One-step Chemical Vapor Deposition Research Articles

A Two-in-One Strategy to Simultaneously Boost the Site Density and Turnover Frequency of Fe-N-C Oxygen Reduction Catalysts.

Site density and turnover frequency are the two fundamental kinetic descriptors that determine the oxygen reduction activity of iron-nitrogen-carbon (Fe-N-C) catalysts. However, it remains a grand challenge to simultaneously optimize these two parameters in a single Fe-N-C catalyst. Here we show that treating a typical Fe-N-C catalyst with ammonium iodine (NH4I) vapor via a one-step chemical vapor deposition process not only increases the surface area and porosity of the catalyst (and thus enhanced exposure of active sites) via the etching effect of the in-situ released NH3, but also regulates the electronic structure of the Fe-N4 moieties by the iodine dopants incorporated into the carbon matrix. As a result, the NH4I-treated Fe-N-C catalyst possesses both high values in the site density of 2.15×1019 sites g-1 (×2 enhancement compared to the untreated counterpart) and turnover frequency of 3.71 electrons site-1 s-1 (×3 enhancement) that correspond to a high mass activity of 12.78 A g-1, as determined by in-situ nitrite stripping technique. Moreover, this catalyst exhibits an excellent oxygen reduction activity in base with a half-wave potential (E1/2) of 0.924 V and acceptable activity in acid with E1/2 = 0.795 V, and superior power density of 249.1 mW cm-2 in zinc-air batteries.

One-step fabrication of high energy storage polymer films with a wide bandgap and high melting temperature induced by the fluorine effect for high temperature capacitor applications with ultra-high efficiency.

The development of polymer dielectrics with both high energy density and low energy loss is a formidable challenge in the area of high-temperature dielectric energy storage. To address this challenge, a class of polymers (Parylene F) are designed by alternating fluorinated aromatic rings and vinyl groups in the polymer chain to confine the conjugating sequence and broaden the bandgap with the fluorine effect. The target films with desired thickness, ultra-high purity, and a wide bandgap are facilely fabricated by a one-step chemical vapor deposition (CVD) technique from monomers. The symmetric and bulky aromatic structures exhibit high crystalline performance and excellent stability at high temperature. The presence of strongly electronegative fluorine atoms effectively enhances bandgap and electron trapping capability, which effectively reduces the conduction loss as well as the possibility of breakdown at high temperatures. CVD technology avoids the post-processing film-forming process, ensuring the fabrication of thin films with high quality. These benefits allow Parylene F films to effectively store electrical energy at temperature up to 150 °C, exhibiting a record discharged energy density of 2.92 J cm-3 at charge-discharge efficiency exceeding 90%. This work provides a new idea for the design and synthesis of all-organic polymer dielectric films for high temperature applications.

Dual chalcogenide coordination engineering on a self-supported alloy electrode for enhanced hydrogen evolution reaction.

The electrochemical hydrogen evolution reaction (HER) holds substantial promise for large-scale green hydrogen production due to its cost-effectiveness, high performance, and scalability for repeated implementation. A promising strategy that involves a novel transition-metal chalcogenide with a self-supported framework can improve the reaction kinetics in the HER. We synthesize a nano three-dimensional self-supported HER catalyst via a straightforward one-step chemical vapor deposition process. This method incorporates a dual co-reaction with sulfur (S) and selenium (Se) onto a commercially available Monel alloy (CNSSe). The dynamics ion exchange redox reactions promote the formation of heterogeneous catalyst structures. Density functional theory (DFT) calculations indicate that the CNSSe catalyst exhibits low hydrogen coverage, as evidenced by a thermoneutral free energy of adsorbed hydrogen (ΔGH*) of 0.105 eV, which can be attributed to the dual introduction of S and Se. Consequently, the optimized CNSSe electrocatalyst achieves an enhancement in HER performance exceeding 100% compared to catalysts introduced exclusively with either S or Se. These results underscore the substantial potential of the optimized CNSSe electrocatalyst to improve both the performance and economic feasibility of HER technologies in alkaline water electrolysis.

A Single-Crystal Antimony Trioxide Dielectric for 2D Field-Effect Transistors.

