工程 TM-N2@C15N5S3H5-基于共价有机框架,用于增强水分裂和氧减少反应:恒定潜力和特征共同评估方法
Yajuan Feng1, Xihang Zhang2, Renxian Qin2
1School of Materials Science and Engineering, North Minzu University, Yinchuan 750021, People's Republic of China.
Langmuir : the ACS journal of surfaces and colloids
|March 11, 2025
概括
高活性单原子催化剂 (SAC) 对于能源应用至关重要. 这项研究确定了对和氧反应有前途的双功能SAC,其性能优于传统催化剂,并提供了具有成本效益的解决方案.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 计算化学计算化学
背景情况:
- 单原子催化剂 (SAC) 为能量转换和储存提供了更高的原子利用率和活性.
- 能够催化演变 (HER) 和氧演变/减少 (OER/ORR) 等多种反应的双功能SAC比单功能对应物具有更高的效率和经济价值.
研究的目的:
- 系统地评估过渡金属 (TM) -N2@C15N5S3H5单层对HER,OER和ORR的催化潜力.
- 确定稳定的TM-N2配置并评估它们在不同条件下的双功能催化活性和性能.
主要方法:
- 密度函数理论 (DFT) 的计算被用来研究TM-N2@C15N5S3H5单层的结构稳定性和电子特性.
- 机器学习 (ML) 技术被用来探索结构-活动关系和预测催化性能.
- 计算包括对反应机制,吸附能量的详细分析,以及pH和应用潜力的影响.
主要成果:
- 发现27个过渡金属原子在N2@C15N5S3H5框架内稳定,形成TM-N2协调点.
- Rh-N2@C15N5S3H5与金相比表现出更高的HER活性,并催化了OER,作为双功能催化剂.
- Ni-N2@C15N5S3H5表现出极好的OER和ORR活性,作为另一种双功能催化剂. 它的性能归因于有利的Ni-d轨道相互作用与O-p轨道,增强OH*吸附.
- 在酸性介质中,Ni-N2@C15N5S3H5和Rh-N2@C15N5S3H5都显示出增强的OER. Ni-N2@C15N5S3H5在性ORR中表现出色,而Rh-N2@C15N5S3H5在酸性条件下对ORR更有效.
结论:
- TM-N2@C15N5S3H5单层系统是开发高效的双功能单原子催化剂的有希望的平台,用于能源应用.
- Rh-N2@C15N5S3H5和Ni-N2@C15N5S3H5代表了先进的双功能催化剂,其性能可以根据反应条件和pH值进行调整.
- 集成的DFT和ML方法有效地将结构性/原子性质与催化活性相关联,为合理的催化剂设计铺平了道路.
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