Engineering eg filling of RuO2 enables a robust and stable acidic water oxidation

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters Pub Date : 2024-11-05 DOI:10.1016/j.cclet.2024.110612

Qing Li , Yumei Feng , Yingjie Yu , Yazhou Chen , Yuhua Xie , Fang Luo , Zehui Yang

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Abstract

Efficient and stable electrocatalyst for oxygen evolution reaction (OER) in acidic environment is vital for polymer electrolyte membrane water electrolysis (PEMWE). In this work, we have devised the formation of heterostructured RuO₂/MnO₂ with nanoflower structure for acidic OER catalysis. Compared to commercial RuO₂, the overpotential at 50 mA/cm² is decreased by 36 mV, corresponding to a 3.7-fold better mass activity. The boosted acidic OER performance is attributed to the heterostructure inducing more electrons are filled in e_g orbital of Ru atom triggering a better deprotonation of bridge oxygen atom in Ru-O_bri-Mn structure evidenced by pH-independent cyclic voltammetry test. Moreover, RuO₂/MnO₂ sustains its acidic OER activity within 20 h, longer than commercial RuO₂. The membrane electrode assembly (MEA) test suggests than only 2.18 V is required to achieve a current density of 5 A/cm². The theoretical calculation reveals that the e_g filling of Ru atom is increased from 2.18 to 2.39 after MnO₂ incorporation, reducing the energy for the formation of *OOH moiety.

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工程上如充注RuO2，使酸性水氧化稳定而有力

高效、稳定的酸性析氧反应电催化剂是实现聚合物电解质膜电解的关键。在这项工作中，我们设计了具有纳米花结构的异质结构的RuO2/MnO2的形成，用于酸性OER催化。与商用RuO2相比，50 mA/cm2下的过电位降低了36 mV，质量活性提高了3.7倍。非ph循环伏安试验证明，异质结构导致Ru原子的eg轨道上填充了更多的电子，从而使Ru- obi - mn结构中的桥氧原子更好地去质子化。此外，RuO2/MnO2的酸性OER活性维持时间为20 h，比商用RuO2长。膜电极组件（MEA）测试表明，只需2.18 V即可达到5 a /cm2的电流密度。理论计算表明，加入MnO2后，Ru原子的eg填充从2.18增加到2.39，降低了*OOH部分的形成能量。

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来源期刊

Chinese Chemical Letters 化学-化学综合

CiteScore

14.10

自引率

15.40%

发文量

8969

审稿时长

1.6 months

期刊介绍： Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.