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Spatial Confinement in Copper-Porphyrin Frameworks Enhances Carbon Dioxide Reduction to Hydrocarbons
Cell Reports Physical Science ( IF 7.9 ) Pub Date : 2020-09-09 , DOI: 10.1016/j.xcrp.2020.100182
Yinzheng Zhou , Shenghua Chen , Shibo Xi , Zhitong Wang , Peilin Deng , Fan Yang , Youjia Han , Yuanjie Pang , Bao Yu Xia

Porphyrin-based catalysts are promising for electrochemical carbon dioxide (CO2) conversion. We report here molecular Cu-porphyrin-constructed porous frameworks for efficient CO2 reduction. This framework catalyst has a high Faradaic efficiency of 73.6% and a partial current density of 7.5 mA cm−2 at −1.4 V versus RHE for the selective production of hydrocarbons, while only carbon monoxide is generated on the Cu-porphyrin building blocks. Experimental results demonstrate that this porous framework has a high CO2 absorption capability, and abundant copper-active sites account for the efficient CO2 conversion. Moreover, finite-element simulations reveal that the spatial confinement of CO intermediates in the porous framework are critical for the efficient generation of hydrocarbons. This work may offer insights into designing efficient catalysts for CO2 reduction to valuable products.



中文翻译:

铜卟啉骨架中的空间限制增强了二氧化碳还原为碳氢化合物的能力

卟啉基催化剂有望用于电化学二氧化碳(CO 2)转化。我们在这里报告了分子铜卟啉构造的有效降低CO 2的多孔框架。与RHE相比,该骨架催化剂具有较高的法拉第效率,效率为73.6%,在-1.4 V时的分流密度为7.5 mA cm -2,用于选择性生产烃,而在铜-卟啉结构单元上仅生成一氧化碳。实验结果表明,该多孔骨架具有较高的CO 2吸收能力,并且大量的铜活性位点构成了有效的CO 2转换。此外,有限元模拟表明,多孔骨架中CO中间体的空间限制对于有效生成烃至关重要。这项工作可以为设计有效的催化剂以减少CO 2还原为有价值的产品提供见识。

更新日期:2020-09-23
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