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新的二维碳材料T-石墨烯支持3D过渡金属单个原子作为高效的氧降解催化剂

Run Jiang¹, Zelong Qiao¹, Haoxiang Xu¹

¹State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, People's Republic of China. caodp@mail.buct.edu.cn.

|October 11, 2023

概括

通过优化电子结构和减少中间吸附,T-石墨烯增强了氧降解反应 (ORR) 的单原子催化剂活性. 这一发现为设计高效的电催化剂提供了新的策略.

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
催化剂是一种催化剂.

背景情况:

在碳支上的单原子催化剂 (SAC) 对氧降解反应 (ORR) 是有前途的.
支持结构显著影响SAC的内在活动.
T-石墨烯具有很高的导电性和稳定性,这表明它有可能作为支材料.

研究的目的:

在T-石墨烯上支持过渡金属 (TM) 单个原子的ORR活性进行系统评估.
为了比较T-石墨烯支持的SAC与其石墨烯支持的对应物的性能.
阐明在这些新型催化剂上控制ORR的结构-活动关系.

主要方法:

使用密度函数理论 (DFT) 的计算.
对TMN4-Tgra,TMC4-Tgra,TMN4-Gra和TMC4-Gra (TM = Sc-Zn) 的ORR活性进行系统评估.
分析轨道杂交和d频段中心对氧介质吸附的影响.

主要成果:

与石墨烯相比,T-石墨烯通过增加d波段中心和减弱*OH吸附来提高SAC ORR活性.
轨道杂交 (TM(d) -O(p,TM(d) -O(p,TM(d) -O(p+s)) 决定了催化性能.
确定了一个d频段中心依赖定律,用于基于支持和主动站点相互作用的ORR催化剂的设计.

结论:

在ORR催化中,T-石墨烯是TM SACs的优越支持.
优化活跃站点的d波段中心对于增强ORR活动至关重要.
这些发现为设计高效的ORR电催化剂提供了理论基础.

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相关概念视频

Properties of Transition Metals

Properties of Transition Metals

Transition metals are defined as those elements that have partially filled d orbitals. As shown in Figure 1, the d-block elements in groups 3–12 are transition elements. The f-block elements, also called inner transition metals (the lanthanides and actinides), also meet this criterion because the d orbital is partially occupied before the f orbitals.