Potential-induced nanoclustering of metallic catalysts during electrochemical CO(2) reduction.
Potential-induced nanoclustering of metallic catalysts during electrochemical CO(2) reduction.
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DOI：
10.1038/s41467-018-05544-3
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发表时间：
2018-08-06
影响因子：
16.6
通讯作者：
Buonsanti R
中科院分区：
文献类型：
--
作者：
Huang J;Hörmann N;Oveisi E;Loiudice A;De Gregorio GL;Andreussi O;Marzari N;Buonsanti R
在催化科学中，稳定性与活性和选择性一样重要。了解运行过程中发生的降解途径并制定缓解策略将最终改进催化剂设计，从而促进基础科学向技术应用的转化。在此，我们揭示了独特的和一般的金属纳米催化剂在电化学CO2还原过程中的降解机制，以不同尺寸的铜纳米立方体为例。我们遵循他们的形态演变过程中的操作，并将其与电催化性能。与最常见的聚结和溶解/沉淀机制相比，我们发现电位驱动的纳米团簇是主要的降解途径。大电位密度泛函理论计算证实了作用的负电位施加到减少CO2作为集群的主要驱动力。这项研究提供了一个新的前景，未来的研究的稳定性和降解反应机制的纳米催化剂在电化学CO2还原，更普遍的是，在电还原反应。虽然材料在使用过程中的降解对于了解其性能至关重要，但了解腐蚀过程具有挑战性。在这里，作者发现铜纳米粒子在二氧化碳还原过程中经历了一种不寻常的电位驱动的纳米簇降解途径。
In catalysis science stability is as crucial as activity and selectivity. Understanding the degradation pathways occurring during operation and developing mitigation strategies will eventually improve catalyst design, thus facilitating the translation of basic science to technological applications. Herein, we reveal the unique and general degradation mechanism of metallic nanocatalysts during electrochemical CO2 reduction, exemplified by different sized copper nanocubes. We follow their morphological evolution during operation and correlate it with the electrocatalytic performance. In contrast with the most common coalescence and dissolution/precipitation mechanisms, we find a potential-driven nanoclustering to be the predominant degradation pathway. Grand-potential density functional theory calculations confirm the role of the negative potential applied to reduce CO2 as the main driving force for the clustering. This study offers a novel outlook on future investigations of stability and degradation reaction mechanisms of nanocatalysts in electrochemical CO2 reduction and, more generally, in electroreduction reactions. While the degradation of materials during usage is crucial in understanding their performance, it is challenging to understand the corrosion processes. Here, authors find copper nanoparticles to undergo an unusual potential-driven nanoclustering degradation pathway during carbon dioxide reduction.
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影响因子：
16.6
作者：
Mistry H;Varela AS;Bonifacio CS;Zegkinoglou I;Sinev I;Choi YW;Kisslinger K;Stach EA;Yang JC;Strasser P;Cuenya BR
通讯作者：
Cuenya BR
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16.6
作者：
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32.5
作者：
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影响因子：
15
作者：
Li, Christina W.;Kanan, Matthew W.
通讯作者：
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