The remarkable potential of two-dimensional (2D) materials in sustaining Moore's law has sparked a research frenzy. Extensive efforts have been made in the research of utilizing 2D semiconductors as channel materials in field-effect transistors. However, the next generation of integrated devices requires the integration of gate dielectrics with wider bandgaps and higher dielectric constants. Here, insulating α-Sb2O3 single-crystal nanosheets are synthesized by one-step chemical vapor deposition method. Importantly, the α-Sb2O3 single-crystal dielectric exhibits a high dielectric constant of 11.8 and a wide bandgap of 3.78 eV. Besides, the atomically smooth interface between α-Sb2O3 and MoS2 enables the fabrication of dual-gated field-effect transistors with the top gate dielectric of α-Sb2O3 nanosheets. The field-effect transistors exhibit a switching ratio of exceeding 108, which achieves the manipulation of field-effect transistors by using 2D dielectric materials. These results hold significant implications for optimizing the performances of 2D devices and innovating microelectronics.

Controlled growth of two-dimensional MoS2/WSe2 heterostructure solar cell by chemical vapor deposition

The development of high-quality type II semiconductor heterostructures is crucial for solar energy conversion applications. Here, we report the sequential growth of MoS2/WSe2 two-dimensional semiconductor type II heterostructure using a one-step chemical vapor deposition. The morphological, Raman, and chemical analysis revealed that the WSe2 layer is deposited on the rhombus-shaped MoS2, forming a vertical MoS2/WSe2 heterostructure. The solar cell fabricated using the grown heterostructure exhibits a photovoltaic response with a conversion efficiency of 2.5 % and an open circuit voltage of 0.22 V, respectively. The numerical simulation study unravels the mechanism of charge separation and transport in the MoS2/WSe2 heterostructure solar cell.

Synthesis of MnFe-C core–shell nanoparticles with tunable microwave absorption performance by designing the Mn/Fe ratio

Metal-C nanoparticles with MnFe nanocores and their microwave absorption performances with design Mn/Fe ratios have been rarely reported in previous studies. In this work, MnFe-C core–shell nanoparticles with tunable Mn/Fe ratios were prepared by a one-step metal organic chemical vapor deposition method. It was found that the magnetic properties and microwave absorption performances of the nanoparticles could be well tunable by designing Mn/Fe ratios in their nanocores. These results suggest that the as-synthesized MnFe-C core–shell nanoparticles have great potential for microwave absorption applications.

Vapor Growth of All-Inorganic 2D Ruddlesden-Popper Lead- and Tin-Based Perovskites.

The 2D Ruddlesden-Popper (RP) perovskites Cs2PbI2Cl2 (Pb-based, n = 1) and Cs2SnI2Cl2 (Sn-based, n = 1) stand out as unique and rare instances of entirely inorganic constituents within the more expansive category of organic/inorganic 2D perovskites. These materials have recently garnered significant attention for their strong UV-light responsiveness, exceptional thermal stability, and theoretically predicted ultrahigh carrier mobility. In this study, we synthesized Pb and Sn-based n = 1 2D RP perovskite films covering millimeter-scale areas for the first time, utilizing a one-step chemical vapor deposition (CVD) method under atmospheric conditions. These films feature perovskite layers oriented horizontally relative to the substrate. Multilayered Cs3Pb2I3Cl4 (Pb-based, n = 2) and Cs3Sn2I3Cl4 (Sn-based, n = 2) films were also obtained for the first time, and their crystallographic structures were refined by combining X-ray diffraction (XRD) and density functional theory (DFT) calculations. DFT calculations and experimental optical spectroscopy support band-gap energy shifts related to the perovskite layer thickness. We demonstrate bias-free photodetectors using the Sn-based, n = 1 perovskite with reproducible photocurrent and a fast 84 ms response time. The present work not only demonstrates the growth of high-quality all-inorganic multilayered 2D perovskites via the CVD method but also suggests their potential as promising candidates for future optoelectronic applications.

