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BIOMATERIALS · 2020 · IF 10.317

Anti-recurrence/metastasis and chemosensitization therapy with thioredoxin reductase-interfering drug delivery system

Jichun Yang,Shuojiong Pan,Shiqian Gao,Yiheng Dai,Huaping Xu

Thioredoxin reductase (TrxR) is an essential mammalian enzyme that possesses a selenocysteine active site. TrxR is overexpressed in many malignant tumors and has a close relationship with apoptosis, drug resistance, recurrence and metastasis of tumors. Recently, TrxR has emerged as a promising target for anticancer therapy. Herein, we developed a TrxR-interfering drug delivery system (DDS) based on RGD-PEG-PUSeSe-PEG-RGD self-assembling micelles for imaging-guided gemcitabine (GEM) chemosensitization and anti-recurrence/metastasis therapy. The diselenide-containing micelles were degraded in response to TrxR stimuli for GEM releasing. In the meantime, the dissociated polymers’ chain segments targeted the active site of TrxR via Se–Se/Se–S dynamic reactions for activity inhibition. This inhibition by the micelles not only provided chemosensitization, but reduced tumor recurrence/metastasis risk via the induction of residual tumor cell apoptosis by triggering ROS production post-chemotherapy. In this work, we took the transformation between Se-containing dynamic covalent bonds developed by our group from in vitro to in vivo , which furthered the knowledge on the biochemistry of selenium and provided aspects to develop new TrxR inhibitors. Overall, the TrxR-interfering DDS combined excellent antitumor effects for primary solid tumors with the inhibition of tumor recurrence/metastasis during post-treatment care, providing new perspectives for efficient cancer therapy.

CAS / MDL: 7782-49-2 16940-66-2
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Advanced Electronic Materials · 2020 ·Vol. 6 ·期 5 ·2000035 · IF 6.593

Exploiting Flexible Memristors Based on Solution-Processed Colloidal CuInSe2 Nanocrystals

Ruiqi Guo,Linxing Zhang,Jie Meng,Aqiang Liu,Jifeng Yuan,Kaibo Zheng,Jianjun Tian

Compared to analogous bulk materials, colloidal nanocrystals have presented a powerful platform for building up electronic devices on the nano/micrometer scale and flexible portable electronic apparatus with the benefits of solution-based processing approach at room temperature. Herein, memristors based on CuInSe 2 (CISe) colloidal nanocrystals prepared using a solution-based process at room temperature are constructed. The memristors exhibit obvious bipolar resistive switching performance with a high–low resistance ratio larger than 5.7 and a steady retention time over 10 4 s. This is attributed to the copper ion redox reaction and the migration of these ions under an applied electric field. When the SET voltage is reached, the ions are separated from one of the electrodes, and the memristor changes from a low-resistance state (LRS) to a high-resistance state (HRS). Conversely, when the voltage reaches the RESET voltage, the memristor switches from a HRS to a LRS. In addition, the flexible memristor can be fabricated by spincoating nanocrystal solution onto polyethylene terephthalate (PET) at room temperature, showing excellent reproducibility of the performance including 100 times of continuous operation, 10 4 s of reproducible reading, 600 times of antifatigue testing, and thermal stability up to 95 °C. The flexible devices demonstrate promising applications for portable electronic devices.

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Nanomaterials · 2020 ·Vol. 10 ·期 4 ·631 · IF 4.324

TiO2 Passivation Layer on ZnO Hollow Microspheres for Quantum Dots Sensitized Solar Cells with Improved Light Harvesting and Electron Collection

Zhen Li,Libo Yu,Hao Wang,Huiwen Yang,Huan Ma

Light harvesting and electron recombination are essential factors that influence photovoltaic performance of quantum dots sensitized solar cells (QDSSCs). ZnO hollow microspheres (HMS) as architectures in QDSSCs are beneficial in improving light scattering, facilitating the enhancement of light harvesting efficiency. However, this advantage is greatly weakened by defects located at the surface of ZnO HMS. Therefore, we prepared a composite hollow microsphere structure consisting of ZnO HMS coated by TiO2layer that is obtained by immersing ZnO HMS architectures in TiCl4aqueous solution. This TiO2-passivated ZnO HMS architecture is designed to yield good light harvesting, reduced charge recombination, and longer electron lifetime. As a result, the power conversion efficiency (PCE) of QDSSC reaches to 3.16% with an optimal thickness of TiO2passivation layer, which is much higher when compared to 1.54% for QDSSC based on bare ZnO HMS.Keywords:TiO2passivation layer;ZnO hollow microspheres;quantum dots sensitized solar cells

