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Materials Today Communications · 2021 · IF 3.383

Synthesis of TiN–TiB2–hBN composite powders with a core-shell structure and preparation of bulk samples

Shi Tian,Wenchao Guo,Qianglong He,Aiyang Wang,Tian Tian,Chun Liu,Lanxin Hu,Zhixiao Zhang,Hao Wang,Weimin Wang,Zhengyi Fu

TiN–TiB 2 –hBN composite powders were synthesized by a nitride boronizing process using TiN and amorphous boron as the raw materials, and the reaction process of TiN–B powder mixture was investigated by heat treatment at elevated temperatures. At 1400 °C in a vacuum, TiN–TiB 2 –hBN composite powders with a core-shell structure of layered hBN-wrapped TiB 2 were obtained, which can be used to prepare ceramic composites with excellent properties. The results showed that B atoms began to diffuse into TiN and replace the N atoms to form TiB 2 at high temperature; then, the substituted N escaped outwards, and upon contacted with B, formed hBN at the surface of the TiB 2 particles. The relative density, bending strength , and fracture toughness of the 70 vol% TiN–17.6 vol% TiB 2 –12.4 vol% hBN (TB73) composite prepared by reactive sintering were 98.90%, 521 MPa, and 4.22 MPa m 1/2 , respectively, which were much higher than that of fabricated via conventional method (TBN73: 88.02%, 198 MPa, and 2.58 MPa m 1/2 ).

CAS / MDL: 7440-31-5
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Nanoscale · 2021 ·Vol. 13 ·期 38 ·16307-16315 · IF 7.79

Electrochemically synthesized SnO2 with tunable oxygen vacancies for efficient electrocatalytic nitrogen fixation

Xiaojia He,Haoran Guo,Tianhao Liao,Yi Pu,Long Lai,Zihao Wang,Hui Tang

Electrochemical nitrogen reduction reaction (NRR) driven by a renewable energy source offers a sustainable and environmentally benign route to produce ammonia (NH3), but it is highly dependent on efficient and specific catalysts to reduce the high reaction barrier and improve the selectivity. Defect engineering is extensively used to regulate the surface properties of materials to improve their catalytic performance. Herein we synthesized SnO2 with different oxygen vacancy concentrations by a controllable electrochemical method for electrocatalytic nitrogen (N2) fixation. The prepared SnO2 was used as an electrocatalyst and exhibited excellent NRR performance with an optimal NH3 yield rate of 25.27 μg h−1 mgcat.−1 and faradaic efficiency of 11.48% at −0.6 V (vs. the reversible hydrogen electrode) in 0.1 M Na2SO4. Oxygen vacancies provide more active sites and greater electron transfer ability on the catalyst surface to facilitate N2 adsorption and activation. The electrocatalytic NRR performance of SnO2 was enhanced with the increase in oxygen vacancy concentration. The density functional theory calculations indicate that the oxygen vacancies in SnO2 promote the electrocatalytic NRR performance by increasing the number of valence electrons of Sn and decreasing the energy barrier of the potential-determining step, thus promoting the activation of the N–N bond to further achieve efficient N2 fixation.

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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Super-Assembled Periodic Mesoporous Organosilica Frameworks for Real-Time Hypoxia-Triggered Drug Release and Monitoring

Yingnan Liu,Lei Xie,Meng Gao,Runhao Zhang,Jingchen Gao,Jiangdong Sun,Qingdong Chai,Tong Wu,Kang Liang,Pu Chen,Qi Wan,Biao Kong

Hypoxia, induced by inadequate oxygen supply, is a key indication of various major illnesses, which necessitates the need to develop new nanoprobes capable of sensing hypoxia environments for the targeted system monitoring and drug delivery. Herein, we report a hypoxia-responsive, periodic mesoporous organosilica (PMO) nanocarrier for repairing hypoxia damage. β-cyclodextrin (β-CD) capped azobenzene functionalization on the PMO surface could be effectively cleaved by azoreductase under a hypoxia environment. Moreover, the nanosystem is equipped with fluorescence resonance energy transfer (FRET) pair (tetrastyrene derivative (TPE) covalently attached to the PMO framework as the donor and Rhodamine B (RhB) in the mesopores as the receptor) for intracellular visualization and tracking of drug release in real-time. The design of intelligent nanocarriers capable of simultaneous reporting and treating of hypoxia conditions highlights a great potential in the biomedical domain.

