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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Preparation of temperature-responsive smart sponge and its application in oil-water separation and dye adsorption

Cai Ling,Dai Yimin,Li Yaqi,Yang Siwen,Wang Junlong,Liu Bo,Ding Xianglong,Zhang Yue-Fei,Li Yan,Wan Li

At present, researchers are committed to studying new intelligent response materials to deal with severe water pollution problems. Using PU sponge as the substrate, dopamine was first modified to construct a rough surface while introducing active groups. The monomer N-isopropylacrylamide (NIPAM) and itaconic acid (IA) were grafted and polymerized onto the polydopamine coating on the sponge surface by vinyltrimethoxysilane (VTMS). The obtained DINA-PU sponge has good temperature response and switchable wettability characteristics, and has good adsorption-desorption cycle function. Moreover, a micro-filtration device was designed to separate heavy (light) oil-water mixtures. The separation efficiency can reach more than 95 % and 99 % for heavy and light oil-water, respectively. In addition, the adsorption capacity of the material for methylene blue (MB) can reach 660 mg·g −1 . The separation efficiency in the oil-water separation-dye adsorption integrated separation experiment can reach more than 99 %.

研究领域: 材料科学 · 环境科学
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY · 2015 · IF 0.795

Preparation of Thermo-Sensitive Magnetic Cationic Hydrogel for the Adsorption of Reactive Red Dye

Wei Yao,Pinhua Rao,Wenqi Zhang,Liang Li,Yingjie Li

In this study, thermo-sensitive magnetic cationic hydrogel (TSMCH) based on (3-acrylamidopropyl) trimethyl ammonium chloride (APTMACl) and N-isopropylacrylamide (NIPAm) was synthesized by free radical copolymerization. The TSMCH was characterized with Fourier transform infrared spectroscopy, thermal gravimetric analysis, x-ray diffraction, scanning electron microscope with energy dispersive x-ray, vibrating sample magnetometer, and zeta potential, and employed as adsorbent for adsorbing reactive red (RR) dye. Effects of molar ratios of APTMACl to NIPAm on the adsorption capacity of TSMCH were studied, and the results showed that a maximum adsorption capacity (1428.57 mg RR g−1 TSMCH) had been achieved when the molar ratio of APTMACl to NIPAm was 1:1. The adsorption isotherm of RR was well fitted by the Langmuir isotherm equation. TSMCH had good selectivity for adsorbing RR. Solution pH hardly affected the adsorption of RR on the TSMCH. The adsorption amount of RR increased with the increase of temperature. The adsorption–desorption of TSMCH was evaluated in three circles and a high regeneration rate was demonstrated.

研究领域: 材料科学 · 环境工程
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DESIGNED MONOMERS AND POLYMERS · 2023 · IF 1.6

Temperature sensitive nanogels for real-time imaging during transcatheter arterial embolization

Hongfu Zhou,Wenjing Xie,Anran Guo,Bin Chen,Sanming Hu,Min Zheng,Houqiang Yu,Hongan Tian,Ling Li

Several vascular embolization materials are commonly used in clinical practice, however, having application defects of varying degrees, such as poor intraoperative imaging and easy recanalization of embolized blood vessels, they are challenging for application during Transcatheter arterial embolization (TAE). Thus, an intraoperative visible vascular embolization material with good embolization effect and biocompatibility can improve transcatheter arterial embolization clinical efficacy to some extent. Our study aimed to synthesize a novel vascular embolization material that can achieve complete embolization of arterial trunks and peripheral vessels, namely poly (N-isopropyl acrylamide)-co-acrylic acid nanogel (NIPAM-co-AA). Iohexol 200 mg/mL was co-assembled with 7 wt% NIPAM-co-AA nanogel to create an intelligent thermosensitive radiopaque nanogel (INCA), which achieves a good intraoperative imaging effect and is convenient for transcatheter arterial bolus injection due to its good fluidity and temperature-sensitive sol-gel phase transition. The normal rabbit kidney embolism model further confirmed that INCA could effectively use Digital subtraction angiography (DSA) to achieve intraoperative imaging, and real-time monitoring of the embolization process could avoid mis-embolization and leakage. Meanwhile, in a 42-day study, INCA demonstrated an excellent embolization effect on the right renal artery of New Zealand white rabbits, with no vascular recanalization and ischemic necrosis and calcification remaining. As a result, this radiopaque thermosensitive nanogel has the potential to be an intelligent thermosensitive medical vascular embolization material, providing dual benefits in TAE intraoperative imaging and long-term postoperative embolization while effectively addressing the shortcomings and challenges of commonly used clinical vascular embolization agents.

