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Developing high performance catalysts for electrochemical water splitting is critical for an efficient and sustainable route to hydrogen production. For this, single-atom catalysts (SACs) are the best candidates, as they offer the highest atom efficiency. However, current methods to produce SACs involve a complex synthesis, often requiring multiple lengthy and expensive steps and yielding an insufficient density of single atoms. Here, we report a one-step chemical vapor deposition (CVD) synthesis to produce free-standing (FS) electrodes with Ni SACs on a matrix of sulfur-doped carbon nanofibers (CNFs), referred to as SACs@nanocarbon. The mechanism is based on a temperature-controlled delamination of thin films, with Au in contact with a SiO2 substrate, leading to the nucleation and growth of SACs@nanocarbon. Advanced characterization methods indicate the presence of Ni and Au single atoms and larger gold aggregates on the CNF matrix surface. These non-platinum group metal (non-PGM) electrodes showed exceptional performance for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). They performed for over 20 000 cycles with negligible change in overpotential at higher currents, with low onset overpotentials of 305 mV at 10 mA cm−2 for the OER and 40 mV at 17 mA cm−2 for the HER. The overpotential decreased to 195 mV at a current density of 100 mA cm−2. Remarkably, the electrode performance improved over cycling, while gold was dissolving in the electrolyte. This novel synthesis yielding SACs@nanocarbon could pave the way for the development of non-PGM, high performance electrodes for many other electrocatalytic applications. Additionally, the new paradigm of temperature-controlled delamination of thin films could be used to synthesize new materials. [ABSTRACT FROM AUTHOR]

Lithiated transition metal oxides are the most important cathode materials for lithium‐ion batteries. Many efforts have been devoted in recent years to improving their energy density, stability, and safety, as demonstrated by thousands of publications. However, the commercialization of several promising materials is limited due to obstacles like stability limitations. To overcome the limitations of energetically high‐voltage or high‐capacity cathode materials, unconventional solutions for their surface engineering were suggested; among them, metal–organic frameworks (MOFs) and zeolites have been employed. MOFs possess favorable characteristics for stabilization goals, including manageable structures, topological control, high porosity, large surface area, and low density. This review article explores promising strategies for improving the electrochemical behavior of favorable cathode materials through surface modifications by using MOFs and zeolites. Investigating the potential of this frameworks‐based surface engineering for high energy density batteries' electrodes is essential for optimal control of their surface chemistry. It may be highly effective to upgrade the performance of high‐energy cathode materials, thus extending the practical use of very high energy density rechargeable batteries. [ABSTRACT FROM AUTHOR]

The high concentration of antibiotics in aquatic environments is a serious environmental issue. In response, researchers have explored photocatalytic degradation as a potential solution. Through chemical vapor deposition (CVD), we synthesized copper selenide (β-Cu2−xSe) and found it an effective catalyst for degrading tetracycline hydrochloride (TC-HCl). The catalyst demonstrated an impressive degradation efficiency of approximately 98% and a reaction rate constant of 3.14 × 10−2 min−1. Its layered structure, which exposes reactive sites, contributes to excellent stability, interfacial charge transfer efficiency, and visible light absorption capacity. Our investigations confirmed that the principal active species produced by the catalyst comprises O2− radicals, which we verified through trapping experiments and electron paramagnetic resonance (EPR). We also verified the TC-HCl degradation mechanism using high-performance liquid chromatography–mass spectrometry (LC-MS). Our results provide valuable insights into developing the β-Cu2−xSe catalyst using CVD and its potential applications in environmental remediation. [ABSTRACT FROM AUTHOR]

Raman spectroscopy in transition metal dichalcogenides (TMDCs) helps determine their structural information and layer dependency. Because it is non‐destructive and fast, it is an archetypal spectroscopic technique to investigate the structure and defects in TMDCs. In our earlier study, we used a metal‐dielectric coating to enhance Raman signal of WS2 because the Raman Spectra measured from WS2 coated on the standard Si/SiO2 was significantly lower. This metal‐dielectric coating allowed access to the otherwise unavailable E12g and A1g modes of WS2. In this study, we compare the Raman spectra of WS2 on a Si/SiO2 to that of metal layers (Au [200 nm] and Al [200 nm]). A significant enhancement in the Raman signal of 2‐3L WS2 is observed for both the Au and Al coatings. Although 200 nm Au coating enhances the Raman Signal better than the 10 nm Au coating, it does not resolve the other signature vibrations other than E12g and A1g. Whereas, coating based on Al (200 nm) and Al (10 nm) both enhance the Raman signal of WS2. In the case of Al coating, we report well‐resolved vibrational modes such as the ones below <300 cm−1in a few layered WS2. This enhancement allows us to quantify the number of layers and also investigate the presence of defects. Photoluminescence measurements on 2–3L and 15L WS2 on Al (200 nm) confirm this. [ABSTRACT FROM AUTHOR]

Correction for 'High performance, binder-free electrodes with single atom catalysts on doped nanocarbons for electrochemical water splitting synthesized using one-step thermally controlled delamination of thin films' by Efrat Shawat Avraham et al., J. Mater. Chem. A, 2024, https://doi.org/10.1039/D4TA04701J. [ABSTRACT FROM AUTHOR]

