Yangfan Shao

Synergistic effect of 2D Ti2C and g-C3N4 for efficient photocatalytic hydrogen production

Photocatalytic water splitting is an environmentally friendly technique for hydrogen production. In this work, we report a novel photocatalyst consisting of two-dimensional (2D) titanium carbide (Ti2C) and graphitic carbon nitride (g-C3N4). We observe substantially enhanced water splitting activities due to the efficient synergistic interaction between Ti2C and g-C3N4. Optimal properties are achieved in the g-C3N4 with a loading of 0.4 wt% Ti2C with a hydrogen production rate of 47.5 μmol h−1, which is 14.4 times as much as that in the case using pure g-C3N4, and it even outperforms Pt-loaded g-C3N4. We further show that the Ti2C/g-C3N4 has high stability and good reproducibility. We expect that the Ti2C/g-C3N4 can be a photocatalyst for large scale applications because both Ti2C and g-C3N4 are low-cost, abundant, and nontoxic.

Ultra-high electrocatalytic activity of VS2 nanoflowers for efficient hydrogen evolution reaction

It is a great challenge to explore cheap, abundant and eco-friendly electrocatalysts for hydrogen evolution reaction (HER). Here, we report the fabrication of VS2 nanoflowers with 1T phase by a simple hydrothermal method and their electrocatalytic performance in the HER. We find that the VS2 nanoflowers show comparable HER performance to Pt in acids, including an ultra-low onset potential of 32 mV, a Tafel slope of 34 mV dec−1 which resembles that of Pt, and a small overpotential of 58 mV (54 mV for Pt) at a current density of 10 mA cm−2. High stability and almost 100% faradaic efficiency indicate the practical application of VS2 nanoflowers in the HER. Our first-principles calculations reveal that the thermoneutral Gibbs free energy of hydrogen adsorption on both the basal and edge sites of the 1T-VS2 monolayer can be achieved under certain hydrogen coverage and the monolayer shows good conductivity, which contribute to the impressive catalytic performance of VS2 nanoflowers. We expect that the VS2 nanostructures may be applicable in electrocatalysis with high efficiency.

Exploring new two-dimensional monolayers: pentagonal transition metal borides/carbides (penta-TMB/Cs)

The development of two-dimensional (2D) materials with high conductivity and catalytic activity is important for the proposed hydrogen economy. Herein, we design a new family of 2D monolayers, pentagonal transition-metal borides/carbides (penta-TMBs and penta-TMCs), as electrocatalysts for the hydrogen evolution reaction (HER) on the basis of density functional theory (DFT). We find that all of the stable 2D penta-TMBs/TMCs are metallic, and 2D WB and HfC are ferromagnetic metals. We demonstrate that penta-TMBs and penta-TMCs show high catalytic performance for the HER. The Gibbs free energy for the adsorption of hydrogen atoms on catalyst surfaces (such as WB and ZrC) is close to the ideal value of zero electron volt (eV). Our findings highlight a new family of promising noble metal-free HER catalysts and provide new insight into the design of advanced 2D materials.

Fullerene/layered antiferromagnetic reconstructed spinterface: Subsurface layer dominates molecular orbitals’ spin-split and large induced magnetic moment

The interfaces between organic molecules and magnetic metals have gained increasing interest for both fundamental reasons and applications. Among them, the C60/layered antiferromagnetic (AFM) interfaces have been studied only for C60 bonded to the outermost ferromagnetic layer [S. L. Kawahara et al., Nano Lett. 12, 4558 (2012) and D. Li et al., Phys. Rev. B 93, 085425 (2016)]. Here, via density functional theory calculations combined with evidence from the literature, we demonstrate that C60 adsorption can reconstruct the layered-AFM Cr(001) surface at elevated annealing temperatures so that C60 bonds to both the outermost and the subsurface Cr layers in opposite spin directions. Surface reconstruction drastically changes the adsorbed molecule spintronic properties: (1) the spin-split p-d hybridization involves multi-orbitals of C60 and top two layers of Cr with opposite spin-polarization, (2) the subsurface Cr atom dominates the C60 electronic properties, and (3) the reconstruction induces a large magnetic moment of 0.58 μB in C60 as a synergistic effect of the top two Cr layers. The induced magnetic moment in C60 can be explained by the magnetic direct-exchange mechanism, which can be generalized to other C60/magnetic metal systems. Understanding these complex hybridization behaviors is a crucial step for molecular spintronic applications.