研究领域: 医学影像学 · 介入放射学 · 生物材料学
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TALANTA · 2021 · IF 6.057

Thermally responsive reduced graphene oxide with electroactive functionality for controllable electroanalysis

Huiting Wang,Li Dong,Ling Zhang,Xiangxiang Chen,Qian Zhang,Lixin Xia

A thermally responsive hybrid poly(NIPAm- b -BVIm[FcCOO])-rGO composed of block co-polymer poly(NIPAm- b -BVImBr), reduced graphene oxide (rGO) and electroactive anions was designed and synthesized to achieve electroactive functionality. It is the polymeric ionic liquids (PILs) segment in the block co-polymer that integrated the three different components into a whole hybrid. Such segment of PILs could not only promote the modification of polar PNIPAm onto the non-polar rGO by cation-π interaction, but also realize the immobilization of ferrocenecarboxylate anion (FcCOO − ) via anion-exchange reaction. The PNIPAm moiety endowed the poly(NIPAm- b -BVIm[FcCOO])-rGO with thermal responsiveness, while the anion moiety provided additional electroactive function. It is noteworthy that the conformational change of PNIPAm segment upon different temperature could reveal or seal the redox probe of FcCOO − , thereby leading to a controllable expression of electroactivity switching by thermal stimuli. Owing to such regulation on surface property and conformation of PNIPAm segment, the modified electrode exhibited excellent thermally responsive electrocatalysis with reversible ‘ON-OFF’ effect toward the detection of ascorbic acid (AA), which led to two different catalytic states at the same electrode. The reversible electrocatalytic performance with switching capability of the poly(NIPAm- b -BVIm[FcCOO])-rGO/GCE is expected to have a broad application in the field of intelligent electrochemical sensors and devices.

研究领域: 材料科学 · 电化学
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MACROMOLECULAR RAPID COMMUNICATIONS · 2022 ·Vol. 43 ·期 19 ·2200320 · IF 5.006

Thermosensitive P(AAc-co-NIPAm) Hydrogels Display Enhanced Toughness and Self-Healing via Ion–Ligand Interactions

Lin Xu,Yu Fu,Robert J. Wagner,Xiang Zou,Qingrui He,Tao Li,Wenlong Pan,Jianning Ding,Franck J. Vernerey

Hydrogels containing thermosensitive polymers such as poly( N -isopropylacrylamide) (P(NIPAm)) may contract during heating and show great promise in fields ranging from soft robotics to thermosensitive biosensors. However, these gels often exhibit low stiffness, tensile strength, and mechanical toughness, limiting their applicability. Through copolymerization of P(NIPAm) with poly(Acrylic acid) (P(AAc)) and introduction of ferric ions (Fe 3+ ) that coordinate with functional groups along the P(AAc) chains, here a thermoresponsive hydrogel with enhanced mechanical extensibility, strength, and toughness is introduced. Using both experimentation and constitutive modeling, it is found that increasing the ratio of m(AAc):m(NIPAm) in the prepolymer decreases strength and toughness but improves extensibility. In contrast, increasing Fe 3+ concentration generally improves strength and toughness with little decrease in extensibility. Due to reversible coordination of the Fe 3+ bonds, these gels display excellent recovery of mechanical strength during cyclic loading and self-healing ability. While thermosensitive contraction imbued by the underlying P(NIPAm) decreases slightly with increased Fe 3+ concentration, the temperature transition range is widened and shifted upward toward that of human body temperature (between 30 and 40 °C), perhaps rendering these gels suitable as in vivo biosensors. Finally, these gels display excellent adsorptive properties with a variety of materials, rendering them possible candidates in adhesive applications.

