Analytical Methods
·
2021
·Vol. 14
·期 3
·278-285
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IF 2.896
Ting Zhou,Meijuan Li,Na Li,Yulin Dong,Dan Liu,Xiaosong Hu,Zhizhong Xie,Deyu Qu,Xi Li,Chaocan Zhang
An ultrasensitive and specific-selection electrochemical sensor was constructed for Hg2+ detection based on Au nanoparticles and molybdenum selenide (Au NPs@MoSe2) as well as the thymine–Hg2+–thymine (T–Hg2+–T) coordination. Herein, Au NPs@MoSe2 not only could improve the sensitivity due to the large surface area and good electrical conductivity but also offered more sites to immobilize thiol-labeled T-rich hairpin DNA probes (P-1), which has a specific recognition for Hg2+ and methylene blue-labeled T-rich DNA probes (MB-P). When Hg2+ and MB-P exist, P-1 and MB-P can form a stable T–Hg2+–T complex. Then, methylene blue can be close to the electrode and detectable via differential pulse voltammetry (DPV). Benefiting from the specific recognition of T–Hg2+–T and the merits of Au NPs and MoSe2, the fabricated biosensor presented an ultrasensitive and highly selective performance. The DPV responses had a positive linear relationship with Hg2+ concentrations over ten orders of magnitude from 1.0 × 10−16 to 1.0 × 10−7 mol L−1. The detection limit was down to 1.1 × 10−17 mol L−1. Moreover, the developed sensor exhibited a promising application for trace Hg2+determination in water samples.
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Advanced Energy Materials
·
2021
·Vol. 12
·期 1
·2102359
·
IF 29.368
Yuan Chang,Panlong Zhai,Jungang Hou,Jijun Zhao,Junfeng Gao
Faced with grave climate change and enormous energy demands, effective catalysts have become more and more important due to their significant effects on reducing fossil fuels consumption. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by water splitting are feasible ways to produce clean sustainable energy. Here, atomic structures and related scanning tunneling microscope images of Se defects in PtSe 2 are systematically explored. The equilibrium fractions of vacancies under variable conditions are predicted in detail. In addition, it is found that the vacancies are highly kinetically stable, without recovering or aggregation. The Se vacancies in PtSe 2 can dramatically enhance the HER performance, comparing to Pt(111). It is also revealed that a PtSe 2 monolayer with Se vacancies is also a good OER catalyst. The excellent bipolar catalysis of Se vacancies is further confirmed by experimental measurements. A defective PtSe 2 made via direct selenization of Pt foil at 773 K using a chemical vapor deposition process is produced. It is shown that the HER and OER performance of defective PtSe 2 is much more efficient than Pt foils by a series of measurements. This work, with its compelling theoretical and experimental studies indicates PtSe 2 with Se defects is an ideal bipolar candidate for HER and OER.
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Nanoscale
·
2021
·Vol. 13
·期 42
·17846-17853
·
IF 7.79
Ting Li,Qing Zhang,Xiao Hu Wang,Juan Luo,Li Shen,Hong Chuan Fu,Fei Gu,Nian Bing Li,Hong Qun Luo
Electrochemical water splitting is widely studied in the hope of solving environmental deterioration and energy shortage. The design of inexpensive metal catalysts exhibiting desired catalytic performance and durable stability for efficient oxygen evolution is the pursuit of sustainable and clean energy fields. Herein, a three-dimensional (3D) flower-like NiSe2 primary structure, modified with highly dispersed CuSe2 nanoclusters as the secondary structure, is obtained by regulating the growth trend of the nanosheets. Benefiting from the metallicity of selenides and the formation of a heterogeneous interface, NiSe2@CuSe2/NF shows comparable performance toward the oxygen evolution reaction (OER) in an alkaline environment. Upon regulating the synthesis conditions, the catalyst exhibits its optimal performance with ultralow overpotential for the OER when the Ni/Cu molar ratio is 1 : 0.2 and the hydrothermal temperature and hydrothermal time are 200 °C and 6 h, respectively. It provides a current density of 10 mA cm−2 when a potential of 201 mV is applied without iR compensation. In this work, the hierarchical heterostructures of NiSe2 and CuSe2 are synthesized, which exhibit high electrocatalytic activity towards the oxygen evolution reaction and provides a new possibility for the extensive application of copper-based compounds in advanced energy fields.
