ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Ziyang Huang,Siyi Zou,Guozhen Liu
It is a long-lasting research topic to avoid the formation of oxidation layers on gallium-based liquid metals. This study has developed a simple general method for modification of the eutectic gallium–indium (EGaIn) surface with p-aniline derivatives to introduce a monolayer of organic molecules with versatile functional groups. The binding affinity of carboxylic acid groups, amine groups, or thiol groups with EGaIn is in the order SH > NH2 > COOH. For the first time, it is evidenced that both NH2 and SH groups can coexist on the EGaIn nanoparticle surface with the binding affinities of 30 and 70%, respectively. The formation of these organic molecules on the EGaIn surface antioxidizes and thus stabilizes the EGaIn nanoparticles, while increasing the conductivity of EGaIn significantly. The resulting EGaIn nanoparticles have very good distribution in both ethanol and aqueous solutions and rich surface chemistry, making them suitable for the following attachment of biomolecules such as aptamers, antibodies, or enzymes for biomedical applications. As an example, the EGaIn surface is successfully modified with p-aminobenzoic acid followed by the attachment of an insulin aptamer, which can be used for the electrochemical detection of insulin with the lowest detectable concentration limit of 1 pM. This study reveals the modification of EGaIn nanoparticles with p-aniline derivatives with versatile functional groups to antioxidize EGaIn in a biological environment, opening a door for gallium-based liquid metals toward biomedical applications.
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 9
·3016
·
IF 4.927
Fangjun Liu,Dun Wang,Jiaqi Wang,Liwei Ma,Cuiyun Yu,Hua Wei
Bottlebrush copolymers with different chemical structures and compositions as well as diverse architectures represent an important kind of material for various applications, such as biomedical devices. To our knowledge, zwitterionic conjugated bottlebrush copolymers integrating fluorescence imaging and tumor microenvironment-specific responsiveness for efficient intracellular drug release have been rarely reported, likely because of the lack of an efficient synthetic approach. For this purpose, in this study, we reported the successful preparation of well-defined theranostic zwitterionic bottlebrush copolymers with unique brush-on-brush architecture. Specifically, the bottlebrush copolymers were composed of a fluorescent backbone of polyfluorene derivate (PFONPN) possessing the fluorescence resonance energy transfer with doxorubicin (DOX), primary brushes of poly(2-hydroxyethyl methacrylate) (PHEMA), and secondary graft brushes of an enzyme-degradable polytyrosine (PTyr) block as well as a zwitterionic poly(oligo (ethylene glycol) monomethyl ether methacrylate-co-sulfobetaine methacrylate) (P(OEGMA-co-SBMA)) chain with super hydrophilicity and highly antifouling ability via elegant integration of Suzuki coupling, NCA ROP and ATRP techniques. Notably, the resulting bottlebrush copolymer, PFONPN9-g-(PHEMA15-g-(PTyr16-b-P(OEGMA6-co-SBMA6)2)) (P2) with a lower MW ratio of the hydrophobic side chains of PTyr and hydrophilic side chains of P(OEGMA-co-SBMA) could self-assemble into stabilized unimolecular micelles in an aqueous phase. The resulting unimolecular micelles showed a fluorescence quantum yield of 3.9% that is mainly affected by the pendant phenol groups of PTyr side chains and a drug-loading content (DLC) of approximately 15.4% and entrapment efficiency (EE) of 90.6% for DOX, higher than the other micelle analogs, because of the efficient supramolecular interactions of π–π stacking between the PTyr blocks and drug molecules, as well as the moderate hydrophilic chain length. The fluorescence of the PFONPN backbone enables fluorescence resonance energy transfer (FRET) with DOX and visualization of intracellular trafficking of the theranostic micelles. Most importantly, the drug-loaded micelles showed accelerated drug release in the presence of proteinase K because of the enzyme-triggered degradation of PTyr blocks and subsequent deshielding of P(OEGMA-co-SBMA) corona for micelle destruction. Taken together, we developed an efficient approach for the synthesis of enzyme-responsive theranostic zwitterionic conjugated bottlebrush copolymers with a brush-on-brush architecture, and the resulting theranostic micelles with high DLC and tumor microenvironment-specific responsiveness represent a novel nanoplatform for simultaneous cell image and drug delivery.Keywords:brush-on-brush;zwitterionic;enzyme-responsive;theranostic;FRET
