Understanding synergistic metal–oxide interactions of in situ exsolved metal nanoparticles on a pyrochlore oxide support for enhanced water splitting,Energy & Environmental Science

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Understanding synergistic metal–oxide interactions of in situ exsolved metal nanoparticles on a pyrochlore oxide support for enhanced water splitting
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-12-24 , DOI: 10.1039/d0ee02935a
Myeongjin Kim _{1,

2,

3,

4} , Jinho Park _{5,

6,

7,

8,

9} , Hyun Ju _{5,

6,

7,

8} , Jin Young Kim _{4,

10,

11,

12} , Hyun-Seok Cho _{4,

13,

14,

15} , Chang-Hee Kim _{4,

13,

14,

15} , Byung-Hyun Kim _{4,

14,

15,

16} , Seung Woo Lee _{5,

6,

7,

8}

Affiliation

Department of Hydrogen & Renewable Energy
Kyungpook National University
Daegu 41566
Republic of Korea
G. W. Woodruff School of Mechanical Engineering
Georgia Institute of Technology
Atlanta
USA
Aerospace
Fuel Cell Research Center
Korea Institute of Science and Technology (KIST)
Seoul 02792
Hydrogen Research Department
Korea Institute of Energy Research
Daejeon 34129
Platform Technology Laboratory

Hybrid catalysts consisting of metal nanoparticles on a metal oxide support have emerged as a new class of catalysts that can improve various electrocatalytic reactions, but the origin of the improved performance is still unclear. Here we demonstrate that rationally designed hybrid catalysts through the in situ exsolution process of metallic nanoparticles on a B-site Ni-substituted lead ruthenate pyrochlore oxide improve both oxygen evolution reaction and hydrogen evolution reaction activity. A combination of operando X-ray absorption spectroscopy measurements and density functional theory calculations reveals that the generated oxygen and cation vacancies in the pyrochlore oxide support during the in situ exsolution process can decrease the charge-transfer energy, thereby facilitating charge transfer between exsolved metal nanoparticles–oxide support as well as hybrid catalyst–electrolyte. These findings establish a structure–property relationship of complicated hybrid catalysts for efficient water splitting, suggesting a new strategy in designing various hybrid catalysts for other electrochemical reactions.

中文翻译：

了解原位溶解的金属纳米粒子在烧绿石氧化物载体上的协同金属-氧化物相互作用，以增强水分解

由金属氧化物载体上的金属纳米颗粒组成的杂化催化剂已经作为可以改善各种电催化反应的新型催化剂出现，但是改进性能的根源仍然不清楚。在这里，我们证明了通过在B位Ni取代的钌酸钌烧绿石氧化物上原位释放金属纳米颗粒而合理设计的杂化催化剂可以改善氧释放反应和氢释放反应活性。结合操作X射线吸收光谱测量和密度泛函理论计算发现，在原位烧绿石氧化物载体中产生的氧和阳离子空位析出过程可以降低电荷转移能，从而促进溶解的金属纳米颗粒-氧化物载体以及杂化催化剂-电解质之间的电荷转移。这些发现建立了用于高效水分解的复杂杂化催化剂的结构-性质关系，为设计用于其他电化学反应的各种杂化催化剂提供了新的策略。

更新日期：2021-01-07

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