MACROMOLECULES
·
2022
·
IF 6.057
Kang Liu,Pengbo Han,Shunfeng Yu,Xinjun Wu,Yueyi Tian,Qianhan Liu,Jinhui Wang,Mingming Zhang,Chuanzhuang Zhao
Stimuli-responsive light-emitting polymers (SRLEPs) have many promising applications. However, the synthesis of SRLEPs from nonconjugated and water-soluble monomers remains a challenge. Herein, for the first time, nonconjugated luminescent polymers with an upper critical solution temperature (UCST) in aqueous solution are reported. The polymer is synthesized through copolymerization of a strong hydrogen-donating monomer, acrylic acid (AAc), and a strong hydrogen-accepting monomer, N-vinylcaprolactam (NVCL). The polymer–polymer hydrogen-bonding rigidifies the chain conformation and enhances the clustering of the heteroatoms and carbonyl groups, resulting in an improved clusteroluminescence. Meanwhile, the polymer–polymer hydrogen bonding also brings in dynamic chain association that can be switched with temperature, yielding a UCST-type thermoresponsiveness in aqueous solution. This work demonstrates a novel and facile method of designing SRLEPs through tailoring the hydrogen bonds in the polymer. The properties of clusteroluminescence and thermoresponsiveness of the AAc–NVCL copolymers may render themselves with applications as temperature-sensitive biosensing.
研究领域:
聚合物科学
·
材料科学
·
化学
·
生物传感
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产品关联
DOI
高影响因子
EUROPEAN POLYMER JOURNAL
·
2019
·
IF 3.621
Zelai Zheng,Lin Zhang,Ying Ling,Haoyu Tang
A series of ABA-type triblock copolymers (PImBF 4 -b-PPG-b-PImBF 4 ) comprising of poly(propylene glycol) (PPG) as middle block and UCST polypeptide on both sides of PPG was synthesized by ring-opening polymerization of γ -chloropropyl- L -glutamic acid-based N -carboxyanhydride (CPLG-NCA) and then side-chain modification including nucleophilic substitution of the chloro group followed by copper-mediated 1,3-dipolar cycloaddition and subsequent ion-exchange reaction. Variable-temperature UV–vis spectroscopy revealed that the upper critical solution temperature (UCST)-type cloud point temperature (T cp ) was highly dependent on both polypeptide and PPG chain length as well as polymer concentration. Increasing the polymer chain length or concentration frequently results in T cp increases. Noticeable hysteresis in a cooling/heating cycle was observed for all resulting triblock copolymers owing to a slow disassembly of large aggregates (d = 145 nm) in the heating cycle. Moreover, the resulting UCST triblock copolymers were used to regulate the release property of ciprofloxacin (CIP)-loaded poly(vinyl alcohol) (PVA) hydrogel. The incorporation of PImBF 4 -b-PPG-b-PImBF 4 hampered the burst release of CIP at 37 °C indicating their potential toward sustained release of drug-loaded hydrogels.
研究领域:
材料科学
·
生物医学工程
·
高分子化学
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产品关联
DOI
高影响因子
Soft Matter
·
2015
·Vol. 11
·期 35
·7059-7065
·
IF 4.029
Lei Hou,Peiyi Wu
The UCST-type transition of poly(acrylamide-co-acrylonitrile) (P(AAm-co-AN)) (molar fraction of AN: 13.3%; PDI = 3.2) in H2O and D2O is explored and compared by applying turbidity, DLS as well as FTIR measurements. The transition temperature of P(AAm-co-AN) in D2O is observed to be almost 10 °C higher than that in H2O at the same concentration, demonstrating a dramatic solvent isotope effect. Such a phenomenon could be rooted from a stronger interaction among polymer chains in D2O than in H2O, as indicated from DLS results. It is also observed in second-derivative analysis of FTIR spectra in the ν(CO) region, where all CO groups participate in the formation of inter-/intra-chain hydrogen bonds (CO⋯H–N) in D2O while there is still part of relatively “free” CO groups in H2O. Moreover, we find in the temperature-dependent FTIR spectra that CN groups exhibit hydrating behavior while CO groups present increased inter-/intra-molecular hydrogen bonding interaction (CO⋯H–N) upon cooling, revealing the later process to be the driving force of the UCST-type transition.
