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Modulating the valence electronic structure using earth-abundant aluminum for high-performance acidic oxygen evolution reaction
Chem ( IF 19.1 ) Pub Date : 2023-09-01 , DOI: 10.1016/j.chempr.2023.08.006
Kangjae Lee , Jaehyuk Shim , Ho Yeon Jang , Hyeon Seok Lee , Heejong Shin , Byoung-Hoon Lee , Megalamane S. Bootharaju , Kug-Seung Lee , Jongmin Lee , Seongbeom Lee , Young-Hoon Lee , Chan Woo Lee , Yoon Jung , Guocheng Deng , Seungwoo Yoo , Seoin Back , Yung-Eun Sung , Taeghwan Hyeon

Iridium oxide (IrO2) is the most widely used anode catalyst for a proton exchange membrane water electrolyzer (PEMWE). However, its high cost and poor intrinsic activity impede its practical application, which calls for the development of catalysts devoid of Ir or with minimal Ir content. Herein, we designed a facile synthetic route incorporating Al, a p-block metal, into RuO2 and RuIrOx for a durable PEMWE. Al dopants favorably modulate the valence electronic structure of Ru–O hybridized orbitals, which tunes the adsorption energy of oxygen intermediates, consequently promoting the formation of O–O bonds. The optimized Al-doped RuIrOx requires an overpotential of 178 mV at 10 mA cm−2 and maintains the high activity for over 300 h at 100 mA cm−2. In a PEMWE, a high current density of 4.1 A cm−2 at 2.0 V was achieved with negligible performance degradation at 1.0 A cm−2 for 60 h.



中文翻译:


利用地球储量丰富的铝调节价电子结构进行高性能酸性析氧反应



氧化铱(IrO 2 )是质子交换膜水电解槽(PEMWE)中使用最广泛的阳极催化剂。然而,其高成本和较差的本征活性阻碍了其实际应用,这就需要开发不含Ir或Ir含量极低的催化剂。在此,我们设计了一种简便的合成路线,将 p 区金属 Al 掺入 RuO 2 和 RuIrO x 中,以获得耐用的 PEMWE。 Al掺杂剂有利于调节Ru-O杂化轨道的价电子结构,从而调节氧中间体的吸附能,从而促进O-O键的形成。优化的 Al 掺杂 RuIrO x 在 10 mA cm −2 下需要 178 mV 的过电势,并在 100 mA cm −2 下保持高活性超过 300 小时。在 PEMWE 中,在 2.0 V 下实现了 4.1 A cm −2 的高电流密度,在 1.0 A cm −2 下持续 60 小时,性能下降可以忽略不计。

更新日期:2023-09-01
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