Chen Chunjun, Yan Xupeng, Wu Yahui, Liu Shoujie, Zhang Xiudong, Sun Xiaofu, Zhu Qinggong, Wu Haihong, Han Buxing
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun North First Street 2, Beijing, 100190, P. R. China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Yuquan Road, Shijingshan District, Beijing, 100049, P. R. China.
Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202202607. doi: 10.1002/anie.202202607. Epub 2022 Apr 7.
Electroreduction of CO into valuable fuels and feedstocks offers a promising way for CO utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO electroreduction by improving diffusion of CO to the surface of catalysts using porous organic cages (POCs) as an additive. It was noted that the Faradaic efficiency (FE) of C2+ products could reach 76.1 % with a current density of 1.7 A cm when Cu-nanorod(nr)/CC3 (one of the POCs) was used, which were much higher than that using Cu-nr. Detailed studies demonstrated that the hydrophobic pores of CC3 can adsorb a large amount of CO for the reaction, and the diffusion of CO in the CC3 to the nanocatalyst surface is easier than that in the liquid electrolyte. Thus, more CO molecules make contact with the nanocatalysts in the presence of CC3, enhancing CO reduction and inhibiting generation of H .
将CO电还原为有价值的燃料和原料为CO的利用提供了一种很有前景的方法。然而,商业化受到低生产率的限制。在此,我们报告一种策略,通过使用多孔有机笼(POC)作为添加剂来改善CO向催化剂表面的扩散,从而提高CO电还原的生产率。值得注意的是,当使用Cu-纳米棒(nr)/CC3(一种POC)时,C2+产物的法拉第效率(FE)在电流密度为1.7 A cm时可达到76.1%,这远高于使用Cu-nr时的效率。详细研究表明,CC3的疏水孔可以吸附大量的CO用于反应,并且CO在CC3中向纳米催化剂表面的扩散比在液体电解质中更容易。因此,在CC3存在下,更多的CO分子与纳米催化剂接触,增强了CO还原并抑制了H的生成。