二维hetero-MXenes体系电催化析氢性能调控的理论研究

电催化分解水由于其产物只有H2和O2，有望作为一种常规手段用于工业制氢。目前，其大规模应用主要受制于催化材料存在活性位点少、导电性能差以及调控手段复杂等问题。因此，寻求调控简单、导电性能好、价格低廉的新型电催化材料是解决上述问题的关键。本项目拟围绕近期实验合成的二维hetero-MXenes结构，基于第一性原理计算并结合溶剂效应，系统地探究其相关的电子结构和催化性质。本项目拟通过施加应力、原子吸附、构造缺陷等手段进一步调控其催化活性，揭示界面处电荷转移影响其析氢活性的内在机理。此外，基于hetero-MXenes结构设计具有本征极性的Janus结构，利用其内建电场影响界面处电荷转移，实现高性能的电催化分解水制氢，并对其内在的反应机理进行深入探究。本项目的研究结果不仅对揭示电催化分解水的内在反应机理具有重要理论意义，还将为实验上指导合成高质量的电催化材料提供理论依据和参考。

Electrocatalytic water splitting has been expected to be used as a conventional strategy for industrial hydrogen production due to the fact that the products are only H2 and O2. The previously reported catalyst systems generally have following shortcomings of few active sites, poor electrical conductivity, complex regulatory means and so on, which greatly hinder their practical applications. Therefore, seeking for new types of electrocatalyst with intrinsic activity, easily regulated, good electrical conductivity and low price is important for to solve the above problems. By using the first-principles calculations and solvent effect, this project aims to systematically explore the electronic structure and catalytic properties related to the recently synthesized two-dimensional hetero-Mxenes structures. This project intends to further regulate its catalytic activity by applying strain, atomic adsorption, and structural defects, and reveal the internal mechanism of their hydrogen evolution activity. What's more, the project will design the intrinsic polarity Janus structure based on the Hetero-MXenes, and investigate the reaction mechanism of electrocatalytic water splitting for hydrogen production by analyzing the charge transfer, which induced by internal electric field. This project will not only reveal the internal reaction mechanism of electrocatalytic water splitting, but also provide theoretical reference for synthesizing high-quality electrocatalysts in experiments.