechanical properties, the AP hydrogel-based flexible sensor exhibits high reliability as a flexible resistance strain sensor and an electric double-layer capacitive pressure sensor. This work not only resolves the inherent constraint of traditional phosphoric acid-based hydrogels but also provides a perspective for the structural regulation of functional hydrogels, enabling broader applications in flexible sensing and human–machine interactions.
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ACS Sensors
·
2026
·
IF 10.9
Peng Xu,Yanlei Guo,Xin Lv,Shuting Wei,Dan Yang,Renquan Guan,Yuxin Wang,Yingmin Teng,Aiceng Li,Huaqiao Tan,Zhongling Lang,Zheng Lou,Lili Wang,Zhao Zhao
The necessity for high-efficiency, low-power room-temperature (RT) ammonia (NH3) sensors is particularly acute in environmental monitoring, industrial safety, and medical diagnostics. However, conventional chemiresistive sensors frequently require elevated temperatures to initiate reactions, leading to high energy consumption and potential safety risks. Inspired by plant photosynthesis, this paper successfully designs a ternary S-scheme heterojunction for a photo-activated RT NH3 sensor. The design effectively mimics the efficient charge transfer process in photosynthesis, thereby significantly promoting the separation and migration of photogenerated carriers and enhancing the sensing performance. Experimental results demonstrate exceptional performance under illumination: a high response value of 1679% (representing a 20-fold improvement over the dark state), rapid response and recovery times of 2.1 s and 1.9 s, respectively, along with outstanding selectivity, excellent stability, and a detection limit as low as 17 ppb. This work demonstrates a novel, efficient RT photo-activated NH3 sensor and provides innovative insights into designing biomimetic, smart gas-sensing materials and devices.
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LANGMUIR
·
2026
·
IF 4.4
Yue Huang,Xiaoxuan Zheng,Guangtao Mei,Haowen Lu,Shuji Ye,Guangming Liu
Understanding the thermodynamic driving force behind the pH-controllable interfacial hydration of strong polyelectrolyte brushes (SPBs) is crucial yet challenging. Using the poly(styrenesulfonate) (PSS) brush as a model system, we elucidate this thermodynamic mechanism by employing advanced femtosecond sum frequency generation vibrational spectroscopy (SFG-VS). SFG-VS identifies the hydrogen bond interactions between the bound hydronium counterions and the grafted PSS chains, along with the ordering of water molecules at the PSS brush surface. As pH increases, more hydrogen bonds are formed between the interfacial water molecules and the PSS brush accompanying the disruption of the integrated hydrogen-bond network inside the brush, concurrently enhancing the ordering of interfacial water molecules, thereby leading to the interfacial hydration of the PSS brush with negative changes in both enthalpy (ΔH < 0) and entropy (ΔS < 0). Consequently, the pH-controllable interfacial hydration of the PSS brush is consistent with enthalpically driven hydration. Moreover, this pH-controllable, enthalpically driven interfacial hydration may extend to other SPB systems, enabling the key properties of SPBs pH-responsive. This work provides a thermodynamic perspective on the pH-controllable interfacial hydration of SPBs, and will pave the way for novel applications of SPBs in material science.
