通过通过异质核双原子兴奋剂调节电催化站点的特定原子轨道来改善性演变反应的综合战略
Meixia Xiao1, Jiangman Xi2, Yibo Wu1
1College of New Energy, Xi'an Shiyou University, Xi'an 710065, China..
Journal of colloid and interface science
|March 11, 2026
概括
为演化反应 (HER) 开发具有成本效益的过渡金属硫化物具有挑战性. 这项研究引入了异核双原子兴奋剂,以增强硫位点,产生具有优越HER性能和稳定的CuNi-Co3S4,用于绿色生产.
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:
- 过渡金属硫化物 (TMS) 是用于演化反应 (HER) 的无贵金属电催化剂.
- 提高HER在TMS的效率受到限制,因为人们对硫 (S) 现场活动的理解有限,超出了传统的p/d带中心原则.
- 开发具有成本效益和高活性的电催化剂对于工业规模的绿色生产至关重要.
研究的目的:
- 开发一个综合战略,将密度函数理论 (DFT) 计算和机器学习 (ML) 结合起来,用于设计高性能TMS电催化剂.
- 确定新的异核双原子兴奋剂策略,以调节硫原子的电子特性,以增强 HER 活性.
- 为了合成和实验验证一个有前途的候选电催化剂有效的进化.
主要方法:
- 密度函数理论 (DFT) 计算用于研究电子结构和反应机制.
- 机器学习 (ML) 分析,以建立用于电催化剂选的多维预测描述符.
- 异核双原子兴奋剂策略调整硫活性位点的电子特性.
- 对于催化剂合成而言,协调共降和水热硫化.
- 在性介质中的电化学表征 (超电位,Tafel斜率,稳定性).
主要成果:
- 建立了包含轨道特征的多维预测描述器,以有效识别催化剂.
- 通过DFT和ML确定CuNi-Co3S4作为一个非常有前途的电催化剂候选者.
- 证明异质核兴奋剂改变了电子分布,并提高了S原子的p轨道能量,增强了HER的活性.
- 合成的CuNi-Co3S4表现出色的HER性能:低超电位 (135 mV) 和Tafel斜率 (81 mV·dec-1) 在10 mA·cm-2.
- 在1M KOH中实现了超过180小时的显著催化稳定性.
结论:
- 集成的DFT,ML和实验方法对于设计先进的电催化剂是有效的.
- 硫位点的异核双原子兴奋剂是一种可行的策略,可以促进HER在过渡金属硫化物中的活性.
- -3S4显示出作为一个具有成本效益和稳定的电催化剂的巨大潜力,用于工业绿色生产.
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