Yan Haohao, Wang Yongjie, Xin Yue, Jiang Zhongqing, Deng Binglu, Jiang Zhong-Jie
Guangzhou Key Laboratory for Surface Chemistry of Energy Materials, Guangdong Engineering and Technology Research Center for Surface Chemistry of Energy Materials, College of Environment and Energy, South China University of Technology, Guangzhou, 510006, P. R. China.
Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems, Harbin Institute of Technology, Shenzhen, 518055, P. R. China.
Small. 2024 Nov;20(47):e2406070. doi: 10.1002/smll.202406070. Epub 2024 Aug 11.
This work reports a strategy that integrates the carbon nanotube (CNT) supporting, ultrathin carbon coating and oxygen defect generation to fabricate the RuO based catalysts toward the pH-universal hydrogen evolution reaction (HER) with high efficiencies. Specifically, the CNT supported RuO nanoparticles with ultrathin carbon loricae and rich oxygen vacancies at the surface (C@OV-RuO/CNTs-325) have been synthesized. The C@OV-RuO/CNTs-325 shows superior activities and excellent durability for the HER. It only requires overpotentials of 36.1, 18.0, and 19.3 mV to deliver -10 mA cm in the acidic, neutral, and alkaline media, respectively. Its HER activities are comparable to that of the Pt/C in the acidic media but higher than those of the Pt/C in the neutral and alkaline media. The C@OV-RuO/CNTs-325 shows excellent HER durability with no activity losses for > 500 h in the acidic, neutral or alkaline media at -250 mA cm. The density-functional-theory calculations indicate that the CNT supporting, the carbon coating, and the OVs can modulate the d-band centers of Ru, increasing the HER activities of C@OV-RuO/CNTs-325, and stabilize the Ru atoms in the catalyst, increasing the durability of the C@OV-RuO/CNTs-325. More interestingly, the C@OV-RuO/CNTs-325 shows great potential for practical applications toward overall seawater splitting.
这项工作报道了一种策略,该策略整合了碳纳米管(CNT)支撑、超薄碳涂层和氧缺陷生成,以制备用于高效pH通用析氢反应(HER)的RuO基催化剂。具体而言,已经合成了表面具有超薄碳壳层和丰富氧空位的CNT负载RuO纳米颗粒(C@OV-RuO/CNTs-325)。C@OV-RuO/CNTs-325在HER中表现出优异的活性和出色的耐久性。在酸性、中性和碱性介质中分别仅需36.1、18.0和19.3 mV的过电位即可实现-10 mA cm的电流密度。其HER活性在酸性介质中与Pt/C相当,但在中性和碱性介质中高于Pt/C。C@OV-RuO/CNTs-325在-250 mA cm的电流密度下,在酸性、中性或碱性介质中>500 h均无活性损失,表现出优异的HER耐久性。密度泛函理论计算表明,CNT支撑、碳涂层和氧空位可以调节Ru的d带中心,提高C@OV-RuO/CNTs-325的HER活性,并使催化剂中的Ru原子稳定,提高C@OV-RuO/CNTs-325的耐久性。更有趣的是,C@OV-RuO/CNTs-325在实际应用于整体海水分解方面显示出巨大潜力。