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ACTA MATERIALIA
·
2021
·
IF 8.203
Jie Chen,Qiang Sun,Deyu Bao,Bang-Zhou Tian,Zegao Wang,Jun Tang,Dali Zhou,Lei Yang,Zhi-Gang Chen
Thermoelectric materials strengthened by defect engineering can also suffer from the compromise of plasticity, and in turn results in negative effect on the processability, reliability and durability of thermoelectric devices. Here, we introduce nano-twinned CuAgSe secondary phase to achieve simultaneously increased compressive strength and plasticity of the β-Ag 2 Se pellets without obviously sacrificing the thermoelectric performance, as evidenced by our thermoelectric measurements. Our pellet shows a maximum compressive strength of 96 MPa, which is ∼104% higher than that of pristine Ag 2 Se, ascribed to the impeded crack propagation by the CuAgSe secondary phase. An extraordinary deformation value of ∼19% is observed at the maximum compressive strength, which is attributed to the intrinsically large plastic deformation of the Ag 2 Se matrix, the deformable nano-twinned CuAgSe secondary as well as the interaction between the Ag 2 Se matrix and the CuAgSe secondary phase. This work indicates that introducing nano-twinned secondary phase in thermoelectric materials is a promising strategy for developing high-performance thermoelectric materials with high strength and plasticity.
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LANGMUIR
·
2021
·
IF 3.882
Huimin Kong,Wenjie Zhang,Ge Shi,Zhe Cui,Peng Fu,Minying Liu,Yanjie He,Xiaoguang Qiao,Xinchang Pang
A colloidal nanocrystal cluster (CNC) is a hierarchical nanostructure formed by clustering several nanocrystals into one nano-ensemble, which may exhibit unique optical or catalytic properties different from individual nanocrystals owing to the mutual interactions among neighboring component nanocrystals. However, there is still no universal synthetic route that could be applicable to diverse material compositions with precisely controlled hierarchical structures (i.e., nanocrystal number density, component nanocrystal size, and overall diameter of the CNC) up to now. Herein, a general and novel synthetic strategy was reported for crafting a wide range of inorganic CNCs (i.e., noble metal, semiconductor, and metal oxide) via utilizing amphiphilic star-like poly(4-vinylpyridine)-block-polystyrene diblock copolymers as nanoreactors prepared by sequential atom transfer radical polymerization. The hierarchical structure of rationally designed CNCs could be readily tailored by varying the P4VP molecular weight of star-like nanoreactors and the parameter optimization during the CNC preparation process, which was inaccessible by conventional synthetic methods.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Danyang He,Liyun Cao,Jianfeng Huang,Yongqiang Feng,Guodong Li,Dan Yang,Qingqing Huang,Liangliang Feng
Developing highly efficient and cost-effective non-noble metal electrocatalysts with prominent operational stability toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is indispensable for large-scale water electrolysis but remains challenging. Here, an innovative superhydrophilic vanadium-modulated Ni3Se2 nanorod@nanosheet array in situ grown on nickel foam (V-Ni3Se2/NF) is synthesized via a solvothermal strategy employing a NiV-LDH nanosheet as a precursor. Experimental investigations disclose that the hierarchical nanostructure endows V-Ni3Se2/NF with abundant electrochemically surface active sites that render the easy accessibility of the electrolyte to the electrode, thereby enhancing the electron transfer efficiency and electrocatalytic activity toward HER and OER. Furthermore, the modulated electronic configuration in V-Ni3Se2/NF not only favors the water dissociation and formation of adsorbed hydrogen but also optimizes the binding energy of key reaction intermediates, thus expediting the water electrolysis kinetics. Consequently, the V-Ni3Se2/NF electrode requires ultralow overpotentials of 275 and 370 mV at a large current density of 500 mA cm–2 in 1.0 M KOH solution toward HER and OER, respectively. The assembled V-Ni3Se2/NF||V-Ni3Se2/NF electrolyzer yields a low cell voltage equaling to 1.56 V to deliver 10 mA cm–2 together with an extraordinary long-term durability for 80 h, far outperforming the benchmark Pt/C/NF||IrO2/NF counterpart (1.76 V, 10 mA cm–2), demonstrating its glorious potentials in large-scale industrial water electrolysis applications. This work puts forward novel synergistic tactics to construct bifunctional electrocatalysts with prominent water splitting performance in a harsh alkaline electrolyte.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Yi-Xin Zhang,Yun-Qiao Tang,Zheng Ma,Ming-Yu Hu,Jing Feng,Zhen-Hua Ge
In this study, Cu2Se1–xSx (x = 0.1, 0.3, and 0.5) alloy powders were prepared by the hydrothermal synthesis method. In the subsequent sintering process, the spontaneous in situ phase separation process of the sample forms a two-phase hybrid structure. The generated Cu2S precipitates in the Cu2Se matrix noticeably enhance phonon scattering, which is beneficial for low thermal conductivity without significantly affecting the electrical transport performance. Ultimately, an optimized thermoelectric performance was obtained in Cu2Se0.9S0.1, reaching a peak zT value of 1.43 at 773 K, the optimum value among the Cu–Se–S systems at this temperature.
