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Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons

2018; Nature Portfolio; Volume: 10; Issue: 9 Linguagem: Inglês

10.1038/s41557-018-0092-x

1755-4349

Yansong Zhou, Fanglin Che, Min Liu, Chengqin Zou, Zhiqin Liang, Phil De Luna, Haifeng Yuan, Jun Li, Zhi-Qiang 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,

Electrocatalysts for Energy Conversion

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. On copper catalysts, Cuδ+ sites play a key role in the electrochemical reduction of CO2 to C2 hydrocarbons, however, they are prone to being reduced (to Cu0) themselves. Now, a Cuδ+-based catalyst is reported that is stable for in excess of ~40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons and that exhibits a Faradaic efficiency for C2 of ~80%.