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Lijing Zhang,Jiaqi Han,Yuchao Wang,Wenbo Yang,Shengyang Tao
Achieving a room-temperature Suzuki–Miyaura coupling (SMC) with high efficiency is of great significance to the development of low-carbon organic synthesis. Nevertheless, it is still a great challenge to construct a promising nanocatalyst with high activity for room-temperature SMC reaction. In this paper, a strong alkaline-supported nanocatalyst Pd/Mg(OH)2/MgO–ZrO2 was rationally developed based on MgO–ZrO2 hybrid nanofibers. Physicochemical characterizations present that the in situ conversion of MgO to Mg(OH)2 on the surface of the nanofibers results in a great increase in surface alkalinity of the carrier. The strong alkalinity can greatly accelerate the oxidation addition and transmetalation of the SMC process, resulting in the obvious reduction of activation energy of the reaction (Ea = 9.0 kJmol–1 for Ph–Br). The coupling conversion can reach up to 100% at room temperature within 8 min with a maximum TOF > 6516 h–1. It also shows an excellent performance in substrate applicability and chlorobenzene activation. The rational design of a high-basicity catalyst for room-temperature SMC will be a rewarding attempt for the development of low-carbon green organic synthesis.
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高影响因子
Small
·
2023
·
IF 13.3
Ziyang Huang,Mingyang Guan,Ziting Bao,Fengyi Dong,Xiaolin Cui,Guozhen Liu
Gallium-based liquid metal systems hold vast potential in materials science. However, maximizing their possibilities is hindered by gallium's native oxide and interfacial functionalization. In this study, small-molecule ligands are adopted as surfactants to modify the surface of eutectic gallium indium (EGaIn) nanoparticles and suppress oxidation. Different p -aniline derivatives are explored. Next, the reduction of chloroanric acid (HAuCl 4 ) onto these p -aniline ligand modified EGaIn nanoparticles is investigated to produce gold-decorated EGaIn nanosystems. It is found that by altering the concentrations of HAuCl 4 or the p -aniline ligand, the formation of gold nanoparticles (AuNPs) on EGaIn can be manipulated. The reduction of interfacial oxidation and presence of AuNPs enhances electrical conductivity, plasmonic performance, wettability, stability, and photothermal performance of all the p -aniline derivative modified EGaIn. Of these, EGaIn nanoparticles covered with the ligand of p -aminobenzoic acid offer the most evenly distributed AuNPs decoration and perfect elimination of gallium oxides, resulting in the augmented electrical conductivity, and highest wettability suitable for patterning, enhanced aqueous stability, and favorable photothermal properties. The proof-of-concept application in photothermal therapy of cancer cells demonstrates significantly enhanced photothermal conversion performance along with good biocompatibility. Due to such unique characteristics, the developed gold-decorated EGaIn nanodroplets are expected to offer significant potential in precise medicine.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 41
·10666-10676
·
IF 5.236
Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao
Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Yuzhu Li,Jiajun Yang,Lai Xie,Yu Li,Xiwen Liang,Xubing Lu,Xingsen Gao,Jinwei Gao,Lingling Shui,Sujuan Wu,Jun-Ming Liu
In this work, 4-bromoaniline (BrAL) is employed to modify the CsPbI2Br/carbon electrode interface to passivate defects of all-inorganic CsPbI2Br perovskite solar cells (PSCs). The effects of BrAL modification on the structure, light absorption, and trap-state density (Ntrap) of CsPbI2Br films and the carrier recombination process, photoelectrical characteristics, and air stability of the PSCs are systematically studied. The results show that the hydrophobic BrAL interlayer modification can lead to a better matched energy-level alignment, reduce the Ntrap to construct uniform CsPbI2Br films, and suppress carrier recombination to promote charge transport and collection. Thus, the modified PSC achieves a higher power conversion efficiency (PCE) of 11.34% with less hysteresis (reference-PSC, 9.50%) and better stability in ambient air. The BrAL passivation provides a good strategy to enhance the photoelectrical performance and air stability of all-inorganic PSCs.
