ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Tao Yang,Yufei Zhang,Liujia Xu,Hao Zhu,Juntao Zhang,Zheng Guo,Fenghong Huang,Mingming Zheng
Herein, a pH-switchable Pickering interfacial biocatalysis (PIB) system is proposed and applied to a solvent-free biphasic biocatalysis. The oil-in-water emulsion was stabilized by amine-functionalized hollow mesoporous silica nanospheres (HMSS-N), which is functioned as emulsifiers of PIB and carriers of lipase AYS. The smart emulsifiers exhibited switch of the surface wettability behaviors in response to abrupt changes of pH. Under the optimality conditions, the immobilized lipase loading amount, activity, and expressed activity were 174.1 mg g–1, 9073 U g–1, and 52.1 U g–1 protein, respectively, at pH 6. Based on it, the hydrolysis of rice bran oil and esterification with phytosterols to produce phytosterol esters (PEs) were successfully performed. Compared with the conventional free enzyme one-phase system, the PIB system displays a higher reaction efficiency (catalytic efficiency value 6.88 mmol g–1 h–1, 20-fold enhancement). In addition, the system maintains 95% residual activity after 10 reaction cycles with 38.3 g products/g biocatalyst average productivity, complying with the requirements of industry-accepted standards. In each cycle, the demulsification is realized simply by in situ pH regulation. Therefore, this paper provides a powerful and green platform for oil–fat modification and stimuli-responsive interfacial biocatalysis with the advantages of a high efficiency, sustainability, a solvent-free process, and multi-recyclability.
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CORROSION SCIENCE
·
2022
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IF 7.72
Tong Liu,Dawei Zhang,Lingwei Ma,Yao Huang,Xiangping Hao,Herman Terryn,Arjan Mol,Xiaogang Li
Herein, we report the development of a self-sensing and active corrosion protection coating which incorporates pH-sensitive multilayer chitosan/alginate-covered CaCO 3 microcontainers containing 1,10-phenanthrolin-5-amine (APhen). The microcontainers can respond to pH variation to release APhen which serves not only as a corrosion indicator but also as an inhibitor. An epoxy coating doped with 5 wt% microcontainers exhibited improved corrosion performance and was capable of inhibiting corrosion spreading from the damaged area in a 3.5 wt% NaCl solution. The salt spray test showed that corrosion damage can be quickly detected by the appearance of a red color within 2 min.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Nini Luo,Yue Shu,Chuanlong Zhu,Xiaoxue Cheng,Lixue Chen,Jiang Wang,Rui Liu,Huangxian Ju,Wei Cheng,Qianfeng Xia
The abnormal protein phosphorylation is closely related to a series of diseases including cancers, neurodegeneration, and other immune/inflammatory disorders. However, a simple, accurate, and pragmatic methodology for the direct detection of phosphorylation levels of target proteins is largely unavailable. Herein, a surface plasma resonance (SPR) biosensor was developed to detect phosphorylated protein based on significant SPR enhancement using UiO-66 and its high affinity for phosphate residues. Furthermore, the pH of the incubation buffer and the NaOH concentration in the washing solution to eliminate nonspecific adsorption of nanoparticles on the chip surface were optimized to adjust the surface charges of UiO-66. This improved the specificity and sensitivity of the proposed method. The designed biosensor could distinguish 1% phosphorylated peptides from non-phosphorylated peptides background. Moreover, the method could directly analyze the phosphorylation level of target protein in complex samples such as cell or tissue extracts without requiring a purification step in a single workflow. This simple and robust biosensor is a sensitive, accurate, and pragmatic toolbox to detect phosphorylated proteins without destroying the protein structure and can significantly facilitate phosphoproteomics and clinical diagnosis research.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Dan Chang,Zhonghua Zhao,Hu Shi,Jianyang Feng,Yongxing Yang,Lihong Shi
Ratiometric fluorescent probes with wavelength-resolved dual target sensing capacity are highly desirable for the simultaneous recognition of target objects. A novel fluorescent carbon dots (CDs) with a yield of 32% was simply synthesized by hydrothermal treatment of neutral red and urea, resulting in discrete dual-emission bands (440 nm/542 nm) under single-wavelength excitation of 380 nm. It was discovered that the fluorescence (FL) signal of CDs at 440 nm enhances with the addition of L -Lysine, whereas the FL intensity at 542 nm remains invariable. Surprisingly, no significant luminescence response is observed after the addition of D -Lysine, implying that as-prepared CDs can serve as fluorescent nanoprobes for chiral recognition of Lysine. On the contrary, it was discovered that the FL band at 542 nm is highly sensitive to pH in linear ranges of 2.0–3.4 and 3.4–8.0, while the FL band at 440 nm is inert to it, providing an effective tool for the ratiometric detection of pH in a “turn-on” mode. Confocal imaging experiments further verify that this nanoprobe can monitor L -Lysine and pH fluctuations in biological systems in real time using ratiometric methods. We believe that our research will provide new insight into the suitable construction of prompt and straightforward ratiometric fluorescent probes for the simultaneous differentiation of two analytes .
