Hatsukade Toru, Kuhl Kendra P, Cave Etosha R, Abram David N, Jaramillo Thomas F
Department of Chemical Engineering, Stanford University, 381 North-South Mall, Stanford, California 94305, USA.
Phys Chem Chem Phys. 2014 Jul 21;16(27):13814-9. doi: 10.1039/c4cp00692e. Epub 2014 Jun 10.
The electrochemical reduction of CO2 could allow for a sustainable process by which renewable energy from wind and solar are used directly in the production of fuels and chemicals. In this work we investigated the potential dependent activity and selectivity of the electrochemical reduction of CO2 on metallic silver surfaces under ambient conditions. Our results deepen our understanding of the surface chemistry and provide insight into the factors important to designing better catalysts for the reaction. The high sensitivity of our experimental methods for identifying and quantifying products of reaction allowed for the observation of six reduction products including CO and hydrogen as major products and formate, methane, methanol, and ethanol as minor products. By quantifying the potential-dependent behavior of all products, we provide insights into kinetics and mechanisms at play, in particular involving the production of hydrocarbons and alcohols on catalysts with weak CO binding energy as well as the formation of a C-C bond required to produce ethanol.
二氧化碳的电化学还原能够实现一个可持续的过程，在此过程中，风能和太阳能等可再生能源可直接用于燃料和化学品的生产。在这项工作中，我们研究了在环境条件下，金属银表面上二氧化碳电化学还原的电位依赖性活性和选择性。我们的结果加深了我们对表面化学的理解，并为设计该反应的更好催化剂的重要因素提供了见解。我们用于识别和定量反应产物的实验方法具有高灵敏度，从而能够观察到六种还原产物，其中一氧化碳和氢气是主要产物，甲酸盐、甲烷、甲醇和乙醇是次要产物。通过量化所有产物的电位依赖性行为，我们深入了解了其中的动力学和机制，特别是涉及在一氧化碳结合能较弱的催化剂上烃类和醇类的生成，以及生成乙醇所需的碳-碳键的形成。