Carbon nanofibers embedded in nanopores decorated graphite felt electrodes for enhanced vanadium redox flow batteries performance

This study introduces a novel electrode design, incorporating carbon nanofibers (CNFs) embedded in nanopores on graphite felt, achieved through a simplified one-step chemical vapor deposition process. The electrodes exhibit a uniform distribution of carbon nanofibers and nanopores, significantly enhancing active sites for vanadium redox reactions. Comprehensive characterization, including X-ray photoelectron spectroscopy (XPS) and Brunauer-Emmett-Teller (BET) surface area analysis, confirmed a significant increase in surface area and catalytic activity. When tested at a current density of 200 mA cm−2, the modified electrodes demonstrated a notable improvement in electrochemical performance, achieving over 75 % energy efficiency and maintaining this efficiency over 300 cycles. The cyclic voltammograms (CV) and electrochemical impedance spectroscopy (EIS) results indicated enhanced kinetics and reduced charge transfer resistance. Post-mortem SEM images confirmed the structural integrity of the nanofibers after extensive cycling tests.

One-step fabrication of P-Co5.47N/Co9S8@NPC heterojunction derived from saccharomycetes cerevisiae as environment-friendly bifunctional high-efficiency electrocatalysts

The one-step green preparation of heterojunction-structured bifunctional high-efficiency electrocatalysts provides a simple method for the green, low-cost, convenient and efficient application of hydrogen energy, meanwhile it is still challenging to achieve. In the present work, the phosphorus-doped two-phase heterojunction P-Co5.47N/Co9S8@NPC nanorods was synthesized on carbon cloth (CC) as a high-quality bifunctional electrode through simple one-step chemical vapor deposition (CVD) method. Saccharomycetes cerevisiae were used for the non-toxic phosphorus doping and formation of a carbon nanolayer wrapping Co5.47N/Co9S8 nanorods. Compared with the single-phase electrocatalyst Co9S8@NPC NSs/CC, P-Co5.47N/Co9S8@NPC NSs/CC exhibited more excellent electrocatalytic performance which required overpotentials of 69 mV for hydrogen evolution reaction (HER), 182.5 mV for oxygen evolution reaction (OER), 1.45 V for over water splitting (OWS) at 10 mA cm−2 in KOH solution. The designed P-Co5.47N/Co9S8@NPC NSs/CC presented multiple advantages of nanorod structure, doped structure, abundant heterointerfaces, as well as dual-phase synergy, which triggered outstanding electrocatalytic performance.

High-performance CsPbBr3-silicon heterojunction photodetectors fabricated by chemical vapor deposition

Inorganic perovskite cesium lead halide (CsPbBr3) has attracted extensive research attention due to its excellent photoelectric properties and long-term stability to water, oxygen, light and heat. In this work, high crystallinity CsPbBr3 microcrystals with different morphologies and grain sizes were synthesized by one-step chemical vapor deposition (CVD) on silicon (Si) wafers and silicon nanowires (SiNWs), respectively. Characterization results show that the CsPbBr3 microcrystals grown on SiNWs (CsPbBr3-SiNWs) display more compact and uniform morphologies than those grown on Si wafer (CsPbBr3-Si). Moreover, CsPbBr3-SiNWs exhibits higher detectivity and larger on/off ratio than CsPbBr3-Si, which are 5.1 × 1012 Jones over 3.4 × 1012 Jones, and 51.3 over 14.7, respectively. Furthermore, CsPbBr3-SiNWs shows a faster photo response with a rise/fall time of 0.22 s/0.28 s than 0.26 s/0.32 s in CsPbBr3-Si. In addition, the CsPbBr3-SiNWs photodetector maintained 90% of its original photocurrent after 60 days of exposure to air, showing excellent stability. These results strongly suggest a promising fabrication approach for constructing perovskite-based heterojunction optoelectronic devices with high performance and excellent stability.

Anti-fouling underwater superoleophobic membranes based on hierarchical double networks for high efficiency oil–water separation

