Two-dimensional transition metal carbides, carbonitrides, and nitrides, called MXenes, exhibit high metallic conductivity, ion intercalation capability, and reversible redox activity, prompting their applications in energy storage and conversion, electromagnetic interference (EMI) shielding, and electronics, among many other fields. It has been shown that replacement of ∼50% of carbon atoms in the most popular MXene family member, titanium carbide (Ti3C2Tx), by nitrogen atoms, forming titanium carbonitride (Ti3CNTx), leads to drastically different properties. Such properties include very high negative charge in solution and extreme EMI shielding effectiveness, exceeding all known materials, even metals at comparable thicknesses. Here, by using ultraviolet photoemission spectroscopy (UPS), the electronic structures of Ti3CNTx and Ti3C2Tx are systematically investigated and compared as a function of charge carrier density. We observe that, in contrast to Ti3C2Tx, the Ti 3p core-level of Ti3CNTx exhibits a counterintuitive shift to a lower binding energy of up to ∼250 meV upon increasing the electron density, which is a spectroscopic signature of negative electronic compressibility (NEC). These experimentally measured chemical potential shifts are well captured by the density functional theory (DFT) calculation. The DFT results also further suggest that the hybridization of titanium–nitrogen bonding in Ti3CNTx helps to promote the available states of Ti atoms for receiving more electrons above the fermi level and leads to the observed NEC. Our findings explain the differences in electronic properties between the two very important and widely studied MXenes and also suggest a new strategy to apply the NEC effect of Ti3CNTx in energy and charge storage applications.
By using angle-resolved photoemission spectroscopy (ARPES), the variation of the electronic structure of HfSe2 has been studied as a function of sodium intercalation. We observe how this drives a band splitting of the p-orbital valence bands and a simultaneous reduction of the indirect band gap by values of up to 400 and 280 meV respectively. Our calculations indicate that such behaviour is driven by the band deformation potential, which is a result of our observed anisotropic strain induced by sodium intercalation. The applied uniaxial strain calculations based on density functional theory (DFT) agree strongly with the experimental ARPES data. These findings should assist in studying the physical relationship between doping and strain, as well as for large-scale two-dimensional straintronics.
Water electrolysis has received much attention in recent years as a means of sustainable H 2 production. However, many challenges remain in obtaining high-purity H 2 and making large-scale production costeffective. This study provides a strategy for integrating a two-cell water electrolysis system with solar energy storage. In our proposed system, CuO-Cu(OH) 2 /Cu 2 O was used as a redox mediator between oxygen and hydrogen evolution components. The system not only overcame the gasmixing issue but also showed high gas generation performance. The redox reaction (charge/discharge) of CuO-Cu(OH) 2 /Cu 2 O led to a significant increase (51%) in the initial rate of H 2 production from 111.7 μmol h −1 cm −2 in the dark to 168.9 μmol h −1 cm −2 under solar irradiation. The effects of light on the redox reaction of CuO-Cu(OH) 2 /Cu 2 O during water electrolysis were investigated by in situ X-ray absorption and photoemission spectroscopy. These results suggest that surface oxygen vacancies are created under irradiation and play an important role in increased capacitance and gas generation. These findings provide a new path to direct storage of abundant solar energy and low-cost sustainable hydrogen production.
In this work, we study and compare the photo-induced conductivity of a two-dimensional electron gas (2DEG) at the bare surface of SrTiO3 (STO) and in the heterostructure of BiFeO3 (BFO) and STO, where BFO was deposited by radio frequency magnetron sputtering. The photo-induced conductance of the BFO/STO interface shows a large increase which is 20.62 times more than the sum of photo-induced conductance from each individual BFO thin film and STO crystal. Since this photo-induced conductance of the BFO/STO heterostructure can be adjusted to become higher and lower by applying an electric field to the top surface, we attribute this large increase to the strong photo-induced electrical polarization of BFO. With the two-point setup of positive bias and negative bias, the conductivity also exhibits diode-like behavior where the forward and backward resistances are different. This work provides methods to interplay between light irradiation, electric field, and conductivity in all-oxide electronics.
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