Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction
Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction
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DOI：
10.1038/s41467-019-10819-4
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发表时间：
2019-06-26
影响因子：
16.6
通讯作者：
Li, Yanguang
中科院分区：
文献类型：
--
作者：
Gong, Qiufang;Ding, Pan;Li, Yanguang
甲酸（甲酸酯）被认为是电化学二氧化碳还原最经济可行的产物之一。然而，其商业可行性取决于高活性和选择性电催化剂的发展。在这里，我们报道了结构缺陷对铋的电催化性能有深远的积极影响。制备了表面碎片化的氧化铋双壁纳米管作为模板，并将其阴极转化为缺陷铋纳米管。这种转化的电催化剂使二氧化碳还原生成具有优异的活性、选择性和稳定性。最重要的是，在-0.61 V下，与流动电池反应器内的可逆氢电极相比，其电流密度达到类似于288 mA cm（-2）。利用密度泛函理论计算，良好的活性和选择性被合理化为丰富的缺陷铋位点稳定*OCHO中间体的结果。此外，该电催化剂与硅光电阴极耦合，实现了高性能的光电化学二氧化碳还原。
Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. However, its commercial viability hinges on the development of highly active and selective electrocatalysts. Here we report that structural defects have a profound positive impact on the electrocatalytic performance of bismuth. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes. This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Most significantly, its current density reaches similar to 288 mA cm(-2) at -0.61 V versus reversible hydrogen electrode within a flow cell reactor under ambient conditions. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate. Furthermore, this electrocatalyst is coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.