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MICROCHIMICA ACTA
·
2026
·Vol. 193
·期 7
·501
·
IF 5.4
Wang Yunan,Zhang Qiang,Cheng Yue,Shi Chenglong,Wang Yong,Ma Xiaofei
A micro-nano structure enhanced chiral separation strategy is proposed by integrating biomimetic liposome assemblies with cyclodextrin (CD) derivatives as composite chiral selectors in capillary electrophoresis (CE). The self-assembly of weakly chiral, poorly soluble phospholipids into liposomes markedly amplifies chiral discrimination when coupled with CD-based molecular recognition, enabling highly efficient separation of multiple 9-fluorenylmethoxycarbonyl (Fmoc)-amino acid enantiomers. This enhancement is proposed to be associated with the formation of interfacial pre-enrichment microzones on liposome surfaces, where locally concentrated selectors and analytes may engage in synergistic hydrogen bonding, hydrophobic interactions, and steric effects, collectively strengthening chiral recognition. The composite system exhibits good selectivity and compatibility in mixed-sample separations, supporting simultaneous enantioseparation of multiple amino acids with high reproducibility. Beyond establishing an effective CE-based approach for amino acid enantiomer separation, this work demonstrates a proof-of-concept for transforming poorly soluble, weakly chiral substances into efficient chiral selectors through micro-nano assembly, offering preliminary insights for synergistic chiral separation systems. Graphical abstract
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Jianqi Ye,Jinhua Lu,Lanqing Li,Xinhao Wan,Jialu Wang,Haoxin Fan,Fangyuan Ma,Shan Chen,Dan Wen
Developing flexible, self-sufficient power generators is of significance for burgeoning wearable electronics. Biofuel cells (BFC) that harness perspiration metabolites can potentially offer a promising route toward simultaneous energy generation and self-powered sensing. However, insufficient power supply and susceptible enzyme-induced instability hinder widespread adoption. Herein, an enzyme-free hybrid glucose BFC is designed employing nitrogen-phosphorus doped carbon (NPC) flexible film derived from self-assembly graphene/polymer hydrogels, incorporating platinum nanoparticles for glucose oxidation and manganese dioxide-based O 2 -independent capacitive cathode. The O 2 -independent design eliminates potential interference to the anodic reaction, enabling a markedly enhanced maximum power density of 680 µW cm −2 and an open circuit voltage of 0.92 V, alongside operational stability exceeding 30 days. When functioning as the self-powered glucose sensor, it offers a wide range of 0.05–20 mM. Integrated into a conformal wearable system, the device enables bioenergy harvesting from human sweat and real-time glucose monitoring via compact signal processing electronics. This work underscores the potential of flexible hybrid BFC systems and paves the way for powering next-generation wearable bioelectronics in personalized healthcare.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2026
·
IF 3.6
Yue Gui,Jincheng Liu,Ping Yang,Jingxian Zhu,Yiran Xu,Jing Wang,Xin Dong,Tongming Sun,Yanfeng Tang,Minmin Wang
This study successfully fabricated a freestanding ZnO@(NiFe)OOH nano-heterostructure array electrocatalyst with high hydrophilicity for efficient electrocatalytic nitrate reduction to ammonia (NO 3 RR) in neutral media. The material integrates the large specific surface area of one-dimensional ZnO nanoarrays with the electronic modulation capability of heterogeneous interfaces, which significantly enhances nitrate adsorption and activation, promotes proton supply, and effectively suppresses the hydrogen evolution side reaction. The highly hydrophilic surface further accelerates electrolyte diffusion, nitrate ion transport, and product desorption. In a neutral electrolyte of 0.1 M PBS containing 0.15 M KNO 3 at a potential of −1.0 V (vs. RHE), the catalyst achieves an ammonia production rate of 4.86 mg·h −1 ·cm −2 with a Faradaic efficiency of 85.58%, while generating minimal byproducts, demonstrating excellent catalytic selectivity and stability. This work provides a new strategy for the structural design and performance enhancement of NO 3 RR electrocatalysts, which holds significance for advancing green ammonia synthesis and enabling efficient conversion of nitrate in water pollution control. Graphical A self-supported ZnO@(NiFe)OOH core-shell array enables efficient nitrate-to-ammonia conversion. The ZnO core accelerates NO 3 -diffusion and prevents active site coverage while enhancing conductivity and stability. The (NiFe)OOH shell facilitates intermediate conversion and suppresses hydrogen evolution by weakening H+ adsorption. Its surface hydroxyl groups promote water dissociation, ensuring a local proton supply. In neutral media, this design achieves superior performance: at −1.0 V vs RHE in 0.15 M KNO 3 , it delivers an NH3 yield of 4.86 mg h −1 cm −2 and a faradaic efficiency of 85.58%.
