对二氧化碳减排和演变反应之间的竞争以及通过加载单原子催化剂在石墨碳化物上调节选择性的机制研究
Joel Jie Foo1,2, Sue-Faye Ng1,2, Mo Xiong3
1School of Energy and Chemical Engineering, Xiamen University Malaysia, Sepang, Selangor Darul Ehsan, 43900, Malaysia. weejun.ong@xmu.edu.my.
Nanoscale
|July 16, 2024
概括
在g-C3N4上的单原子催化剂可以通过选择性地引导催化二氧化碳减排 (CO2RR) 而不是进化来改善酸生产. 催化剂通过*OCHO通路显示出有希望的选择性.
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
- 计算化学的计算化学
背景情况:
- 催化二氧化碳减排 (CO2RR) 面临着竞争的进化 (HER) 和对酸等所需产品的低选择性所带来的挑战.
- 在碳支上的单原子催化剂 (SAC) 对于调整CO2RR活性和选择性至关重要.
研究的目的:
- 研究各种单原子金属催化剂对g-C3N4支持CO2RR选择性的影响.
- 使用密度函数理论 (DFT) 来分析反应路径和中间选择性 (*COOH与*OCHO).
主要方法:
- 使用DFT计算系统地检查一系列单原子金属载荷g-C3N4单层 (MCN).
- 对不同金属原子 (M = Ni, Cu, Zn, Ga, Cd, In, Sn, Pb, Ag, Au, Bi, Pd, Pt) 的*COOH和*OCHO中间体之间的反应途径和选择性进行了分析.
主要成果:
- 与原始的CN系统 (1.36 eV) 相比,NiCN表现出对*OCHO通路的偏好,其速度决定潜力显著降低 (0.36 eV).
- 单个Ni原子的低协调增强了CO2吸附,使CO2RR比HER更受欢迎.
- DFT计算预测特定的SAC可以有效调节反应路径以提高选择性.
结论:
- 选择单原子金属催化剂是控制CO2RR选择性的可行策略.
- 在g-C3N4上以Ni为基础的SAC显示了通过CO2RR.通过有效和选择性酸生产的潜力.
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