We designed a heterostructure of Fe3S4@Ni3S2, as a potent oxygen evolution reaction (OER) electrocatalyst in an alkaline medium. Intriguingly, Fe3S4@Ni3S2 exhibits low onset potential of 290 mV and overpotential of 360 mV at a current density of 10 mA cm−2. We examined the OER kinetics of Fe3S4@Ni3S2 using distribution function of relaxation times (DFRT), which are attained with the help of impedance spectroscopy genetic programming (ISGP). ISGP reveals the occurrences of three events of OER, manifested as peaks in the DFRT, such as active material or pores (P2), charge transfer (P1'), and production rate of intermediates (P1) in case of Fe3S4@Ni3S2 at different faradic overpotentials. The effective resistance of each phenomenon can be easily calculated. It decreases with an increase in conductivity at high overpotentials for all the three, which suggests the high performance of the as‐synthesized composite due to faster kinetics. Further, structural investigation of the catalyst employing x‐ray photoelectron spectroscopy is elaborated and it is suggested that the catalyst activation takes place by the constant exchange of anions between electrode and electrolyte during electrochemical oxidation. [ABSTRACT FROM AUTHOR]

Transition-metal dichalcogenides (TMDCs) are unique layered materials with exotic properties. So, examining their structures holds tremendous importance. 2H-MoSe 2 (analogous to MoS 2 ; Gr. 6 TMDC) is a crucial optoelectronic material studied extensively using Raman spectroscopy. In this regard, low-frequency Raman (LFR) spectroscopy can probe this material's structure as it reveals distinct vibration modes. Here, we focus on understanding the microstructural evolution of different 2H-MoSe 2 morphologies and their layers using LFR scattering. We grew phase-pure 2H-MoSe 2 (with variable microstructures) directly on a Mo foil using a two-furnace ambient-pressure chemical vapor deposition (CVD) system by carefully controlling the process parameters. We analyzed the layers of exfoliated flakes after ultrasonication and drop-cast 2H-MoSe 2 of different layer thicknesses by choosing different concentrations of 2H-MoSe 2 solutions. Further detailed analyses of the respective LFR regions confirm the presence of newly identified Raman signals for the 2H-MoSe 2 nanosheets drop-cast on Raman-grade CaF 2 . Our results show that CaF 2 is an appropriate Raman-enhancing substrate compared to Si/SiO 2 as it presents new LFR modes of 2H-MoSe 2 . Therefore, CaF 2 substrates are a promising medium to characterize in detail other TMDCs using LFR spectroscopy., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

We report a facile and robust room-temperature NO 2 sensor fabricated using bi- and multi-layered 2H variant of tungsten di-selenide (2H-WSe 2 ) nanosheets, exhibiting high sensing characteristics. A simple liquid-assisted exfoliation of 2H-WSe 2 , prepared using ambient pressure chemical vapor deposition, allows smooth integration of these nanosheets on transducers. Three sensor batches are fabricated by modulating the total number of layers (L) obtained from the total number of droplets from a homogeneous 2H-WSe 2 dispersion, such as ∼2L, ∼5-6L, and ∼13-17L, respectively. The gas-sensing attributes of 2H-WSe 2 nanosheets are investigated thoroughly. Room temperature (RT) experiments show that these devices are specifically tailored for NO 2 detection. 2L WSe 2 nanosheets deliver the best rapid response compared to ∼5-6L or ∼13-17L. The response of 2L WSe 2 at RT is 250, 328, and 361% to 2, 4, and 6 ppm NO 2 , respectively. The sensor showed nearly the same response toward low NO 2 concentration even after 9 months of testing, confirming its remarkable long-term stability. A selectivity study, performed at three working temperatures (RT, 100, and 150 °C), shows high selectivity at 150 and 100 °C. Full selectivity toward NO 2 at RT confirms that 2H-WSe 2 nanosheet-based sensors are ideal candidates for NO 2 gas detection.

We report a facile two-furnace APCVD synthesis of 2H-WSe 2 . A systematic study of the process parameters is performed to show the formation of the phase-pure material. Extensive characterization of the bulk and exfoliated material confirm that 2H-WSe 2 is layered (i.e., 2D). X-ray diffraction (XRD) confirms the phase, while high-resolution scanning electron microscopy (HRSEM), high-resolution transmission electron microscopy (HRTEM), and atomic force microscopy (AFM) clarify the morphology of the material. Focused ion beam scanning electron microscopy (FIB-SEM) estimates the depth of the 2H-WSe 2 formed on W foil to be around 5-8 μm, and Raman/UV-vis measurements prove the quality of the exfoliated 2H-WSe 2 . Studies on the redox processes of lithium-ion batteries (LiBs) show an increase in capacity up to 500 cycles. On prolonged cycling, the discharge capacity up to the 50th cycle at 250 mA/g of the material shows a stable value of 550 mAh/g. These observations indicate that exfoliated 2H-WSe 2 has promising applications as an LiB electrode material., Competing Interests: The authors declare no competing financial interest., (Copyright © 2020 American Chemical Society.)