研究领域:
高分子化学
·
物理化学
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产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 7
·2738-2746
·
IF 10.182
Feiyun Li,Feiyang Qin,Yuxia Pang,Hongming Lou,Cheng Cai,Weifeng Liu,Yong Qian,Xueqing Qiu
In order to reduce the enzyme cost of lignocellulosic enzymatic hydrolysis, upper critical solution temperature (UCST) additives are used to recover and reuse cellulase by regulating the temperature. A sulfobetaine polymer, PSPE, showed a sensitive UCST response in buffer, and its UCST-performance was optimised by adjusting the molecular weight of the polymer. PSPE-3 (Mw = 355.1 kDa) was added to the cellulase buffer at 50 °C, and PSPE-3 and cellulase were co-precipitated by cooling to the room temperature of 25 °C. PSPE-3 and cellulase co-precipitated mainly through hydrophobic interactions via cooling. Compared with octadecyl sulfobetaine (SB3–18), PSPE-3 had a more sensitive UCST response and stronger cellulase recovery ability. Adding only 40% PSPE-3 (accounting for the mass fraction of cellulase) can save more than 50% cellulase in the enzymatic hydrolysis system of eucalyptus chips pre-treated with dilute acid (Eu-DA). However, for the Eu-DA system, adding 100% SB3–18 can only save about 30% of cellulase. In this work, efficient recycling of cellulase was achieved at room temperature by adding UCST-type PSPE. The process is green without consuming acid and alkali, and this work provides a new idea for reducing the production cost of cellulosic ethanol.
研究领域:
生物化学
·
可再生资源与环境工程
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DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2024
·
IF 5.4
Yuanyuan Wang,Weimin Guan,Yulin Yang,Huiling Lan,Yu Wang,Yun Wang,Juan Han,Lei Wang
Immobilization of enzymes in porous organic framework (POF) materials is popular strategy to stabilize enzymes. For such solid enzyme catalysis system, improving the catalytic efficiency is challenging due to the diffusion resistance from solid-liquid interface and inner pores. Here, UCST-pH dual responsive polymeric carrier (PEG- b -PAAm- b -P(GMA- co -AAc)) was synthesized to immobilize cytochrome c (Cyt c), which impart the reversibly insoluble-soluble property to the immobilized Cyt c. The PEG- b -PAAm- b -P(GMA- co -AAc) could serve as an insoluble-soluble matrix to fast and efficiently immobilize Cyt c via covalent attachment, achieving a remarkable 92 % loading efficiency within just 120 min. The obtained insoluble PEG- b -PAAm- b -P(GMA- co -AAc)-Cyt c micelles exhibited an improvement in thermal, pH stability and reusability. The completely soluble PEG- b -PAAm- b -P(GMA- co -AAc)-Cyt c conjugates accelerated substrate diffusion and then enhanced the catalytic efficiency. These excellent advantages led to low detection limit (1.99 μM), lower than the presently reported biosensors based on enzyme mimics in the colorimetric detection of phenol. This UCST-pH dual responsive window presents a new platform to efficiently control the immobilization and release of enzymes, which will achieve excellent stability and catalytic efficiency.
研究领域:
生物化学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 5
·1039
·
IF 4.2
Zhaohui Chen,Jiacong Wu,Juan Han,Yun Wang,Liang Ni
This paper reports an innovative study that aims to address key issues in the efficient recycling of wastepaper cellulose. The research team utilized the temperature-responsive upper critical solution temperature (UCST) polymer P(NAGA-b-DMA) in combination with the LytA label’s affinity for choline analogs. This innovative approach enabled them to successfully develop a novel soluble immobilized enzyme, P(NAGA-b-DMA)-cellulase. This new enzyme has proven highly effective, significantly enhancing the degradation of wastepaper cellulose while demonstrating exceptional stability. Compared with the traditional insoluble immobilized cellulase, the enzyme showed a significant improvement in the pH, temperature stability, recycling ability, and storage stability. A kinetic parameter calculation showed that the enzymatic effectiveness of the soluble immobilized enzyme was much better than that of the traditional insoluble immobilized cellulase. After the immobilization reaction, the Michaelis constant of the immobilized enzyme was only increased by 11.5%. In the actual wastepaper degradation experiment, the immobilized enzyme was effectively used, and it was found that the degradation efficiency of wastepaper cellulose reached 80% of that observed in laboratory conditions. This novel, thermosensitive soluble immobilized cellulase can efficiently catalyze the conversion of wastepaper cellulose into glucose under suitable conditions, so as to further ferment into environmentally friendly biofuel ethanol, which provides a solution to solve the shortage of raw materials and environmental protection problems in the paper products industry.
