Hyun Gayea, Song Jun Tae, Ahn Changui, Ham Youngjin, Cho Donghwi, Oh Jihun, Jeon Seokwoo
Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 34141 Daejeon, Republic of Korea.
Graduate School of Energy, Environment, Water, and Sustainability, KAIST 34141 Daejeon, Republic of Korea.
Proc Natl Acad Sci U S A. 2020 Mar 17;117(11):5680-5685. doi: 10.1073/pnas.1918837117. Epub 2020 Mar 4.
Electrocatalytic CO reduction is a promising way to provide renewable energy from gaseous CO The development of nanostructures improves energy efficiency and selectivity for value-added chemicals, but complex nanostructures limit the CO conversion rates due to poor mass transport during vigorous electrolysis. Herein, we propose a three-dimensional (3D) hierarchically porous Au comprising interconnected macroporous channels (200-300 nm) and nanopores (∼10 nm) fabricated via proximity-field nanopatterning. The interconnected macropores and nanopores enable efficient mass transport and large active areas, respectively. The roles of each pore network are investigated using reliable 3D nanostructures possessing controlled pore distribution and size. The hierarchical nanostructured electrodes show a high CO selectivity of 85.8% at a low overpotential of 0.264 V and efficient mass activity that is maximum 3.96 times higher than that of dealloyed nanoporous Au. Hence, the systematic model study shows the proposed hierarchical nanostructures have important value in increasing the efficiency of expensive Au.
电催化CO还原是一种从气态CO中获取可再生能源的有前景的方法。纳米结构的发展提高了能源效率和对增值化学品的选择性,但复杂的纳米结构由于在剧烈电解过程中传质较差而限制了CO转化率。在此,我们提出了一种三维(3D)分级多孔金,其由通过近场纳米图案化制造的相互连接的大孔通道(200 - 300 nm)和纳米孔(约10 nm)组成。相互连接的大孔和纳米孔分别实现了高效的传质和大的活性面积。使用具有可控孔分布和尺寸的可靠3D纳米结构研究了每个孔网络的作用。分级纳米结构电极在0.264 V的低过电位下显示出85.8%的高CO选择性和高效的质量活性,其最大比脱合金化纳米多孔金高3.96倍。因此,系统的模型研究表明所提出的分级纳米结构在提高昂贵金的效率方面具有重要价值。