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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

In-Situ doping-induced crystal form transition of amorphous Pd–P catalyst for robust electrocatalytic hydrodechlorination

Yanju Chen,Zhi Liu,Shoujie Liu,Yuansheng Cheng,Chao Zhang,Jiqing Jiao,Yukun Lu,Wenhong Wang,Kaian Sun,Xiaolong Bi,Aiyan Han,Bin Liu,Yuan Pan,Yunqi Liu,Chenguang Liu

Developing catalysts with high activity and high atom utilization as well as exploring catalytic active sites are the biggest challenges for the electrocatalytic hydrodechlorination technology. Herein, a novel strategy of Pd crystal transformation induced by in-situ doping was proposed, and a series of amorphous Pd–P nanoparticles (NPs) with controllable coordination environment were synthesized successfully. The amorphous Pd–P NPs catalyst exhibits the highest activity for electrocatalytic hydrodechlorination and good cycling stability when the Pd–P coordination number is 3 and the Pd–Pd coordination number is 4. The 4-chlorophenol hydrodechlorination efficiency of Pd–P-60 NPs reaches 100 % within 2 h, and the mass activity is 8.58 min −1 g −1 , which is 5.57 times as high as that for crystalline Pd NPs catalyst. Theoretical calculation shows that Pd–P catalyst facilitates the desorption of phenol and weakens the toxic effect on active sites. Density of states indicate that the doping of P results in a downshift of d -band center, facilitating the desorption of phenol. This work discovers the crystal effect and coordination effect of amorphous Pd–P NPs for electrocatalytic hydrodechlorination, which lays an important theoretical foundation for the design and development of high-performance Pd-based catalysts for electrocatalytic hydrodechlorination.

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OPTICAL MATERIALS · 2021 · IF 3.08

Solvothermal synthesis and upconversion luminescence of ultra-small Sc2O3: Yb, Er nanoparticles

Huilian Qin,Jing Li,Meijuan Yuan,Yaru Peng,Yuxin Huang,Li Chen

Monodisperse sub-10 nm Sc 2 O 3 : Yb, Er upconverting nanoparticles (UCNPs) were firstly synthesized via solvothermal method in three-neck round-bottom flask. The X-ray diffraction (XRD) shows that the prepared UCNPs possess cubic structure. The transmission electron microscopy (TEM) shows that sample has monodisperse spheroid morphology with high crystallinity . The average size of spheroid UCNPs could be controllable manipulated as small as 3 nm. Furthermore, the sample exhibits stronger red and green upconversion luminescence (UCL) than reported Sc 2 O 3 : Yb, Er nanostructure by biphasic solvothermal method. The Fourier-transform infrared (FTIR) spectra and decay curve reveal that ultra-small Sc 2 O 3 : Yb, Er UCNPs exhibit the reduced surface groups and long decay time of Er 3+ ions. The results indicate Sc 2 O 3 : Yb, Er UCNPs is a probable oxide material with small size and intense UCL for biological applications.

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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 48 ·17403-17409 · IF 7.059

Synthesis of single CsPbBr3@SiO2 core–shell particles via surface activation

Cuifang Meng,Dandan Yang,Ye Wu,Xuejia Zhang,Haibo Zeng,Xiaoming Li

Encapsulating cesium lead halide (CsPbX3, X = Cl, Br, and I) perovskite quantum dots (PQDs) into stable shells has been proved to be an effective strategy for improving their stability, which however usually forms agglomerated particles or alters PQDs’ original morphology and optical properties. Herein, we propose a surface activation strategy to prepare single CsPbBr3@SiO2 core–shell particles. (3-Aminopropyl)triethoxysilane (APTES) is used as a bifunctional surface ligand, which not only effectively passivates the surface defects of PQDs, but also provides –SiOCH3 and –SiOH groups for the formation of Si–O–Si covalent bonds with the subsequently introduced silanes. Furthermore, by controlling the hydrolysis rate of silanes, we realized the preparation of single CsPbBr3@SiO2 core–shell particles with an average shell thickness from 1 to 2.7 nm, and the PQDs maintained their initial cubic morphology and optical properties after coating. The stability of CsPbBr3@SiO2 in harsh environments has been effectively improved owing to the complete encapsulation of the SiO2 shell. As a result, the emission peak of CsPbBr3@SiO2 remains constant at 515 nm after being heated at 60 °C for 84 h, and the photoluminescence (PL) intensity still remains 90% after storage for 6 h in a high humidity environment. This work not only enhances the stability of PQDs for practical applications but also provides a reliable method to synthesize single core–shell particles, which can be instructive to other PQD systems.