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JOURNAL OF PERIODONTOLOGY
·
2026
·
IF 4.5
Bei Gao,Jin Bai,Rui Xiao,Jiaqi Li,Mengying Wang,Ziyi Wang,Zhihui Feng,Jianfeng Shi,Zhongbo Liu
Background Postmenopausal osteoporosis (PMOP) leads to systemic bone metabolism disorders, significantly affecting oral bone health and complicating treatment. Osteocytes, the most abundant cells in bone tissue, play a crucial role in bone remodeling through cellular communication. However, the mineralized bone matrix surrounding osteocytes presents significant challenges for studying their dendritic networks. Methods Eight week old C57BL/6J female mice were randomly assigned to either a Sham group or an ovariectomized (OVX) group. The PMOP animal model was established via bilateral ovariectomy and analyzed after 12 weeks. Osteocyte dendrites and the lacuno-canalicular network (LCN) were examined via SEM and immunohistochemical staining. Quantification of nodes and connectomic measurements were performed for LCN and phalloidin network analyses. Furthermore, the expression levels of MMP13 and CTSK were assessed via immunohistochemical staining and real-time PCR. Results Our findings revealed that both Sham and OVX mice exhibited two distinct morphological types of osteocyte lacunar structures in the mandible. In Sham mice, direct communication was observed between osteocytes, adjacent cells, and blood vessels via canaliculi. In contrast, connectivity analysis of the osteocyte dendritic network in OVX mice revealed a reduced material transport capacity between cells compared with Sham controls. OVX-induced systemic osteoporosis altered the osteocyte dendritic network and lacunar canaliculi in the mandible, potentially due to periluminal canalicular remodeling. Conclusions This study offers new insights into the changes and mechanisms affecting the dendritic network and lacunar canaliculi of mandibular osteocytes in postmenopausal osteoporosis, contributing to a deeper understanding of oral bone lesions in this condition. Plain Language Summary After menopause, many women develop osteoporosis—a condition where bones become weak and break easily. This not only affects bones such as the spine or hips but also damages the jawbone, making dental treatments harder. We wanted to understand how osteoporosis weakens the jawbone by studying tiny bone cells called osteocytes, which act like “messengers” controlling bone health. Using advanced microscopy and special staining techniques, we mapped communication networks between osteocytes in the jawbone (like tracing telephone wires between cells). We then compared bone structures between healthy mice and mice with osteoporosis after ovary removal. Osteoporosis damaged the “wires” (dendrites) connecting osteocytes, reducing their ability to share nutrients and signals. It also widened tunnels (canaliculi) around osteocytes—like potholes in roads—disrupting their links to blood vessels and neighboring cells. These changes likely occur because osteoporosis impairs the bone's self-repair system around these tunnels. Our discovery that osteoporosis breaks bone cell networks reveals a new mechanism for jawbone weakening, paving the way for better dental treatments, protective drugs, and patient education.
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PHYTOTHERAPY RESEARCH
·
2026
·
IF 8.1
Huimao Liu,Dan Yang,Hanyan Cheng,Lijuan Cao,Xu Song,Xun Zhou,Yuanfeng Zou,Lixia Li,Renyong Jia,Dongmei Zhang,Mingyue Li,Zhongqiong Yin
Resveratrol (RSV), a dietary polyphenol widely present in traditional medicinal plants and foods, exhibits antioxidant and anti-inflammatory properties that are relevant to ethnopharmacological strategies for protecting against environmental neurotoxicants. Given increasing real-world co-exposure to lead (Pb) and cadmium (Cd), elucidating RSV's capacity to preserve gut–brain axis (GBA) homeostasis has direct translational relevance for populations relying on phytochemical interventions. Sprague–Dawley rats were randomized into control, Pb–Cd model, and RSV treatment groups (10, 20, or 40 mg/kg). For 4 weeks, rats received Pb (300 mg/L) and Cd (50 mg/L) in drinking water with daily RSV. Cognitive function was assessed by Morris water maze; barrier integrity by Evans blue assay, histology, and Western blot for ZO-1/Occludin; synaptic ultrastructure by TEM; microbiota composition by 16S rRNA sequencing; and short-chain fatty acids (SCFAs) by GC-MS. Neurotransmitters (5-HT, GABA, SP, VIP) and cytokines (IL-6, IL-1β, TNF-α) were measured by ELISA. RSV improved spatial learning, reduced EB extravasation, preserved synaptic ultrastructure and proteins (BDNF, SYN, PSD-95), and restored intestinal architecture with increased ZO-1/Occludin. RSV attenuated cytokine release, normalized goblet cells, reversed dysbiosis by restoring Lactobacillaceae/Prevotellaceae, and increased acetate, propionate, and butyrate. It reinstated 5-HT and GABA while reducing SP and restoring VIP across serum, colon, and hippocampus. RSV attenuated Pb–Cd–associated neurotoxicity and was accompanied by improved intestinal and BBB-related readouts, partial normalization of gut microbiota features and SCFA levels, and preservation of synaptic and neurotransmitter-related markers, consistent with a link to gut–brain axis function. This study is among the first to test RSV in a Pb–Cd co-exposure model using a multi-dose regimen with integrated behavioral, barrier, microbial, and neurochemical endpoints.
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