研究领域:
生物技术
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Zhaomiao Chu,Chengzhu Yu,Chuang Li
Dynamic phase transitions are important in living organisms for sustaining their adaptive structures and functions. The design of artificial dynamic systems using light as a noninvasive input fuel has gained significant interest to mimic such adaptive features. Here the development of light-fueled dissipative phase transitions of upper critical solution temperature polymers by introducing pendant spiropyrans as photoactive units, is reported. The reversible open-close photoisomerization of spiropyrans is designed to undergo either an enhancement or a decline of their net charge, which is subsequently used to regulate the electrostatic interactions between polymer chains, and ultimately shift their phase transition temperatures to either a lower or a higher direction. The degree and speed of such bidirectional shifting are flexibly modulated by manipulating the external illumination parameters or varying the compositions/concentrations of the polymers. The diametrically opposite transmittance changes driven by light are utilized to produce a series of complementary patterns and shapes for application in transient information storage and encryption with improved accuracy and security. This work offers a bidirectional spatiotemporal modulation of dissipative phase transitions of polymers using visible light that allows highly tunable and adaptable features shared with their natural counterparts.
研究领域:
材料科学
·
高分子化学
·
光学材料
·
信息技术
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yangyang Wang,Shuwen Chen,Ronghao Liu,Lixin Zhang,Wenfeng Xue,Yanzhao Yang
The development of efficient ionic liquids (ILs) for disposable separation and recovery of various precious metals was of great importance, but still faced difficult challenges. A phase change temperature-controlled system composed of IL and HCl solution was developed for the extraction and separation of Au(III), Pd(II) and Pt(IV) from secondary resources. UCST (upper critical solution temperature)-type IL ([1,4,7-TMTA][Tf 2 N]) possessed outstanding selectivity of precious metals and the property of temperature-controlled phase transition. The ability of ILs to form solvated hydrogen bonds was confirmed by quantum-chemical calculation to be correlated with their corresponding UCST. Different experimental parameters were optimized to explore the extraction behavior of IL. It is noteworthy that homogeneous liquid-liquid extraction system (HLLE) constructed by UCST-type IL could significantly enhance the extraction kinetic of Au(III), Pd(II) and Pt(IV) by decreasing phase interface resistance. For Au(III), Pd(II) and Pt(IV), when the system temperatures were higher than 40 °C, 49 °C and 65 °C, the maximum values were 98.5%, 98.3% and 93.2% at the highest efficiency. In addition, the extraction mechanism of anion exchange was revealed by UV–vis, IR, NMR and LC-MS spectrometry. At last, Au(III), Pd(II) and Pt(IV) could be selectively separated from multi-metal solutions where impurity ions coexist by K 2 C 2 O 4 , NH 3 ·H 2 O and CS(NH 2 ) 2 /HCl, respectively. After 5 cycles, the extraction performance of [1,4,7-TMTA][Tf 2 N] maintained. In summary, this paper overcame the obstacle of slow kinetics of solvent extraction technology, and pointed out a way for polymetallic co-extraction and separation in HLLE system.
研究领域:
材料科学
·
环境化学
·
分析化学
·
绿色化学
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产品关联
DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 3
·2288-2299
·
IF 8.897
Du Yan,Liu Di,Sun Mingchen,Shu Gaofeng,Qi Jing,You Yuchan,Xu Yiting,Fan Kai,Xu Xiaoling,Jin Feiyang,Wang Jun,Shen Qiying,Zhu Luwen,Ying Xiaoying,Ji Jiansong,Wu Liming,Liu Daren,Du Yongzhong
Hepatocellular carcinoma (HCC) is a life-threatening disease for which there is no effective treatment currently. Novel theranostics simultaneously having excellent imaging and therapeutic functions are highly desired in cancer therapy. Herein, we develop the sialic acid (SA) modified polymeric micelles at an upper critical solution temperature (UCST) of 43 °C (sialic acid-polyethylene glycol)-poly(acrylamide- co -acrylonitrile), SA-PEG-p(AAm- co -AN)), which further encapsulated with doxorubicin (DOX) and Gd-CuS nanoparticles (Gd-CuS NPs) for chemo-photothermal treatment of HCC guided by magnetic resonance (MR)/photoacoustic (PA) dual-mode imaging. The resultant SA-PEG-p(AAm- co -AN)/DOX/Gd-CuS (SPDG) had an excellent photothermal conversion efficiency, enabling SPDG with an instantaneous release behavior of DOX under near-infrared (NIR) irradiation. This study also revealed that SPDG could actively target to HCC, which was due to that SA had a high affinity with E-selectin overexpressed at the tumor site. Moreover, benefiting from the HCC-targeted ability and NIR light-controlled on-demand delivery of DOX, SPDG showed a superior potential in MR/PA dual-mode imaging-guided chemo-photothermal treatment. Overall, our study reveals that the designed SPDG may be used as an ideal multifunctional nanoplatform for cancer theranostics.
