含铁well - dawson多金属氧酸盐与碳纳米材料组成的杂化物作为氧还原反应的电催化剂

Hugo C. Novais, Bruno Jarrais, Israël-Martyr Mbomekallé, Anne-Lucie Teillout, Pedro de Oliveira, Cristina Freire, Diana M. Fernandes
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摘要

氧还原反应(ORR)是燃料电池(fc)等能量转换系统中一个关键的阴极反应。因此,开发经济高效的无贵金属电催化剂替代pt基电催化剂是十分重要的。本文主要研究了基于聚金属氧酸盐(POM)的ECs在ORR中的应用。A well - dawson POM盐K7 [P2W17(FeOH2)O61]。·将20H2O固定在石墨烯薄片和掺杂氮的多壁碳纳米管上,命名为P2W17Fe@GF_N8和P2W17Fe@MWCNT_N8。通过FTIR、XPS和SEM等多种表征技术证明了复合材料的成功制备。两种材料在碱性介质中表现出良好的ORR性能,相对于RHE的电位起始值相似,为~0.84 V, P2W17Fe@MWCNT_N8和P2W17Fe@GF_N8的扩散限制电流密度分别为−3.9和−3.3 mA cm−2。此外,两种复合材料都具有较低的Tafel斜率(48-58 mV dec−1)。计时安培测试显示,与Pt/C相比,制备的纳米复合材料对甲醇的耐受性显著提高,电流保留率达到90%至94%,长期电化学稳定性中等至良好,电流保留率在68%至88%之间。这项工作加强了聚甲醛作为重要电活性物质制备替代ORR电催化剂的使用,在甲醇存在下对ORR表现出良好的活性、稳定性和选择性。
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Hybrids Composed of an Fe-Containing Wells–Dawson Polyoxometalate and Carbon Nanomaterials as Promising Electrocatalysts for the Oxygen Reduction Reaction
The oxygen reduction reaction (ORR) is a key cathodic reaction in energy-converting systems, such as fuel cells (FCs). Thus, it is of utmost importance to develop cost-effective and efficient electrocatalysts (ECs) without noble metals to substitute the Pt-based ones. This study focuses on polyoxometalate (POM)-based ECs for ORR applications. A Wells–Dawson POM salt K7 [P2W17(FeOH2)O61].·20H2O was immobilised onto graphene flakes and multiwalled carbon nanotubes doped with nitrogen, denominated as P2W17Fe@GF_N8 and P2W17Fe@MWCNT_N8. The successful preparation of the composites was proved with various characterisation techniques, including FTIR, XPS and SEM. Both materials showed good ORR performance in an alkaline medium with similar potential onset values of ~0.84 V vs. RHE and diffusion-limiting current densities of −3.9 and −3.3 mA cm−2 for P2W17Fe@MWCNT_N8 and P2W17Fe@GF_N8, respectively. Furthermore, both composites presented low Tafel slopes (48–58 mV dec−1). Chronoamperometric tests revealed that the as-prepared nanocomposites rendered a significant improvement achieving between 90 and 94% of current retention in tolerance to methanol in comparison with Pt/C, and moderate to good long-term electrochemical stability with current retentions comprised between 68 and 88%. This work reinforces the use of POMs as important electroactive species for the preparation of alternative ORR electrocatalysts, exhibiting good activity, stability and selectivity towards the ORR in the presence of methanol.
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