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Elucidation of Structure–Activity Relations in Proton Electroreduction at Pd Surfaces: Theoretical and Experimental Study
Small ( IF 13.3 ) Pub Date : 2022-06-20 , DOI: 10.1002/smll.202202410 Thorsten O Schmidt 1 , Apinya Ngoipala 2 , Ryan L Arevalo 2 , Sebastian A Watzele 1 , Raju Lipin 2 , Regina M Kluge 1 , Shujin Hou 1, 3 , Richard W Haid 1 , Anatoliy Senyshyn 4 , Elena L Gubanova 1 , Aliaksandr S Bandarenka 1, 3 , Matthias Vandichel 2
Small ( IF 13.3 ) Pub Date : 2022-06-20 , DOI: 10.1002/smll.202202410 Thorsten O Schmidt 1 , Apinya Ngoipala 2 , Ryan L Arevalo 2 , Sebastian A Watzele 1 , Raju Lipin 2 , Regina M Kluge 1 , Shujin Hou 1, 3 , Richard W Haid 1 , Anatoliy Senyshyn 4 , Elena L Gubanova 1 , Aliaksandr S Bandarenka 1, 3 , Matthias Vandichel 2
Affiliation
The structure–activity relationship is a cornerstone topic in catalysis, which lays the foundation for the design and functionalization of catalytic materials. Of particular interest is the catalysis of the hydrogen evolution reaction (HER) by palladium (Pd), which is envisioned to play a major role in realizing a hydrogen-based economy. Interestingly, experimentalists observed excess heat generation in such systems, which became known as the debated “cold fusion” phenomenon. Despite the considerable attention on this report, more fundamental knowledge, such as the impact of the formation of bulk Pd hydrides on the nature of active sites and the HER activity, remains largely unexplored. In this work, classical electrochemical experiments performed on model Pd(hkl) surfaces, “noise” electrochemical scanning tunneling microscopy (n-EC-STM), and density functional theory are combined to elucidate the nature of active sites for the HER. Results reveal an activity trend following Pd(111) > Pd(110) > Pd(100) and that the formation of subsurface hydride layers causes morphological changes and strain, which affect the HER activity and the nature of active sites. These findings provide significant insights into the role of subsurface hydride formation on the structure–activity relations toward the design of efficient Pd-based nanocatalysts for the HER.
中文翻译:
阐明 Pd 表面质子电还原的结构-活性关系:理论和实验研究
构效关系是催化领域的基石课题,为催化材料的设计和功能化奠定了基础。特别令人感兴趣的是钯 (Pd) 对析氢反应 (HER) 的催化作用,预计这将在实现基于氢的经济中发挥重要作用。有趣的是,实验者观察到此类系统中产生过多热量,这被称为备受争议的“冷聚变”现象。尽管该报告引起了相当多的关注,但更多的基础知识,例如散装 Pd 氢化物的形成对活性位点性质和 HER 活性的影响,在很大程度上仍未得到探索。在这项工作中,在模型 Pd(hkl) 表面上进行的经典电化学实验、“噪声”电化学扫描隧道显微镜 (n-EC-STM)、结合密度泛函理论来阐明HER活性位点的性质。结果揭示了Pd(111)> Pd(110)> Pd(100)的活性趋势,并且亚表面氢化物层的形成引起形态变化和应变,从而影响HER活性和活性位点的性质。这些发现为深入了解表面下氢化物的形成对结构-活性关系的作用提供了重要的见解,从而有助于设计用于 HER 的高效 Pd 基纳米催化剂。
更新日期:2022-06-20
中文翻译:
阐明 Pd 表面质子电还原的结构-活性关系:理论和实验研究
构效关系是催化领域的基石课题,为催化材料的设计和功能化奠定了基础。特别令人感兴趣的是钯 (Pd) 对析氢反应 (HER) 的催化作用,预计这将在实现基于氢的经济中发挥重要作用。有趣的是,实验者观察到此类系统中产生过多热量,这被称为备受争议的“冷聚变”现象。尽管该报告引起了相当多的关注,但更多的基础知识,例如散装 Pd 氢化物的形成对活性位点性质和 HER 活性的影响,在很大程度上仍未得到探索。在这项工作中,在模型 Pd(hkl) 表面上进行的经典电化学实验、“噪声”电化学扫描隧道显微镜 (n-EC-STM)、结合密度泛函理论来阐明HER活性位点的性质。结果揭示了Pd(111)> Pd(110)> Pd(100)的活性趋势,并且亚表面氢化物层的形成引起形态变化和应变,从而影响HER活性和活性位点的性质。这些发现为深入了解表面下氢化物的形成对结构-活性关系的作用提供了重要的见解,从而有助于设计用于 HER 的高效 Pd 基纳米催化剂。