Piontek Stefan, Junge Puring Kai, Siegmund Daniel, Smialkowski Mathias, Sinev Ilya, Tetzlaff David, Roldan Cuenya Beatriz, Apfel Ulf-Peter
Inorganic Chemistry I , Ruhr-University Bochum , Universitätsstrasse 150 , 44780 Bochum , Germany . Email:
Fraunhofer UMSICHT , Osterfelder Straße 3 , 46047 Oberhausen , Germany.
Chem Sci. 2018 Nov 6;10(4):1075-1081. doi: 10.1039/c8sc03555e. eCollection 2019 Jan 28.
The electrocatalytic reduction of carbon dioxide (CORR) to valuable bulk chemicals is set to become a vital factor in the prevention of environmental pollution and the selective storage of sustainable energy. Inspired by structural analogues to the active site of the enzyme CODH, we envisioned that bulk Fe/Ni sulfides would enable the efficient reduction of CO. By careful adjustment of the process conditions, we demonstrate that pentlandite (FeNiS) electrodes, in addition to HER, also support the CORR reaching a peak faradaic efficiency of 87% and 13% for the formation of CO and methane, respectively at 3 mA cm. The choice of solvent, the presence of water/protons and CO solubility are identified as key-properties to adjust the balance between HER and CORR in favour of the latter. Such experiments can thus serve as model reactions to elucidate a potential catalyst within gas diffusion electrodes.
将二氧化碳电催化还原（CORR）为有价值的大宗化学品，有望成为预防环境污染和选择性存储可持续能源的关键因素。受酶CODH活性位点结构类似物的启发，我们设想块状铁/镍硫化物能够实现一氧化碳的高效还原。通过仔细调整工艺条件，我们证明，除析氢反应（HER）外，镍黄铁矿（FeNiS）电极还能支持CORR，在3 mA cm时，生成一氧化碳和甲烷的法拉第效率分别达到87%和13%的峰值。溶剂的选择、水/质子的存在以及一氧化碳的溶解度被确定为调节HER和CORR之间平衡以利于后者的关键特性。因此，此类实验可作为模型反应，以阐明气体扩散电极中的潜在催化剂。