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JOURNAL OF ELECTRONIC MATERIALS · 2022 ·Vol. 51 ·期 2 ·486-494 · IF 2.047

Achieving High Thermoelectric Performance of SnTe Composites with 2D WSe2

Wang Xiaochun,Zhou Zhiwei,Lin Xuesong

In this work, we introduced two-dimensional (2D) WSe 2 with the lowest heat conductivity to enhance thermoelectric properties of the non-toxic and cost-effective SnTe. On one hand, the improved power factor can be attributed to the enhancement of Seebeck coefficient due to the decrease of low-energy carriers and minority carriers by the addition of WSe 2 -SnTe p - p -type heterojunction interface barriers. On the other hand, the thermal conductivity also decreased sharply by the heightened phonon scattering from the high-density stacking faults and multiscale hierarchical architectures. Ultimately, benefiting from the dual regulation effect of the introduction of 2D WSe 2 on the electro-acoustic decoupling, an improved figure of merit ( ZT ) of 1.0 is achieved for the composition of SnTe + 6 wt% WSe 2 at 873 K, which is enhanced by 134% in comparison with the pure SnTe sample. Moreover, the meaningful attempt represents an effective and feasible strategy for mixing SnTe with other compounds by the method of ball milling. Graphical Abstract

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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Integration of black phosphorene and MXene to improve fire safety and mechanical properties of waterborne polyurethane

Lingxin He,Xin Jiang,Xia Zhou,Zhaoxin Li,Fukai Chu,Xin Wang,Wei Cai,Lei Song,Yuan Hu

The low exfoliation yield and large solvents consumption have become the major issue that limits the commercial application of two-dimensional nanomaterials. Emerging as an effective and environmentally friendly approach, electrochemical exfoliation has been attached by extensive concern. Hence, a simple and environmentally friendly two-electrode electrochemical exfoliation method was put forward to prepare black phosphorus-MXene (BP-Ti 3 C 2 ) nanohybrids without consumption of any organic solvents. The integration of BP and Ti 3 C 2 also imparts higher fire safety and mechanical properties to waterborne polyurethane (WPU). With the incorporation of 2.0 wt% BP-Ti 3 C 2 , the peak heat release rate, total heat release, total smoke production and total CO 2 yield of WPU were decreased by 42.2%, 12.9%, 12.6% and 16.5%, respectively, exhibiting a great flame retardancy effect. The employment of electrochemical exfoliation method towards BP and Ti 3 C 2 nanosheets not only imparts higher fire safety to polymer composites, but also provides a referable environmentally friendly preparation for two-dimensional nanomaterials.

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MICROCHEMICAL JOURNAL · 2021 · IF 4.821

An electrochemical biosensor of Sn@C derived from ZnSn(OH)6 for sensitive determination of acetaminophen

Yuxuan Qin,Chen Hang,Liping Huang,Haiyun Cheng,Junqing Hu,Wenyao Li,Jianghong Wu

In this study, Sn@C composite was fabricated from ZnSn(OH) 6 through a green thermal calcination method. For the first time, this composite was used as a modifier on glassy carbon electrode (GCE) to construct an electrochemical biosensor to detect acetaminophen (AC). The Sn@C sensor exhibited distinctly enhanced performance in electrochemical response to AC compared with bare GCE, GCE modified with Sn and GCE modified with graphene. The linear range is 0.2–100 μM and the limit of detection (LOD) is 0.020 μM based on DPV analysis. The excellent electrochemical behavior can be ascribed to the outstanding conductivity of metal Sn and carbon, and the strong adsorption of the carbon layer to AC. Most importantly, the chemical interaction between Sn and C through Sn-C bond facilitated the electron transfer process in the electrooxidation of AC. Finally, the Sn@C sensor was successfully applied in pharmaceutical samples and spiked serum samples to detect AC with satisfactory recoveries.

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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 11 ·110537 · IF 4.316

Preparation and Electrochemical Properties of Bicontinuous Solid Electrolytes Derived from Porous Li6.4La3Zr1.4Ta0.6O12 Incorporated with Succinonitrile

Fei Chen,Leana Ziwen Rannalter,Xing Xiang,Yanhua Zhang,Shangbin Song,Shiyu Cao,Qiang Shen