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Theranostics
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2022
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IF 11.6
Huang Yang,Yuan Ding,Zongrui Tong,Xiaohui Qian,Hao Xu,Fenghao Lin,Guoping Sheng,Liangjie Hong,Weilin Wang,Zhengwei Mao
Background: Despite their outstanding properties in high surface-to-volume ratio and deep penetration, the application of ultrasmall nanoparticles for tumor theranostics remains limited because of their dissatisfied targeting performance and short blood circulation lifetime. Various synthetic materials with complex structures have been prepared as a multifunctional platform for loading ultrasmall nanoparticles. However, their use in nanomedicine is restricted because of unknown metabolic processes and potential physiological toxicity. Therefore, versatile and biocompatible nanoplatforms need to be designed through a simple yet effective method for realizing specific delivery and responsible release of ultrasmall nanoparticles. Methods: Iron-gallic acid coordination polymer nanodots (FeCNDs) exhibits outstanding photothermal ability and Fenton catalytic performance, which can be applied for tumor inhibition via hyperthermia and reactive oxygen species. A pH-responsive platelet-based hybrid membrane (pH-HCM) was prepared via co-extrusion and acted as a safe nanoplatform to load FeCNDs (pH-HCM@FeCNDs). Subsequently, their responsive performance and penetration ability were valued considering the multicellular sphere (MCS) model in an acidic or neutral environment. Thereafter, in vivo fluorescence image was performed to assess targeting capability of pH-HCM@FeCNDs. Finally, the corresponding antitumor and antimetastatic effects on orthotropic breast cancer were investigated. Results: In 4T1 MCS model, pH-HCM@FeCNDs group exhibited higher penetration efficiency (72.84%) than its non-responsive counterparts (17.77%) under an acidic environment. Moreover, the fluorescence intensity in pH-HCM@FeCNDs group was 3.18 times higher than that in group without targeting performance in the in vivo fluorescence image experiment. Finally, through in vivo experiments, pH-HCM@FeCNDs was confirmed to exhibit the best antitumor effect (90.33% tumor reduction) and antimetastatic effects (only 0.29% tumor coverage) on orthotropic breast cancer. Conclusions: Hybrid cell membrane was an ideal nanoplatform to deliver nanodots because of its good responsibility, satisfactory targeting ability, and excellent biocompatibility. Consequently, this study provides novel insights into the delivery and release of nanodots in a simple but effect method.
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高影响因子
Acta Pharmaceutica Sinica B
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2022
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IF 14.903
Lujing Geng,Tong Lu,Huaqing Jing,Yue Zhou,Xiaoyang Liang,Jiao Li,Nan Li
Ferroptosis (FPT), a novel form of programmed cell death, is characterized by overwhelming iron/reactive oxygen species (ROS)-dependent accumulation of lipid peroxidation (LPO). However, the insufficiency of endogenous iron and ROS level limited the FPT therapeutic efficacy to a large extent. To overcome this obstacle, the bromodomain-containing protein 4 (BRD 4 )-inhibitor (+)-JQ1 (JQ1) and iron-supplement ferric ammonium citrate (FAC)-loaded gold nanorods (GNRs) are encapsulated into the zeolitic imidazolate framework-8 (ZIF-8) to form matchbox-like [email protected] /ZIF-8 for the amplified FPT therapy. The existence of matchbox (ZIF-8) is stable in physiologically neutral conditions but degradable in acidic environment, which could prevent the loaded agents from prematurely reacting. Moreover, GNRs as the drug-carriers induce the photothermal therapy (PTT) effect under the irradiation of near-infrared II (NIR-II) light owing to the absorption by localized surface plasmon resonance (LSPR), while the hyperthermia also boosts the JQ1 and FAC releasing in the tumor microenvironment (TME). On one hand, the FAC-induced Fenton/Fenton-like reactions in TME can simultaneously generate iron (Fe 3+ /Fe 2+ ) and ROS to initiate the FPT treatment by LPO elevation. On the other hand, JQ1 as a small molecule inhibitor of BRD 4 protein can amplify FPT through downregulating the expression of glutathione peroxidase 4 (GPX4), thus inhibiting the ROS elimination and leading to the LPO accumulation. Both in vitro and in vivo studies reveal that this pH-sensitive nano-matchbox achieves obvious suppression of tumor growth with good biosafety and biocompatibility. As a result, our study points out a PTT combined iron-based/BRD 4 -downregulated strategy for amplified ferrotherapy which also opens the door of future exploitation of ferrotherapy systems.
