以宽禁带 SrTiO3 为电催化剂，高掺杂 Ru 打破析氧反应活性与稳定性之间的关系,ACS Catalysis

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以宽禁带 SrTiO3 为电催化剂，高掺杂 Ru 打破析氧反应活性与稳定性之间的关系
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-05-09 , DOI: 10.1021/acscatal.1c05539
Heng-Jui Liu, Ching-Yu Chiang, Yun-Sheng Wu, Li-Ren Lin, Yi-Chen Ye, Yi-Hong Huang, Jai-Lin Tsai, Ying-Chih Lai, Ratiporn Munprom

长期以来，创造高效电催化剂以加速析氧反应 (OER) 一直是降低可再生能源技术成本的目标。电催化剂的活性和耐久性通常是两种相互竞争的特性，几乎不会共存。为了实现活性和耐久性的一致性，混合异质结构、成分调制和缺陷工程的策略已被广泛研究。作为一种高活性但耐用性差的电催化剂，钙钛矿 SrRuO ₃ (SRO) 遇到了特定的困境，阻碍了其实际应用。在这项工作中，我们应用了另一个材料设计方向，以宽带隙半导体钙钛矿 SrTiO _3为基础(STO)，在碱性介质中高度稳定。通过在STO中掺杂~30原子%的Ru，与SRO相比，这种固溶体电催化剂可以表现出更好的OER性能和耐久性。以来自电子结构表征和Ru掺杂STO的电化学测量的信息作为直接证据，晶格-氧介导的机制与小电阻率协同提高了OER活性。稳定的STO晶格矩阵还可以防止钙钛矿结构的进一步分解，大大延长了运行时间。我们的工作表明，通过适当调整宽带隙半导体氧化物中的化学成分，可以同时提高电催化活性和耐久性。

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Breaking the Relation between Activity and Stability of the Oxygen-Evolution Reaction by Highly Doping Ru in Wide-Band-Gap SrTiO3 as Electrocatalyst

The creations of efficient electrocatalysts to accelerate the oxygen-evolution reaction (OER) has long been an objective to decrease the cost of renewable energy techniques. The activity and durability of an electrocatalyst are generally two competing properties, which scarcely coexist. To achieve a coincidence of activity and durability, strategies of hybrid heterostructures, composition modulation, and defect engineering have been widely investigated. As a highly active but poorly durable electrocatalyst, the perovskite SrRuO₃ (SRO) encounters the specified dilemma, hampering its practical application. In this work, we applied another direction of material design, which adopted as its base the wide-band-gap semiconductor perovskite SrTiO₃ (STO), which is highly stable in an alkaline medium. Through doping of Ru to extent ∼30 atom % into STO, this solid-solution electrocatalyst can exhibit better OER performance and durability in comparison to SRO. With the information from the characterization of the electronic structures and the electrochemical measurement of Ru-doped STO as direct evidence, a lattice-oxygen-mediated mechanism synergistic with small resistivity increased the OER activity. A stable STO lattice matrix can also prevent the further decomposition of the perovskite structure, substantially extending the period of operation. Our work demonstrates that, through appropriate tuning of the chemical composition in wide-band-gap semiconductor oxides, a simultaneous improvement of electrocatalytic activity and durability is achievable.

更新日期：2022-05-09

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