Polymers
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2022
·Vol. 14
·期 3
·406
·
IF 4.967
Xiao Wang,Xianghong Zheng,Xinyu Liu,Birong Zeng,Yiting Xu,Conghui Yuan,Lizong Dai
Due to unique chelating and macrocyclic effects, crown ether compounds exhibit wide application prospects. They could be introduced into amphiphilic copolymers to provide new trigger mode for drug delivery. In this work, new amphiphilic random polymers of poly(lipoic acid-methacrylate-co-poly(ethylene glycol) methyl ether methacrylate-co-N-isopropylacrylamide-co-benzo-18-crown-6-methacrylamide (abbrev. PLENB) containing a crown ether ring and disulphide bond were synthesized via RAFT polymerization. Using the solvent evaporation method, the PLENB micelles were formed and then used to load substances, such as doxorubicin hydrochloride (DOX) and gold nanoparticles. The results showed that PLENB exhibited a variety of lowest critical solution temperature (LCST) in response to the presence of different ions, such as K+, Na+and Mg2+. In particular, the addition of 150 mM K+increased the LCST of PLENB from 31 to 37 °C and induced the release of DOX from the PLENB@DOX assemblies with a release rate of 99.84% within 12 h under 37 °C. However, Na+and Mg2+ions could not initiate the same response. Furthermore, K+ions drove the disassembly of gold aggregates from the PLENB-SH@Au assemblies to achieve the transport of Au NPs, which is helpful to construct a K+-triggered carrier system.Keywords:crown ether;amphiphilic copolymers;K+-triggered;Au NPs;disassembly
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ANALYTICA CHIMICA ACTA
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2022
·
IF 6.911
Yu Du,Siqi Yu,Huangxian Ju
A quenching-typed electrochemiluminescence (ECL) immunosensing method was proposed for protein detection by the redox reaction of tungsten-based polyoxometalate nanoclusters (W-POM NCs) with free radical (O 2 •– ) as the intermediate of co-reactant H 2 O 2 . The immunosensor was constructed by co-immobilizing luminol loaded CeVO 4 /Au nanohybrids and capture antibody on an indium tin oxide electrode, which showed strong ECL emission in the presence of H 2 O 2 due to the catalysis of CeVO 4 /Au toward its electro-oxidation to produce O 2 •– via the reversible conversion between Ce 3+ and Ce 4+ . The W-POM NCs were encapsulated in the uniformly sized amino-silica nanosphere (SiO 2 ) to act as a label ( [email protected] 2 ) of the secondary antibody. Upon the sandwich-typed immunoreactions with the target, the W-POM NCs were introduced onto the immunosensor surface to reduce O 2 •– , and thus quenched the ECL emission of luminol-H 2 O 2 system. Using neuron-specific enolase (NSE) as a target, the proposed method showed a detection limit of 0.19 pg/mL and detectable range of 0.5 pg/mL to 18 ng/mL. The excellent performance of the proposed “ON-OFF” strategy demonstrated that the W-based quenching offers an effective tag for immunoassay of protein biomarkers.
