| 孙楠楠,赵志超,张宇,赵翠莲,董海阳.二维四角TiC单层片上的析氢反应研究[J].分子催化,2022,36(1):12-21 |
| 二维四角TiC单层片上的析氢反应研究 |
| Investigation of the Hydrogen Evolution Reaction on Two-dimensional Tetragonal TiC Monolayer Sheet |
| 投稿时间：2021-10-12 修订日期：2021-12-07 |
| DOI：10.16084/j.issn1001-3555.2022.01.002 |
| 中文关键词: 密度泛函理论 TiC单层片 覆盖率 催化性能 |
| 英文关键词:density functional theory TiC monolayer sheet coverage rate catalytic ability |
| 基金项目:高等学校基本科研业务费研究项目（SYKY2011，SYKY2102）、河北省高等学校青年拔尖人才计划项目（BJ2019055），河北省自然科学基金（B2021412001）和沧州市自然科学基金项目（204001001）资助 |
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| 中文摘要: |
| 电解水是目前获得氢气的高效方法之一.过渡金属碳化物因其廉价且在析氢反应（HER）中表现出较高的催化活性而备受关注.我们利用第一性原理首先计算了新型二维四角TiC单层片的稳定性及电子性质，进而计算其表面不同活性位点、不同氢覆盖率下的吸附能、吉布斯自由能（ΔGH*）等属性，并且将对应的微观结构进行了系统分析比较，同时结合差分电荷密度理论，分析了TiC单层片氢吸附的电荷转移及成键特性.结果发现TiC单层片表面的topC2位点在氢覆盖率为100%时，吉布斯自由能是-0.0611eV，表明四角TiC二维片表面的topC2位点在高覆盖率下具有很好的HER催化性能.为电化学还原水的析氢反应提供了一种有前景的二维催化剂材料. |
| 英文摘要: |
| Electrochemical water splitting is one of the most efficient ways to generate long-term hydrogen energy. Transition metal carbides have received increased attention due to their low cost and high catalytic activity in hydrogen evolution reactions(HER). This research used the first principles of the density functional theory to investigate the stability and electronic properties of the two-dimensional(2D) tetragonal titanium carbide(t-TiC) sheet. Then, we selected five hydrogen adsorption sites, and optimized results reveal two ideal adsorbed sites:topC1 and topC2. To compare their catalytic ability in the HER, the adsorption energy and Gibbs free energy(ΔGH) of the hydrogen adsorption on the t-TiC surface with different active sites and hydrogen coverage rates are investigated. The results show that the of the topC2 site at the 100% hydrogen coverage is about -0.0611 eV, indicating that the topC2 site can have good catalytic activity for the HER. The charge density difference and electronegativity are used to analyze the charge transfers and bonding details of the two carbon-hydrogen adsorptions as the associated structures and relative ΔGH are explained further. This research demonstrates a promising 2D catalyst material for the HER of electrochemical reducing water. |
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