Oil fouling is a key problem of superwettable oil–water separation membranes because the membranes are inevitably susceptible to varying degrees of oil contamination during the ongoing separation processes, which usually results in a severe impact on separation performance. Consequently, it is a great challenge to construct oil-removal membranes with superior resistance to oil contamination. Herein, we fabricated hierarchical double networks (HDT)-modified porous glass membrane with superhydrophilicity/underwater superoleophobicity. Firstly, a layer of silicone nanofilament (SNF) network bearing tremendous C = C double bonds were fabricated on a porous glass membrane surface by one-step chemical vapor deposition (CVD) using vinyltrichlorosilane (VTCS) as a precursor. Subsequently, the second network layer was constructed by copolymerization of the C = C double bonds on the SNF network and those in sulfobetaine-derived monomer (sulfobetaine methacrylate, SBMA), using N,N′-methylenebisacrylamide (MBA) as the cross-linkering agent. It was observed that the obtained HDT-modified glass membranes displayed excellent superhydrophilicity/underwater superoleophobicity accompanied with superior self-cleaning performance and oil-resistance properties. As a result, the HDT-modified membranes showed high separation flux and high efficiency for both oil/water mixtures (7500 L m−2h−1, above 99.98%) and surfactant-stabilized oil-in-water emulsions (1100 L m−2h−1, above 99.96%) with excellent cyclability. The outstanding advantages with characteristics of excellent oil resistance and superior separation performance enable the HDT-modified glass membrane promising applications in a wide range of industries related to oil–water separations.

Improving the capacitive performance of wood-derived carbon monolith by anchoring heteroatom-doped carbon nanotubes in the vessels via in situ chemical vapor deposition

Wood, with high carbon contents and abundant vertically oriented channels, has unique advantages in preparing high mass-loading carbon-based freestanding supercapacitor electrodes. However, there is considerable room for enhancing the capacitive performance of wood-derived carbon electrodes. A one-step chemical vapor deposition (CVD) method mediated by dicyandiamide using iron-based nanoparticles as catalysts was proposed to enhance the utilization of vertical channels in wood-based carbon electrodes and improve their pore structure and chemical composition. This approach aimed to fabricate composite electrodes with enhanced mass loading, interwoven conductive carbon nanotube networks, well-developed hierarchical porous structure, and abundant nitrogen/oxygen-containing functional groups. The effect of CVD temperature on the physical/chemical properties and capacitance performance of the composite material was investigated. Consequently, the optimal electrode (CW/NCNTs-800) attained a competitive initial specific capacitance of 5762 mF cm−2 at 5 mA cm−2 and demonstrated a satisfactory rate performance with the specific capacitance of 3520 mF cm−2 at 300 mA cm−2. In addition, the durable electrode demonstrated commendable cycle stability, maintaining a capacitance retention of 93 % through 30,000 cycles at 30 mA cm−2. This study on wood-derived high mass-loading supercapacitor electrodes can provide a novel perspective on the application of high-performance energy storage devices.

Effects of CaCO3/MgO on Fe-Co-Mo catalyst in the reprocessing of recycled polypropylene to carbon nanotubes

In recent times, there has been a global discourse on the menace of plastic waste (PW) materials on the ecosystem and ways for effective management of PW. This has resulted in the utilization of PW in the research arena in the synthesis of smart nanomaterials of high value as a sustainable solution. In this study, the catalytic-pyrolysis procedure was used to develop carbon nanotubes (CNTs) from recycled polypropylene (PP) plastic in a one-step chemical vapour deposition (CVD) reactor. The impacts of CaCO3 and MgO as supports for Fe-Co-Mo catalysts in the production of CNTs were studied. Kinetic and thermodynamic parameters were determined from the thermal profile of the catalysts to establish the nature of the reaction in CNTs synthesis. Transmission electron microscopy (TEM), energy Dispersive X-ray (EDX), selected area electron diffraction pattern, particle size distribution (PSD), thermogravimetric analysis (TGA), Raman spectroscopy, Fourier transforms infrared (FTIR) and X-ray diffraction (XRD) were employed to characterize the catalysts and CNTs. The results obtained showed the impact of the supports on the yield, quality, and morphology of the synthesized CNTs. The CNTs yield from catalysts supported with CaCO3 and MgO were 35.12 % and 37.24% respectively. The average outer diameters of CNTs produced over the catalyst with CaCO3 and MgO supports were 36 and 29 nm respectively. The ID/IG ratio for CaCO3 and MgO supports were 0.6724 and 0.8401 respectively. The change in entropy for all phases were −274.41 and −1032.97 J/mol/K and −213.0, −318.48 and −1022.13 J/mol/K for CaCO3 and MgO supported catalyst respectively which confirmed non-spontaneous endothermic reaction. It was observed that MgO support showed better catalytic activity toward CNTs growth in terms of yield while those with CaCO3 support showed higher graphitization.