研究领域: 材料科学 · 生物医学工程
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Feasibility of thermo-sensitive P(NIPAM-MBA) hydrogels as novel stripping agents for osmotic membrane distillation

Jing Ren,Jianfeng Li,Zhaozan Xu,Zhiping Du,Fangqin Cheng

As thermo-sensitive hydrogels could absorb water quickly and squeeze the water out by their insoluble cross-linked networks under thermal stimulus, a novel osmotic membrane distillation (OMD) process was proposed for the first time. In the OMD process of this study, water vapor diffused across the membrane under the swelling pressure of thermo-sensitive hydrogels. Poly-N-isopropylacrylamide (PNIPAM) hydrogels with 0.02%, 0.1% and 0.5% N,N′-methylenebisacrylamide (MBA) were synthesized and incorporated into the OMD system. The hydrogel properties were characterized by UV–vis spectrophotometer, FTIR and SEM . The effects of MBA content, membrane characteristics, operating temperature on OMD flux were investigated. The initial fluxes for the 0.02%, 0.1% and 0.5% MBA hydrogel-OMD systems were 1.68, 1.09 and 0.76 kg/m 2 ·h, respectively. And the hydrogels transformed to dehydrated state after 150 min of water absorption. The fastest water absorption rates for PNIPAM hydrogels with 0.02%, 0.1% and 0.5% MBA were obtained at the initial swelling ratios of 16, 14 and 12 folds, respectively. Besides, the optimal feed temperatures for the maximum flux were 40 °C, 50 °C and 50 °C for hydrogels with 0.02%, 0.1% and 0.5% MBA, respectively. The membranes with higher porosity and lower thickness demonstrated higher fluxes. According to our results, the swelling pressure of hydrogel acted as a driving force of the hybrid hydrogel-OMD system, and it was greatly affected by the hydrogel structure. Typically, a hydrogel with the balanced water absorbing and dewatering behaviors and a membrane with good mass transfer performance were two essential prerequisites for this process.

研究领域: 材料科学 · 环境工程
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ACS Omega · 2021 · IF 3.512

Temperature and pH Dual Responsive Nanogels of Modified Sodium Alginate and NIPAM for Berberine Loading and Release

Shuhua Chang,Dawei Qin,Rongjun Yan,Mengli Zhang,Binglin Sui,Hui Xu,Zhaomin Zheng,Xiaoli Hou,Yonggang Wang,Chenggang Qi

pH- and temperature-sensitive nanogels (NGs) were prepared from sodium alginate (SA) and N-isopropylacrylamide (NIPAM), as the sensitivity at pH 5.5 and 31 °C. SA was pH-modified with glutamic acid (Glu) and ethylenediamine (EDA). The products Glu-SA (Glu-modified SA) and EGSA (EDA- and Glu-modified SA) were characterized by ninhydrin color reaction, infrared spectroscopy, and zeta potential, and the best reactant ratio was selected. Moreover, temperature-sensitive, pH-sensitive EGSA-NGs possessing a semi-interpenetrating network structure were prepared by radical polymerization using N-isopropylacrylamide. The morphology of EGSA-NGs was characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), and atomic force microscopy (AFM). The cytotoxicity test shows the low cytotoxicity and high biocompatibility of the NGs. The newly prepared NGs were also subjected to pH-sensitive temperature-sensitive in vitro drug-loading and drug-release experiments. The pH-sensitive and temperature-sensitive experiments showed that the particle size of EGSA-NGs was reduced at pH 5.5 and above 31 °C. The drug-loading and drug-release experiments also confirmed this finding, indicating that the newly synthesized NGs could release the drug according to the environmental changes. Therefore, the material has potential application value in solid tumor targeted therapy.

