COLLOIDS AND SURFACES B-BIOINTERFACES
·
2026
·
IF 5.9
Xingchun Jiang,Zhen Qin,Jun Li,Yunjiao Chi,Zhenhao Zhou,Zhiyun Qi,Xiaoying Chen,Xiaorui Feng,Shuangshuang Qi,Enlian Tang,Cui Wang,Sha Guo,Xueyan Hu,Hao Wu
Hydrophobic patterning, container surface, and Hofmeister salts drive aggregation. • Adsorbed protein amount does not predict subvisible particle concentration after shaking. • Hydrophobic patch continuity modulates interface-induced protein aggregation. • Spearman and PCA analysis enable interfacial-stability risk assessment. Antibody formulations are routinely exposed to air–liquid and solid–liquid interfaces during manufacturing, transportation, and drug administration, yet formulation design still relies mainly on bulk-phase stability parameters, which poorly predict aggregation under interfacial stress. Here we combined interfacial experiments and dissipative particle dynamics (DPD) simulations to dissect how Hofmeister-series salts and container-wall hydrophobicity jointly govern the stability of two monoclonal antibodies (mAb-1 and mAb-2) under mechanical stress. When bulk-phase stability was comparable, hydrophobizing the vial surface by octyltriethoxysilane silanization suppressed the growth of insoluble subvisible particles in mAb-1 by promoting stable protein layer adsorption. DPD simulations resolved the molecular basis of this stabilization: mAb-1 formed a flat, immobilized monomolecular protective layer at the solid–liquid interface (sliding-transition frequency 0.7), whereas mAb-2 underwent frequent adsorption–desorption cycles (transition frequency 3.6) that released denatured monomers back into the bulk and caused protein aggregation. Beyond bulk electrostatic effects, Hofmeister anions reshaped the interfacial hydration environment and thereby tuned how much protein adsorbed, how strongly it was retained, and how often it desorbed, kosmotropic sulfate enriched protein at interfaces through preferential exclusion, chaotropic thiocyanate strengthened retention at hydrophobic surfaces. Interfacial experiments and DPD simulations together show that profiling antibody adsorption dynamics across surfaces and Hofmeister salts identifies stabilizing combinations that bulk-phase stability metrics alone cannot predict, offering a practical strategy for formulation and packaging design. Download: Download high-res image (234KB) Download: Download full-size image
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LANGMUIR
·
2026
·Vol. 42
·期 29
·21195-21206
·
IF 4.4
Liu Qixin,Zhu Manyu,Li Shanshan,Zhang Yuqi,Li Zihao,Wang Yiran,Wu Lie,Ishibashi Takaaki,Jiang Xiue
Accurately understanding the water structure around multiple
groups
and their synergistic effect at electrified interfaces has been challenging
due to the complexity of the interface. The interfacial chiral symmetry-breaking
effect leads to differences in the spatial distribution of functional
groups and the consequent water structure, thereby providing a possibility
for the accurate analysis of molecular group-associated water. On
the basis of this model and combined with surface-enhanced infrared
absorption spectroscopy and ab initio molecular dynamics simulation,
we have systematically investigated the precise water structure around
carboxyl and amino groups, including the influence of carboxyl groups
on tetrahedrally coordinated water, the effect of amino groups in
tightening the surrounding water organization, and their synergy in
directing the first-layer water toward the surface. The presence of
methyl groups can enhance the interaction between amino groups and
water due to their electron-donating function. Furthermore, we revealed
a ligand-induced enhancement in the hydrogen evolution reaction at
the single group level. Our research provides a new methodology for
obtaining comprehensive insights into the impact of each functional
group, how they synergize to regulate the water structure and proton
reduction in complex systems, and their contribution to proton-coupled
electron-transfer reactions.
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ANALYTICAL CHEMISTRY
·
2026
·Vol. 98
·期 29
·21514-21524
·
IF 7.3
Xiao Jiaxin,Lu Guoci,Yuan Haoran,Wu Yangtao,Zhu Shumin,Bu Lingjun,Zhou Shiqing
The pervasive contamination of groundwater
by highly
toxic oxyanions
necessitates advanced sensing technologies capable of high-throughput
screening. To overcome the intrinsic single-analyte limitation of
conventional ion-selective electrodes (ISEs), we developed a biomimetic
sensor array inspired by the cross-reactive principles of biological
taste systems, which was constructed by self-assembling quaternary
ammonium salts (QACs) with tailored alkyl chain lengths (Cn) within
MXene interlayers (MXene/QAC-Cn). When integrated with a machine learning
model, the array successfully enabled the simultaneous identification
of four kinds of oxyanions (CrO 4 2– , SeO 4 2– , BrO 3 – ,
and ClO 4 – ) with a discrimination accuracy
of 97.1%. The sensor demonstrated exceptional sensitivity, achieving
a detection limit of 1.2 × 10 –9 M, and a 32-fold
enhancement in analytical throughput compared to single-analyte approaches.
