Jeng Emily, Qi Zhen, Kashi Ajay R, Hunegnaw Sara, Huo Ziyang, Miller John S, Bayu Aji Leonardus B, Ko Byung Hee, Shin Haeun, Ma Sichao, Kuhl Kendra P, Jiao Feng, Biener Juergen
Center for Catalytic Science & Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, Delaware 19716, United States.
Materials Science Division, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550, United States.
ACS Appl Mater Interfaces. 2022 Feb 16;14(6):7731-7740. doi: 10.1021/acsami.1c17860. Epub 2022 Feb 7.
Electrochemical CO reduction (ECR) promises the replacement of fossil fuels as the source of feedstock chemicals and seasonal storage of renewable energy. While much progress has been made in catalyst development and electrochemical reactor design, few studies have addressed the effect of catalyst integration on device performance. Using a microfluidic gas diffusion electrolyzer, we systematically studied the effect of thickness and the morphology of electron beam (EB) and magnetron-sputtered (MS) Cu catalyst coatings on ECR performance. We observed that EB-Cu outperforms MS-Cu in current density, selectivity, and energy efficiency, with 400 nm thick catalyst coatings performing the best. The superior performance of EB-Cu catalysts is assigned to their faceted surface morphology and sharper Cu/gas diffusion layer interface, which increases their hydrophobicity. Tests in a large-scale zero-gap electrolyzer yielded similar product selectivity distributions with an ethylene Faradaic efficiency of 39% at 200 mA/cm, demonstrating the scalability for industrial ECR applications.
电化学CO还原(ECR)有望取代化石燃料,成为原料化学品的来源和可再生能源的季节性储存方式。虽然在催化剂开发和电化学反应器设计方面已经取得了很大进展,但很少有研究探讨催化剂集成对器件性能的影响。我们使用微流控气体扩散电解槽,系统地研究了电子束(EB)和磁控溅射(MS)铜催化剂涂层的厚度和形态对ECR性能的影响。我们观察到,在电流密度、选择性和能量效率方面,EB-Cu优于MS-Cu,400 nm厚的催化剂涂层表现最佳。EB-Cu催化剂的优异性能归因于其多面体形表面形态和更清晰的Cu/气体扩散层界面,这增加了它们的疏水性。在大规模零间隙电解槽中的测试产生了类似的产物选择性分布,在200 mA/cm下乙烯法拉第效率为39%,证明了其在工业ECR应用中的可扩展性。