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过渡金属氧化物/碳化物@碳纳米管复合材料作为用于挑战性氧化和还原反应的多功能电催化剂

Transition-Metal Oxides/Carbides@Carbon Nanotube Composites as Multifunctional Electrocatalysts for Challenging Oxidations and Reductions.

作者信息

Xing Xiaolin, Liu Rongji, Cao Kecheng, Kaiser Ute, Streb Carsten

机构信息

Institute of Inorganic Chemistry I, Ulm University, Ulm, 89081, Germany.

Institute of Process Engineering, Key Laboratory of Green Process and Engineering, Chinese Academy of Sciences, Beijing, 100190, China.

出版信息

Chemistry. 2019 Aug 22;25(47):11098-11104. doi: 10.1002/chem.201901400. Epub 2019 Jul 28.

Abstract

The rapid development of renewable-energy technologies such as water splitting, rechargeable metal-air batteries, and fuel cells requires highly efficient electrocatalysts capable of the oxygen-reduction reaction (ORR) and the oxygen-evolution reaction (OER). Herein, we report a facile sonication-driven synthesis to deposit the molecular manganese vanadium oxide precursor [Mn V O (OAc) ] on multiwalled carbon nanotubes (MWCNTs). Thermal conversion of this composite at 900 °C gives nanostructured manganese vanadium oxides/carbides, which are stably linked to the MWCNTs. The resulting composites show excellent electrochemical reactivity for ORR and OER, and significant reactivity enhancements compared with the precursors and a Pt/C reference are reported. Notably, even under harsh acidic conditions, long-term OER activity at low overpotential is reported. In addition, we report exceptional activity of the composites for the industrially important Cl evolution from an aqueous HCl electrolyte. The new composite material shows how molecular deposition routes leading to highly active and stable multifunctional electrocatalysts can be developed. The facile design could in principle be extended to multiple catalyst classes by tuning of the molecular metal oxide precursor employed.

摘要

诸如水分解、可充电金属空气电池和燃料电池等可再生能源技术的快速发展,需要能够催化氧还原反应(ORR)和析氧反应(OER)的高效电催化剂。在此,我们报道了一种通过超声驱动的简便合成方法,将分子锰钒氧化物前驱体[Mn V O (OAc) ]沉积在多壁碳纳米管(MWCNT)上。该复合材料在900 °C下进行热转化,得到纳米结构的锰钒氧化物/碳化物,它们与MWCNT稳定相连。所得复合材料对ORR和OER表现出优异的电化学反应活性,与前驱体相比有显著的活性增强,并且与Pt/C参比电极相比也有显著提升。值得注意的是,即使在苛刻的酸性条件下,也报道了其在低过电位下的长期OER活性。此外,我们还报道了该复合材料对从HCl水溶液电解质中进行工业上重要的析氯反应具有优异的活性。这种新型复合材料展示了如何开发出能够生成高活性和稳定的多功能电催化剂的分子沉积路线。通过调整所使用的分子金属氧化物前驱体,这种简便的设计原则上可以扩展到多种催化剂类别。

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