CAS / MDL: 6461-04-7
研究领域: 药学 · 材料科学 · 生物医学工程
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2019 · IF 2.298

Dual-Responsive Graphene Oxide/Poly(NIPAM-co-AA) Hydrogel as an Adsorbent for Rhodamine B and Imidacloprid

Guohong Yao,Sisi Li,Jun Xu,Hui Liu

A dual-responsive hydrogel based on graphene oxide (GO) was prepared by in situ radical copolymerization of N-isopropyl acrylamide (NIPAM) as a temperature-sensitive component and acrylic acid (AA) as a pH-sensitive unit. The resulting hydrogels (GO/poly(NIPAM-co-AA) (PNA) were systematically characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, thermogravimetric analysis, differential scanning calorimetry, and scanning electron microscopy. With the change of AA content, the lower critical solution temperature of hydrogels changed from 26.91 to 24.38 °C. The swelling ratio under alkaline condition was higher than that under acidic condition. The adsorption of rhodamine B (RB) followed Langmuir isotherm model and pseudo-second-order model, and nearly 93% of RB could be released within 10 h at pH 4.01 and 60 °C. With imidacloprid as the model drug, the higher cumulative release rate of the GO/PNA hydrogel was obviously observed at pH = 4.01 than at pH = 9.18. On the basis of their good adsorption–desorption, loading-releasing, and regeneration ability, the GO/PNA hydrogel as a multifunctional adsorbent might have broad application prospects in environmental protection and biomedical engineering.

研究领域: 材料科学 · 环境科学 · 生物医学工程
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Soft Matter · 2015 ·Vol. 11 ·期 14 ·2771-2781 · IF 4.029

Comparison of LCST-transitions of homopolymer mixture, diblock and statistical copolymers of NIPAM and VCL in water

Lei Hou,Peiyi Wu

The LCST-transitions of linear, well-defined polymers of N-isopropylacrylamide (NIPAM) and N-vinylcaprolactam (VCL), including a homopolymer mixture, diblock and statistical copolymers, in water are explored and compared by applying turbidity and FTIR measurements in combination with two-dimensional correlation spectroscopy (2Dcos). Only one transition is observed in all polymer systems, suggesting a dependent aggregation of poly(N-isopropylacrylamide) (PNIPAM) and poly(N-vinylcaprolactam) (PVCL) parts in the phase transition processes. With the help of 2Dcos analysis, it is discovered that the hydrophobic interaction among C–H groups is the driving force for simultaneous collapse of the two distinct thermo-responsive segments. Additionally, the delicate differences within the LCST-transitions thereof have been emphasized, where the phase separation temperatures of the homopolymer mixture and the diblock copolymer are close while that of the statistical copolymer is relatively higher. Moreover, both diblock and statistical copolymers exhibit rather sharp phase transitions while the homopolymer mixture demonstrates a moderately continuous one.

CAS / MDL: 78-67-1 2210-25-5
研究领域: 高分子化学 · 物理化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Temperature-controlled electrochemical sensor based on environmentally responsive polymer/BiPO4/BiOCl/multi-walled carbon nanotube composite for the detection of catechol in water

Yilin Wang,Qian Fu,Jia Chen,Yueli Lin,Yaqi Yang,Chenxi Wang,Yixi Xie,Pengcheng Zhao,Junjie Fei

Catechol is a phenolic environmental pollutant that is highly toxic to living organisms and is released into the environment, where it is difficult to degrade in the ecosystem, thereby contaminating the environment and groundwater. Here, P(NIPAM-co-BMA)/BiPO 4 /BiOCl/MWCNTs nanocomposites were synthesized, and a temperature-controlled "on/off" electrochemical sensor was constructed. In addition, the P(NIPAM-co-BMA)/BiPO 4 /BiOCl/MWCNTs/GCE sensor shows good thermal sensitivity and electrochemical detection of catechol. Reproducible "on/off" switching on the CVs curve can be achieved by controlling the temperature of the solution. Under optimal conditions, the sensor was able to detect catechol in the linear range of 0.5–86.51 μM with a limit of detection of 0.2 μM (S/N = 3). Satisfactory results were obtained for the detection of natural environmental samples (tap water). In addition, the redox mechanism and electrochemical reaction sites of catechol were investigated by scanning rates. This work demonstrates for the first time the combination of temperature-sensitive polymers, bismuth-based compounds and multi-walled carbon nanotubes as electrochemical sensors for the detection of catechol, opening a new window for the sensitive detection of catechol. At the same time, the constructed switch-like electrochemical sensors can be better applied to different special scenarios.