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LANGMUIR
·
2022
·
IF 4.331
Qiangtao Zhu,Dongyu Pan,Yangyi Sun,Dongming Qi
Hollow structures in TiO2 materials can enhance the photocatalytic properties by reducing the diffusion length and improving the accessibility of active sites for the reactants. However, existing approaches for preparing hollow TiO2 materials have two drawbacks that restrict their engineering applicability: first, a heavy reliance on templates to form a hollow structure, which makes the preparation laborious, complicated, and costly; second, difficult-to-achieve high crystallization while maintaining the small grain size in calcinated TiO2, which is crucial for enhancing photocatalytic activity. Herein, a simple, effective method is proposed that not only enables the preparation of hybrid TiO2–SiO2 hollow spheres without the template fabrication and removal process via microemulsion technology but also achieves both high crystallization and a small grain size in calcinated TiO2 at once through the calcination of amorphous TiO2 with organosilane at a high temperature of 850 °C. The prepared TiO2–SiO2 hollow spheres with tunable sizes demonstrate high photocatalytic activity with a maximum k value of 133.74 × 10–3 min–1, which is superior to commercial photocatalyst P25 (k = 114.97 × 10–3 min–1). In addition, Au can be doped in the hybrid TiO2–SiO2 shell to gain Au-doped hollow spheres that show a high k value of up to 694.14 × 10–3 min–1, which is 6 times larger than that of P25 and much better than that reported in the literature. This study not only provides an effective approach to stabilize and tune the grain growth of the TiO2 photocatalyst during calcination but also enables the simple preparation of hollow TiO2-based materials with controllable hollow nanostructures.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 16
·7385-7394
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IF 3.925
Xia Xu,Meirong Fu,Min Yang,Bing Hu,Jitao Yang,Wenjun Gui,Jinxiu Guo
4-Nitrophenol (4-NP) is one of the main toxic water pollution substances. Most 4-NP fluorescence detection methods are based on the change in the fluorescence intensity of a single emission peak, which has low sensitivity, accuracy, and narrow analytical ranges. Herein, NaYF4:Yb3+(58%),Tm3+@NaYF4@Au were designed and synthesized for the quantitative detection of 4-NP due to the fluorescence intensity ratio of two upconversion emission peaks, the analytical range is 0.01–100 μg mL−1 and the detection limit is 0.01 μg mL−1. In addition, 1.66 nm Au nanoparticles randomly distributed on the surface of composite nanomaterials can effectively cause the catalytic reduction of 4-NP. Therefore, NaYF4:Yb3+(58%),Tm3+@NaYF4@Au is a type of composite nanomaterial with great development potential and application prospects in the detection and catalysis of 4-NP.
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Journal of Materials Chemistry B
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2022
·Vol. 10
·期 12
·2028-2037
·
IF 7.571
Chen Yang,Wenli Jiang,Yongqi Yu,Hui Zhang,Chenxin Cai,Qingming Shen
The integration of photothermal therapy (PTT) and photodynamic therapy (PDT) has become a promising cancer treatment method. Herein, anisotropic metal hetero-nanostructure Pd-tipped Au nanorods (PTA NRs) were fabricated, which exhibit plasmon-enhanced photothermal performance under near-infrared laser irradiation. Due to their anisotropic nanostructure, PTA NRs promote the generation of energetic hot electrons and prolong the separation time of electrons and holes. The hot electrons could generate heat energy through the electron–phonon relaxation process and produce reactive oxygen species through energy and electron transformation processes. Because of their high NIR absorption cross-section, as well as good photostability, PTA NRs can be used for NIR-activated photoacoustic imaging-guided PTT-PDT combination cancer therapy. Experiments in tumor-bearing mice proved that PTA NRs exhibit excellent anti-tumor effects, with little side effects on normal organs, making them promising for NIR cancer phototherapy.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
De Ping Chen,Lei Yuan,Meng Jue Li,Wen Jing Han,Xu Dong Liu,Xi Chuan Liu,Chao Yang Wang
Pd is a highly active non-Pt anode in direct ethanol fuel cells, and its morphology and structural composition heavily influence its electrocatalytic efficiency. In this study, three-dimensional (3D)-hollow Au microspheres (HNPs-Au) as a support for the Pd monolayer (HNPs-Au@Pd) were synthesized using a simple template method and galvanic replacement reaction. The experimental results and theoretical calculations show that the presence of HNPs-Au enhances the catalytic activity of ethanol oxidation in alkaline media, improving the electroactivity of metallic Pd. Benefiting from the 3D-hollow-porous structure and the significant synergistic impact between Au and Pd (balancing the adsorption energy of the intermediate and reactant molecules), HNPs-Au@Pd achieves a 10.8-fold mass activity and a 3.3-fold enhancement of the specific activity for the ethanol oxidation reaction when compared to commercial Pd/C. The present work not only enriches the preparation strategy of porous metal materials but also opens up a sector for the construction of anodic electrocatalysts with a wide range of applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Qiang Huang,Jiayu Yang,Fei Qi,Wenxia Zhang,Nan Zhang,Zhiyu Liang,Jiaxin Liu,Changqing Tian,Xiaosheng Tang,Daofu Wu,Benjun Huo