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Photonics Research · 2020 ·Vol. 8 ·期 8 ·1301-1308 · IF 6.099

Self-powered, flexible, and ultrabroadband ultraviolet-terahertz photodetector based on a laser-reduced graphene oxide/CsPbBr3 composite

Yifan Li,Yating Zhang,Zhiliang Chen,Qingyan Li,Tengteng Li,Mengyao Li,Hongliang Zhao,Quan Sheng,Wei Shi,Jianquan Yao,Jianquan Yao

Self-powered and flexible ultrabroadband photodetectors (PDs) are desirable in a wide range of applications. The current PDs based on the photothermoelectric (PTE) effect have realized broadband photodetection. However, most of them express low photoresponse and lack of flexibility. In this work, high-performance, self-powered, and flexible PTE PDs based on laser-scribed reduced graphene oxide (LSG)/CsPbBr3 are developed. The comparison experiment with LSG PD and fundamental electric properties show that the LSG/CsPbBr3 device exhibits enhanced ultrabroadband photodetection performance covering ultraviolet to terahertz range with high photoresponsivity of 100 mA/W for 405 nm and 10 mA/W for 118 μm at zero bias voltage, respectively. A response time of 18 ms and flexible experiment are also acquired at room temperature. Moreover, the PTE effect is fully discussed in the LSG/CsPbBr3 device. This work demonstrates that LSG/CsPbBr3 is a promising candidate for the construction of high-performance, flexible, and self-powered ultrabroadband PDs at room temperature.

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MATERIALS & DESIGN · 2020 · IF 6.289

Chemical and morphological mechanisms of synthesizing rectangular cesium tungsten bronze nanosheets with broadened visible-light absorption and strong photoresponse property

Guanghui Liu,Ju Xu,Ruixing Li

Recently, nano-cesium tungsten bronze (Cs x WO 3 ) is found to be a new candidate for the application in solar filter due to its high visible transmittance and excellent near-infrared shielding ability. However, a typical two-dimensional (2D) Cs x WO 3 has not been reported since 2D nanomaterials have attracted great attention due to their fascinating properties, e.g., graphene. Herein, a novel synthesis system and related mechanisms are tried to develop for synthesizing 2D Cs x WO 3 via hydrothermal method, which an original inspiration derived from the morphology control of sulfides. The results indicate that morphology modifier represents a new strategy in which thiourea and oleylamine interact synergistically rather than independently to synthesize 2D Cs 0.3 WO 3 . The more regular and larger the rectangular nanosheet, the broader and stronger the light absorption, the rectangular Cs 0.3 WO 3 nanosheets with the maximum size are synthesized from thiourea, oleylamine and HCl concentrations of 4, 0.061 and 320 mmol/L, respectively, and exhibit a broad and strong absorption spectrum. The above nanosheet shows excellent instantaneous photo-thermal conversion property resulting in an obvious temperature increases from 20 °C to 88.5 °C when it was irradiated by 50 W halogen lamp for 10 s. Finally, both chemical reaction and morphological evolution in the synthesis processes are revealed.

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ACS Applied Materials & Interfaces · 2017 · IF 7.504

AIEgen-Functionalized Mesoporous Silica Gated by Cyclodextrin-Modified CuS for Cell Imaging and Chemo-Photothermal Cancer Therapy

Qing-Lan Li,Duo Wang,Yuanzheng Cui,Zhiying Fan,Li Ren,Dongdong Li,Jihong Yu

A novel multifunctional drug delivery system has been constructed by assembling per-6-thio-β-cyclodextrin-modified ultrasmall CuS nanoparticles (CD-CuS) onto fluorescent AIEgen-containing mesoporous silica nanoparticles (FMSN). The CD-CuS nanoparticles are anchored on the surface of benzimidazole-grafted FMSN, acting as a gatekeeper and photothermal agent. The prepared blue-emitting nanocomposite (FMSN@CuS) exhibits good biocompatibility and cell imaging capability. Anticancer drug doxorubicin hydrochloride (DOX) molecules are loaded into FMSN@CuS, and zero prerelease at physiological pH (7.4) and on-demand drug release at an acidic environment can be achieved due to the pH-responsive gate-opening of CD-CuS only at an acidic condition. The FMSN@CuS nanocomposite can generate obvious thermal effect after the exposure of 808 nm laser, which can also accelerate the DOX release. Meanwhile, the fluorescence intensity of DOX-loaded FMSN@CuS increases with the release of DOX, and the intracellular drug release process can be tracked according to the change of luminescence intensity. More importantly, DOX-loaded FMSN@CuS displays efficient anticancer effects in vitro upon 808 nm laser irradiation, demonstrating a good synergistic therapeutic effect via combining enhanced chemotherapy and photothermal therapy.

