用高效率的双功能Cu-Nx单原子催化剂对糖醇进行电氧化,并与演变/二氧化碳减少相结合的描述剂
Mingyue Lv1, Hao Sun1, Hui Wang2
1Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130023 China.
这项研究使用DFT来研究用于电化学甘油氧化的配合石墨烯支持的铜单原子催化剂. CuN3@Gra显示了最高的活性,产生酸,并为高效的电催化剂设计提供了见解.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 计算化学的计算化学
背景情况:
- 电化学甘氧化 (GOR) 是一个有前途的途径,用于增值甘.
- 了解GOR机制和实现产品选择性仍然具有挑战性.
- 用添加的石墨烯支持的铜单原子催化剂 (CuNx@Gra SACs) 为GOR研究提供了稳定和导电平台.
研究的目的:
- 为了阐明GOR在CuNx@Gra SACs (x=2-4) 上的催化机制.
- 确定管理GOR业绩的结构-活动关系.
- 确定用于预测电催化剂效率的描述符.
主要方法:
- 密度函数理论 (DFT) 计算以探索反应路径和能量.
- 微动力学分析以验证预测的活动趋势.
- 对像吸附自由能量和d频段中心等描述物的分析.
主要成果:
- CuN2@Gra和CuN3@Gra通过最佳途径有利于酸生产.
- GOR活动遵循这一趋势:CuN3@Gra > CuN2@Gra > CuN4@Gra.
- 吸附自由能量 (ΔGGLY*) 与GOR活性和其他吸附剂能量很好地相关.
结论:
- CuN3@Gra被认为是高活性和选择性的GOR催化剂.
- ΔGGLY* 作为预测 GOR 催化剂性能的可靠描述符.
- CuN2@Gra和CuN3@Gra对GOR和其他电化学反应都具有双功能催化能力.
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