Plasma-Modified Dendritic Cu Catalyst for CO2 Electroreduction
Plasma-Modified Dendritic Cu Catalyst for CO2 Electroreduction
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DOI：
10.1021/acscatal.9b00483
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发表时间：
2019-06-01
期刊：
影响因子：
12.9
通讯作者：
Roldan Cuenya, Beatriz
中科院分区：
文献类型：
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作者：
Scholten, Fabian;Sinev, Ilya;Roldan Cuenya, Beatriz
在稳定运行期间对碳氢化合物和其他有价值的化学品具有高选择性的高效活性催化剂至关重要。我们利用低压氧等离子体对树枝状Cu催化剂进行改性，并能够提高C-2和C-3产物的选择性。利用操作光谱的方法，如X射线吸收精细结构光谱（XAFS）和准原位X射线光电子能谱（XPS），我们观察到，在这些催化剂中的氧化物的反应前的初始存在起着劣化的作用，在确定其催化性能相比，整体催化剂的形态。这归因于在CO2的电催化转化（CO2 RR）的条件下这些材料中的CuxO物种的差的稳定性。我们的研究结果揭示了强大的结构/化学状态选择性的相关性，在CO2 RR和开放场地的合理设计，更有效的催化剂，通过等离子体预处理。
Efficient and active catalysts with high selectivity for hydrocarbons and other valuable chemicals during stable operation are crucial. We have taken advantage of low-pressure oxygen plasmas to modify dendritic Cu catalysts and were able to achieve enhanced selectivity toward C-2 and C-3 products. Utilizing operando spectroscopic methods such as X-ray absorption fine-structure spectroscopy (XAFS) and quasi in situ X-ray photoelectron spectroscopy (XPS), we observed that the initial presence of oxides in these catalysts before the reaction plays an inferior role in determining their catalytic performance as compared to the overall catalyst morphology. This is assigned to the poor stability of the CuxO species in these materials under the conditions of electrocatalytic conversion of CO2 (CO2RR). Our findings shed light into the strong structure/chemical state-selectivity correlation in CO2RR and open venues for the rational design of more effective catalysts through plasma pretreatments.