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Composites composed of a chlorophyll‐a derivative and Ti3C2Tx MXene recently showed promising results as photocatalysts for the hydrogen evolution reaction. Herein, this type of composites is prepared by using a layered Ti3C2Tx material via an HCl@LiF etching technique, instead of the previously adopted HF etching technique. The performance of H2 evolution, therefore, showed a fourfold increase in this photocatalytic system, compared with the reported data in our previous works. The underlying reason for such a large improvement of the chlorophyll‐MXene photocatalyst performance would be attributed to a more suitable surface chemistry, higher conductivity, fewer defects, higher surface area, and larger interlayer space of Ti3C2Tx introduced by the Li+ ions from LiF in the etching process. Herein, it is revealed that the preparation method of MXenes used as the cocatalysts is key to improve the H2 evolution efficiency in photocatalytic water splitting. [ABSTRACT FROM AUTHOR]

The Z‐scheme process is a photoinduced electron‐transfer pathway in natural oxygenic photosynthesis involving electron transport from photosystem II (PSII) to photosystem I (PSI). Inspired by the interesting Z‐scheme process, herein a photocatalytic hydrogen evolution reaction (HER) employing chlorophyll (Chl) derivatives, Chl‐1 and Chl‐2, on the surface of Ti3C2Tx MXene with two‐dimensional accordion‐like morphology, forming Chl‐1@Chl‐2@Ti3C2Tx composite, is demonstrated. Due to the frontier molecular orbital energy alignments of Chl‐1 and Chl‐2, sublayer Chl‐1 is a simulation of PSI, whereas upper layer Chl‐2 is equivalent to PSII, and the resultant electron transport can take place from Chl‐2 to Chl‐1. Under the illumination of visible light (>420 nm), the HER performance of Chl‐1@Chl‐2@Ti3C2Tx photocatalyst was found to be as high as 143 μmol h−1 gcat−1, which was substantially higher than that of photocatalysts of either Chl‐1@Ti3C2Tx (20 μmol h−1 g−1) or Chl‐2@Ti3C2Tx (15 μmol h−1 g−1). [ABSTRACT FROM AUTHOR]

The unique properties of MXenes that arise from terminating functional groups and oxidation of MXenes make them attractive for application in photovoltaic devices like perovskite solar cells (PSCs). Here, oxidation of Ti3C2Tx hydrocolloid was carried out to tune its properties desirable for an electron transport layer (ETL) in low-temperature processed PSCs. The calculations of the energy levels were carried out using the Vienna ab initio simulation package (VASP) code based on density functional theory (DFT). Oxidation of Ti3C2Tx can generate Ti–O bonds and effectively reduce the macroscopic defects of the film fabricated by spin-coating, while a transition from metallic material to semiconductor occurred after heavy oxidation. A better matching of energy levels between perovskite and ETL layer in the case of a hybrid of oxidized and pristine Ti3C2Tx renders a champion power conversion efficiency (PCE) of 18.29%. The improvement in PCE can be attributed to the increased electron mobility in the ETL, which promotes electron transport and reduces the electron–hole recombination. Hence, by presenting a simple method for high performance in PSCs by MXene-derived materials, this work demonstrates the great potential of these materials for applications in low-temperature processed PSCs and other photovoltaic technologies. [ABSTRACT FROM AUTHOR]

MXenes derived from 413 MAX phases are rarely studied but they have the potential to have superior electrical and mechanical properties thanks to a thicker monolayer (four layers of transition metal and three layers of carbon or nitrogen). In this paper, Nb4C3Tx MXene nanosheets are delaminated and freestanding film with 1.77 nm interlayer spacing is obtained, which is larger than that of most previous MXenes. When Nb4C3Tx freestanding films are tested as supercapacitors electrodes, Nb4C3Tx shows high volumetric capacitance, 1075, 687, and 506 F cm−3 in 1 m H2SO4, 1 m KOH, and 1 m MgSO4, respectively, at the scan rate of 5 mV s−1. An in situ X‐ray diffraction technique is used to study the structural changes during the electrochemical charging in 1 m H2SO4 and 1 m MgSO4. There is almost no change in the 21 Å interlayer spacing during the cycling, because the space between the MXene layers is sufficient to accommodate the insertion and deinsertion of cations. This can lead to stable performance of Nb4C3Tx MXene energy storage devices. [ABSTRACT FROM AUTHOR]

Efficient photocatalytic hydrogen evolution reaction (HER) in the visible‐to‐near infrared region at a low cost remains a challenging issue. This work demonstrates the fabrication of organic‐inorganic composites by deposition of supramolecular aggregates of a chlorophyll derivative, namely, zinc methyl 3‐devinyl‐3‐hydroxymethyl‐pyropheophorbide a (Chl) on the surface of Ti3C2Tx MXene with 2D accordion‐like morphology. This composite material is employed as noble metal‐free catalyst in photocatalytic HER under the white light illumination, where Chl serves as a small molecule organic semiconductor component instead of ordinary inorganic and polymer organic semiconductors such as TiO2 and g‐C3N4, and Ti3C2Tx serves as a co‐catalyst. Different composition ratios of Chl/Ti3C2Tx are compared for their light‐harvesting ability, morphology, charge transfer efficiency, and photocatalytic performance. The best HER performance is found to be as high as 52 ± 5 µmol h−1 gcat−1 after optimization. Such a large HER activity is attributed to the efficient light harvesting followed by exciton transfer in Chl aggregates and the resultant charge separation at the interface of Chl/Ti3C2Tx. [ABSTRACT FROM AUTHOR]

2D carbides and nitrides (MXenes) are widely recognized for their exceptional promise for numerous applications. However, physical property measurements of their individual monolayers remain very limited despite their importance for revealing the intrinsic physical properties of MXenes. The first mechanical and electrical measurements of individual single‐layer flakes of Nb4C3Tx MXene, which are prepared via an improved synthetic method are reported. Characterization of field‐effect transistor devices based on individual single‐layer Nb4C3Tx flakes shows an electrical conductivity of 1024 ± 165 S cm−1, which is two orders of magnitude higher than the previously reported values for bulk Nb4C3Tx assemblies, and an electron mobility of 0.41 ± 0.27 cm2 V−1 s−1. Atomic force microscopy nanoindentation measurements of monolayer Nb4C3Tx membranes yield an effective Young's modulus of 386 ± 13 GPa, assuming a membrane thickness of 1.26 nm. This is the highest value reported for nanoindentation measurements of solution‐processable 2D materials, revealing the potential of Nb4C3Tx as a primary component for various mechanical applications. Finally, the agreement between the mechanical properties of 2D Nb4C3Tx MXene and cubic NbC suggests that the extensive experimental data on bulk carbides could be useful for identifying new MXenes with improved functional characteristics. [ABSTRACT FROM AUTHOR]