Photocatalytic conversion of CO 2 to value-added chemicals and fuels is a green and sustainable approach to solve the problems of CO 2 concentration increment and fossil fuels shortage. Employing photocatalysts with high catalytic activity and selectivity to realize CO 2 conversion has attracted extensive attention. However, the efficiency of photocatalysts is still unsatisfied and the selectivity of products is hard to be regulated, hindering their practical applications in large scale commercial purpose. In this work, for the first time, the Au and Pt was co-deposited on the heterostructure consisted of Cu 2 O quantum dots and ReS 2 nanosheets to achieve high efficiency and controllable selectivity during CO 2 photoreduction. The Au-Pt/Cu 2 O/ReS 2 photocatalysts show superior efficiency of CO 2 reduction than that of Au/Cu 2 O/ReS 2 , Pt/Cu 2 O/ReS 2 , Cu 2 O/ReS 2 , Cu 2 O. Such distinct improvement is attributed to the indirect Z-scheme mechanism and Schottky junction effect. Moreover, the synergetic effect of Au and Pt plays an important role of improving the photocatalytic activity, and the Au1-Pt5/Cu 2 O/ReS 2 exhibits the highest R electron of 516.86 μmol/g during one hour of visible light illumination, which is much larger than many recently reported photocatalysts under comparable condition. Meanwhile, the selectivity of CO and CH 4 is effortlessly tunable from 0 to 100% by modulating Au/Pt metal mass ratio due to the strong CO adsorption on Pt metals and the intensive interaction between Au and Pt atoms at the Au/Pt interface. This controllable selectivity provides admirable strategy to tune the component proportion of the gas products for the subsequent conversion into high value-added chemicals or liquid fuels. Our study proposes novel and deep insights into the design and fabrication of practical photocatalysts with high catalytic activity and controllable selectivity to perform efficient CO 2 photoconversion.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Akihiro Nakayama,Ryusei Sodenaga,Yuvaraj Gangarajula,Ayako Taketoshi,Toru Murayama,Tetsuo Honma,Norihito Sakaguchi,Tetsuya Shimada,Shinsuke Takagi,Masatake Haruta,Botao Qiao,Junhu Wang,Tamao Ishida
Cation- and anion-substituted hydroxyapatites (sHAPs) supported gold catalysts showed strong metal-support interaction (SMSI) under oxidative atmosphere. Mg- and Ce-substituted sHAPs stabilized Au clusters and imparted positively charged Au. The Au on these sHAPs became more positively charged upon formation of the oxidative SMSI. The catalytic activities for transvinylation of benzoic acid with vinyl acetate and isomerization of 3,4-diacetoxybut-1-ene (34DABE) correlated well with the cationic properties of Au; Au/Mg0.1SrHAP and Au/Ce0.1SrHAP with SMSI exhibited higher catalytic activity than other Au/sHAPs and the same catalysts without SMSI. The enhanced cationic properties of Au particles induced by oxidative SMSI surpassed the disadvantages of the reduction of the exposed surface Au atoms caused by SMSI. This work reveals that controlling the degree of SMSI is an efficient methodology to tune an optimal electronic state of metal NPs for target reactions and to provide highly active and durable catalysts.
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Shiyue Wu,Qinglei Jia,Yi Wang,Feng Liu,Gongguo Zhang,Haifeng Zhang,Haiwen Zhang,Maochang Liu,Yiqun Zheng
Plasmonic semiconductor nanomaterials have been widely accepted as promising candidates for photothermal conversion, while the efficiency is yet to optimize. Herein, we report a facile synthesis of Au@Cu x O mesoporous nanospheres anchored with branched Ag nano-islands on the surface and explore their applications as photothermal conversion agent. Due to the intimate hybridization of two materials, the Au@Cu x O-Ag hybrid nanocomposites display a unique dual-plasmonic absorption that covers the visible-NIR range, benefiting the utilization efficiency of light energy . The synthesis is realized by reacting Au@Cu x O with Ag + , the galvanic replacement reaction between them enables a preferential depletion of Cu phase, leaving Ag and Cu 2 O as dominate crystal phases. The resulting hybrid nanocomposites are featured with a core-shell structure but incomplete coverage, as well as the mesoporous interior and dendritic outer shell. In addition to the enhanced photothermal conversion efficiency, the current nano-hybrids show excellent structural stability and no decay in conversion after five successive rounds of measurement. The advantages in both morphological and electronic structure aspects are discussed. The present study validates the promising synergetic use of distinct hot charge carriers originating from metal and semiconductor that are photoexcited in the same hybrid nanoparticle for photothermal conversion, shedding light on rational design of photothermal materials based on metal-semiconductor hybrid nanocomposites.