研究领域:
生物医学工程
·
纳米技术
·
癌症治疗
·
分子成像
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Ning Wang,Qi Wang,Yuqi Geng,Xu Sun,Duokun Wu,Yanzhao Yang
Three novel ionic liquids were synthesized. Their binary mixtures with water exhibit tunable thermomorphic behaviors involving monophasic–biphasic transition. Through electrostatic potential maps, we predicted the ability of the three ionic liquids to form solvated hydrogen bonding to estimate the upper critical solution temperature (UCST) ordering of their binary mixture with water. Then, experimental verifications were carried out of the prediction. Three homogeneous liquid–liquid extraction systems were used to extract Au(III) from acidic chloride media based on the thermodynamic property. By comparing the UCST and extraction efficiency of the three systems, the N-carboxymethyl-ethyl-ester-N-methylmorpholinium bis(trifluoromethylsulfonyl)imide ([EtbetmMor][Tf2N]) was selected for subsequent systematic extraction study. High-efficiency extraction and extraordinary selectivity of gold were achieved by optimizing a series of factors affecting the extraction process. The extraction mechanism was confirmed in further. Finally, the extracted gold could be recovered from the ionic liquid phase by precipitation stripping with oxalic acid. The [EtbetmMor][Tf2N] could be regenerated simply by mixing the raffinate containing [Tf2N]− with the [HbetmMor]Cl phase separated with gold after stripping. It is reasonable to think that the environmental friendliness and high efficiency of this new extraction system make it a strong candidate in the field of gold recycling.
研究领域:
化学工程
·
材料科学
·
环境化学
·
分析化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meirong Zhang,Shidong Zou,Dingwen Shi,Qingqing Zhang,Mengqin Guo,Xiangliang Yang,Yanbing Zhao
Transcatheter arterial chemoembolization (TACE) exhibits an important role in the treatment of some solid tumors. However, incomplete embolization and angiogenesis-induced tumor relapse and metastasis remain the biggest challenges for TACE. Here, we synthesized metformin-conjugated poly(N-acryloyl glycinamide) ( p Met) nanogels for precisely synergizing TACE with radiofrequency ablation (RFA) to improve antitumor efficacy. p Met nanogels exhibited RF-heating effect and UCST-type gel-sol phase transition, with high performance of sol syringeability, gel strength and thermal stability. Meanwhile, p Met nanogels showed distinct cytotoxicity and suppression of CD24. By the synergistic efficacy with RF-heating, p Met nanogels exhibited significant tumor regression (0.37 ± 0.5) over 36 d in H22-bearing mice. p Met nanogels further down-regulated the levels of PD-1 and Tim-3 of CD8 + T cells and CD25 and CD38 of CD4 + T cells, suggesting their improvement on tumor immunosuppressive microenvironment. The blood-vessel embolization of p Met nanogels was well validated on rabbit ear vessel model. p Met nanogels provide a new paradigm for constructing RF responsive embolic platform.
研究领域:
肿瘤学
·
生物医学工程
·
药学
✓ 已验证
DOI
高影响因子
PLoS One
·
2023
·Vol. 18
·期 8
·e0290237
·
IF 3.7
Xiaoya Niu,Yi Fu,Lei Feng,Maodi Xie,Bei Li,Lin Que,Zhen You
Recently, bioinspired material such as nanoparticle has been successfully applied in the cancer therapy. However, how to precisely control the drug release from nanomedicine in tumor tissue and overcome the hypoxic microenvironment of tumor tissue is still an important challenge in the development of nanomedicine. In this work, a new type of drug-loaded nanoparticles P(AAm-co-AN)-AuNRs@CeO 2 -DOX (PA-DOX) was prepared by combining high-efficiency photothermal reagents, critical up-conversion temperature polymer layer and anti-cancer drug doxorubicin (DOX) for the treatment of hepatocellular carcinoma (HCC). In this system, CeO 2 can decompose hydrogen peroxide to H 2 O and O 2 alleviate the anaerobic microenvironment of liver cancer cells. As a photothermal reagent, AuNRs@CeO 2 can convert near-infrared light into heat energy to achieve local heat to kill cancer cells and ablate solid tumors. In addition, the elevated temperature would enable the polymer layer to undergo a phase transition to release more DOX to achieve a controlled release mechanism, which will open up a new horizon for clinical cancer treatment.
研究领域:
纳米技术
·
癌症治疗
·
材料科学
·
药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）