The development of solid electrolytes is a key step to break through the technical bottleneck of lithium batteries and obtain lithium batteries with high safety and high energy density. Combining the advantages of both inorganic and organic solid electrolytes, the form of inorganic fillers for composite solid electrolytes is extended from nanoparticles, nanofibers to a 3D matrix. In this study, a porous Li6.4La3Zr1.4Ta0.6O12 (LLZTO) ceramic framework was fabricated by adding a pore-forming agent, which was then infiltrated by succinonitrile (SN)-LiTFSI to take full advantage of the inorganic and organic parts of the composite electrolyte. The interconnected porous structure allows continuous ion transport pathways in both parts. The effect of the porosity, namely the amount proportion of inorganic and organic materials, on the electrochemical performance of composite electrolytes was investigated by regulating the amount of pore-forming agent. The presented composite solid electrolyte achieves a very high ionic conductivity of 1.08 × 10−3 S cm−1 at 30 °C, while it is stable up to 5.1 V at room temperature. The repeated lithium stripping/plating is stable over 250 h without short circuit.

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Journal of Physical Chemistry C · 2021 · IF 4.126

Palladium Phosphide/Black Phosphorus Heterostructures with Enhanced Ethanol Oxidation Activity and Stability

Qian Zhang,Jian Weng,Jun Xu

Electrocatalytic performance for the ethanol oxidation reaction (EOR) under alkaline conditions can be improved by the rational design of catalysts. Palladium phosphates have shown higher electrical conductivities and activity compared with Pd. Nevertheless, the synthesis of palladium phosphide is complex and requires a relatively high temperature. Here, we report a simple synthesis method of palladium phosphide/black phosphorus heterostructure (Pd3P/BP) with enhanced EOR activity. BP is used instead of other phosphorus sources for several reasons: (i) BP has a lone pair of electrons, which easily coordinate with the metal atoms to form palladium phosphides. (ii) As a two-dimensional layered structure material, BP has a large specific surface area, which is beneficial for the dispersion of metal nanoparticles, and thus improves the utilization rate of catalysts owing to the expanded active sites. (iii) Phosphorus species (P0) might inhibit the adsorption of CO on the catalyst surface. (iv) BP has an excellent adsorption capacity to water molecules, thereby promoting the generation of OH groups and stripping of reaction intermediates, contributing to superior EOR activity and stability of Pd3P/BP. The activity of Pd3P/BP (7411.2 mA mgPd–1) is about 9.1-fold higher than the commercial Pd/C (814.8 mA mgPd–1) and significantly higher than that of Pd3P + BP (3065.4 mA mgPd–1).

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Nanoscale Advances · 2021 ·Vol. 3 ·期 19 ·5650-5655 · IF 4.553

Conjugated polymer coating enabled light-resistant black phosphorus with enhanced stability

Xingyun Li,Bin Han,Yaojie Xu,Xiao Liu,Chunhui Zhao,Jun Xu

As an advanced two-dimensional (2D) material with unique properties, black phosphorus (BP) has attracted great attention in a variety of fields. One of the main obstacles for the practical application of BP is the poor ambient stability of few-layer BP, especially under light irradiation. In this study, a light-absorbing conjugated polymer is functionalized on the surface of BP during the exfoliation process, yielding BP nanosheets with light-resistance. The obtained BP/polymer nanosheets demonstrate enhanced stability compared to pure BP under sunlight. Systematic characterization reveals that the crystal structure and electronic characteristics of BP are well retained after 30 days of sun exposure. This convenient and efficient conjugated polymer passivation provides a novel light-prohibited method to improve the stability of BP for future applications.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Enhancing thermoelectric performance of K-doped polycrystalline SnSe through band engineering tuning and hydrogen reduction

