Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, 210023, Nanjing, China.
MOE Key Laboratory of Functional Small Organic Molecule College of Chemistry and Chemical Engineering, Jiangxi Normal University, 330022, Nanchang, China.
Nat Commun. 2018 Oct 26;9(1):4466. doi: 10.1038/s41467-018-06938-z.
The design of highly stable, selective and efficient electrocatalysts for CO reduction reaction is desirable while largely unmet. In this work, a series of precisely designed polyoxometalate-metalloporphyrin organic frameworks are developed. Noted that the integration of {ε-PMoMoOZn} cluster and metalloporphyrin endows these polyoxometalate-metalloporphyrin organic frameworks greatly advantages in terms of electron collecting and donating, electron migration and electrocatalytic active component in the CO reduction reaction. Thus-obtained catalysts finally present excellent performances and the mechanisms of catalysis processes are discussed and revealed by density functional theory calculations. Most importantly, Co-PMOF exhibits remarkable faradaic efficiency ( > 94%) over a wide potential range (-0.8 to -1.0 V). Its best faradaic efficiency can reach up to 99% (highest in reported metal-organic frameworks) and it exhibits a high turnover frequency of 1656 h and excellent catalysis stability ( > 36 h).
设计高稳定性、高选择性和高效率的电催化剂对于 CO 还原反应是非常理想的，但目前尚未完全实现。在这项工作中，设计并制备了一系列精确设计的多金属氧酸盐-金属卟啉有机框架。值得注意的是，{ε-PMoMoOZn} 簇和金属卟啉的集成赋予了这些多金属氧酸盐-金属卟啉有机框架在 CO 还原反应中在电子收集和提供、电子迁移和电催化活性组分方面的巨大优势。最终获得的催化剂表现出优异的性能，并通过密度泛函理论计算讨论和揭示了催化过程的机制。最重要的是，Co-PMOF 在很宽的电位范围内（-0.8 至-1.0 V）表现出显著的法拉第效率（>94%）。其最佳的法拉第效率可达 99%（在报道的金属-有机框架中最高），并具有高达 1656 h-1 的高周转频率和出色的催化稳定性（>36 h）。
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