摘要：Conversion of inert N2 molecules into NH3 via electrochemical methods is an environmentally friendly alternative to replace the traditional Haber-Bosch ***,the development of highly efficient catalyst is still ***,we report a density functional theory(DFT)based high-throughput screening to investigate the potential of 23 atomic transition metals(Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Y,Zr,Nb,Mo,Tc,Ru,Rh,Pd,Ag,Cd,W,Pt and Au)supported on phosphorene monolayer as electrocatalyst for nitrogen reduction reaction(NRR).Our theoretical results demonstrate that V single atom anchoring on phosphorene monolayer exhibits good thermal stability,selectivity and excellent catalytic activity with a low overpotential of 0.18 ***,rational design principles and electronic descriptor between the intrinsic electronic properties and activation barrier have been *** work offers a new promising noble metal-free catalyst for NRR and reveals profound insights into the activity origin to guide further design.

摘要：As a clean and renewable future energy source, hydrogen fuel can be produced via solar water splitting. Two-dimensional (2D) black phosphorene (black-P) can harvest visible light due to the desirable band gap, which promises it as a metal-free photocatalyst. However, black-P can be only used to produce hydrogen since the oxidation potential of water locates lower than the position of the valence band maximum. To improve the photocatalytic performance of black-P, here, using black-P and blue phosphorene (blue-P) monolayers, we propose a 2D van der Waals (vdW) heterojunction. Theoretical results, including the band structures, density of states, Bader charge population, charge density di erence, and optical absorption spectra, clearly reveal that the visible light absorption ability is obviously improved, and the band edge alignment of the proposed vdW heterojunction displays a typical type-II feature to effectively separate the photogenerated carriers. At the same time, the built-in interfacial electric field prevents the electron-hole recombination. These predictions suggest that the examined phosphorene-based vdW heterojunction is an efficient photocatalyst for solar water splitting.

摘要：The selective detection of harmful gases is of great significance to human health and air quality,triggering the need for special customizations of sensing material *** this study,we prepared a novel Sn S_(2)/black phosphorus(BP)two-dimensional(2D)-2D heterostructure via the in situ hydrothermal growth of Sn S_(2)nanosheets on exfoliated BP lamellae for NO_(2)sensing *** the Sn S_(2)/BP composite,the holes with high oxidizability in p-type BP could oxidize Sn^(2+)into Sn^(4+),thus inhibiting the formation of Lewis acidic S *** Sn^(2+)/Lewis acidity suppression of the composite was further confirmed by X-ray photoelectron spectroscopy and acidic double-layer capacitance analyses,and promoted the adsorption and detection of acidic NO_(2).Owing to its valence and Lewis acidity engineering,the Sn S_(2)/BP heterostructure sensor could detect trace levels of NO_(2)as low as 100 ppb(parts per billion)with high response,fast response/recovery,good stability,and selectivity at room *** high absorption energy of NO_(2)(à0.74 e V),as indicated by the density functional theory calculations,suggests that NO_(2)was chemically adsorbed on the Sn S_(2)/BP surface,which was also evidenced by the in situ Raman spectroscopy *** work opens up interesting opportunities for the rational design of highly efficient NO_(2)gas sensors through Lewis acidity modification and interface engineering.

摘要：As the base of modern electronic industry,field-effect transistor(FET) requires the channel material to have both moderate bandgap and high mobility. The recent progresses indicate that few-layer black phosphorus has suitable bandgap and higher mobility than two-dimensional(2D) MoS_2, but the experimentally achieved maximal mobility(1000 cm^2 V^(-1) s^(-1)) is still obviously lower than those of classical semiconductors(1,400 and 5,400 cm^2 V^(-1) s^(-1) for Si and InP). Here, for the first time, we report on monolayer antimonide phosphorus(SbP) as a promising 2D channel material with suitable direct bandgap, which can satisfy the on/off ratio, and with mobility as high as 10~4 cm^2 V^(-1) s^(-1)based on density functional theory calculation. In particular,α-Sb_(1-x)P_x monolayers possess 0.3–1.6 eV bandgaps when0.1 ≤ x ≤ 1, which are greater than the minimum bandgap(0.4 eV) required for large on/off ratio of FET. Surprisingly,the carrier mobilities of α-Sb_(1-x)P_x monolayers exhibit very high upper limit approaching 2×10~4 cm^2 V^(-1) s^(-1) when 0 ≤x ≤ 0.25 due to the ultra-small effective mass of holes and electrons. This work reveals that 2D SbP with both suitable bandgap and high mobility could be a promising candidate as eco-friendly high-performance FET channel materials avoiding short-channel effect in the post-silicon era, especially when considering the recent experimental success in realizing arsenide phosphorus(AsP) with similar structure.