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TALANTA
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2022
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IF 6.556
Xiaoqing Cui,Yu Bao,Tingting Han,Zhenbang Liu,Yingming Ma,Zhonghui Sun
Here, we developed a wearable electrochemical sensor for pH and K + monitoring in sweat. The sensor was composed of flexible reference electrode, pH response electrode and K + selective electrode, which were prepared through printing β-CD functionalized graphene (β-CD/RGO) water suspension on conductive PET substrate with microelectronic printer. β-CD/RGO not only served as the pH sensitive material for pH response electrode with good sensitivity, selectivity and reproducibility due to its abundant oxygen-containing functional groups, but also worked as the ion-to-electron transducer for K + selective electrode with good sensitivity. The wearable sensor exhibited good potential stability at different bending states. On-body sweat pH and K + measurements showed high accuracy compared with ex-situ analysis.
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CHEMOSPHERE
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2022
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IF 8.943
Guohua Li,Xianjin Qi,Nina Yang,Xiaoxu Duan,Aimin Zhang
Molecular sieves have also been used for arsenic adsorption in recent years because of their special structure. In order to solve the problem of arsenic pollution in drinking water and/or industrial wastewater , ZSM-5/Fe adsorbent was prepared by loading iron on ZSM-5 molecular sieve. It is also used as an excellent adsorbent for removing arsenic and other heavy metal ions from industrial wastewater. At room temperature, the concentration of arsenic was reduced from 100 mg/L to 0.006 mg/L after the solution pH was adjusted to the range of weak acid to weak base (4–10) and 0.5 g of ZSM-5/Fe adsorbent was added for reacting 2 h. The adsorption capacity reached 40.00 mg/g, the adsorption efficiency reached 99.99%, reaching the national standard of drinking water. Adsorption thermodynamics, kinetics and isotherms showed that the adsorption mechanism of arsenic is heterogeneous nucleation adsorption (including electrostatic attraction and chemical precipitation). Moreover, ZSM-5/Fe adsorbent can adjust pH spontaneously by using non-skeleton Si–Al phase to achieve effective adsorption from weak acid to weak base. At the same time, ZSM-5/Fe adsorbent showed good reusability and stability in five cycles. This study provides an important idea for the application of ZSM-5 molecular sieve in many fields and the efficient removal of arsenic from drinking water and industrial wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Gang Peng,Mingxue Xiang,Wenzhe Wang,Zilin Su,Huilin Liu,Yuting Mao,Yu Chen,Ping Zhang
Microplastics (MPs) elimination is becoming an intractable environmental issue due to their nonbiodegradable nature and wide spreading，especially in the case of wastewater containing acid or alkaline effluent. To target the dilemma, this work rationally engineered a robust three-dimensional graphene-like carbon assembled layered double oxide material (defined as G@LDO) from hierarchical organic LDH ( i.e. , 3D OLDH) via a “precursor-calcination” strategy. In virtue of the mutually protection effect of graphene-like carbon (G) and LDO, the engineered G@LDO featured the preeminent acid and base resistance for polystyrene (PS, as representative of MPs) removal. Especially and importantly, the removal efficiency of PS was ≥ 80% at pH= 3–11, even nearly 60% PS was removed at pH= 1 and 13. The maximum adsorption ability of G@LDO for PS was estimated to be 209.39 mg/g by a Langmuir isotherm model, much superior to that of pure G, LDO, and 2D G@LDO. Furthermore, the removal pathway was analyzed by kinetic together with thermodynamic study, revealing that the PS removal on G@LDO was an exothermic reaction controlled by chemisorption . By systematical characterization and DFT calculation , the removal mechanism of PS was revealed to be hydrogen bond and complexation associated with LDH recovered from LDO and π-π conjunction from G. Notably, the existence of sulfure (S) in the carbon network was also identified as significant component in PS removal via p-π interaction. Overall, this work not only provides a effective candidate for microplastics removal in a wide applicable scope (especially acid/alkaline effluent), shedding light on environmental remediation, but also opens a new anvenue for the disposal of LDHs adsorbed organic in a high value-added manner.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xuzhuo Sun,Wenhui Li,Jing Chen,Xinli Yang,Baofan Wu,Zhengxi Wang,Bo Li,Haibo Zhang
