有效的N2电还原是通过在原子分散的W位点上线性电荷转移而实现的
Jin Wan1, Dong Liu1, Chuanzhen Feng1
1The School of Chemistry and Chemical Engineering, Chongqing University 174 Shazheng Street, Shapingba District Chongqing City 400044 P. R. China.
Chemical science
|August 16, 2024
概括
研究人员开发了用于电催化降解反应 (NRR) 的新型单/双原子催化剂,实现了创纪录的氨生产效率,并揭示了对催化机制的见解.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 电催化降解反应 (NRR) 为生产氨 (NH3) 的哈伯-博什工艺提供了一个可持续的替代方案.
- 开发高效的NRR催化剂和理解它们的机制是重大挑战.
研究的目的:
- 设计和合成新的原子分散 (W) 催化剂,以提高NRR.
- 为了研究电荷转移和NRR性能之间的关系.
- 阐明用于氨合成的基于W的催化剂的催化机制.
主要方法:
- 用自捕捉方法将原子分散的W原子嵌入V2-xCTz中.
- 电催化性能通过测量氨产量和法拉第效率 (FE) 来评估.
- 密度函数理论 (DFT) 的计算被用来研究反应机制和能量障碍.
主要成果:
- 在n-W/V2-xCTz催化剂实现了121.8μg h-1 mg-1和FE的34.2%的的记录产量在-0.1V与RHE.
- DFT计算显示了邻近W原子的协同效应,将限制电位 (UL) 降至0.32V.
- UL和集成晶体轨道汉密尔顿群体 (ICOHP) 之间的线性关系被确立为活动描述符.
结论:
- 原子分散的W催化剂在电催化NRR方面表现出了卓越的性能.
- 邻近的单个原子在通过协同效应增强反应动力学方面发挥着至关重要的作用.
- 该研究为NRR活动提供了一个新的描述符,并对基础电子结构-性能关系提供了洞察力.
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