Journal of the American Chemical Society
·
2025
·
IF 15.6
Jingyu Li,Zheng Ma,Hao Wang,Lanwei Li,Jianbo Zhu,Huaican Chen,Yuanpeng Zhang,Zhuoyang Ti,Jiajun Zhong,Yuanguang Xia,Peng-Fei Liu,Yongsheng Zhang,Wen Yin
Controlling the local structure of high-entropy materials offers a promising pathway to resolve the trade-off of electron and phonon transport behaviors, which unlocks their full potential in thermoelectric applications. Herein, utilizing time-of-flight neutron total scattering and advanced multiscale simulations, we unveil the intricate local structures spanning both short- and long-range scales in high-entropy chalcogenides AgMnPbSbTe4 and AgMnGePbSbTe5, characterized by pronounced long-range cation disordering and well-defined short-range ordering. Notably, pair distribution function refinements revealed substantial discrepancies near 3 Å, unequivocally indicating significant local distortions from PbTe. Besides enhancing Pb-site asymmetry, the high-entropy strategy also triggers chemical bonding evolutions from purely ionic interactions in PbTe to mixed covalent-ionic features in AgMnPbSbTe4, and ultimately to more robust covalent-ionic interactions in AgMnGePbSbTe5. This transformation produces a 3-fold enhancement in electrical conductivity for AgMnGePbSbTe5 relative to AgMnPbSbTe4, and an orders-of-magnitude improvement over PbTe. Due to the enhanced covalent character imparted by Ge–Te bonding and weakened local octahedral structural distortions with long-ranged scales, the lattice thermal conductivity of AgMnGePbSbTe5 surpasses that of AgMnPbSbTe4 across the entire temperature range. By optimizing high-entropy materials from the local chemical order, we achieve a maximum ZT of 1.66 at 750 K in pure AgMnGePbSbTe5, significantly outperforming intrinsic PbTe (∼ 0.26 at 720 K) and other PbTe-based composites. Our findings not only elucidate the underlying mechanisms governing the anomalously low thermal conductivity in high-entropy materials but also establish a correlation between local structural distortions and thermoelectric performance, thereby providing critical insights for the rational design of next-generation thermoelectric materials.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Xiao Wang,Tongxin Di,Wei Li,Debao Liu,Xiaohao Sun
Nowadays, Zinc (Zn)-based biocomposites as biodegradable implant materials have been recognized as a promising approach to overcome the insufficient mechanical performance of Zn matrix and to endow the Zn-based materials with biofunctionality. However, the strengthening effect on Zn-based matrix composite remains far from expectation mainly due to the poor interfacial bonding between the reinforcement and Zn matrix, and the relatively coarse grain size of the Zn matrix. Herein, we have developed a novel in situ wetting strategy to ameliorate the interfacial bonding and mechanical performance of Zn-Ag-based composites using cuprous oxide-modified graphene oxide (Cu 2 O-GO) sheets as reinforcement. The enhanced interfacial bonding between GO sheets and Zn matrix owing to the in situ generated ZnO interlayer and the ultrafine microstructure with an average grain size of 360 nm were simultaneously achieved in the hot extruded (HEed) 1 wt%Cu 2 O-GO/Zn-2 wt%Ag biocomposites. Consequently, HEed biocomposites possessed excellent tensile properties, including ultimate tensile strength (UTS) of 344.0 ± 2.4 MPa, yield stress (YS) of 314.0 ± 4.8 MPa, and elongation at failure of 15.5% ± 1.3%. Ultrafine and uniform microstructure of the HEed biocomposites resulted in a relatively uniform corrosion morphology and a degradation rate of 0.195 ± 0.004 mm y −1 in simulated body fluid (SBF) solution. The 2-fold diluted extract of the HEed biocomposites exhibited satisfying cytocompatibility with MC3T3-E1 pre-osteoblast comparable to that of Ti-6Al-4 V ELI alloys. More importantly, the synergistic effect of metallic ions, Ag-rich nanoparticles, and GO sheets contributed to the remarkable antibacterial activity of the experimental biocomposites against both S. aureus and E. coli. These results demonstrated that the 1Cu 2 O-GO/Zn-2Ag biocomposites should be anticipated as a promising biodegradable material for orthopedic applications.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
·
IF 5.7
Liangliang Tang,Dongxu Yao,Yongfeng Xia,Hanqin Liang,Yu-Ping Zeng
Gas-pressure sintered silicon nitride (Si 3 N 4 ) ceramic was brazed to oxygen-free copper (OFC) foil using 20.22 ± 0.93 mg/cm 2 of Ag-Cu-TiH 2 filler at 875 ◦ C for 0.5 h. The effect of TiH 2 content on the 3D morphology, including the cross-section microstructure and etched surface morphology of Si 3 N 4 ceramic/OFC foil joints, was analyzed. An evolution model of the interfacial microstructure for joints was proposed based on 3D morphological analysis. The reaction between the brazing alloy and Si 3 N 4 ceramic formed the interfacial reaction layer and the inside reaction zones during brazing. The growth mechanism of the interfacial reaction layer was discussed in detail. The peeling test was used to evaluate the bonding strength of the Si 3 N 4 ceramic/OFC foil joints, and the optimum peeling strength of 25.1 N/mm was achieved at 5 wt% TiH 2 content. The interfacial microstructure of the joints changed with TiH 2 content, leading to different main fracture mechanisms and corresponding peeling strengths.
