Oxygen reduction reaction (ORR) in fuel cells on carbon-based metal-free electrocatalysts by first-principles multiscale simulations.

通过第一原理多尺度模拟，在碳基无金属电催化剂上进行燃料电池中的氧还原反应（ORR）。

基本信息

批准号：
22KJ2131
负责人：
WANG YUELIN
金额：
$ 1.09万
依托单位：
Osaka University
依托单位国家：
日本
项目类别：
Grant-in-Aid for JSPS Fellows
财政年份：
2023
资助国家：
日本
起止时间：
2023-03-08 至 2024-03-31
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-22KJ2131/
关键词：
fuel cell DFT AIMD

项目摘要

In order to improve the ORR electrocatalytic activity, by doping atoms to modification structure is good way to improve the activity. Here, we choose the N doped GDY to investigate the ORR activity. And So, my research purpose is focus on three issues, namely (1) screening the suitable metal-free atoms doped on GDY as electrocatalysts for ORR first-principles multiscale simulations and figure out the doping principle of metal-free atoms by analysis of the intrinsic properties (such as electronic properties). (2) investigating the ORR electrocatalytic activity in water condition. (3) analysis the ORR reaction paths in thermodynamics and kinetics level. At present, we have studied sp-N and pyridine N doped GDY to investigate the electrocatalytic activity of ORR. To simulate the real experiment condition, (1) Graphene (G) is applied as support under the N-doped GDY to enhance the electrode conductivity. (2) we used the ab inito molecular dynamics (AIMD) calculations to simulate the water environment with some H2O on surface to calculate the solvation energy of ORR intermediates. Finally, we performed the free energy diagram (based on thermodynamic analyses) to proving and predicting the experimentally observed activity trends for a range of materials. All calculations will be performed using simulation tool for atom technology (STATE) code and investigated the ORR mechanisms using NEB method.

为了改善ORR电催化活性，通过掺杂原子对修饰结构是改善活性的好方法。在这里，我们选择N掺杂的GDY来研究ORR活性。因此，我的研究目的是关注三个问题，即（1）筛选在GDY上掺杂的无金属原子，作为ORR第一原理多尺度模拟的电催化剂，并通过分析对无金属原子的兴奋剂原理进行分析。内在特性（例如电子特性）。（2）研究水条件下的ORR电催化活性。（3）分析热力学和动力学水平的ORR反应路径。目前，我们研究了SP-N和吡啶n掺杂GDY来研究ORR的电催化活性。为了模拟真实的实验条件，（1）石墨烯（g）被用作N掺杂GDY下的支撑，以增强电极电导率。（2）我们使用AB Inito分子动力学（AIMD）计算来模拟水上环境，并在表面上进行一些H2O来计算ORR中间体的溶剂化能。最后，我们进行了自由能图（基于热力学分析），以证明和预测一系列材料的实验观察到的活性趋势。所有计算将使用用于Atom技术（状态）代码的仿真工具进行，并使用NEB方法研究了ORR机制。