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

General surfactant-free synthesis of binary silver chalcogenides with tuneable thermoelectric properties

Hengyang Wang,Xiaofang Liu,Bin Zhang,Lisi Huang,Meiling Yang,Xiang Zhang,Hong Zhang,Guoyu Wang,Xiaoyuan Zhou,Guang Han

Binary silver chalcogenides (Ag 2 X, X  = S, Se, Te) are a group of intriguing thermoelectric materials. When utilised for thermoelectrics, however, the syntheses of these chalcogenides commonly require energy-intensive, high-temperature melting-annealing processes. Herein, we have developed a general surfactant-free and scalable solution synthesis strategy to nano/micro-particles of binary silver chalcogenides, which requires neither high temperature nor long reaction duration. The chalcogenide particles were spark plasma sintered into pellets with porous structures. By modifying the Ag + /X 2− molar ratios in the solution precursors from 2:1 to 2:1.1, the thermoelectric properties of the pellets have been effectively optimised, leading to maximum ZT values of 0.84 at 380 K for Ag 2 Se, 0.59 at 650 K for Ag 2 Te and 0.27 at 540 K for Ag 2 S that are comparable to those of samples fabricated by other synthetic methods, such as melting and annealing. This study provides a general surfactant-free solution approach to binary silver chalcogenide nano/micro-materials with tuneable thermoelectric properties.

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ACS Sustainable Chemistry & Engineering · 2020 · IF 7.632

Heterostructured CoSe2/FeSe2 Nanoparticles with Abundant Vacancies and Strong Electronic Coupling Supported on Carbon Nanorods for Oxygen Evolution Electrocatalysis

Wei Li,Yanli Niu,Xiuju Wu,Fawang Wu,Tianhao Li,Weihua Hu

Metal selenides attract great research interest as oxygen evolution reaction (OER) electrocatalysts. Herein, we report heterostructured bimetallic cobalt–iron diselenide nanoparticles with abundant vacancies and strong electronic coupling supported on carbon nanorod (CoSe2/FeSe2@C) as a highly efficient OER electrocatalyst. It is synthesized with a facile templating-engaged synthetic strategy and exhibits outstanding OER catalytic performance including high activity and good durability in alkaline medium. It affords a current density of 10 mA cm–2 at a low overpotential of 291 mV with small Tafel slope of 62 mV dec–1, which significantly outperforms the benchmarking RuO2 catalyst. The outstanding OER performance is found to be arising from its integrated advantages of the modulated electronic structure, abundant active sites, high electric conductivity, and large surface area endowed by its unique heterostructure and composition. This work exemplifies a feasible route to designing heterogeneous nanomaterials and enriches the OER electrocatalytic application of transition metal selenide-based hybrid materials.

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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 11 ·5699-5708 · IF 11.301

Contrasting roles of small metallic elements M (M = Cu, Zn, Ni) in enhancing the thermoelectric performance of n-type PbM0.01Se

Xin Qian,Dongyang Wang,Yang Zhang,Haijun Wu,Stephen J. Pennycook,Lei Zheng,Pierre F. P. Poudeu,Li-Dong Zhao

The metallic elements with a small atomic radius can not only compensate for the intrinsic vacancies to improve the carrier mobility, but also can form interstitials to reduce lattice thermal conductivity. In this work, we investigate the contrasting roles of three different metallic elements with small atomic radius on the thermoelectric properties of n-type PbM0.01Se (M = Cu, Zn, Ni). We find that all the metallic elements can increase the carrier concentration as electron donors and improve the electrical transport properties. In addition, the lattice thermal conductivity of PbSe can be significantly decreased through the formation of interstitials by the incorporated extra metallic elements. We also find that the PbCu0.01Se sample exhibits a unique and complex behavior compared with the other samples due to the diffusion and the thermally activated oxidation of Cu+ ions. When the temperature increased to 673 K, the carrier concentration of PbCu0.01Se sample increases suddenly and continues to increase by nearly two folds, which we ascribe to the release of 3d orbital electrons in Cu+ ions. This results in a strong decoupling of the charge and heat transport in the material, which can be manifested by the overestimation of the electronic thermal conductivity when assuming strong electron–phonon coupling in Wiedemann–Franz law. A maximum ZT of ∼1.6 can be reached at 773 K and the average ZT of ∼0.96 can be achieved in PbCu0.01Se. Our results demonstrate the exceptional contrasting behavior of Cu in PbSe by comparing with Zn and Ni, and the thermoelectric performance of n-type PbSe can be enhanced through the introduction of extra metallic elements with small radius.