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ORGANIC ELECTRONICS
·
2023
·
IF 3.2
Jinyao Zhong,Haitao Xu,Junwei Zhao,Fuhao Gao,Jinxin Zhou,Yongbing Long
Microcavity-based semitransparent organic solar cells (ST-OSCs) have become a hot issue in the research field of green energy harvesting due to their wider potential applications in colored photovoltaic glass, building-integrated photovoltaics, and so on. However, for this kind of ST-OSCs, high photoelectric conversion efficiency (PCE) and high peak transmittance cannot usually be achieved simultaneously. To circumvent the problem, this paper proposes MgF 2 microcavity with a structure of Au/Ag/MgF 2 /Ag for ST-OSCs so that high peak transmittance can be achieved at low cost of PCE. The device structure of ST-OSCs is Glass/ITO/ZnO/PTB7-Th: IEICO-4F/MoO 3 /Au/Ag/MgF 2 /Ag. By combining the high transmittance of MgF 2 microcavities with the low absorption of IEICO-4F in the blue light, a colorful ST-OSCs with high blue light transmittance can be obtained. The IEICO-4F in the active layer shows strong optical absorption in the near-infrared wavelength region, but weak absorption in the visible region. The results demonstrate that the peak transmittance of ST-OSCs reached a high value of 48% at 440 nm and the PCE reached 10.4%. Such a high peak transmittance is achieved while the PCE reduction compared to the control opaque device is about 5%. The PCE loss rate at each peak transmittance is the lowest among the reported values for the similar ST-OSCs devices. By adjusting the thickness of MgF 2 , ST-OSCs with different colors can be obtained, the peak transmittance of which is over 32% and the PCE loss rate is less than 7.25%. This report provides a new approach to solve the trade-off between efficiency and transmittance of ST-OSCs.
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JOURNAL OF DENTISTRY
·
2023
·
IF 4.4
Tiantian Guo,Mengyu Yang,Dai Wang,Jing Zheng,Sherry Shiqian Gao
Background Glass ionomer cement (GIC) is a commonly used restorative material in dentistry , but GIC does not have significant antibiofilm effects and its mechanical strength is limited. Objective To investigate the antibiofilm and mechanical properties of a newly developed silver nanowire (AgNW) modified GIC. Methods GICs were modified with different nanosilver formulations including 0.05%wt AgNW, 0.5%wt AgNW, 0.05%wt silver nanoparticle (AgNP) and 0.5%wt AgNP. Biofilms of Streptococcus mutans were cultured for 72 h on GIC specimens. Scanning electron microscopy (SEM) was conducted to observe the accumulation and morphology of Streptococcus mutans on the material surfaces. Another set of biofilm/specimens was treated with SYTO-9 and the biofilm development was evaluated by quantifying the visible stain with an inverted fluorescence microscope. The compressive strength of the specimens was assessed according to ISO 9917–1:2007. The colour of GICs was compared using the VITA Easyshade system. Results SEM images showed that fewer biofilms were accumulated on nanosilver-modified GICs. The Streptococcus mutans quantity was significantly lower in all nanosilver-modified groups compared to conventional GIC ( p <0.0001). GIC modified with 0.5% AgNP showed slightly lower compressive strength than the negative control (58.3 ± 12.9 MPa vs 78.3 ± 13.8 MPa); but there is no significant difference between all study groups. The colour change between AgNW-modified GIC and conventional GIC was significantly lower than that between AgNP-modified GIC and conventional GIC. Conclusion AgNW-modified GIC showed superior antibiofilm effect and comparable compressive strength to conventional GIC. In addition, the complement of AgNW would not influence the colour stability of GIC as much as AgNP. Clinical Significance This study developed a novel AgNW-modified GIC material. It showed good antibiofilm and mechanical properties and would not influence the colour stability of GIC. The AgNW-modified GIC has a large potential for clinical use and biomedical application.
