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Design of atomically precise Au2Pd6 nanoclusters for boosting electrocatalytic hydrogen evolution on MoS2†
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2018-09-27 00:00:00 , DOI: 10.1039/c8qi00697k Yuanxin Du 1, 2, 3, 4, 5 , Ji Xiang 1, 2, 3, 4, 5 , Kun Ni 6, 7, 8, 9, 10 , Yapei Yun 1, 2, 3, 4, 5 , Guodong Sun 1, 2, 3, 4, 5 , Xiaoyou Yuan 1, 2, 3, 4, 5 , Hongting Sheng 1, 2, 3, 4, 5 , Yanwu Zhu 6, 7, 8, 9, 10 , Manzhou Zhu 1, 2, 3, 4, 5
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2018-09-27 00:00:00 , DOI: 10.1039/c8qi00697k Yuanxin Du 1, 2, 3, 4, 5 , Ji Xiang 1, 2, 3, 4, 5 , Kun Ni 6, 7, 8, 9, 10 , Yapei Yun 1, 2, 3, 4, 5 , Guodong Sun 1, 2, 3, 4, 5 , Xiaoyou Yuan 1, 2, 3, 4, 5 , Hongting Sheng 1, 2, 3, 4, 5 , Yanwu Zhu 6, 7, 8, 9, 10 , Manzhou Zhu 1, 2, 3, 4, 5
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Atomically precise nanoclusters (NCs) have been widely used as catalysts in many reactions to investigate the structure–activity relationship due to their ultrasmall sizes, well-defined structures and precise compositions, especially bimetallic NCs can further promote the catalytic activity by the synergistic effects of heteroatoms. For electrocatalytic hydrogen evolution reaction (HER) catalysts, a common method to improve the performance is coupling with a nano-metal, but the origin of the enhancement is still unclear due to the diversity and complexity of the nanometal supported composites. Here, we take MoS2 (a star HER electrocatalyst) as an example, to report a strategy to boost the activity and give insight into the activity enhancement of it by combining with bimetallic atomically precise NCs. The crystal structure of this new NC is determined by X-ray crystallography, and its precise composition is identified as Au2Pd6S4(PPh3)4(C6H4F2S)6 (Au2Pd6 for short). The Au2Pd6/MoS2 show significantly improved HER activity and robust durability compared to the single component Pd3 or Au2/MoS2 and bare MoS2. This is attributed to the appropriate adsorption behavior of H atoms on Au2Pd6/MoS2 and the electronic interactions between NCs and MoS2, according to the combination of experiment and theory. This study presents a new strategy to improve the electrocatalytic activity of 2D materials such as MoS2 and sheds light on the origin of the promotion effects at the atomic level.
中文翻译：
原子精确Au 2 Pd 6纳米团簇的设计，以促进MoS 2 †上的电催化氢释放
原子精确的纳米团簇（NCs）由于其超小尺寸，定义明确的结构和精确的组成而在许多反应中被广泛用作催化剂，以研究结构与活性之间的关系，尤其是双金属NCs可以通过协同作用进一步促进催化活性。杂原子。对于电催化放氢反应（HER）催化剂，提高性能的常用方法是与纳米金属偶联，但是由于纳米金属负载的复合材料的多样性和复杂性，增强的起源仍不清楚。在这里，我们采用MoS 2（以星型HER电催化剂为例），以报告一种通过与双金属原子精确NC结合来增强活性并深入了解其活性的策略。这个新的NC的晶体结构通过X射线晶体学测定，并且其精确组成被鉴定为金2的Pd 6小号4（PPH 3）4（C 6 H ^ 4 ˚F 2 S）6（AU 2的Pd 6为短）。与单组分Pd相比，Au 2 Pd 6 / MoS 2显示出显着改善的HER活性和耐用性3或Au 2 / MoS 2和裸MoS 2。根据实验和理论的结合，这归因于H原子在Au 2 Pd 6 / MoS 2上的适当吸附行为以及NC和MoS 2之间的电子相互作用。这项研究提出了一种新的策略，以改善诸如MoS 2的2D材料的电催化活性，并阐明了在原子水平上促进作用的起源。
更新日期：2018-09-27
中文翻译：
原子精确Au 2 Pd 6纳米团簇的设计，以促进MoS 2 †上的电催化氢释放
原子精确的纳米团簇（NCs）由于其超小尺寸，定义明确的结构和精确的组成而在许多反应中被广泛用作催化剂，以研究结构与活性之间的关系，尤其是双金属NCs可以通过协同作用进一步促进催化活性。杂原子。对于电催化放氢反应（HER）催化剂，提高性能的常用方法是与纳米金属偶联，但是由于纳米金属负载的复合材料的多样性和复杂性，增强的起源仍不清楚。在这里，我们采用MoS 2（以星型HER电催化剂为例），以报告一种通过与双金属原子精确NC结合来增强活性并深入了解其活性的策略。这个新的NC的晶体结构通过X射线晶体学测定，并且其精确组成被鉴定为金2的Pd 6小号4（PPH 3）4（C 6 H ^ 4 ˚F 2 S）6（AU 2的Pd 6为短）。与单组分Pd相比，Au 2 Pd 6 / MoS 2显示出显着改善的HER活性和耐用性3或Au 2 / MoS 2和裸MoS 2。根据实验和理论的结合，这归因于H原子在Au 2 Pd 6 / MoS 2上的适当吸附行为以及NC和MoS 2之间的电子相互作用。这项研究提出了一种新的策略，以改善诸如MoS 2的2D材料的电催化活性，并阐明了在原子水平上促进作用的起源。
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