Wen-Jin Yin

R-graphyne: a new two-dimensional carbon allotrope with versatile Dirac-like point in nanoribbons

A novel two-dimensional carbon allotrope, rectangular graphyne (R-graphyne) with tetra-rings and acetylenic linkages, is proposed by first-principles calculations. Although the bulk R-graphyne exhibits metallic property, the nanoribbons of R-graphyne show distinct electronic structures from the bulk. The most intriguing feature is that band gaps of R-graphene nanoribbons oscillate between semiconductor and metal as a function of width. Particularly, the zigzag edge nanoribbons with half-integer repeating unit cell exhibits unexpected Dirac-like fermions in the band structures. The Dirac-like fermions of the R-graphyne nanoribbons originate from the central symmetry and two sub-lattices. The extraordinary properties of R-graphene nanoribbons greatly expand our understanding on the origin of Dirac-like point. Such findings uncover a novel fascinating property of nanoribbons, which may have broad potential applications for carbon-based nano-size electronic devices.

CO2 Capture and Conversion on Rutile TiO2(110) in the Water Environment: Insight by First-Principles Calculations.

The conversion of CO2 by the virtue of sunlight has the great potential to produce useful fuels or valuable chemicals while decreasing CO2 emission from the traditional fossil fuels. Here, we use the first-principles calculations combined with the periodic continuum solvation model (PCSM) to explore the adsorption and reactivity of CO2 on rutile TiO2(110) in the water environment. The results exhibit that both adsorption structures and reactivity of CO2 are greatly affected by water coadsorption on rutile TiO2(110). In particular, the solvation effect can change the most stable adsorption configuration of CO2 and H2O on rutile TiO2(110). In addition, the detailed conversion mechanism of CO2 reduction is further explored in the water environment. The results reveal that the solvation effect cannot only greatly decrease the energy barrier of CO2 reduction but also affect the selectivity of the reaction processes. These results presented here show the importance of the aqueous solution, which should be helpful to understand the detailed reaction processes of photocatalysts.

High performance NiO nanosheets anchored on three-dimensional nitrogen-doped carbon nanotubes as a binder-free anode for lithium ion batteries

Transition metal oxides (TMOs) have attracted extensive research attention as promising anode materials for lithium ion batteries due to their high theoretical capacities. However, their applications have been hindered by their poor electronic conductivity and drastic volume change in the reversible conversion reaction. Here three-dimensional NiO ultrathin nanosheets were grown on the composites of N-doped carbon nanotubes (N-CNTs) and Ni foam by chemical vapor deposition and electrochemical deposition methods, and the 3D Ni foam/N-CNT/NiO nanosheet electrode thus obtained exhibits larger capacity, better cycling stability, superior rate capability and higher ionic conductivity. The first-principles calculations suggest that N-doping can improve the interaction between NiO and N-CNTs, which can facilitate fast electron hopping from N-CNTs to NiO to enhance the electronic conductivity. The results indicate that the introduction of N-doped carbon nanotubes can greatly improve the electrochemical performance of NiO. The understanding between N-CNTs and NiO can be extended to the preparation of N-CNTs coated with other high-performance electrode materials for energy-storage devices.

Electronic structures and optical properties of two-dimensional ScN and YN nanosheets

Two-dimensional (2D) materials exhibit different electronic properties than their bulk materials. Here, we present a systematic study of 2D tetragonal materials of ScN and YN using density functional theory calculations. Several thermodynamically stable 2D tetragonal structures were determined, and such novel tetragonal structures have good electronic and optical properties. Both bulk ScN and YN are indirect band gap semiconductors while the electronic structures of 2D ScN and YN are indirect gap semiconductors, with band gaps of 0.62–2.21 eV. The calculated optical spectra suggest that 2D tetragonal ScN and YN nanosheets have high visible light absorption efficiency. These electronic properties indicate that 2D ScN and YN have great potential for applications in photovoltaics and photocatalysis.

The Effect of Excess Electron and hole on CO2 Adsorption and Activation on Rutile (110) surface.

CO2 capture and conversion into useful chemical fuel attracts great attention from many different fields. In the reduction process, excess electron is of key importance as it participates in the reaction, thus it is essential to know whether the excess electrons or holes affect the CO2 conversion. Here, the first-principles calculations were carried out to explore the role of excess electron on adsorption and activation of CO2 on rutile (110) surface. The calculated results demonstrate that CO2 can be activated as CO2 anions or CO2 cation when the system contains excess electrons and holes. The electronic structure of the activated CO2 is greatly changed, and the lowest unoccupied molecular orbital of CO2 can be even lower than the conduction band minimum of TiO2, which greatly facilities the CO2 reduction. Meanwhile, the dissociation process of CO2 undergoes an activated CO2− anion in bend configuration rather than the linear, while the long crossing distance of proton transfer greatly hinders the photocatalytic reduction of CO2 on the rutile (110) surface. These results show the importance of the excess electrons on the CO2 reduction process.