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2020
·
IF 4.192
Shichao Xu,Xiaojing Zeng,Songlin Dai,Jing Wang,Yuxiang Chen,Jie Song,Yunfei Shi,Xian Cheng,Shengliang Liao,Zhendong Zhao
In this study, we will report on the synthesis and application of efficient botanical agrochemicals from turpentine for sustainable crop protection. Two series of turpentine derived secondary amines were synthesized and identified by FT-IR, 1H NMR, 13C NMR, and HRMS. The herbicidal activities against Echinochloa crus-galli were evaluated. The potential toxicity of the synthesized compounds was tested by MTT cytotoxicity analysis. The effect of structure of the synthesized secondary amines and corresponding Schiff base compounds on their activities was investigated by quantitative structure–activity relationship (QSAR) study. All target products were found to be low toxicity, with similar or higher herbicidal activities than commercial herbicides diuron and Glyphosate. Results of QSAR study showed that a best four-descriptor QSAR model with R2 of 0.880 and Rloo2 of 0.818 was obtained. The four descriptors most relevant to the herbicidal activities are the min valency of a N atom, the max total interaction for a C−H bond, the relative number of aromatic bonds, and the min partial charge (Qmin).
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高影响因子
Catalysts
·
2020
·Vol. 10
·期 4
·432
·
IF 3.52
Li-Hua Du,Rui-Jie Long,Miao Xue,Ping-Feng Chen,Meng-Jie Yang,Xi-Ping Luo
A continuous-flow procedure for the synthesis of β-amino acid esters has been developed via lipase-catalyzed Michael reaction of various aromatic amines with acrylates. Lipase TL IM fromThermomyces lanuginosuswas first used to catalyze Michael addition reaction of aromatic amines. Compared with other methods, the salient features of this work include green reaction conditions (methanol as reaction medium), short residence time (30 min), readily available catalyst and a reaction process that is easy to control. This enzymatic synthesis of β-amino acid esters performed in continuous-flow microreactors is an innovation that provides a new strategy for the fast biotransformation of β-amino acid esters.Keywords:enzymatic synthesis;β-amino acid esters;microreactor;aromatic amines;Michael addition
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2021
·
IF 3.196
Chenglu Zhang,Lu Zhang,Yuqing Li,Zhixuan Ren,Lu Li,Yanpeng Zhang,Yizheng Li,Cui Liu
A novel 1,8 - naphthalimide - ebselen fluorescent probe BPHN was synthesized. BPHN has great fluorescence properties: high quantum yield (0.5932), large Stokes shift (125 nm) and remarkable stability at wide pH range (5–11). The results of fluorescence spectroscopy experiments show that BPHN can recognize H 2 S selectively and sensitively. BPHN exhibits low LOD (0.129 μM) and fast response (90 s). The potential of BPHN as a biosensor for H 2 S was demonstrated by imaging of exogenous H 2 S in living cells. BPHN can also detect H 2 S qualitatively and quantitatively in actual water samples.