Nan Xin,Yifei Li,Guihua Tang,Longyun Shen

High-efficient and environment-friendly thermoelectric materials have attracted much attention. The single crystal tin selenide (SnSe) has a record high thermoelectric figure of merit ( ZT ) of 2.6 at ~800 K. Polycrystalline SnSe has better mechanical-strength but inferior ZT values than the single crystal, attribute to the paradoxically higher thermal conductivity ( κ ). In this work, we synthesized K x Sn 1−x Se (x = 0, 0.01, 0.02, 0.03 and 0.04) by doping K 2 CO 3 . A large number of point defects and dislocations generated with CO 2 volatilization, which possibly reduces κ . Based on this process, the K x Sn 1−x Se powders were followed by the hydrogen reduction with 4% H 2 − 96% Ar atmosphere to reduce tin oxide and potassium oxide which have high κ . These strategies lead to an ultra-low κ 0.32 Wm −1 K −1 in K 0.03 Sn 0.97 Se at 798 K. The effects of K doping on electronic transport performance of SnSe were studied by density functional theory calculation and experimental measurement. Doing K can narrow the band gap, increase hole concentration and enhance the electrical conductivity ( σ ) of SnSe. At 298 K, the σ of K x Sn 1−x Se increased by more than 2.5 times compared with the pristine SnSe. In high temperature region (623 K<  T  < 823 K), the σ is mainly affected by thermal excitation. High doping level of K (x = 0.03 and 0.04) suppresses the thermal excitation and limits the maximum of ZT . As the result, A high ZT of 1.06 is obtained at 798 K from K 0.01 Sn 0.99 Se perpendicular to the pressing direction, which is 103.8% larger than that of pristine SnSe. In addition, the hot-pressing polycrystalline K x Sn 1−x Se remains obvious lamellar morphology and show anisotropy. The σ and κ of K x Sn 1−x Se samples perpendicular to the pressure direction are much higher than those of the samples parallel to the pressure direction. This anisotropy decreases with the increasing K content.

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Materials · 2021 ·Vol. 14 ·期 20 ·6166 · IF 3.623

Syntheses, Structures and Properties of Alkali and Alkaline Earth Metal Diamond-Like Compounds Li2MgMSe4 (M = Ge, Sn)

Hongbo Gao,Kewang Zhang,Ailijiang Abudurusuli,Chen Bai,Zhihua Yang,Kangrong Lai,Junjie Li,Shilie Pan

Two new diamond-like (DL) chalcogenides, Li2MgGeSe4and Li2MgSnSe4, have been successfully synthesized using a conventional high-temperature solid-state method. The two compounds crystallize in the non-centrosymmetric space groupPmn21witha= 8.402 (14) Å,b= 7.181 (12) Å,c= 6.728 (11) Å,Z= 2 for Li2MgSnSe4, anda= 8.2961 (7) Å,b= 7.0069 (5) Å,c= 6.6116 (6) Å,Z= 2 for Li2MgGeSe4. The calculated results show that the second harmonic generation (SHG) coefficients of Li2MgSnSe4(d33= 12.19 pm/v) and Li2MgGeSe4(d33= −14.77 pm/v), mainly deriving from the [MSe4] (M = Ge, Sn) tetrahedral units, are close to the one in the benchmark AgGaS2(d14= 13.7 pm/V). The calculated band gaps for Li2MgSnSe4and Li2MgGeSe4are 2.42 and 2.44 eV, respectively. Moreover, the two compounds are the first series of alkali and alkaline-earth metal DL compounds in the I2-II-IV-VI4family, enriching the structural diversity of DL compounds.Keywords:diamond-like structure;chalcogenides;infrared nonlinear optical materials;second harmonic generation

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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Partial congener substitution induced centrosymmetric to noncentrosymmetric structural transformation and nonlinear optical properties of PbSnSiS4

Jiazheng Zhou,Ling Luo,Yu Chu,Peng Wang,Zhiyong Guo,Xin Su,Junjie Li

The Pb x Sn 2−x SiS 4 series from 0 ≤ x ≤ 2 were investigated to study the influence of partial congener cationic substitution on structure and properties. While the centrosymmetric (CS) compounds Pb 2 SiS 4 and Sn 2 SiS 4 crystallizing in the centrosymmetric (CS) P 2 1 / c space group have been reported previously, the partial congener cationic substitution induced CS to noncentrosymmetric (NCS) structural transformation in this system and the formed NCS substitution variant PbSnSiS 4 are introduced here for the first time. PbSnSiS 4 crystallizes in P 2 1 space group with the cell parameters a  = 6.4334(8) Å; b  = 6.6912(8) Å, c  = 8.5037(10) Å, β  = 108.576(4) °, Z = 2. The title compound shows a strong second harmonic generation (SHG) response (~ 1.1 × AgGaS 2 ), high laser induced damage threshold (LIDT) (~3 × AgGaS 2 ), and wide IR transparent region from 0.58 to 16.85 µm (down to zero). What’s more, PbSnSiS 4 exhibits good crystal growth habits, and millimeter-scale single crystals (~ 2 × 2 × 1 mm 3 ) were obtained in a spontaneous crystallization way. The theoretical calculations indicate that the optical band gaps decrease with increasing Sn content from Pb 2 SiS 4 (1.94 eV), PbSnSiS 4 (1.82 eV), to Sn 2 SiS 4 (1.69 eV). The results give an insight into the exploration of new NCS compounds with the congener cationic substitution strategy.

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