Two-dimensional GeS synthesized by one-step space-confined APCVD and its self-powered photodetector

Germanium sulfide (GeS) is a notable two-dimensional (2D) layered material that has gained attention across various research domains. However, challenges remain in realizing large areas of high-quality 2D GeS, despite the efforts made. Recently, we have successfully synthesized rectangular 2D single-crystal GeS flakes with a thickness of about 52 nm and a lateral length of 100 μm by one-step space-confined atmospheric pressure chemical vapor deposition (APCVD) using sulfur and germanium powders as raw materials. There is a direct relationship between the area size and the growth time. The further prepared GeS device has good photoresponsivity in the visible range. At 532 nm, it includes a responsivity of 40 mA/W, a detectivity of 8 × 108 Jones and a fast response time of 199 ms. In addition, the GeS device exhibits p-type conductive behavior and a unique self-powered effect. After prolonged storage, the GeS photodetector still exhibits good and stable photoswitching characteristics.

Lead-free CsCu2I3 thin films prepared by one-step chemical vapor deposition method for ultraviolet photodetector

In recent years, inorganic lead-free perovskite materials have garnered attention for their non-toxicity, high carrier mobility, and strong light absorption capabilities, showing promising application prospects in photoelectric sensing. CsCu2I3 perovskite has been mentioned as one of the representatives and as a potential material for short-wavelength optoelectronic devices. This study employs a one-step chemical vapor deposition (CVD) process to fabricate CsCu2I3 thin films, which exhibit a vibrant yellow emission at 560 nm. Ultraviolet photodetectors utilizing CsCu2I3 films demonstrate an exceptional responsivity and a detectivity of 1.43 A/W and 1.15 × 1012 Jones (254 nm, 5 V bias), along with rapid response times (trise ≈ 50 ms, tdecay ≈ 70 ms). Moreover, this work examines the factors affecting device performance, including wavelength, operating voltage, and film thickness. It presents a straightforward, ecofriendly CVD method for producing lead-free perovskite films and optoelectronic devices, which has significant implications for the development of lead-free perovskite-based photoelectric technologies.

Band Gap Engineering of MoxW1-xS2 Alloy Monolayers with Wafer-Scale Uniformity.

Modulating the band gap of two-dimensional (2D) transition metal dichalcogenide (TMDC) semiconductors is critical for their application in a wider spectral range. Alloying has been demonstrated as an effective method for regulating the band gap of 2D TMDC semiconductors. The fabrication of large-area 2D TMDC alloy films with centimeter-scale uniformity is fundamental to the application of integrated devices. Herein, we report a liquid-phase precursor one-step chemical vapor deposition (CVD) method for fabricating a MoxW1-xS2 alloy monolayer with a large size and an adjustable band gap. Good crystalline quality and high uniformity on a wafer scale enable the continuous adjustment of its band gap in the range of 1.8-2.0 eV. Density functional theory calculations provided a deep understanding of the Raman-active vibration modes of the MoxW1-xS2 alloy monolayer and the change in the conductivity of the alloy with photon energy. The synthesis of large-area MoxW1-xS2 alloy monolayers is a critical step toward the application of 2D layered semiconductors in practical optoelectronic devices.

Controllable Synthesis of Transferable Ultrathin Bi2Ge(Si)O5 Dielectric Alloys with Composition-Tunable High-κ Properties.

Two-dimensional (2D) alloys hold great promise to serve as important components of 2D transistors, since their properties allow continuous regulation by varying their compositions. However, previous studies are mainly limited to the metallic/semiconducting ones as contact/channel materials, but very few are related to the insulating dielectrics. Here, we use a facile one-step chemical vapor deposition (CVD) method to synthesize ultrathin Bi2SixGe1-xO5 dielectric alloys, whose composition is tunable over the full range of x just by changing the relative ratios of the GeO2/SiO2 precursors. Moreover, their dielectric properties are highly composition-tunable, showing a record-high dielectric constant of >40 among CVD-grown 2D insulators. The vertically grown nature of Bi2GeO5 and Bi2SixGe1-xO5 enables polymer-free transfer and subsequent clean van der Waals integration as the high-κ encapsulation layer to enhance the mobility of 2D semiconductors. Besides, the MoS2 transistors using Bi2SixGe1-xO5 alloy as gate dielectrics exhibit a large Ion/Ioff (>108), ideal subthreshold swing of ∼61 mV/decade, and a small gate hysteresis (∼5 mV). Our work not only gives very few examples on controlled CVD growth of insulating dielectric alloys but also expands the family of 2D single-crystalline high-κ dielectrics.