Theoretical calculations revealed that the confined microenvironment
of the MXene/QAC-Cn composite promotes partial dehydration of the
oxyanions, reducing the adsorption energy by 1.09 eV. This mechanism
is pivotal for generating high-quality and differentiable response
fingerprints, which in turn ensures the high accuracy of the machine
learning model. The programmable design of this platform underscores
its potential for extension to a broader spectrum of oxyanions, offering
a versatile and scalable solution for comprehensive water quality
monitoring.
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Nanoscale
·
2026
·
IF 5.1
Xiaofang Ma,Yuhao Cai,Yang Gao,Hairong Zhao,Xiaxia Liu,Yuanyuan Tian,He Xiao
The design and fabrication of highly active hydrogen evolution reaction (HER) electrocatalysts that can outperform Pt/C are extremely desirable but remain challenging. Herein, the fabrication of S-doped hollow mesoporous carbon anchored Ru nanoclusters (Ru NCs/S-HMCs) is reported as a novel and highly active HER electrocatalyst through modified Stöber process and subsequent hydrothermal treatment, in which Ru NCs (1.64 nm in size) are uniformly anchored into S-HMCs channels. Benefiting from the unique electronic structure induced by S doping and the spatial confinement effect of the mesoporous carbon, the Ru NCs/S-HMCs catalyst exhibits excellent pH-universal HER activity, requiring only 3.5, 61.0, and 63.5 mV of overpotential to achieve a current density of 10 mA cm-2 in alkaline, neutral, and acidic electrolytes, respectively. In 1 M KOH, 0.5 M H2SO4, and 0.5 M PBS solutions, Ru NCs/S0.5-HMCs exhibits high mass activities of 21542, 2998 and 7088 mA mgRu−1 at an overpotential of -50 mV, respectively. The excellent activity stems from: (1) the pore confinement effect, which promotes the formation of ultrasmall Ru NCs (1.64 nm) and suppresses metal leaching; (2) S doping, which modulates the electronic structure of Ru and reduces the water dissociation barrier; and (3) the hollow mesoporous architecture, which accelerates mass and electron transport. This work provides insights for designing high-efficiency pH-universal electrocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaoping Huang,Kai Jin,Shengkai Yang,Jianxian Zeng,Hu Zhou,Rui Zhang,Jianrong Xue,Yuan Liu,Guoqing Liu,Huan Peng
Silver-containing wastewater poses a great threat to the surrounding living areas due to its toxicity and non-biodegradable. In this study, a novel polyvinylidene fluoride (PVDF)-based composite membrane (PVDF/BDBTU) was fabricated by blending PVDF and N-benzoyl-N′,N′-dibutyl thiourea (BDBTU) for the enrichment of Ag + ions from the aqueous solution. The structure and morphology of the membrane were characterized using FTIR, XPS, AFM and SEM, and its adsorption performances for Ag + ions were deeply studied. The results revealed that the adsorption amount of Ag + ions adsorbed by the membrane was 1.45 mmol/g at pH 6.0, and the adsorption can be described very well by the pseudo-second-order and Langmuir models, respectively, showing a monolayer chemisorption process. The coexisting substances had little impact on the adsorption of PVDF/BDBTU membrane to Ag + ions, suggesting an excellent adsorption selectivity to Ag + ions. In addition, the membrane showed a noticeable reusability for Ag + ions since no significant loss in adsorption capacity was observed after ten cycles of adsorption-desorption. The adsorption mechanism elucidated that the binding reaction between the C O and C S groups in BDBTU and Ag + ions contributed to the adsorption of Ag + ions onto the PVDF/BDBTU membrane surface, as confirmed by FTIR, XPS and DFT calculation.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1284-1296
·
IF 7.3
Yuxuan Lin,Weihua Qin,Yuwei Lu,Mingye Ren,Pan Gao,Feng Xiao,Shaoxia Yang
Improving the performance of single-atom catalysts (SACs) is still challenging in Fenton-like reactions for degrading refractory organic pollutants. Here, we designed P and N co-doped Fe SACs to regulate the electronic structure of Fe active sites and enhance the reaction kinetics of peroxymonosulfate (PMS) activation. The obtained heteroatom-doped Fe SACs for the first time exhibited an ultra-low activation energy (ca. 3.7 kJ mol−1) and excellent degradation efficiency for bisphenol A (BPA) in a wide pH range (4.3–9.2). The superior reaction kinetics of the Fe SACs were attributed to enriching the electron density of atomic Fe and then forming dual electron-rich/-deficient sites, which accelerated the electron transformation to generate reactive oxygen species (ROS). In this study the heteroatom-doped Fe SACs with rapid reaction kinetics are achieved, and provides an idea to design SACs with superior performance in heterogeneous Fenton-like reactions.
