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Surface reconstruction of RuO2/Co3O4 amorphous-crystalline heterointerface for efficient overall water splitting
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2023-12-09 , DOI: 10.1016/j.jcis.2023.12.045
Qiaohong Su 1 , Rui Sheng 1 , Qingcui Liu 1 , Juan Ding 1 , Pengyue Wang 1 , Xingchao Wang 1 , Jiulin Wang 1 , Yonggang Wang 2 , Bao Wang 3 , Yudai Huang 1
Affiliation  

The rational construction of amorphous-crystalline heterointerface can effectively improve the activity and stability of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, RuO2/Co3O4 (RCO) amorphous-crystalline heterointerface is prepared via oxidation method. The optimal RCO-10 exhibits low overpotentials of 57 and 231 mV for HER and OER at 10 mA cm−2, respectively. Experimental characterization and density functional theory (DFT) results show that the optimized electronic structure and surface reconstruction endow RCO-10 with excellent catalytic activity. DFT results show that electrons transfer from RuO2 to Co3O4 through the amorphous-crystalline heterointerface, achieving electron redistribution and moving the d-band center upward, which optimizes the adsorption free energy of the hydrogen reaction intermediate. Moreover, the reconstructed Ru/Co(OH)2 during the HER process has low hydrogen adsorption free energy to enhance HER activity. The reconstructed RuO2/CoOOH during the OER process has a low energy barrier for the elementary reaction (O*→*OOH) to enhance OER activity. Furthermore, RCO-10 requires only 1.50 V to drive 10 mA cm−2 and maintains stability over 200 h for overall water splitting. Meanwhile, RCO-10 displays stability for 48 h in alkaline solutions containing 0.5 M NaCl. The amorphous-crystalline heterointerface may bring new breakthroughs in the design of efficient and stable catalysts.



中文翻译:


RuO2/Co3O4 非晶态异质界面的表面重构,实现高效的整体水分解



合理构建非晶-结晶异质界面可以有效提高析氢反应(HER)和析氧反应(OER)的活性和稳定性。本文通过氧化法制备了RuO 2 /Co 3 O 4 (RCO)非晶-结晶异质界面。最佳RCO-10在10 mA cm -2下对HER和OER分别表现出57和231 mV的低过电势。实验表征和密度泛函理论(DFT)结果表明,优化的电子结构和表面重构赋予RCO-10优异的催化活性。 DFT结果表明,电子通过非晶-结晶异质界面从RuO 2转移到Co 3 O 4 ,实现电子重新分布并使d带中心向上移动,从而优化了氢反应中间体的吸附自由能。此外,在HER过程中重构的Ru/Co(OH) 2具有较低的氢吸附自由能,从而增强了HER活性。 OER过程中重构的RuO 2 /CoOOH对基元反应(O*→*OOH)具有较低的能垒,从而增强了OER活性。此外,RCO-10仅需要1.50 V即可驱动10 mA cm -2并在整个水分解过程中保持稳定性超过200小时。同时,RCO-10 在含有 0.5 M NaCl 的碱性溶液中表现出 48 小时的稳定性。非晶-结晶异质界面可能为高效稳定催化剂的设计带来新的突破。

更新日期:2023-12-09
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