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MACROMOLECULAR BIOSCIENCE
·
2021
·Vol. 21
·期 12
·2100229
·
IF 4.979
Fangqin Song,Siqi Li,Chuanhao Sun,Ying Ji,Yan Zhang
The integration of hypoxia-activated chemotherapy with photodynamic therapy (PDT) has newly become a potent strategy for tumor treatment. Herein, a reactive oxygen species (ROS)-responsive drug carriers (PS@AQ4N/mPEG- b -PSe NPs) are fabricated based on the amphiphilic selenium-containing methoxy poly(ethylene glycol)-polycarbonate (mPEG- b -PSe), the hydrophobic photosensitizer (PS), and hypoxia-activated prodrug Banoxantrone (AQ4N). The obtained nanoparticles are spherical with an average diameter of 100 nm as characterized by transmission electron microscope (TEM) and dynamic laser scattering (DLS) respectively. The encapsulation efficiency of the PS and AQ4N reaches 92.83% and 51.04% at different conditions, respectively, by UV–vis spectrophotometer. It is found that the drug release is accelerated due to the good ROS responsiveness of mPEG- b -PSe and the cumulative release of AQ4N is up to 89% within 30 h. The cell test demonstrates that the nanoparticles dissociate when triggered by the ROS stimuli in the cancer cells, thus the PS is exposed to more oxygen and the ROS generation efficiency is enhanced accordingly. The consumption of oxygen during PDT leads to the increased tumor hypoxia, and subsequently activates AQ4N into cytotoxic counterpart to inhibit tumor growth. Therefore, the synergistic therapeutic efficacy demonstrates this drug delivery has great potential for antitumor therapy.
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Applied Materials Today
·
2021
·
IF 10.041
Wenshuai Feng,Manman Bu,Shuting Kan,Xiaohui Gao,Aimin Guo,Hongtao Liu,Lianwen Deng,Wei Chen
In this work, a novel hetero-phase interface structure (NiMoSe/NF-2), consisting of crystalline (NiSe) and amorphous (MoSe x ), was constructed by annealing Ni 0.85 Se/MoSe x hybrid (NiMoSe/NF-1), synthesized through hydrothermal and selenylation steps. For hydrogen evolution and oxygen evolution reaction, the NiMoSe/NF-2 exhibited an overpotential of 91 mV (10 mA cm −2 ) and 307 mV (100 mA cm −2 ) with the Tafel slope of 48.1 mV dec −1 and 30.9 mV dec −1 , respectively, superior to NiMoSe/NF-1. Meanwhile, much higher stability with 10 and 14 h tests was also respectively achieved for HER and OER. Using the NiMoSe/NF-2 as anode and cathode, the electrolyzer showed a long-time stability up to 14 h with the current density of 100 mA cm −2 at the potential of 1.91 V for overall water splitting. The density functional theory calculation validates that the crystalline/amorphous hetero-phase structure remarkably reduces the Gibbs free energy difference for both HER/OER and the increased occupation densities of electronic states near Fermi level accelerated charge transfer rate during electrocatalytic process. The hydrogen and oxygen intermediates desorption are facilitated by the downshift of Ni d-band center. The proposed crystalline/amorphous hetero-phase structure is prospective for designing bifunctional catalysts for water splitting.