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Joule
·
2023
·
IF 39.8
Tiancheng He,Haiyan Wang,Bing Lu,Tianlei Guang,Ce Yang,Yaxin Huang,Huhu Cheng,Liangti Qu
Ubiquitous moisture is of particular attraction for sustainable power generation. However, rigorous assembly procedures limit the efficient large-scale integration for moisture-enabled electric generators (MEGs). Herein, we develop fully printed planar MEG (PMEG) arrays using modulated polycation and polyanion inks, which maximize access to moisture and make it free of strict assembly and device packaging. Thus, a PMEG unit (only 0.3 cm 2 ) generates an open-circuit voltage of up to 1.1 V, along with a power density of 2.6 μW cm −2 . A small piece of sheet with 200 PMEG units offers a maximum voltage of 200 V and a current of 1.3 mA. A standard power module is constructed to meet the on-demand power supply requirements of compact electronics. Furthermore, scalable and customizable PMEG arrays can be compatibly integrated with flexible circuits, as demonstrated by a fully printed self-powered functional system including PMEG arrays and energy-storage and electrochromic devices.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Kaiqi Liu,Luminita Marin,Xinjian Cheng
In this work, fluorescent β- cyclodextrin (β-CD) based probes containing naphthalimide group were synthesized to realize the specific recognition of Hg 2+ /Hg + in aqueous system. Firstly, three small fluorescent molecules (N1, N2 and N3) with -NH 2 groups were synthesized from 4-bromo-1, 8-naphthalene anhydride . Secondly, CH CCH 2 - group was introduced into β-CD by Williamson ether formation reaction. Finally, the target probes (β-CD-PI, β-CD-PY and β-CD-TP) were obtained by Amino-Yne click reaction. These probes can efficiently recognize Hg 2+ /Hg + . β-CD-PI emits bright yellow fluorescence after binding with Hg 2+ /Hg + , which is a turn-on fluorescent probe . When the Hg 2+ /Hg + concentration exceeds 26 μM, the fluorescence intensity amplifies sharply (20 folds). The hydrophobic parts of the probes aggregated together to form a micelle-like structure due to complexation with Hg 2+ /Hg + , resulting in special micelle-sensitizing properties. Meanwhile, the HOMO-LUMO energy levels of the probes were calculated by cyclic voltammetry (CV). The probe is expected to be used for the detection of Hg 2+ /Hg + in aqueous solutions without any organic solvents.
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Advanced Science
·
2023
·Vol. 10
·期 28
·2302976
·
IF 15.1
Jianhua Xiao,Yang Wang,Liu Yuan,Yin Long,Zhi Jiang,Qingxia Liu,Deen Gu,Weizhi Li,Huiling Tai,Yadong Jiang
The recent emergence of non-fullerene acceptors (NFAs) has energized the field of organic photodiodes (OPDs) and made major breakthroughs in their critical photoelectric characteristics. Yet, stabilizing inverted NF-OPDs remains challenging because of the intrinsic degradation induced by improper interfaces. Herein, a tin ion-chelated polyethyleneimine ethoxylated (denoted as PEIE-Sn) is proposed as a generic cathode interfacial layer (CIL) of NF-OPDs. The chelation between tin ions and nitrogen/oxygen atoms in PEIE-Sn contributes to the interface compatibility with efficient NFAs. The PEIE-Sn can effectively endow the devices with optimized cascade alignment and reduced interface defects. Consequently, the PEIE-Sn-OPD exhibits properties of anti-environmental interference, suppressed dark current, and accelerated interfacial electron extraction and transmission. As a result, the unencapsulated PEIE-Sn-OPD delivers high specific detection and fast response speed and shows only slight attenuation in photoelectric performance after exposure to air, light, and heat. Its superior performance outperforms the incumbent typical counterparts (ZnO, SnO 2 , and PEIE as the CILs) from metrics of both stability and photoelectric characteristics. This finding suggests a promising strategy for stabilizing NF-OPDs by designing appropriate interface layers.
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Advanced Healthcare Materials
·
2023
·Vol. 12
·期 24
·2202707
·
IF 10
Kai Li,Yuting Zhu,Qiang Zhang,Yahong Shi,Tun Yan,Xi Lu,Huizhen Sun,Tingting Li,Zhongxian Li,Xiaoli Shi,Dong Han
Injectable hydrogels have been extensively used in tissue engineering where high mechanical properties are key for their functionality at sites of high physiological stress. In this study, an injectable, conductive hydrogel is developed exhibiting remarkable mechanical strength that can withstand a pressure of 500 kPa (85% deformation rate) and display good fatigue resistance, electrical conductivity, and tissue adhesion. A stable covalent cross-linked network with a slip-ring structure by threading amino β -cyclodextrin is formed onto the chain of a four-armed (polyethylene glycol) amino group, and then reacted with the four-armed (polyethylene glycol) maleimide under physiological conditions. The addition of silver nanowires enhances the hydrogel's electrical conductivity, enabling it to act as a good conductor in vivo. The hydrogel is injected into the fascial space, and the results show that the weight and muscle tone of the atrophied gastrocnemius muscle improve, subsequently alleviating muscle atrophy. Overall, this study provides a simple method for the preparation of a conductive hydrogel with high mechanical properties. In addition, the interstitial injection provides a strategy for the use of hydrogels in vivo.
