Using density functional theory coupled with Boltzmann transport equation with relaxation time approximation, we investigate the electronic structure and predict the charge mobility for a new carbon allotrope, the graphdiyne for both the sheet and nanoribbons. It is shown that the graphdiyne sheet is a semiconductor with a band gap of 0.46 eV. The calculated in-plane intrinsic electron mobility can reach the order of 10(5) cm(2)/(V s) at room temperature, while the hole mobility is about an order of magnitude lower.

Aqueous zinc‐ion batteries are largely restricted by the unsatisfactory performance of zinc (Zn) anodes, including their poor stability and irreversibility. In particular, the mechanism behind the electrochemical contrast caused by the surface crystal plane, which is a decisive factor of the electrochemical characteristics of the hostless Zn anode, is still relatively indistinct. Hence, new insight into a novel anode with a surface‐preferred (002) crystal plane is provided. The interfacial reaction and morphology evolution are revealed by theoretical analysis and post‐mortem/operando experimental techniques, indicating that Zn anodes with more exposed (002) basal planes exhibit free dendrites, no by‐products, and weak hydrogen evolution, in sharp contrast to the (100) plane. These features benefit the Zn (002) anode by enabling a long cyclic life of more than 500 h and a high average coulombic efficiency of 97.71% for symmetric batteries, along with delivering long cycling stability and reversibility with life spans of over 2000 cycles for full batteries. This work provides new insights into the design of high‐performance Zn anodes for large‐scale energy storage and can potentially be applied to other metal anodes suffering from instability and irreversibility.

We summarize our recent progresses in developing first-principles methods for predicting the intrinsic charge mobility in carbon and organic nanomaterials, within the framework of Boltzmann transport theory and relaxation time approximation. The electron-phonon couplings are described by Bardeen and Shockley's deformation potential theory, namely delocalized electrons scattered by longitudinal acoustic phonons as modeled by uniform lattice dilation. We have applied such methodology to calculating the charge carrier mobilities of graphene and graphdiyne, both sheets and nanoribbons, as well as closely packed organic crystals. The intrinsic charge carrier mobilities for graphene sheet and naphthalene are calculated to be 3 × 10(5) and ∼60 cm(2) V(-1) s(-1) respectively at room temperature, in reasonable agreement with previous studies. We also present some new theoretical results for the recently discovered organic electronic materials, diacene-fused thienothiophenes, for which the charge carrier mobilities are predicted to be around 100 cm(2) V(-1) s(-1).

First-principles density functional theory coupled with deformation potential calculations indicate a strong width-dependent carrier mobility: for an armchair graphene ribbon whose width (i.e., number of carbons along the edge) is N = 3k, the room-temperature electron mobility is calculated to be approximately 10(6) cm(2) V(-1) s(-1) and the hole mobility approximately 10(4) cm(2) V(-1) s(-1), while for N = 3k + 1 or 3k + 2, the hole mobility is calculated to be 4-8 x 10(5) cm(2) V(-1) s(-1) and the electron mobility approximately 10(4) cm(2) V(-1) s(-1). Such alternating behavior is absent in zigzag-type graphene.