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Dopant-induced electron localization drives CO 2 reduction to C 2 hydrocarbons
Nature Chemistry ( IF 21.8 ) Pub Date : 2018-07-16 , DOI: 10.1038/s41557-018-0092-x
Yansong Zhou , Fanglin Che , Min Liu , Chengqin Zou , Zhiqin Liang , Phil De Luna , Haifeng Yuan , Jun Li , Zhiqiang Wang , Haipeng Xie , Hongmei Li , Peining Chen , Eva Bladt , Rafael Quintero-Bermudez , Tsun-Kong Sham , Sara Bals , Johan Hofkens , David Sinton , Gang Chen , Edward H. Sargent

The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C2 products. Here, we use boron to tune the ratio of Cuδ+ to Cu0 active sites and improve both stability and C2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C2 products. We report experimentally a C2 Faradaic efficiency of 79 ± 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of ~40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons.



中文翻译:

掺杂剂引起的电子局域化将CO 2还原为C 2烃

将CO 2电化学还原为多碳产品备受关注,因为它为利用可再生电力合成增值的碳基燃料和原料提供了途径。不幸的是,CO 2转化为C 2产品的效率仍然低于大规模实施所需的效率。据预测,用正价位修饰铜的局部电子结构将促进向C 2产物的转化。在这里,我们使用硼来调整Cuδ+与Cu 0活性位点的比例,并提高稳定性和C 2产品生成。仿真表明,调节铜的平均氧化态的能力可以控制CO的吸附和二聚化,并可以实现对C 2产物的电合成的偏爱。我们通过实验报告了在掺硼铜催化剂上的C 2法拉第效率为79±2%,并且进一步表明,掺硼导致催化剂在超过40小时的时间内保持稳定,同时将CO 2电化学还原为多碳烃。

更新日期:2018-07-18
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