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Biosensors-Basel
·
2022
·Vol. 12
·期 6
·387
·
IF 5.743
Sen Li,Defu He,Shuning Li,Ruipeng Chen,Yuan Peng,Shuang Li,Dianpeng Han,Yu Wang,Kang Qin,Shuyue Ren,Ping Chen,Zhixian Gao
Bisphenol A (BPA) has emerged as a contaminant of concern because long-term exposure may affect the human endocrine system. Herein, a novel aptamer sensor based on magnetic separation and surface-enhanced Raman scattering (SERS) is proposed for the extremely sensitive and specific detection of trace BPA. Moreover, the capture unit was prepared by immobilizing thiolated (SH)-BPA aptamer complementary DNA on AuNP-coated magnetic halloysite nanotubes ([email protected]), and SH-BPA aptamer-modified[email protected]@Ag core–shell SERS nanotags acted as signal units. By the complementary pairing of the BPA aptamer and the corresponding DNA,[email protected]and[email protected]@AgCS were linked together through hybridization-ligation, which acted as the SERS substrate. In the absence of BPA, the constructed aptamer sensor generated electromagnetic enhancement and plasmon coupling to improve the sensitivity of SERS substrates. Owing to the high affinity between BPA and the aptamer, the aptamer probe bound to BPA was separated from the capture unit by an externally-induced magnetic field. Thus, the Raman intensity of the[email protected]@AuCS core–satellite assemblies was negatively correlated with the BPA concentration. High sensitivity measurements of BPA might be performed by determining the decline in SERS signal strength together with concentration variations. The proposed aptasensor is a promising biosensing platform for BPA detection.Keywords:surface-enhanced Raman scattering (SERS);aptasensor;bisphenol A;core–satellite assemblies
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CATALYSIS TODAY
·
2022
·
IF 6.562
Peng Bai,Tao Zhou,Xiaohua Wang,Xiaofei Liu,Yi Wang,Yue Wang,Edgar Muhumuza,Yonghui Zhang,Pingping Wu
A series of γ-Al 2 O 3 supported gold-palladium (Au-Pd) alloy nanoparticles (NPs) catalysts were synthesized by a one-pot approach applying mercapto-propyl-trimethoxysilane (MPTMS) as an anchoring ligand. Homogeneously dispersed Au-Pd alloy NPs were observed on the prepared catalysts and their catalytic performance in benzyl alcohol partial oxidation was investigated. Results showed that the highest benzaldehyde yield was achieved on catalyst Au-Pd/7%MPTMS-γ-Al 2 O 3 with a benzaldehyde selectivity of 90%. By establishing the structure-performance relationship, the high activity of catalysts with MPTMS modification was attributed to the anchoring and dispersion effect of MPTMS on Au-Pd NPs, while the high benzaldehyde selectivity was due to the formation of more surface Lewis acid sites after introducing MPTMS, protecting the benzaldehyde from over-oxidation to byproducts.
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ELECTROANALYSIS
·
2022
·Vol. 35
·期 2
·e202200152
·
IF 3.077
Zeping Lv,Mingli Zhang,Huali Jin,Min Wei
An ultrasensitive electrochemical DNA sensor was designed for Hg 2+ assay using cooperative signal amplification effect of electrodeposited Au/carbon nanofibers-chitosan (DpAu/CNFs-CS) and reduced graphene oxide (RGO). CNFs-CS was prepared to modify gold electrode (AuE). Then, Au was electrodeposited on CNFs-CS/AuE to form DpAu/CNFs-CS/AuE for the first signal amplification. With TH as signal probe and ssDNA as recognition component, RGO/ssDNA and RGO/TH interaction were used for the second signal amplification. The prepared sensor had wider linear range of 0.0001–460 nM and lower detection limit of 5.7×10 −5 nM, high selectivity, and performed well in Hg 2+ assay of tap water.
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