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Polymers
·
2023
·Vol. 15
·期 8
·1892
·
IF 5
Lijuan Chen,Changchang Chen,Yehan Yan,Linlin Yang,Renyong Liu,Jiajia Zhang,Xin Zhang,Chenggen Xie
Polydopamine fluorescent organic nanomaterials present unique physicochemical and biological properties, which have great potential application in bio-imaging and chemical sensors. Here, folic acid (FA) adjustive polydopamine (PDA) fluorescent organic nanoparticles (FA-PDA FONs) were prepared by a facile one-pot self-polymerization strategy using dopamine (DA) and FA as precursors under mild conditions. The as-prepared FA-PDA FONs had an average size of 1.9 ± 0.3 nm in diameter with great aqueous dispersibility, and the FA-PDA FONs solution exhibit intense blue fluorescence under 365 nm UV lamp, and the quantum yield is ~8.27%. The FA-PDA FONs could be stable in a relatively wide pH range and high ionic strength salt solution, and the fluorescence intensities are constant. More importantly, here we developed a method for rapidly selective and sensitive detection of mercury ions (Hg2+) within 10 s using FA-PDA FONs based probe, the fluorescence intensities of FA-PDA FONs presented a great linear relationship to Hg2+concentration, the linear range and limit of detection (LOD) were 0–18 µM and 0.18 µM, respectively. Furthermore, the feasibility of the developed Hg2+sensor was verified by determination of Hg2+in mineral water and tap water samples with satisfactory results.Keywords:polydopamine;folic acid;mercury ions;fluorescence probe
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JOURNAL OF BIOMEDICAL MATERIALS RESEARCH PART A
·
2023
·
IF 4.9
Yuying Bai,Dawei Tian,Zhengxin Ren,Dangyang Yue,Qian Ren,Li Pei,Jun Pan
Though magnetic iron oxide nanoparticles (IONPs) are approved for clinical use as contrast agents for MR imaging in United States and Europe, and are widely used to label cells in research, the relationship between IONPs and mesenchymal stem cells (MSCs) is not fully addressed. Here the effects of consistently appeared γ-Fe 2 O 3 on the lineage commitment of MSCs were studied to optimize applications of IONPs in MSCs upon verification of viability. 30 nm 10 μg/mL induced highest promotions on osteogenesis, while 30 and 50 nm of 100 μg/mL elicited most chondrogensis in 14 days, where the effects on ALP, GAG and SOX9 appeared after 7 days, while on RUNX2 came out after 10 days. γ-Fe 2 O 3 enhanced intracellular and extracellular Fe 3+ and ROS, modulated F-actin and decreased Lamin A of MSCs at different time scale. The disturbances of F-actin, Lamin A or ROS altered the effects of γ-Fe 2 O 3 on MSC differentiation. Our results demonstrate that different size, concentration and modulation of γ-Fe 2 O 3 are needed in its MSC applications for bone and cartilage tissues. Furthermore, an undocumented phenomenon that the modulation of F-actin affected the Lamin A expression in MSCs was observed.
