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Hydrogen energy is a high-efficiency and clean energy, but the problem of storage still prevents its extensive use. Large-surface-area, two-dimensional (2D) layered materials have an advantage in hydrogen storage applications. Monolayer MoS2 is a typical 2D material that has been widely studied recently. And the 1T' phase of MoS2 is a focus especially for studies concerning hydrogen. Here, first-principles calculations are carried out to investigate the adsorption behaviors of hydrogen molecules on 1T' MoS2. Comparing with other MoS2-based materials, such as doped or decorated 2H-MoS2, 1T' MoS2 has even better performance in hydrogen adsorption, and its preparation is easier. In multiple hydrogen molecule adsorption, the material shows good stability and appropriate adsorption energy while adsorbing hydrogen molecules. With the researches in this paper, the connection between the adsorption energy and hydrogen mass fraction was set up. This can provide a reference for further studies on hydrogen storage applications.
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InAs doping superlattice-based solar cells have great advantages in terms of the ability to generate clean energy in space or harsh environments. In this paper, multi-period InAs doping superlattice solar cells have been prepared.. Current density-voltage measurements were taken both in the dark and light, and the short-circuit current was estimated to be 19.06 mA/cm2. Efficiency improvements were achieved with a maximum one sun AM 1.5 G efficiency of 4.14%. Additionally, external quantum efficiency and photoluminescence with different temperature-dependent test results were taken experimentally. The corresponding absorption mechanisms were also investigated.
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The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built-in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2OâS@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g-1 h-1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g-1 h-1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p-n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials-by-design of high-performance heterojunctions.
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Photodetectors with a broad-band response range are widely used in many fields and are regarded as pivotal components of the modern miniaturized electronics industry. However, commercial broad-band photodetectors composed of traditional bulk semiconductor materials are still limited by complex preparation techniques, high costs, and a lack of mechanical strength and flexibility, which are difficult to satisfy the increasing demand for flexible and wearable optoelectronics. Therefore, researchers have been devoted to finding new strategies to obtain flexible, stable, and high-performance broad-band photodetectors. In this work, a novel self-assembled BiGaSeAs composite superlattice-structured nanowire was developed with a simple chemical vapor deposition method for easy fabrication. After the device assembling, the photodetector showed outstanding performance in terms of obvious Ion/Ioff (13.9), broad-band photoresponse (365-940 nm), excellent responsivity (1007.67 A/W), high detectivity (9.38 × 109 Jones), and rapid response (21 and 23 ms). The formation of microheterojunctions among various materials inside the nanowires also contributed to their extended broad-spectrum response and outstanding detection ability. These results indicate that the BiGaSeAs nanowires have potential applications in the field of flexible and wearable electronics.
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With their fascinating properties, emerging two-dimensional (2D) materials offer innovative ways to prepare high-performance infrared (IR) detectors. However, the current performance of 2D IR photodetectors is still below the requirements for practical application owing to the severe interfacial recombination, sharply raised contact resistance, and deteriorated metal conductivity at nanoscale. Here, we introduce a vertical barrier heterojunction with a structure of PtSe2/GaAs that combines the excellent optoelectronic properties of transition metal sulfides with topological semi-metals, which allows for an adjustable bandgap and high carrier mobility. The heterojunction was fabricated using the wet transfer method. The heterostructures show significant rectification behaviors and photovoltaic effects, which allow it to operate as a self-driven photodetector at zero bias. The photoresponse parameters at 850 nm with zero bias voltage are 67.2 mA W-1, 6.7 × 1012 Jones, 9.8%, 3.8 × 105, 164 µs, and 198 µs for the responsivity, specific detectivity, external quantum efficiency, Ilight/Idark ratio, rise time, and fall time, respectively. Moreover, the heterojunction is highly sensitive to a wide spectral band from ultraviolet to near-infrared (360-1550 nm). At the same time, this heterostructure demonstrates significant potential for applications in IR polarized light detection and room-temperature high-resolution IR imaging. The excellent properties of the heterojunction make it well-suited for high-performance, self-powered IR detection.
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The construction of heterojunction photocatalysts is an effective method to improve photocatalytic efficiency since the potential gradient and built-in electron field established at the junction could enhance the efficiency of charge separation and interfacial charge transfer. Nevertheless, heterojunction photocatalysts with strong built-in electron fields remain difficult to build since the two adjacent constitutes must be satisfied with an appropriate band alignment, redox potential, and carrier concentration gradient. Here, an efficient charge transfer-induced doping strategy is proposed to enhance the heterojunction built-in electron field for stable and efficient photocatalytic performance. Carrier transfer tests show that the rectification ratio of the n-TiO2-X/n-BiOI heterojunction is significantly enhanced after being coated with graphene oxide (GO). Consequently, both the hydrogen production and photodegradation performance of the GO composite heterojunction are considerably enhanced compared with pure TiO2-X, BiOI, and n-TiO2-X/n-BiOI. This work provides a facile method to prepare heterojunction photocatalysts with a high catalytic activity.
