Screening Highly Effective Electrocatalyst for N2 Reduction on Anatase TiO2(101) Surface: By Tuning Electronic and Geometry Features

Tuning the Electronic Structure of Anatase Through Fluorination

A highly fluorinated anatase lattice has been recently reported, providing a new class of materials whose general chemical formula is $\rm Ti_{1- \mathit x}\square_{\mathit x}X_{4\mathit x}O_{2- 4\mathit x}$ (X$^-$ = F$^-$ or OH$^-$). To characterise the complex structural features of the material and the different F environments, we here apply a computational screening procedure. After deriving a polarisable force--field from DFT simulations, we screen in a step-wise fashion a large number of possible configurations differing in the positioning of the titanium vacancies ($\square$) and of the…

通过机器学习势加速发现氮配位双原子析氢反应电催化剂

Accelerated Discovery of Nitrogen-Coordinated Dual-Atom Hydrogen Evolution Reaction Electrocatalysts via Machine Learning Potentials

本研究利用机器学习势（MLP）高效筛选石墨烯负载的TM2@Nx-Gr双原子催化剂，发现中等氮配位（2N-4N）可实现近最优ΔGH*，并鉴定出多种可合成的优异候选催化剂。

Large polaron evolution in anatase TiO2 due to carrier and temperature dependence of electron-phonon coupling

The electronic and magneto transport properties of reduced anatase TiO2 epitaxial thin films are analyzed considering various polaronic effects. Unexpectedly, with increasing carrier concentration, the mobility increases, which rarely happens in common metallic systems. We find that the screening of the electron-phonon (e-ph) coupling by excess carriers is necessary to explain this unusual dependence. We also find that the magnetoresistance (MR) could be decomposed into a linear and a quadratic component, separately characterizing the transport and trap behavior of carriers as a function of te…

Oxygen Reduction Reaction: Rapid Prediction of Mass Activity of Unstrained Nanostructured Platinum Electrocatalysts

Tailored Pt nanoparticle catalysts are promising candidates to accelerate the oxygen reduction reaction (ORR) in fuel cells. However, the search for active nanoparticle catalysts is hindered by laborious effort of experimental synthesis and measurements. On the other hand, DFT-based approaches are still time consuming and often not efficient. In this study, we introduce a computational model which enables rapid catalytic activity calculation of unstrained pure Pt nanoparticle electrocatalysts. The generic setup of the computational model is based on DFT results and experimental data obtained w…

Quasiparticle and Optical Properties of Rutile and Anatase TiO$_{2}$

Quasiparticle excitation energies and optical properties of TiO$_{2}$ in the rutile and anatase structures are calculated using many-body perturbation theory methods. Calculations are performed for a frozen crystal lattice; electron-phonon coupling is not explicitly considered. In the GW method, several approximations are compared and it is found that inclusion of the full frequency dependence as well as explicit treatment of the Ti semicore states are essential for accurate calculation of the quasiparticle energy band gap. The calculated quasiparticle energies are in good agreement with avail…

锆-氮功能化材料中用于 N2 还原的配位工程：第一性原理模拟

Coordination Engineering in Zirconium-Nitrogen-Functionalized Materials for N2 Reduction: A First-Principles Simulation

本文通过第一性原理计算与四步筛选研究 ZrPP-A 电催化剂，揭示不对称配位环境调控电荷转移、N2 极化及混合 NRR 路径的机制。