Design of Frustrated Lewis Pair in Defective TiO2 for Photocatalytic Non-Oxidative Methane Coupling

The efficient C-H polarization is the prerequisite for the low-temperature photocatalytic CH4 conversion, which however is restricted by the poor stretching ability of short-distanced lattice atoms. Herein, frustrated Lewis pair (FLP) composed of doped ion in TiO2 as Lewis acid (LA) and neighboring Ti-OH as Lewis base (LB) with a long distance (0.31-0.37 nm) were designed through DFT calculation and fabricated by hydrogenation treatment of metal-doped TiO2-SiO2 with macroporous-mesoporous structure. Benefitting from the long LA-LB distance and matched acid-base intensity, hydrogenated Ga-doped composite achieves superior C-H stretching with a high CH4 conversion rate (139 µmol g−1 h−1) to ethane. The photo-irradiation causes the electron excitation from Ga to Ti-OH according to the time-dependent DFT calculation and in situ EPR analysis, which promotes the formation and coupling of ·CH3. This work provides a key underpinning for regulating the characteristics of FLP for C-H activation and C-C coupling via light irradiation.

Hydrogenation treatment under several gigapascals assists diffusionless transformation in a face-centered cubic steel

The use of hydrogen in iron and steel has the potential to improve mechanical properties via altering the phase stability and dislocation behavior. When hydrogen is introduced under several gigapascals, a stoichiometric composition of hydrogen can be introduced for steel compositions. In this study, a face-centered cubic (fcc) stainless steel was hydrogenated under several gigapascals. When the steel was not hydrogenated, the microstructure after depressurization was an fcc with a hexagonal close-packed (hcp) structure. In contrast, the hydrogenation treatment resulted in a fine lath body-centered cubic (bcc) structure arising from diffusionless transformation. In particular, the bcc phase formed through the following transformation sequence: fcc → hcp → dhcp (double hexagonal close-packed phase) → bcc. That is, the use of hydrogenation treatment realized fine microstructure evolution through a new type of diffusionless transformation sequence, which is expected to be used in future alloy design strategies for developing high-strength steels.

Reversible hydrogenation restores defected graphene to graphene

Graphene as a two-dimensional material is prone to hydrocarbon contaminations, which can significantly alter its intrinsic electrical properties. Herein, we implement a facile hydrogenation-dehydrogenation strategy to remove hydrocarbon contaminations and preserve the excellent transport properties of monolayer graphene. Using electron microscopy we quantitatively characterized the improved cleanness of hydrogenated graphene compared to untreated samples. In situ spectroscopic investigations revealed that the hydrogenation treatment promoted the adsorption ofytyt water at the graphene surface, resulting in a protective layer against the re-deposition of hydrocarbon molecules. Additionally, the further dehydrogenation of hydrogenated graphene rendered a more pristine-like basal plane with improved carrier mobility compared to untreated pristine graphene. Our findings provide a practical post-growth cleaning protocol for graphene with maintained surface cleanness and lattice integrity to systematically carry a range of surface chemistry in the form of a well-performing and reproducible transistor.

(Invited) Improve Electrodes' Electrochemical Performance for HER and OER By Hydrogenation Treatment

Hydrogen production through electrolysis has been regarded as one of the most promising solutions for large-scale production of clean fuels. However, most electrodes have large overpotentials in the HER and OER reactions during the water splitting process. Many approaches and methods have been developed to enhance the electrodes' performance. Here, we would like to present our studies on the hydrogenation of various electrode materials for HER and OER applications. We aim to reveal the structure-property-performance relationship for those electrodes after hydrogenation treatment. We wish our work could provide useful information and will be honored if our work can inspire new discovery and finding in the related fields to advance our understanding and technologies for efficient hydrogen production through electrolysis.

Study on the Effect of γ-Irradiation on Gadolinium Oxysulfide Nanophosphors (Gd2O2S-NPs)

Gadolinium oxysulfide nanophosphors (Gd2O2S-NPs) have been successfully synthesized using γ-irradiation and hydrogenation treatment. The primary stage of Gd2O2S-NPs synthesis was carried out using various doses of γ-irradiation to form diverse sizes of Gd2(SO4)3 precursor, followed by hydrogenation treatment at 900°C for 2 hours to form Gd2O2S-NPs. Then, the nanophosphors were characterized for the structure, morphology, and luminescence properties through X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), and photoluminescence spectrometer (PL). Pure hexagonal phase of Gd2O2S-NPs was obtained with high crystallinity and without any impurities. The morphologies were observed from grain-like nanostructures transformed to spherical shape as the irradiation dose reached 40 kGy. Besides, Gd2O2S-NPs which were prepared at highest irradiation dose of 40 kGy show highest intensity of emission peak at 548 nm and corresponded to Stark level transition from the GJ6 state of Gd3+ ion. It can be emphasized that the different doses of γ-irradiation influenced the nucleation event of Gd2(SO4)3 precursor thus affecting the morphology and size particles of Gd2O2S-NPs. Hence, from the results, it can be suggested that Gd2O2S-NPs can be a promising host for optical applications.