Electrochemical Evolution of Ru-Based Polyoxometalates into Si,W-Codoped RuOx for Acidic Overall Water Splitting,Advanced Materials

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Electrochemical Evolution of Ru-Based Polyoxometalates into Si,W-Codoped RuOx for Acidic Overall Water Splitting
Advanced Materials ( IF 27.4 ) Pub Date : 2023-11-11 , DOI: 10.1002/adma.202304468
Dasom Jeon _{1,

2} , Dong Yeon Kim ₃ , Hyeongoo Kim _{1,

2} , Nayeong Kim _{1,

2} , Cheolmin Lee _{1,

2} , Dong-Hwa Seo ₃ , Jungki Ryu _{1,

2,

4,

5}

Affiliation

Despite intensive studies over decades, the development of electrocatalysts for acidic water splitting still relies on platinum group metals, especially Pt and Ir, which are scarce, expensive, and poorly sustainable. Because such problems can be alleviated, Ru-based bifunctional catalysts such as rutile RuO₂ have recently emerged. However, RuO₂ has a relatively low activity for hydrogen evolution reactions (HER) and low stability for oxygen evolution reactions (OER) under acidic conditions. In this study, the synthesis of a RuO_x-based bifunctional catalyst (RuSiW) for acidic water splitting via the electrochemical evolution from Ru-based polyoxometalates at cathodic potentials is reported. RuSiW consists of the nanocrystalline RuO₂ core and Si,W-codoped RuO_x shell. RuSiW exhibits outstanding HER and OER activity comparable to Pt/C and RuO₂, respectively, with high stability. Computational analysis suggests that the codoping of RuO_x with W and Si synergistically improves the HER activity of otherwise poor RuO₂ by shifting the d-band center and optimizing atomic configurations beneficial for proper hydrogen adsorption. This study provides insights into the design and synthesis of unprecedented bifunctional electrocatalysts using catalytically inactive and less explored elements, such as Si and W.

中文翻译：

Ru基多金属氧酸盐电化学演化为Si,W共掺杂RuOx用于酸性全水分解

尽管经过数十年的深入研究，酸性水分解电催化剂的开发仍然依赖于铂族金属，特别是铂和铱，它们稀缺、昂贵且可持续性差。由于这些问题可以得到缓解，最近出现了基于Ru的双功能催化剂，例如金红石RuO ₂ 。然而，RuO ₂在酸性条件下具有相对较低的析氢反应(HER)活性和较低的析氧反应(OER)稳定性。在这项研究中，报道了通过在阴极电位下基于 Ru 的多金属氧酸盐的电化学演化来合成用于酸性水分解的基于 RuO _x的双功能催化剂（RuSiW）。 RuSiW由纳米晶RuO ₂核和Si,W共掺杂RuO _x壳组成。 RuSiW 表现出出色的 HER 和 OER 活性，分别可与 Pt/C 和 RuO ₂相媲美，并且具有高稳定性。计算分析表明，RuO _x与 W 和 Si 的共掺杂通过移动 d 带中心和优化有利于适当氢吸附的原子构型，协同提高了原本较差的 RuO ₂的 HER 活性。这项研究为使用硅和钨等催化惰性和较少探索的元素设计和合成前所未有的双功能电催化剂提供了见解。

更新日期：2023-11-11

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