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Nanoscale
·
2021
·Vol. 13
·期 39
·16487-16498
·
IF 7.79
Jingwen Wang,Shoufu Cao,Likun Yang,Yan Zhang,Kun Xing,Xiaoqing Lu,Jun Xu
The incorporation of catalytic components is a promising strategy to promote redox reaction kinetics and suppress polysulfide shuttling for high-performance lithium–sulfur batteries (LSBs). In this work, metastable marcasite NiSe2 nanodendrites grown on carbon fiber clothes (m-NiSe2/CFC) were synthesized to improve chemical adsorption and electrocatalytic activity towards lithium polysulfides. The multifunctional m-NiSe2/CFC film was utilized as both the interlayer and the three-dimensional (3D) current collector in LSBs. In comparison with the stable pyrite NiSe2 nanodendrite–covered CFC (p-NiSe2/CFC) counterpart, the m-NiSe2/CFC film exhibits even stronger chemisorption, higher catalytic activity and faster reaction kinetics, thereby resulting in significantly improved lithium storage performance. The Al@S/rGO@m-NiSe2/CFC cell has a high reversible capacity of 1646 mA h g−1 at 0.2C, a high QL/QH ratio of 3.00 at 0.2C, a high rate capability of 900 mA h g−1 at 4C, and an outstanding cyclic stability exhibiting a low capacity decay of 0.028% per cycle for 600 cycles at 4C. Moreover, a symmetrically sandwiched cathode of m-NiSe2/CFC@S/rGO@m-NiSe2/CFC was designed for high sulfur loading LSBs (4.5 mg cm−2) with superior electrochemical performance of 3.73 mA h cm−2 after 100 cycles at 1C rate. Our work opens up a new opportunity to enhance the electrochemical performance of LSBs by phase engineering of NiSe2 catalysts in sandwiched structural cathodes.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 37
·21340-21346
·
IF 12.732
Yuan Ji,Yundan Liu,Bin-Wei Zhang,Zhongfei Xu,Xiang Qi,Xun Xu,Long Ren,Yi Du,Jianxin Zhong,Shi Xue Dou
Hydrogen peroxide (H2O2) is widely used as a green oxidant for varying applications. Electrosynthesis is an economical and environmentally-friendly strategy to directly produce H2O2. Its practical production is hindered, however, by the lack of highly efficient and selective as well as low-cost electrocatalysts. Transition metal chalcogenide materials have been proved to be good catalysts for the oxygen evolution reaction, but their selectivity towards conversion of O2 to H2O2 remains unsatisfactory. In this work, 3 atomic-layer defect-rich CoSe2 nanosheets have been successfully grown on carbon cloth as a high performance electrocatalyst. The morphology of CoSe2 can be tuned by regulating the wettability of the growth substrate. The atomic-layer CoSe2 nanosheets showed unprecedented 92% selectivity towards H2O2 production in alkaline solutions, and the yields of H2O2 in alkaline and acidic solutions were 1227.7 mg L−1 h−1 and 894 mg L−1 h−1, respectively. The high efficiency and selectivity originate from the rich defects in the atomic-layer CoSe2 nanosheets, which can accelerate the adsorption of OOH by the exposed Co defect sites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yuhang Han,Jie Yuan,Yuhang Zhu,Qiangqiang Wang,Lin Li,Maosheng Cao
Microwave absorption materials can protect humanity from harmful electromagnetic radiation , but it is still a challenge to absorb electromagnetic radiation with different bands simultaneously. Herein, an effective strategy for obtaining WSe 2 @CNTs nanohybrids is reported. The conductive network and polarization of WSe 2 @CNTs nanohybrids can be tailored by confinedly implanting WSe 2 nanosheets on multi-walled carbon nanotubes. The electromagnetic properties and microwave absorption performance of the nanohybrids are effectively adjusted via changing the hybrid ratio of WSe 2 and CNTs . Multi-band microwave absorption is achieved with up to three bands. The reflection loss (RL) of the sample can reach −60.1 dB, and the bandwidth can reach 4.24 GHz (RL ≤ −10 dB). The excellent microwave absorption performance is attributed to the conductance and multiple relaxations, as well as the synergistic effect of the two. This result confirms that WSe 2 @CNTs nanohybrids are potential candidates for high-efficiency microwave absorbers and provide a valuable pathway for designing high-performance microwave absorption materials in the future.
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