Gouda Abdelaziz, Hannouche Karen, Mohan Abhinav, Mao Chengliang, Nikbin Ehsan, Carrière Alexandre, Ye Jessica, Howe Jane Y, Sain Mohini, Hmadeh Mohamad, Ozin Geoffrey A
Department of Chemistry, University of Toronto, Toronto, ON, Canada.
Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, ON, Canada.
Nat Commun. 2025 Jan 15;16(1):695. doi: 10.1038/s41467-025-55891-1.
As the global quest for sustainable energy keeps rising, exploring novel efficient and practical photocatalysts remains a research and industrial urge. Particularly, metal organic frameworks were proven to contribute to various stages of the carbon cycle, from CO capture to its conversion. Herein, we report the photo-methanation activity of three isostructural, nickel-based metal organic frameworks incorporating additional niobium, iron, and aluminum sites, having demonstrated exceptional CO capture abilities from thin air in previous reports. The niobium version exhibits the highest performance, with a CO to CH conversion rate in the order of 750-7500 µmolgh between 180 °C and 240 °C, achieving 97% selectivity under light irradiation and atmospheric pressure. The in-depth characterization of this framework before and after catalysis reveals the occurrence of an in-situ restructuring process, whereas active surface species are formed under photocatalytic conditions, thus providing comprehensive structure-performance correlations for the development of efficient CO conversion photocatalysts.
随着全球对可持续能源的追求不断升温，探索新型高效实用的光催化剂仍然是科研和产业界的迫切需求。特别是，金属有机框架已被证明有助于碳循环的各个阶段，从二氧化碳捕获到其转化。在此，我们报告了三种同构的、含额外铌、铁和铝位点的镍基金属有机框架的光催化甲烷化活性，这些框架在之前的报告中已展示出从稀薄空气中捕获二氧化碳的卓越能力。铌基框架表现出最高的性能，在180°C至240°C之间，一氧化碳到甲烷的转化率为750 - 7500 μmol·g⁻¹·h⁻¹，在光照和大气压下选择性达到97%。对该框架催化前后的深入表征揭示了原位重构过程的发生，即在光催化条件下形成了活性表面物种，从而为开发高效二氧化碳转化光催化剂提供了全面的结构 - 性能关联。