Compositional design of C-coated multi-elemental alloy nanoparticles for superior microwave absorption

Exploring improved electromagnetic wave absorption performance in magnetic components involves capitalizing on dual dielectric relaxation and multiple magnetic resonances, ultimately giving rise to a dielectric-magnetic matching effect. Herein, a one-step Metal-organic Chemical Vapor Deposition (MOCVD) method has been utilized to fabricate C-coated ternary and quaternary alloy nanoparticles (FeCoNi, FeCoNiCu, FeCoNiMg, and FeCoNiMn) with tunable magnetization. The results affirm that the capabilities of impedance matching and electromagnetic wave attenuation can be significantly regulated by compositing nanoparticles with different elements. The optimized C-coated FeCoNiMg nanoparticles demonstrate an exceptional capacity for electromagnetic wave attenuation, achieving a reflection loss value of −51.8 dB at a matched thickness of 2.9 mm. Moreover, the absorption bandwidth significantly broadens to 7.60 GHz (10.4 – 18.0 GHz) with a thickness of 2.7 mm. The exceptional performance in electromagnetic attenuation is credited to the dielectric loss and improved impedance matching characteristics induced by the C-coated FeCoNiMg nanoparticles. The findings from this study will be beneficial in the development of lightweight and highly effective electromagnetic wave absorbers using magnetic alloy nanoparticles.

Core-shell designed high entropy alloy CoNiFeCuV-C nanoparticles for enhanced microwave absorption

The widespread interest in high entropy alloy nanostructures stems from their potential utilization in a variety of technological and scientific fields. This study presents an innovative approach employing a one-step metal organic chemical vapor deposition to synthesize quinary high entropy alloy (CoNiFeCuV-C) core-shell nanoparticles designed for microwave absorption applications. Superior microwave absorption performance is attained through the optimization of conduction loss via thermal treatment, coupled with the interfacial polarization across the interfaces between CoNiFeCuV cores and C shell. The paraffin composite filled with an optimal 20% content of CoNiFeCuV-C core-shell nanoparticles demonstrates a minimal reflection loss (RLmin) of −51.8 dB at 13.76 GHz, achieving this performance with a thickness of 2.2 mm. Moreover, the absorbing bandwidth spans 7.44 GHz at a thickness of 2.4 mm. The outstanding accomplishments underscore the potential of utilizing CoNiFeCuV-C core-shell nanoparticles as a promising choice for lightweight, effective microwave absorber material.

Thermal transport and optical anisotropy in CVD grown large area few-layer MoS2 over an FTO substrate

Atomically thin MoS2 is a promising candidate for its integration into devices due to its strikingly unique electronic, optical, and thermal properties. Here, we report the fabrication of a few-layer MoS2 thin film over a conducting fluorine-doped tin oxide-coated glass substrate via a one-step chemical vapor deposition method. We have quantitatively analyzed the nonlinear temperature-dependent Raman shift using a physical model that includes thermal expansion and three- and four-phonon anharmonic effects, which exhibits that the main origin of nonlinearity in both the phonon modes primarily arises from the three-phonon anharmonic process. We have also measured the interfacial thermal conductance (g) and thermal conductivity (ks) of the synthesized film using the optothermal Raman spectroscopy technique. The obtained values of g and ks are ∼7.218 ± 0.023 MW m−2 K−1 and ∼40 ± 2 W m−1 K−1, respectively, suggesting the suitability of thermal dissipation in MoS2 based electronic and optoelectronic devices. Furthermore, we performed a polarization study using the angle resolved polarized Raman spectroscopy technique under non-resonance and resonance excitations to reveal the electron–photon–phonon interaction in the prepared MoS2, based on the semi-classical theory that includes deformation potential and Fröhlich interaction. Our study provides much needed experimental information about thermal conductivity and polarization response in a few-layer MoS2 grown over the conducting substrate, which is relevant for applications in low power thermoelectric and optoelectronic devices.