研究领域: 环境科学 · 分析化学
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SENSORS AND ACTUATORS A-PHYSICAL · 2026 · IF 5.1

Synergistically crosslinked P(NIPAM-AM)/TA-Fe3+/CS composite hydrogel enabling NIR-driven actuation and resistive self‑sensing

Zhibo Zhou,Yunqing Gu,Yun Ren,Zhou Li,Denghao Wu,Zhenxing Wu,Chengqi Mou

P(NIPAM-AM)/CS/TA-Fe 3+ hydrogel integrates NIR actuation and self-sensing. • Optimized network enables a 4.7 s fast response and 104° maximum bending. • TA-Fe 3+ coordination offers a high photothermal conversion efficiency of 27.76%. • Linear resistance-strain mapping predicts bending angles with ≤ 2.67% error. • The dual-function material allows real-time feedback for closed-loop control. Conventional hydrogel actuators often suffer from single functionality and a lack of real-time state feedback, restricting their potential in closed-loop control and intelligent applications. To address this, we designed a synergistically crosslinked composite hydrogel based on poly(N-isopropylacrylamide-co-acrylamide) (P(NIPAM-AM)), tannic acid-iron ion (TA-Fe 3+ ) complexes, and chitosan (CS). This hydrogel integrates near‑infrared (NIR)‑driven actuation with resistive self‑sensing and exhibits excellent shape programming and multidirectional actuation capabilities. By systematically optimizing the composition, the hydrogel with 0.1 mL of CS solution achieves a rapid response time of only 4.7 s and a maximum bending angle of 104°. Furthermore, at an Fe 3+ content of 120 mg, the hydrogel demonstrates a high photothermal conversion efficiency of 27.76% and an initial conductivity of 2.549 (Ω·m) −1 . It exhibits excellent self-sensing characteristics, with a bending gauge factor of 0.019 and high angle-sensing accuracy with an error of ≤ 2.67%. This work provides a simple and efficient strategy for developing intelligent soft materials that integrate actuation and sensing. Download: Download high-res image (220KB) Download: Download full-size image

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SENSORS AND ACTUATORS B-CHEMICAL · 2017 · IF 5.401

A facile synthesis of thermo-responsive copolymer stabilized fluorescent silver nanoclusters and their application in pH sensing

Jianhua Lü,Yuqin Fu,Dongmei Wang,Changli Lü

Luminescent silver nanoclusters (NCs) decorated with temperature-responsive copolymer P(NIPAm-co-MQ) have been fabricated in aqueous solution as a new fluorescent pH stimuli-responsive functional materials. P(NIPAm-co-MQ) was prepared by a conventional free-radical copolymerization of isopropylacrylamide (NIPAm) as thermo-responsive units and 5-(2-methacryloylethyloxymethyl)-8-quinolinol (MQ) as coordinating groups. The obtained fluorescent Ag NCs with various sizes showed different morphologies from single sphere to chain structure induced by the copolymer ligand. Upon changing the temperature, the fluorescence intensity of the Ag NCs exhibited temperature triggered response simultaneously. The copolymer stabilized Ag NCs as a pH probe exhibited reversible pH-dependent PL properties over the pH range of 3.04–5.25. With the pH decreased, the fluorescence intensity of Ag NCs under a UV lamp decreased and it was almost completely quenched after pH 3.04. Also, the properties of this fluorescence change with pH are reversible.

研究领域: 材料科学 · 纳米技术 · 分析化学
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