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Materials Today Physics
·
2023
·
IF 11.5
Wen-Fa Chen,Xiao-Ming Jiang,Bin-Wen Liu,Guo-Cong Guo
Infrared (IR) nonlinear optical (NLO) material with a concurrently wide band gap and significant NLO coefficient in a single crystal is an incompatible but addressable challenge. Hence, for the first time, the AgGaS 2 structure evolved into an Ag-based sulfide system integrating dual s -block elements, guiding the discovery of two NLO crystals named AMgAgGa 6 S 11 (A = K, 1 ; Rb, 2 ). Structurally, title phases possess a novel NLO functional motif [AgGa 6 S 17 ] assembled by two C 2 -type supertetrahedra through a shared [AgS 4 ] tetrahedron, in which the electropositive cations A + and Mg 2+ are embedded. Thus, compounds 1 and 2 display emulative band gaps (3.15 and 3.25 eV, exceeding that of 2.65 eV in AgGaS 2 ) toward optimizing the laser-induced damage thresholds (3.1 and 3.2 × AgGaS 2 @1064 nm). Remarkably, the noncentrosymmetric phases 1 and 2 exhibit moderate second-harmonic generation (SHG) responses (0.6 and 0.7 × AgGaS 2 @1910 nm), the greater-than-commercial half of the AgGaS 2 . To the best of our current knowledge, an experimental birefringence of 1 and 2 (0.029 and 0.027, @546 nm) is first observed in quinary ordered chalcogenides , indicating that samples 1 and 2 meet phase-matching conditions at the incident laser of 1910 nm. All these observations demonstrate that crystals 1 and 2 can become prospective NLO materials. This research will pave the way for discovering excellent IR NLO crystals with wide band gaps and impressive NLO coefficients by incorporating multiple strong electropositive elements into chalcogenides .
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Journal of the American Chemical Society
·
2022
·
IF 16.383
Ling Luo,Linan Wang,Jianbang Chen,Jiazheng Zhou,Zhihua Yang,Shilie Pan,Junjie Li
Large second-harmonic generation (SHG) response and broad band gap are two important and competitive parameters. It is difficult to balance them out in one material. In this work, by coupling alkali earth metal (AEM) octahedra with large highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap and nonlinear optical (NLO)-active tetrahedra units, nine noncentrosymmetric (NCS) compounds, belonging to a new quaternary chalcogenide family AIB3IIC3IIIQ8VI with unique windmill-like [Mg3M3IIIQ24] (MIII = Al, Ga; Q = S, Se) units constructed by alternated [MgQ6] octahedra and [MIIIQ4] tetrahedra, are rationally designed and fabricated. The compounds show a stable structural framework but adjustable optical properties. Among them, NaMg3Ga3Se8 shows a large SHG response (∼1 × AgGaS2 (AGS)), wide band gap (in selenide) (2.77 eV), high laser-induced damage threshold (LIDT) (∼2.3 × AGS), and suitable birefringence (0.079@546 nm). It should be a potential candidate for infrared (IR) nonlinear optical (NLO) materials. The results enrich the chemical diversity of chalcogenides and open an avenue for the development of new IR NLO materials through the octahedra and tetrahedra coupled strategy.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhiqiang Shi,Shuyue Wu,Siyuan Lin,Jia Sun,Han Huang,Deming Kong,Yongli Gao,Conghua Zhou
Silver nanowire based transparent conductor is expected to be widely used in optoelectronic devices. However, when used in perovskite solar cells, it suffers from heavy corrosion caused by the lead halide hybrid perovskite. To solve the problem, nickel electroplating is used to modify the transparent conductor in this study. It is observed that nickel electroplating not only improves the conductance, but also upgrades the corrosion resistance and the oxidization resistance of the transparent conductor. In addition, SnO 2 quantum dots are applied to flatten the conductor surface, while ITO sputtering is used to further improve the film conductance. After that, perovskite solar cells are fabricated on the modified transparent conductors. Current-voltage curves scanning under simulated irradiation shows that, power conversion efficiency of 18.37 % is achieved. Transient photocurrent / photovoltage decay curves and impedance spectroscopy tests show that, nickel treated transparent conductors could ensure efficient charge-extraction process, while retard charge recombination. Storage-stability of the devices is monitored, 80 % of initial performance is reserved after storage in dark for 432 h. The study paves the way for the application of silver nanowire basing transparent conductor in devices when heavy corrosion is involved.
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