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ADVANCED POWDER TECHNOLOGY
·
2023
·
IF 5.2
Xiaoping Huang,Xulu Yuan,Huifang Yang,Rui Zhang,Guoqing Liu,Jianxian Zeng
The selective adsorption of surfactants on minerals can strengthen the differences of physical and chemical properties of mineral surfaces, thereby improving the separation efficiency of the refractory minerals. Herein, a novel surfactant S-carboxyethyl- N -benzoyl thiocarbamate (CEBTB) was prepared and utilized as a collector to selective separation of chalcopyrite from pyrite. The adsorption performances and mechanism of CEBTB on chalcopyrite and pyrite surface were studied. It showed that the functional groups (C O, C S and –COOH) of CEBTB could selectively anchor on the chalcopyrite surface and increase its surface hydrophobicity, whereas the adsorption of CEBTB on pyrite surface was weak with the surface hydrophobicity improved insignificantly. Flotation experimental indicated that CEBTB exhibited superior flotation selectivity for chalcopyrite against pyrite than the common collector of SIBX. Batch adsorption experimental results demonstrated that the adsorption of CEBTB onto chalcopyrite surface was performed by a monolayer chemisorption, as well as the adsorption process was endothermic and spontaneous.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zilong Zhao,Yatao Ren,Shuyu Qi,Zigong Ning,Xing Wang,Wenyi Dong,Hongjie Wang
Heavy metal complexes pose a challenge in terms of their resistance to removal due to their stable and intricate structure. In this study, we explored the utilization of Fe and N co-doped biochar derived from rice husk (Fe-N-RHBC) as catalytic particle electrodes in a three-dimensional electro-Fenton (3D-EF) system for the decomplexation and removal of a model pollutant, Ni-EDTA. The characterization analysis and comparison of catalytic activities confirmed the beneficial effects of Fe and N co-doping on various aspects, such as the types of active sites, interfacial electron transfer properties, and H 2 O 2 decomposition capacity. Compared to other investigated oxidation systems, the 3D-EF process demonstrated rapid removal of Ni-EDTA within the initial minute, with a maximum H 2 O 2 utilization of 99.1% after 30 min. The prepared catalytic particle electrodes exhibited high stability and catalytic capacity even after three consecutive cycles. Throughout the reaction, several processes, including anode oxidation, particle electrode polarization, catalysis, and adsorption of Fe-N-RHBC, as well as cathodic electro-deposition, synergistically contributed to the treatment of Ni-EDTA. The surface-bound O 2 − radicals and 1 O 2 generated by the Fe-N-RHBC catalytic particle electrode played a crucial role in the decomplexation and removal of Ni-EDTA. Building upon these findings, we further proposed potential mechanisms for the removal of Ni-EDTA in the 3D-EF system using the Fe-N-RHBC catalytic particle electrode.
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Nano Research
·
2023
·
IF 9.9
Su Zhen,Li Depeng,Zhang Lixin,Tian Si,Su Yuhong,Hu Xiaoyun,Xiong Duan,Guan Qingqing
Smart materials that integrate multi-stimuli response, full reversibility, and dual-visual read-out channel are highly desired for anti-counterfeiting and information encryption applications. Herein, we developed a multiresponsive perchlorate terpyridyl Pt(II) nano complex which could undergo fully reversible conversion between three forms stimulated by water or formaldehyde molecule due to the extent of Pt–Pt interaction. Meanwhile, a dual-visual channel, i.e., the colorimetric channel changed from yellow to orange or red and the corresponding luminescent channel from orange to orange-red or red, has also been found. The weak and equivalent strength of ion-dipole interaction and hydrogen bond that generated between formaldehyde/water and Pt(II) salt result in the easy-control reversibility between the three forms. Furthermore, by introducing different polymer matrices, 1 Cl·ClO 4 @PMMA ( 1 Cl·ClO 4 : [Pt(tpy)Cl]·ClO 4 , tpy: 2,2′:6′,2″-terpyridine), PMMA: poly(methyl methacrylate)) and 1 Cl·ClO 4 @PVA (PVA: polyvinyl alcohol) are successfully constructed, which exhibit different reversible behaviors since the PMMA and PVA matrix exert different influences on the strength of hydrogen-bond. Those smart Pt(II) salt nanostructures present great potential for high-security-level anticounterfeiting application.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Shi-Long Xu,Peng Yin,Lu-Jie Zuo,Shi-Yi Yin,Yue Lin,Wanqun Zhang,Sheng-Qi Chu,Hai-Wei Liang,Xian-Zhu Fu
Proton exchange membrane fuel cells (PEMFCs) as electrochemical-generating devices with zero contaminants can promise a carbon-neutral future, but the usage of the costly platinum group metal catalysts hindered the widespread adoption of PEMFCs. Here, we present the synthesis of a highly active low-Pt PtCu3 intermetallic oxygen reduction catalyst via a sulfur-containing inorganic salt-assisted strategy. We identify that the success of the catalyst synthesis lies in the use of inorganic negative bivalent sulfur salts that leads to the formation of the CuS2 intermediate at low temperatures. The CuS2 intermediate serves as a passivator and releases Cu source at high temperatures to facilitate the formation of the PtCu3 intermetallic catalyst. The prepared small-sized PtCu3 intermetallic catalyst exhibits a high mass-based activity of 3.0 A mgPt–1 and a large electrochemically active surface area of 74 m2 gPt–1 for oxygen reduction, along with an outstanding durability (18% mass activity loss after 30,000 cycles).
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