使用Cu嵌入式WS2单层作为单原子催化剂高选择性电催化降低NO到NH:A DFT研究
Rinu Jacob1, Thamarainathan Doulassiramane1, Ramanathan Padmanaban1
1Department of Chemistry, School of Physical Chemical and Applied Sciences, Pondicherry University, Puducherry, 605 014, India.
概括
我们开发了新的单原子催化剂 (SACs),用于电催化氧化还原反应 (NORR),以产生氨 (NH3). WS2上的基于铜的SAC表现出高效率和选择性,抑制不必要的进化反应 (HER).
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
- 计算化学计算化学
背景情况:
- 电催化氧化还原反应 (NORR) 提供了氨 (NH3) 合成和有害氧化 (NO) 污染物减轻的双重好处.
- 为NH3生产开发具有成本效益和高效率的NORR催化剂仍然是可持续化学的一个重大挑战.
研究的目的:
- 为NORR设计和研究一系列基于嵌入硫真空WS2单层中的过渡金属的单原子催化剂 (SAC).
- 用计算方法评估这些SACs用于NH3合成的催化性能,选择性和稳定性.
主要方法:
- 密度函数理论 (DFT) 的计算被用来选九种不同的过渡金属SAC (TM@WS2).
- 最初的分子动力学 (AIMD) 模拟用于评估有希望的催化剂的热稳定性.
- 使用能量描述器,探索通过NORR.R.进行NH3生产的所有可能反应途径.
主要成果:
- 基于铜的SAC (Cu@WS2) 对WS2表面表现出强烈的结合,并且对NORR具有优越的选择性.
- Cu@WS2有效地抑制了竞争中的进化反应 (HER).
- Cu@WS2 SAC通过N-交替通路表现出了显著的催化活性,通过N-交替通路的低限制电位为-0.41V,并显示出了高达500K的优异热稳定性.
结论:
- 基于过渡金属二甲基化物 (TMDC) 的SAC,特别是Cu@WS2,是高效和选择性的电催化转化NO到NH3的有希望的候选者.
- 这项工作为设计先进的NORR催化剂开辟了新的途径,用于可持续的氨合成和环境修复.
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