De Gregorio Gian Luca, Burdyny Thomas, Loiudice Anna, Iyengar Pranit, Smith Wilson A, Buonsanti Raffaella
Laboratory of Nanochemistry for Energy, Institute of Chemical Sciences and Engineering, Ecole Politechnique Fédérale de Lausanne, Sion CH-1950, Switzerland.
Materials for Energy Conversion and Storage, Department of Chemical Engineering, Delft University of Technology, Delft 2629 HZ, Netherlands.
ACS Catal. 2020 May 1;10(9):4854-4862. doi: 10.1021/acscatal.0c00297. Epub 2020 Mar 27.
Despite substantial progress in the electrochemical conversion of CO into value-added chemicals, the translation of fundamental studies into commercially relevant conditions requires additional efforts. Here, we study the catalytic properties of tailored Cu nanocatalysts under commercially relevant current densities in a gas-fed flow cell. We demonstrate that their facet-dependent selectivity is retained in this device configuration with the advantage of further suppressing hydrogen production and increasing the faradaic efficiencies toward the CO reduction products compared to a conventional H-cell. The combined catalyst and system effects result in state-of-the art product selectivity at high current densities (in the range 100-300 mA/cm) and at relatively low applied potential (as low as -0.65 V vs RHE). Cu cubes reach an ethylene selectivity of up to 57% with a corresponding mass activity of 700 mA/mg, and Cu octahedra reach a methane selectivity of up to 51% with a corresponding mass activity of 1.45 A/mg in 1 M KOH.
尽管在将CO电化学转化为高附加值化学品方面取得了重大进展,但要将基础研究转化为具有商业相关性的条件仍需付出额外努力。在此,我们研究了在气体进料流动池中具有商业相关性的电流密度下定制的铜纳米催化剂的催化性能。我们证明,在这种装置配置中,它们的晶面依赖性选择性得以保留,与传统的H型电池相比,具有进一步抑制析氢和提高对CO还原产物的法拉第效率的优势。催化剂和系统的综合效应在高电流密度(100-300 mA/cm范围内)和相对较低的外加电位(低至-0.65 V vs RHE)下实现了先进的产物选择性。在1 M KOH中,Cu立方体的乙烯选择性高达57%,相应的质量活性为700 mA/mg,Cu八面体的甲烷选择性高达51%,相应的质量活性为1.45 A/mg。