Spatial separation of photo-generated electron-hole pairs in BiOBr/BiOI bilayer to facilitate water splitting

The electronic structures and photocatalytic properties of bismuth oxyhalide bilayers (BiOX1/BiOX2, X1 and X2 are Cl, Br, I) are studied by density functional theory. Briefly, their compositionally tunable bandgaps range from 1.85 to 3.41 eV, suitable for sun-light absorption, and all bilayers have band-alignments good for photocatalytic water-splitting. Among them, heterogeneous BiOBr/BiOI bilayer is the best as it has the smallest bandgap. More importantly, photo-excitation of BiOBr/BiOI leads to electron supply to the conduction band minimum with localized states belonging mainly to bismuth of BiOBr where the H+/H2 half-reaction of water-splitting can be sustained. Meanwhile, holes generated by such photo-excitation are mainly derived from the iodine states of BiOI in the valence band maximum; thus, the O2/H2O half-reaction of water splitting is facilitated on BiOI. Detailed band-structure analysis also indicates that this intriguing spatial separation of photo-generated electron-hole pairs and the two half-reactions of water splitting are good for a wide photo-excitation spectrum from 2–5 eV; as such, BiOBr/BiOI bilayer can be an efficient photocatalyst for water-splitting, particularly with further optimization of its optical absorptivity.

Atomic structure and electronic properties of folded graphene nanoribbons: A first-principles study

Folded graphene nanoribbons (FGNRs) have attracted great attentions because of extraordinary properties and potential applications. The atomic structure, stacking sequences, and electronic structure of FGNRs are investigated by first-principle calculations. It reveals that the common configurations of all FGNRs are racket-like structures including a nanotube-like edge and two flat nanoribbons. Interestingly, the two flat nanoribbons form new stacking styles instead of the most stable AB-stacking sequences for flat zone. The final configurations of FGNRs are greatly affected by the initial interlayer distance, stacking sequences, and edge styles. The stability of folded graphene nanoribbon depends on the length, and it can only be thermodynamically stable when it reaches the critical length. The band gap of the folded zigzag graphene nanoribbons becomes about 0.17 eV, which provides a new way to open the band gap.

Progress of theoretical research on titanium dioxide and water interface

Titanium dioxide (TiO 2 ) have excellent electrical properties and unique optical properties, which has broad application prospects in optical materials, photoelectrochemical and photovoltaic cells, photo catalysis and environmental governance. However, these functions achieved needs in aqueous environments, so it is very important to study on TiO 2 -water interfacial interaction. Now, people can discuss and understand TiO 2 and water problems at the atomic level with the development of computing method and theory. Especially the quantum chemistry calculation method based on the first principle, is very suitable to study and solve the fundamental problem with TiO 2 -water interface, such as the water molecules adsorbed structure and dynamics research at the interface. In this article we review current understanding of TiO 2 -water interfaces from first-principles calculations, and forecast its development prospect.

Low-dimensional ScO2 with tunable electronic and magnetic properties: first-principles studies.

Transition metal dichalcogenides (TMDs) have attracted extensive attention due to their appealing properties for device applications. In this work, we explored the structure stability, electronic structure and magnetism of low-dimensional scandium dioxides, ScO2, by using the first-principles calculations. The results demonstrate that bulk ScO2, monolayers and nanoribbons (NRs) are thermodynamically stable, implying a high possibility of fabricating ScO2 nanocrystals in experiments. Despite the metallic characteristics of bulk ScO2, low-dimensional ScO2 possesses various electronic behaviors that can be further modulated by crystal structure and dimensionality. The results also show that the ground states of ScO2 monolayers and NRs are ferromagnetic (FM) with about 1 μ B per ScO2 formula. Our studies expand a new realm in low-dimensional TMDs, with tunable electronic and magnetic properties.

Resonant splitting in periodic T-shaped photonic waveguides

Resonant splitting phenomena of photons in periodic T-shape waveguide structure are investigated by the Greens function method. It is found that, except for the (n-1)-fold resonant splitting in the low frequency region, (n-2)-fold resonant splitting occurs in the high frequency region of the transmission spectra. The (n-2)-fold resonant splitting peaks are induced by the high quasi-bound states where the photons are mainly localized in the constrictions rather than in the stubs. To this kind of quasi-bound state, the stub acts as a potential barrier rather than a well, which is the inverse of the case of the low quasi-bound states corresponding to the (n-1)-fold splitting peaks. These resonant peaks can be modulated by adjusting the periodic number and geometry of the waveguide structures.