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ACS Applied Bio Materials · 2020 · IF 0

Selenium-Containing Carrier-Free Assemblies with Aggregation-Induced Emission Property Combine Cancer Radiotherapy with Chemotherapy

Tianyu Li,Shuojiong Pan,Hao Zhuang,Shiqian Gao,Huaping Xu

Developing multifunctional carrier-free nanomedicine with high efficacy attracts tremendous attention in cancer treatment. Here, we develop selenium-containing carrier-free assemblies with aggregation-induced emission (AIE) property, which achieve the combination of cancer radiotherapy with chemotherapy. Under γ-radiation, diselenide bonds in the assemblies can be cleaved to form seleninic acid, which exhibits anticancer activity by upregulating the reactive oxygen species (ROS) levels in cancer cells. The incorporation of AIE groups further endows the selenium-containing assemblies with the ability of bioimaging. Their self-assembly behavior change under γ-radiation can be consequently observed in situ. The system combines cancer radiotherapy with chemotherapy, which exhibits improved anticancer activity.

CAS / MDL: 7782-49-2 16940-66-2
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Effects of surface ligands on localized surface plasmon resonance and stabilization of Cu2−xSe nanocrystals

Dongxu Zhu,Lijin Wang,Zheming Liu,Aiwei Tang

Cubic Cu 2−x Se nanocrystals (NCs) exhibit a strong localized surface plasmon resonance (LSPR) absorption in the near-infrared (NIR) region, in which the LSPR wavelength and stability are significant for the NIR-region applications in photo-thermal therapy and photoacoustic imaging. Herein, we have systematically studied the effects of surface ligands with varying the feeding ratio of oleylamine (OM) to oleic acid (OA) on LSPR behavior and stabilization of Cu 2−x Se NCs, which were synthesized by using a typical hot-injection method. The LSPR wavelength of the as-obtained Cu 2−x Se NCs could be tuned from 1260 to 1030 nm with an increase of the feeding ratio of OM to OA. Furthermore, these Cu 2−x Se NCs showed different LSPR stability with varying feeding ratios of OM to OA. For the Cu 2−x Se NCs synthesized in the presence of only OM, the LSPR could keep stable basically after exposure to air for 60 days. However, in the feeding ratio of OM to OA of 7:3 and 5:5 cases, the LSPR extinction spectra showed an obvious blue-shift in the wavelength. The characterized results indicated the different surface ligands had significant effects on the LSPR behavior and stabilization, and the LSPR change was in good agreement with the calculated results based on the Mie-Drude model. This work provides a new research idea for tuning the LSPR behavior of copper chalcogenide NCs.

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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Promoting the hydrogen evolution performance of 1T-MoSe2-Se: Optimizing the two-dimensional structure of MoSe2 by layered double hydroxide limited growth

Chao Yu,Zhanfang Cao,Shuang Chen,Shuai Wang,Hong Zhong

Designing of catalysts with high activity and earth abundance which can further enhance the electrocatalytic hydrogen evolution performance so as to improve the hydrogen production efficiency. In this paper, we synthesized 1T-MoSe 2 -Se/MgAl-LDH composites by in-situ hydrothermal reduction method. The high proportion 1T phase (73.73%) of ultra-thin layer 1T-MoSe 2 -Se was obtained by acid dissolution operation, which can be ascribed to the limiting growth effect of MgAl-LDH. Compared to Pure MoSe 2 , it dramatically improved HER catalytic activity. the optimal 1T-MoSe 2 -Se (24 h) exhibits superior HER performance with a small overpotential (122 mV at the current density of 10 mA cm −2 ) and Tafel slope (54 mV dec −1 ) as well as excellent electrochemical stability. The introduction of Se can promote the conductivity of 1T-MoSe 2 -Se catalyst. Moreover, the best electrocatalytic hydrogen evolution performance can be exhibited synergistically only when the optimal match between MoSe 2 and Se is achieved, which are confirmed by XPS analysis and HER test results.

