Microstructural origin of locally enhanced CO2 electroreduction activity on gold
Microstructural origin of locally enhanced CO2 electroreduction activity on gold
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DOI：
10.1038/s41563-021-00958-9
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发表时间：
2021-03-18
期刊：
影响因子：
41.2
通讯作者：
Kanan, Matthew W.
中科院分区：
文献类型：
--
作者：
Mariano, Ruperto G.;Kang, Minkyung;Kanan, Matthew W.
了解材料的整体结构如何影响其表面的催化作用，对于制定可操作的催化剂设计原则至关重要。体缺陷已被证明会影响电催化材料，这是重要的能量转换系统，但这些影响的结构起源尚未完全阐明。在这里，我们使用高分辨率的扫描电化学电池显微镜和电子背散射衍射的组合来可视化的电位依赖的电催化二氧化碳（CO2）电还原和氢气（H-2）的演变活动的Au电极和探测体缺陷的影响。将同位活动图和视频与底层微观结构和晶格变形进行比较，支持了一种模型，其中CO2电还原通过表面终止位错选择性增强，该位错可以在晶界和滑移带处积累。我们的研究结果表明，有意识地将位错引入到材料中是改善催化性能的一种有前途的策略。
Understanding how the bulk structure of a material affects catalysis on its surface is critical to the development of actionable catalyst design principles. Bulk defects have been shown to affect electrocatalytic materials that are important for energy conversion systems, but the structural origins of these effects have not been fully elucidated. Here we use a combination of high-resolution scanning electrochemical cell microscopy and electron backscatter diffraction to visualize the potential-dependent electrocatalytic carbon dioxide (CO2) electroreduction and hydrogen (H-2) evolution activity on Au electrodes and probe the effects of bulk defects. Comparing colocated activity maps and videos to the underlying microstructure and lattice deformation supports a model in which CO2 electroreduction is selectively enhanced by surface-terminating dislocations, which can accumulate at grain boundaries and slip bands. Our results suggest that the deliberate introduction of dislocations into materials is a promising strategy for improving catalytic properties.