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ORGANIC ELECTRONICS · 2020 · IF 3.31

Highly efficient Ag–In–Zn–S quantum dot light-emitting diodes with a hole-spacing interlayer

Rongmei Yu,Furong Yin,Chunying Pu,Haizhen Song,Xiumei Xu,Han Zhang,Wenyu Ji

Although much effort has been made to the cadmium-free quantum dot light emitting diodes (QLEDs), it is still a big challenge to achieve an efficient eco-friendly QLED. Here, an extremely efficient QLED based on Ag–In–Zn–S QDs is constructed with the insertion of an 1,3,5-tris(N-phenylbenzimidazole-2-yl)benzene (TPBi) hole-spacing interlayer. The electrical properties of single carrier devices demonstrate the TPBi blocks the hole injection, leading to a more balanced charge injection in the device. Transient electroluminescence measurements confirm that the hole accumulation adjacent QDs is dramatically suppressed after the insertion of TPBi, hence limiting the interactions between excitons and holes. Consequently, the peak current (power) efficiency of 6.0 cd/A (6.5 lm/W) is achieved. To the best of our knowledge, this is the record efficiency for the Ag–In–Zn–S QLEDs reported to date. We anticipate this work will provide a new route for optimizing the performance of Cd-free QLEDs.

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MATERIALS CHEMISTRY AND PHYSICS · 2020 · IF 3.408

PtRhCu ternary alloy nanodendrites with enhanced catalytic activity and durability toward methanol electro-oxidation

Biao Sun,Long Huang,Shan Su,Sai Luo,Chunfeng Meng,Hafiz Muhammad Abdul Basit,Jiankun Xiao,Ting Bian,Shichuan Su

Despite the great progress has been made in the research of Pt-based catalysts toward methanol oxidation reaction (MOR), it is still remaining a great challenge for direct methanol fuel cells (DMFCs) to simultaneously satisfy both excellent activity and good durability. Herein, we report a facile one-pot approach for the successful fabrication of PtRhCu ternary alloy nanodendrites. For the methanol oxidation reaction (MOR), the electrocatalytic performances of the as-prepared nanocrystals can be optimized by simply varying the amount of Rh precursor. The mass activity and specific activity of the as-obtained Pt 47 Rh 8 Cu 45 nanodendrites are 2.9 and 5.8 times as high as that of commercial Pt/C catalyst, respectively. Besides, after the accelerated durability test (ADT) for 1500 cycles, the remaining specific activity of Pt 47 Rh 8 Cu 45 nanodendrites is 7.8 folds enhancement compared to commercial Pt/C, indicating the excellent stability of the PtRhCu catalyst. We believe that the improved electrochemical activity and stability could be resulted from the highly dendritic nanostructure and the synergetic effect of the three metallic elements in the alloy.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Magnetothermally responsive composite submicron particles for recyclable catalytic applications

Zeying Liu,Lingze Zhang,Peng Xiao,Lingfeng Liu,Peng Tang,Ya Wang,Shihong Shen,Jiajun Liu,Zhenhai Gan,Daocheng Wu

To improve the recycling efficiency of magnetic recycling system, magnetothermally responsive composite submicron particles (CFMNs@PEG CSPs) were designed and prepared for recyclable catalytic applications, in which poly(ethylene glycol) gel was used as the shell and clusters of cobalt ferrite magnetic nanoparticles as the core. A novel strategy for recycling both loadings and carriers was proposed based on loadings immobilized CFMNs@PEG CSPs via magnetic separation at first and then magnetothermally responsive release. The morphology and core–shell structure were observed by transmission electron microscope . The physicochemical characteristics were investigated by Fourier transform infrared, 1 H NMR, Magnetic property measurement system, thermogravimetric analysis and X-ray photoelectron spectroscopy. The size of CFMNs@PEG CSPs was 285.1 ± 7.6 nm (the core was 160.0 ± 13.2 nm and PEG gel shell was 62.6 nm). The shell thickness of CFMNs@PEG CSPs shrunk from 62.6 nm to 35.5 nm when the temperature changed from 25 °C to 50 °C, and more than 95% of the loadings were released in 30 min by magnetothermally responsive release. Combing magnetic separation and magnetothermally responsive release, CFMNs@PEG CSPs were recycled over 42 times for horseradish peroxidase catalysis (horseradish peroxidase was re-immobilized for six times and reused seven times for each re-immobilization) and 25 times for gold nanoparticles catalysis (reactivated gold nanoparticles were re-immobilized for five times and reused five times for each re-immobilization) without significant catalytic activity loss, indicating their extensive potential in recyclable catalytic applications and other applications.

