在单个Ni-N4-C位点上通过MXene合来增强电化学CO2降低CO的刚性轴向O协调诱导的旋转极化
Guanping Wei1, Zongchang Mao1, Lingli Liu1
1Key Laboratory of Organo-Pharmaceutical Chemistry of Jiangxi Province, Gannan Normal University, Ganzhou 341000, China.
ACS applied materials & interfaces
|September 17, 2024
概括
单个Ni原子催化剂 (SAC) 中的旋转调节是减少二氧化碳的关键. 在MXene上,新的Ni-N4O配置增强了自旋两极化,显著改善了CO2RR活动,降低了发病潜力.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 计算化学计算化学
背景情况:
- 过渡金属单原子催化剂 (SAC) 需要自旋状态调节才能达到最佳活性.
- 在电化学二氧化碳还原反应 (CO2RR) 中,旋转对单个Ni原子的影响仍未得到充分研究.
研究的目的:
- 研究Ni-N4-C SACs在CO2RR的O端MXene上的电催化性能.
- 阐明了 CO2RR 的 Ni-N4O 配置中自旋两极化的作用.
主要方法:
- 使用第一原则模拟来研究MXene纳米片上的Ni-N4-C SAC.
- 对电子结构,电荷转移和反应能量进行了分析.
主要成果:
- 有O结尾的MXene与Ni原子诱导轴相互作用和电荷转移,形成Ni-N4O位点.
- Ni-N4O配置呈现出显著的旋转极化,打破了旋转退化,并创造了大的净旋转时刻 (1.4 μB).
- 通过少数旋转通道中的减弱的Ni-d-π*轨道稳定*COOH中间体,增强了CO2RR活动.
结论:
- 四种类型的MXenes (Hf3C2,Zr3C2,Hf2C,Zr2C) 在Ni位点上有效诱导旋转极化.
- 在MXene上的Ni-N4O配置显著改善了CO2RR到CO,与纯Ni SACs (-1.17V) 相比,实现了较低的发作潜力 (-0.75V与SHE).
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