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Hydrogen-air proton exchange membrane fuel cells (PEMFCs) and direct methanol fuel cells (DMFCs) are excellent fuel cells with high limits of energy density. However, the low carbon monoxide (CO) tolerance of the Pt electrode catalyst in hydrogen-air PEMFCs and methanol permanent in DMFCs greatly hindered their extensive use. Applying polybenzimidazole (PBI) membranes can avoid these problems. The high thermal stability allows PBI membranes to work at elevated temperatures when the CO tolerance can be significantly improved; the excellent methanol resistance also makes it suitable for DMFCs. However, the poor proton conductivity of pristine PBI makes it hard to be directly applied in fuel cells. In the past decades, researchers have made great efforts to promote the proton conductivity of PBI membranes, and various effective modification methods have been proposed. To provide engineers and researchers with a basis to further promote the properties of fuel cells with PBI membranes, this paper reviews critical researches on the modification of PBI membranes in both hydrogen-air PEMFCs and DMFCs aiming at promoting the proton conductivity. The modification methods have been classified and the obtained properties have been included. A guide for designing modifications on PBI membranes for high-performance fuel cells is provided.
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Hydrogen is a clean energy with high efficiency, while the storage and transport problems still prevent its extensive use. Because of the large specific surface area and unique electronic structure, two-dimensional materials have great potential in hydrogen storage. Particularly, monolayer 2H-WS2 has been proven to be suitable for hydrogen storage. But there are few studies concerning the other two phases of WS2 (1T, 1T') in hydrogen storage. Here, we carried out first-principle calculations to investigate the hydrogen adsorption behaviors of all the three phases of WS2. Multiple hydrogen adsorption studies also evaluate the hydrogen storage abilities of these materials. Comprehensive analysis results show that the 1T'-WS2 has better hydrogen storage performance than the 2H-WS2, which means phase engineering could be an effective way to improve hydrogen storage performance. This paper provides a reference for the further study of hydrogen storage in two-dimensional materials.
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Two-dimensional transition metal disulfides such as MoS2 and WS2 exhibit multiple phases. Altering their phase makes it possible to change their chemical and physical properties significantly. Although several phase-induced modification mechanisms have been reported, their effects on the gas-sensing performance of these substrates remain unknown. Here, the effects of phase selection on the gas-sensing characteristics of 1T' and 2H monolayer MoS2 and WS2 were explored using a density functional theory-based first-principles approach. The theoretical computations took into account the binding energy, band structure, theoretical recovery time, density of states, electron difference density, and total electron density. The results showed that there is a significant change in the density of states near the Fermi level as well as greater charge transfer between the gas in question and the substrate when the gas is adsorbed onto 1T' MoS2 and WS2. Thus, phase selection is important for improving the gas-sensing performance of monolayer MoS2 and WS2. This study provides theoretical evidence for increasing the sensing performance of polymorph films of these materials.
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Two-dimensional transition metal dichalcogenides (2D TMDs), such as WS2, are considered to have the potential for high-performance gas sensors. It is a pity that the interaction between gases and pristine 2D WS2 as the sensitive element is too weak so that the sensor response is difficult to detect. Herein, the sensing capabilities of Al- and P-doped WS2 to NO, NO2, and SO2 were evaluated. Especially, we considered selectivity to target gases and dopant concentration. Molecular models of the adsorption systems were constructed, and density functional theory (DFT) was used to explore the adsorption behaviors of these gases from the perspective of binding energy, band structure, and density of states (DOS). The results suggested that doping atoms could increase the adsorption strength between gas molecules and substrate. Besides, the sensitivity of P-doped WS2 to NO and NO2 was hardly affected by CO2 or H2O. The sensitivity of Al-doped WS2 to NO2 and SO2 was also hard to be affected by CO2 or H2O. For NO detection, the WS2 with 7.4% dopant concentration had better sensitive properties than that with a 3.7% dopant concentration. While for SO2, the result was just the opposite. This work provided a comprehensive reference for choosing appropriate dopants (concentration) into 2D materials for sensing noxious gases.