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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

One-pot synthesis of copper nanowire-graphene composite with excellent stability and electrical performance for flexible electrodes

Rahul Navik,Ding Xiao,Yanzhe Gai,Huijun Tan,Yaping Zhao

Copper nanowires (CuNWs) endowed with oxidation stability without impairing their conductivity is highly desirable for their practical applications. This work demonstrates a green and cost-effective method to produce a stable copper nanowires-graphene nanosheets composite (CuNWs-GNs), and the electrodes based on CuNWs-GNs were fabricated. The CuNWs with a high-aspect-ratio of 1778 in-situ grown directly between the high crystalline GNs interlayers, thereby obtained a multilayer protective shield of GNs. The electrodes fabricated by a filtration method possessed high electrical conductivity of 2.77 × 10 6 S·m −1 . The relative resistance ratio of the electrodes increased only 1.27 and 1.92, respectively, after aging at 25 ℃ and 60 ℃ for 46 days, which suggested that the electrodes had excellent oxidation stability. The transparent flexible electrodes (TFEs) fabricated on a polyethylene terephthalate sheet by a spray coating method presented an excellent transmittance of about 89% at an electrical resistance of 81.42 Ω/sq. The TFEs demonstrated impressive mechanical flexibility against 1000 bending cycles and in different radius curvature ranging from 1 mm to 30 mm. This approach sheds light on solving the big issue of the instability of CuNWs and promote their applications in a modern electronic device.

CAS / MDL: 112-90-3
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Journal of Physics Communications · 2020 ·Vol. 4 ·期 4 ·045016 · IF 0

Synthesis of emission tunable AgInS2/ZnS quantum dots and application for light emitting diodes

Jiahu Wei,Feng Li,Chun Chang,Qin Zhang

Indium-rich environmentally-friendly quantum dots (QDs) have received widespread attention due to the absence of cadmium. In this paper, AgInS2 (AIS) QDs are synthesized by hot injection method. By adjusting the ratio of indium/silver (In/Ag = 1, 2, 3, 4, 5), the AIS QDs exhibit a blue shift from 868 nm to 603 nm with the indium composition increases. Therein, the AIS QDs with the ratio of In/Ag = 4 show a highest photoluminescent (PL) quantum yields (QYs) up to 57%. AIS QDs are coated with ZnS shell to passivate the surface defects, and the PL QYs of obtained core/shell AIS/ZnS QDs is increased to 72%. By using these AIS/ZnS QDs as light emitters, light emitting diodes are assembled with a stacked multi-layer structure ITO/PEDOT:PSS/Poly-TPD/QDs/ZnO:Mg/Al. The resulted electroluminescent (EL) device exhibits a maximum external quantum efficiency (EQE) of 1.25% and an open circuit voltage of 4.6 V corresponding to a maximum brightness of 1120 cd m−2. Although the performances of the as fabricated AIS/ZnS-based device lag much behind than those of the Cd-based ones, they are expected to be enhanced with much more studies on the synthesis of the QDs and the optimization of device structure.

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Nanoscale · 2020 ·Vol. 12 ·期 20 ·11288-11296 · IF 6.895

AgFeS2 nanoparticles as a novel photothermal platform for effective artery stenosis therapy

Xuan Peng,Junchao Liu,Chen Ming,Bo Li,Zhen Zhao,Kaichuang Ye,Min Zeng,Rujia Zou,Xinwu Lu,Junqing Hu

Ternary I–III–VI2 semiconductors usually have narrow band gaps and large absorption coefficients arising from the unique characteristics of their outer-d valence electrons, which are intimately connected with the photothermal conversion properties. AgFeS2 is known as one such material that has the potential to absorb near-infrared light. In this work, we utilized density functional theory (DFT) calculations to evaluate the electronic structure and optical absorption properties of AgFeS2. Strong absorptions were predicted over a wide Vis-NIR region due to the localized 3d electron of Fe atoms, which agree quite well with the UV-Vis-NIR spectra measured by experiment. The as-prepared AgFeS2 nanoparticles were then modified with mPEG-DSPE, an efficient photothermal agent for artery stenosis therapy. Its photothermal conversion effect has been systematically studied, indicating the potential for causing the hyperthermia of macrophages, an essential part of the artery inflammation response. More importantly, both in vitro cell experiments and in vivo mouse-model studies show that the induction of hyperthermia in artery stenosis by using AgFeS2 nanoparticles is safe and effective when injected at a very low concentration. This study provides a novel photothermal platform derived from the inheritability of bandgap structure and also promotes the process of artery inflammation and stenosis therapy.

CAS / MDL: 112-90-3
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