CAS / MDL: 7782-49-2
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JOURNAL OF PHYSICS D-APPLIED PHYSICS · 2020 ·Vol. 53 ·期 12 ·125105 · IF 3.169

General and fast patterning of semiconductor nanocrystals by femtosecond laser direct writing

Yanan Liu,Zhijun Luo,Changsheng Xie,Zongsong Gan

Semiconductor nanocrystals have shown remarkable performance in the field of displays, solar cells, and photodetectors. But, a rapid method to produce localized stable nanocrystals remains a challenge, impeding the step toward device miniaturization. Here, we present a general and fast approach, femtosecond laser direct writing, for manufacturing these nanocrystals as well as integrating them into substrates in one step. The high peak power of the femtosecond laser induces a nonlinear absorption of the CatX (Cat  =  Cd or Pb, X  =  S, Se or Te) precursor at the focal spot. Once the temperature reaches the nucleation temperature, the CatX nanocrystals form immediately. By moving the displacement platform, arbitrary microscale patterns made of nanoscale crystals are obtained, which shows great potential in high-resolution displays and on-chip light sources.

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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 5 ·2777-2788 · IF 11.301

Ferroconcrete-inspired design of a nonwoven graphene fiber fabric reinforced electrode for flexible fast-charging sodium ion storage devices

Zexin Liu,Xin Zhang,Cai Liu,Dongyang Li,Miaoxin Zhang,Fuxing Yin,Guoqing Xin,Gongkai Wang

Flexible fast-charging sodium ion storage devices are poised to transform the future wearable electronics industry, if the materials used to build such devices can present a versatile integration. Herein, inspired by ferroconcrete, nonwoven graphene fiber (GF) fabric reinforced electrodes were successfully demonstrated in flexible sodium ion capacitors (SICs). For the fabrics, the functionalities of fast electron transport and an ion permeation network, a highly compatible electrode material host, an efficient capacity contributor, and a robust flexible framework are synergistically integrated. These were provided by the high conductivity of the graphene sheets, the tunable porosity of the GF, and the interlocked structure, compatibility with materials, and the surface capacitive contribution of the fabrics. The nonwoven fabrics hosted multi-dimensional active materials as the ferroconcrete electrode exhibits exceptional electrochemical and mechanical properties individually. The SICs can complete an entire charge–discharge process within 15 s. A digital LED and watch powered using the flexible SICs with superior volumetric performances (12 mW h cm−3@37 mW cm−3, and 6 mW h cm−3@1.9 W cm−3) proved the practical capability of our design. We believe that the proposed nonwoven GF fabrics and the ferroconcrete electrode structure will become a universal design, and shed new light on flexible fast-charging sodium ion storage devices.

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CERAMICS INTERNATIONAL · 2020 · IF 3.83

Understanding the growth of NiSe nanoparticles on reduced graphene oxide as efficient electrocatalysts for methanol oxidation reaction

Jingchun Jia,Linghui Zhao,Ying Chang,Meilin Jia,Zhenhai Wen

With the development of direct methanol fuel cell (DMFC), methanol oxidation reaction (MOR) becomes the crux of the application of DMFC, and the preparation of cheap, efficient MOR electrocatalyst is still the focus of researchers. Hence, we have prepared NiSe/RGO nanoparticles by a simple and universal way using pyrolyzation and selenylation. The MOR of NiSe/RGO is tested in 0.5 M MeOH/1 M KOH solution. Compared with the precursor Ni, NiSe/RGO-550 has outstanding performance for MOR with onset potential is 1.35 V vs. RHE, and 59.84 mA cm −2 for peak current density, and it can stable catalytic oxidation of methanol more than 4000 s. Because of the augment of active sites after selenization and the load of RGO enhanced electroconductibility, NiSe/RGO-550 has remarkable performance for MOR. This work provides the possibility of high performance, low cost catalysts for energy storage, conversion and practical applications.

CAS / MDL: 112-90-3 7782-49-2
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