As a promising dopant , electron deficient B atom not only tunes the electronic structure of electrocatalysts for improving their intrinsic catalytic activities, but also combines with hydroxy radical as strong adsorption sites for accelerating the water dissociation during the hydrogen evolution reaction (HER). In this paper, we report an electrocatalyst based on boron-modified Ru anchored on carbon nanotubes (B-Ru@CNT) that shows impressive HER activity in acidic and alkaline media. The boron-rich closo -[B 12 H 12 ] 2- borane was selected as a moderately strong reductant for the in situ reduction of a Ru salt, which yielded B-doped Ru nanoparticles . The experimental and theoretical results indicate that the incorporation of B not only weakens the Ru-H bond and downshifts the d-bond centre of Ru from the Fermi level by reducing the electron density at Ru but also accelerates the water dissociation reaction by providing B sites, which strongly adsorb OH* intermediates, and nearby Ru sites, which act as sites for the adsorption of the H* intermediate, thus boosting the HER performance and enhancing the HER kinetics. As a result of the tuning of the electronic structure via B doping, B-Ru@CNT showed excellent HER performance, yielding overpotentials of 17 and 62 mV at a current density of 10 mA cm −2 in alkaline and acidic solutions, respectively. These results indicate that our synthetic method is a promising route to B-doped metallic Ru with enhanced pH-independent HER performance.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jie Bai,Jie Wang,Yecheng Feng,Yongfang Yao,Xubo Zhao
Polymeric micelles from block copolymers have gained increasing attention in cancer drug delivery. However, the fabrication of polymeric micelles that are stable in biological fluids and unstable at tumor sites remains a principal challenge. To achieve the tunable stability for the polymeric micelles, Zn coordination-induced core-crosslinked polymeric micelles have been proposed and confirmed. Herein, a block copolymer bearing imidazole pendants is synthesized which is capable of self-assembling into polymeric micelles in water. After core-crosslinking, it can be found that the critical micelle concentration (CMC) of the core-crosslinked polymeric micelles is significantly lower than that of non-crosslinked polymeric micelles. Particularly, the drug-loaded core-crosslinked polymeric micelles are fragile and easily affected by the slightly acidic environments, which makes it possible to turn the polymeric micelles back to hydrophilic polymers and therefore disassemble micelles to unload cargoes. The drug-loaded core-crosslinked polymeric micelles display adequate toxicity as a result of their low IC 50 value of 3.713 ± 0.166 μg/mL. Collectively, Zn coordination-induced core-crosslinked polymeric micelles offer a design idea for practicable drug delivery system in cancer therapy.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 21
·2112717
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IF 19.924
Yi-Ming Zhao,Lin Cheng,Kai-Yao Wang,Xin Hao,Juan Wang,Jia-Ying Zhu,Meng Sun,Cheng Wang
Switchable coadsorption and separation for elimination/partitioning of Cs + and Sr 2+ is achieved by pH-controlled ion exchange using a potassium thioantimonate K 2 Sb 4 S 7 ·2H 2 O ( SbS-1K ) with fantastic pH durability from diluted NaOH (pH 12) to concentrated HCl (3 m ). At pH 6, SbS-1K exhibits ultrafast adsorption kinetics ( R ≈ 90% in 2 min for Cs + and 20 min for Sr 2+ ) and high removal rates ( R ≈ 98–99%) at equilibrium for both Cs + and Sr 2+ . At pH 2, the Sr 2+ adsorption is inhibited by H + with a great loss in R Sr to 11.18%, whereas the R Cs remains at 96.99%, contributing to a top-ranked separation factor SF Cs/Sr of 256. The SbS-1K -filled ion exchange column can be switched between the eliminating ( R Cs > 99.91%; R Sr > 98.19%) and separating ( R Cs > 98.99%; R Sr ≈ 0±3%) modes for treating continuous flow with a variation from pH 6 to pH 2 or vice versa. The SbS-1K /PTFE membrane exhibits coadsorption and separation effects for filtration of low concentrated mixed Cs + and Sr 2+ solution (1 ppm for each), even at an ultrafast vacuum filtration speed (30 mL min –1 ). Combined with easy synthesis and high β/γ irradiation resistance, SbS-1K represents a new-concept bifunctional exchanger with discriminating intelligence for equipment innovation.
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