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In this paper, we report a novel catalyst using Ni2P as a cocatalyst of Pt supported on graphene for methanol oxidation. The results reveal that the electrocatalytic activity and stability of the as-prepared catalyst for methanol oxidation are significantly enhanced by the addition of Ni2P. The reason for the increased activity and stability is ascribed to complex electron transfer between Pt, Ni2P, and graphene, which gives rise to the eventual promotion of COads electrooxidation reaction kinetics. The present study implies that the as-prepared Pt-Ni2P/graphene will be a promising candidate as an anode electrocatalyst in direct methanol fuel cells.
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When using water splitting to achieve sustainable hydrogen production, low-cost, stable, and naturally abundant electrocatalysts are required to replace Pt-based ones for the hydrogen evolution reaction (HER). Herein, for the first time, a novel nanostructure with one-dimensional (1D) MoS2/Ni3S2 nanoarrays directly grow on a three-dimensional (3D) Ni foam is developed for this purpose, showing excellent catalytic activity and stability. The as-prepared 3D MoS2/Ni3S2/Ni composite has an onset overpotential as low as 13 mV in 1 M KOH, which is comparable to Pt-based electrocatalyst for HER. According to the classical theory, the Tafel slope of the new composite is relatively low, as it goes through a combined Volmer-Heyrovsky mechanism during hydrogen evolution. All the results attribute the excellent electrocatalytic activity of the nanostructure to the electrical coupling among Ni, Ni3S2, and MoS2, the super hydrophilic interface, the synergistic catalytic effects produced by the MoS2/Ni3S2 nanoarrays, and abundant exposed active edge sites. These unique and previously undeveloped characteristics of the 3D MoS2/Ni3S2/Ni composite make it a very promising earth-abundant electrocatalyst for HER.
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Unique hybrid nanostructure, which consists of multi-wall carbon nanotube (MWCNT) stems and MoS2 nanosheet (NS) leaves, are prepared by a hydrothermal method. The fabricated material can be potentially used as an electrocatalyst for the hydrogen evolution reaction (HER). To our knowledge, as the reaction medium, water is firstly utilized to the synthesis of the 1T phase MoS2 NSs which uniformly grow on the carbon-based materials. As a result, a nanohybrid catalyst with excellent HER electrocatalytic properties, which included an onset potential of as low as 50 mV, a Tafel slope of 43 mV dec-1, and remarkable cycling stability, is produced. The observed outstanding catalytic performance can be attributed to the uniform distribution of the metallic 1T phase of the MoS2 NSs, which are characterized by the presence of multiple active edges as well as the effective electron transport route provided by the conductive MWCNT substrate. This work demonstrates the high potential of the synthesized HER catalyst and proposes a novel, efficient, environmentally friendly, and inexpensive method for its fabrication.
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Molybdenum disulfide nanosheets/reduced graphene oxide (MoS2 NSs/rGO) nanohybrid as a highly effective catalyst for hydrogen evolution reaction (HER) have been successfully synthesized by a facile microwave-assisted method. The results clearly reveal that direct grown of MoS2 NSs on rGO have been achieved. Electrochemical tests show that the as-prepared hybrid material exhibited excellent HER activity, with a small Tafel slope of 57 mV dec-1, an overpotential of 130 mV and remarkable cycling stability. After analysis, the observed outstanding catalytic performance can be attributed to the uniform distribution of the MoS2 NSs, which are characterized by the presence of multiple active sites as well as the effective electron transport route provided by the conductive rGO substrate. Moreover, according to the classic theory, the mechanism governing of the catalytic HER on the MoS2 NSs/rGO nanohybrid has been clarified.
Asunto(s)
Disulfuros/química , Técnicas Electroquímicas/métodos , Grafito/química , Hidrógeno/química , Molibdeno/química , Óxidos/química , Catálisis , Microscopía Electrónica de Transmisión , Difracción de Rayos XRESUMEN
Advanced approaches to preparing non-noble-metal electrocatalysts for the hydrogen evolution reaction (HER) are considered to be a significant breakthrough in promoting the exploration of renewable resources. In this work, a hybrid material of MoS2 nanoflowers (NFs) on reduced graphene oxide (rGO) was synthesized as a HER catalyst via an environmentally friendly, efficient approach that is also suitable for mass production. Small-sized MoS2 NFs with a diameter of ca. 190 nm and an abundance of exposed edges were prepared by a hydrothermal method and were subsequently supported on rGO by microwave-assisted synthesis. The results show that MoS2 NFs were distributed uniformly on the remarkably reduced GO and preserved the outstanding original structural features perfectly. Electrochemical tests show that the as-prepared hybrid material exhibited excellent HER activity, with a small Tafel slope of 80 mV/decade and a low overpotential of 170 mV.