Entropy engineering has emerged as a promising paradigm for tailoring the electronic and photoelectric properties of materials. Although high-entropy transition metal sulfides have been achieved, entropy engineering in two-dimensional (2D) tellurides remains challenging. In this work, we report the successful synthesis of a 1T' monolayer heptanary medium-entropy (ME) alloy (MoaWbFecCodSxSeyTez) via a one-step chemical vapor deposition method. Advanced characterizations, including scanning transmission electron microscopy, energy dispersive X-ray spectroscopy, and electron energy loss spectroscopy confirm the uniform atomic-level distribution of the seven constituent elements within the alloy. The 1T' ME alloy device exhibits a high drain current of ~ 6.5 mA, which is 216 times higher than the ~ 30 μA observed in pristine 1T' MoTe2. Furthermore, the 1T' ME alloy photodetector exhibits responsivities of 27.92 A/W at 1064 nm and 63.74 A/W at 1550 nm, outperforming those of the pristine 1T' MoTe2 by more than two orders of magnitude. This remarkable enhancement is attributed to the reduced Schottky barrier (15.9 meV) at the 1T' ME alloy/electrode interface, along with the enhanced conductance (0.43 S) and reduced thermal activation energy (4.1 meV) in the 1T' ME alloy, collectively facilitating more efficient carrier injection and transport. Our work provides a distinct pathway for tailoring the properties of transition metal dichalcogenides through entropy engineering and offers valuable insights for the design of high-performance infrared photodetectors.
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The remarkable advantages of heterojunction engineering have injected significant vitality into the design of high-performance electromagnetic wave absorption (EWA) materials. Understanding interface effects, rather than semi-empirical rules, can facilitate the rational design of heterostructures, thereby enabling effective modulation of impedance matching and the EWA properties of materials. Herein, FeTe@expanded graphite (FeTe@EG) heterostructures are in-situ constructed via a one-step chemical vapor deposition (CVD) method, which effectively generates abundant Mott–Schottky heterojunctions and exhibit a strong built-in electric field (BIEF) effect. The optimal sample, featuring only 10 wt.% filler content and a thickness of 1.8 mm, achieved an effective absorption bandwidth (EAB) of 4.6 GHz and a minimum reflection loss (RLmin) of −63.8 dB. Density functional theory (DFT) calculations and finite element simulations demonstrate that the BIEF effectively modulates charge separation, promotes electron migration, and ultimately improves polarization relaxation loss, leading to superior EWA performance. This study elucidates the intrinsic mechanism by which the FeTe-based heterojunction couples with polarization responses, providing a feasible strategy for the design of lightweight, efficient, and high-performance electromagnetic wave absorbers based on other high-density transition metal telluride (TMT) materials.
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Electrocatalytic hydrogen evolution reaction (HER) faces challenges in alkaline due to competitive adsorption of *OH and *H at the same active site, which hinders H2 generation. Single-atom alloys (SAAs), particularly Ni-based systems like NiPt1 SAAs, show considerable performance through dual-site mechanisms, where Ni adsorbs *OH while Pt facilitates H2 desorption. However, *OH blockage on Ni hinders *OH desorption and triggers slow water dissociation kinetics. Herein, supported NiPt1 alloy nanoclusters embedded with Ni3ZnC0.7 (Ni3ZnC0.7@NiPt1) are synthesized through pyrolysis of zeolitic imidazolate framework-8 (ZIF-8)@Ni coordination compound (ZIF-8@NCC) coupled with Pt galvanic replacement reactions. Experiments and calculations reveal that the embedded Ni3ZnC0.7 modulates electronic structure of Ni, promoting *OH desorption and enhancing water dissociation. Thus, supported Ni3ZnC0.7@NiPt1 achieves exceptional low overpotential (η10 = 23 mV) and high mass activity (MA50 = 1.67 mA·μgPt−1) in alkaline, which remarkably surpass Ni@NiPt1 (η10 = 127 mV and MA50 = 0.101 mA·μgPt−1). The corresponding alkaline anion-exchange membrane water electrolyzer (AEMWE) requires only 1.91 V at 1 A·cm−2, demonstrating industrial viability. This work provides new insights into addressing *OH blockage on SAAs catalysts in alkaline HER.
Intrinsic ferroelectric materials play a critical role in the development of high-density integrated device. Despite some two-dimensional (2D) ferroelectrics have been reported, the research on one-dimensional (1D) intrinsic ferroelectric materials remains relatively scare since 1D atomic structures limit their van der Waals (vdW) epitaxy growth. Here, we report the synthesis of 1D intrinsic vdW ferroelectric SbSI nanowires via a confined-space chemical vapor deposition. By precisely controlling the partial vapor pressure of I2 and reaction temperature, we can effectively manipulate kinetics and thermodynamics processes, and thus obtain high quality of SbSI nanowires, which is determined by Raman spectroscopy and high-resolution scanning transmission electron microscopy characterizations. The ferroelectricity in SbSI is confirmed by piezo-response force microscopy measurements and the ferroelectric transition temperature of 300 K is demonstrated by second harmonic generation. Moreover, the in-plane polarization switching can be maintained in the thin SbSI nanowires with a thickness of 20 nm. Our prepared 1D vdW ferroelectric SbSI nanowires not only enrich the vdW ferroelectric systems, but also open a new possibility for high-power energy storage nanodevices.
Aggregation of polyoxometalates (POM) is largely responsible for the reduced performance of POM-based energy-storage systems. To address this challenge, here, the precise confinement of single Keggin-type POM molecule in a porous carbon (PC) of unimodal super-micropore (micro-PC) is realized. Such precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM, which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron redox-activity. In particular, the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical calculation. Meanwhile, the molecularly dispersed POM molecules confined steadily in the "cage" of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of ~11.4 wt%. As a result, the fabricated solid-state supercapacitor achieves a remarkable areal capacitance, ultrahigh energy and power density of 443 mF cm−2, 0.12 mWh cm−2 and 21.1 mW cm−2, respectively. This work establishes a novel strategy for the precise confinement of single POM molecule, providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.
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