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高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2019
·Vol. 220
·期 9
·1800553
·
IF 2.622
Da Xu,Yanwei Gao,Yang Sun,Zhaoyang Wang,Zhenhua Jiang,Xiangyu Jiang,Haibo Zhang
Polyaryletherketones (PAEKs) with pendant pyrene groups are prepared and used to functionalize and disperse graphene nanoplates (GNPs). A variety of polymers with a range of pyrene contents are studied. A monomer with pyrene and two hydroxyl groups is designed and synthesized through the Suzuki reaction and used to prepare a series of pyrene-functioned PAEKs (Py-PAEKs) by copolymerization. Experiments demonstrate that Py-PAEKs have not only excellent solubility, but also excellent mechanical properties and outstanding heat resistance. In the same treatment condition, the concentration of GNPs that are modified by Py-PAEK with 40 molar percentage of pyrene (Py-40) increases 88 times of the concentration of pure GNPs in NMP. In addition, adding 0.5% GNPs, which is functionalized by Py-40 to PEEK resin, improves the flexural strength of polymer composite nearly 12% and while the tensile strength of these composites improves nearly 10% with a doubling of the strain at break.
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高影响因子
CARBON
·
2019
·
IF 7.466
Chungui Cheng,Pan Jia,Linhong Xiao,Jianxin Geng
Scalable and sustainable preparation of graphene is urgently needed to address its increasing demands in basic research and practical applications. Here, we present a simple preparation of surface-functionalized graphene by ball milling graphite in the presence of an aryl diazonium salt. The efficient exfoliation of graphite is achieved through the tandem surface reaction of graphite with aryl diazonium salt and mechanical shear by ball milling. Moreover, the surface functionalities of the resultant graphene platelets are readily tuned using various aryl diazonium salts, which also provide routes for the further modification of the graphene platelets. More importantly, with 93% of the graphene platelets having layers less than 5, they contain a low quantity of structural defects (I D /I G ratio = 0.30) and a low oxygen content (10.1 atom%). Such features not only facilitate the restoration of the π-conjugated structure of graphene by thermal reduction, with the I D /I G ratio reduced to 0.11 comparable to the value of graphite, but also enhance the structural stability of the graphene platelets at low temperature. This method is ideal for scaling up, since the techniques used are industrially compatible, the chemicals employed are commercially available, and no highly polluting wastes are produced in the synthesis.
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高影响因子
MACROMOLECULES
·
2019
·
IF 5.997
Chao Qian,Runxin Bei,Tianwen Zhu,Weiwen Zheng,Siwei Liu,Zhenguo Chi,Matthew. P. Aldred,Xudong Chen,Yi Zhang,Jiarui Xu
An original design strategy for the preparation of polymers with a low dielectric constant is presented. The key to this design strategy is taking the most advantage of the secondary relaxation behavior of the polymer chains to obtain more free volume in the bulk, which can effectively reduce the dielectric constant of the polymer. By using this design strategy, we have successfully synthesized a novel polyimide TmBPHF with a pendant group that consists of a biphenyl unit attached to the meta-position of a phenyl ring that is part of a triaryl unit. The intrinsic k and dielectric loss values of the TmBPHF are 2.09 and 0.0012 at 10 kHz, respectively. More importantly, such outstanding low-k performance remains stable up to 300 °C. The excellent low-k performance of TmBPHF is mainly due to the secondary relaxation, especially the β relaxation, which occurs from the rotation of the pendant group. The TmBPHF film shows an ultralow moisture rate (∼0.17%), which is able to maintain the low-k property stability in different humid environments. Meanwhile, the TmBPHF film also shows excellent thermal stability and excellent mechanical properties, with a glass transition temperature (Tg) of 302 °C, 5 wt % decomposition temperature (Td5%) of 549 °C, and residual of 70% at 800 °C under N2. The tensile strength and tensile modulus of the polyimide film are equal to 85.8 MPa and 2.02 GPa, respectively. In addition, the TmBPHF film is soluble in common solvents, which allows simple solution processing and efficient, low-cost, and continuous roll-to-roll processes. The design strategy is beneficial for lowering the k value and simultaneously maintaining the overall properties of polyimides, which possibly could also be extended to other novel high-performance polymer systems.
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