Noble-metal-free Co(3)S(4)-S/G porous hybrids as an efficient electrocatalyst for oxygen reduction reaction.

Noble-metal-free Co(3)S(4)-S/G porous hybrids as an efficient electrocatalyst for oxygen reduction reaction.
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DOI:
10.1039/c6sc00357e
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发表时间:
2016-07-01
期刊:
影响因子:
8.4
通讯作者:
Wang E
Wang E
中科院分区:
化学1区
文献类型:
--
作者:
Gu W;Hu L;Hong W;Jia X;Li J;Wang E

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以廉价的前驱体二硫代钴(S4-络合物)为原料,同时还原的氧化石墨烯(GO)为载体,制备了一种高效的无贵金属氧还原反应催化剂。开发一种新型的无贵金属催化剂来替代铂基催化剂在碱性和酸性条件下的氧还原反应(ORR)对燃料电池具有极其重要的意义。本文基于廉价的前驱体二硫代钴(S4-络合物)在同时还原的氧化石墨烯(GO)上的热解反应,制备了以多孔硫掺杂石墨烯包裹的Co3S4纳米粒子为载体的高效无贵金属氧还原杂化催化剂(简称Co3S4-S/G)。在800℃下制得的催化剂(Co3S4-S/G-800)表现出良好的氧还原活性。值得注意的是,Co3S4-S/G-800杂化催化剂在酸性电解液中也表现出高选择性(主要是4E反应过程)和很低的H_2O_2产率。优化的Co3S4-S/G-800杂化催化剂表现出比铂/C更强的耐甲醇能力和更高的稳定性,这些优异的性能表明Co3S4-S/G-800电催化剂在燃料电池中具有很大的潜力。同时,本工作也为利用低成本、易合成的S4-络合物制备硫族钴化合物提供了一种简单实用的方法。
A high-efficiency noble-metal-free oxygen reduction reaction (ORR) catalyst was obtained based on the pyrolysis of the inexpensive precursor cobalt dithiolene (an S4-chelate complex) on simultaneously reduced graphene oxide (GO) as a support matrix. Developing of a new noble-metal-free catalyst to replace Pt-based catalysts of the oxygen reduction reaction (ORR) both in alkaline and acidic conditions is extremely significant for the fuel cell. In this paper, based on the pyrolysis of an inexpensive precursor cobalt dithiolene (a S4-chelate complex) on simultaneously reduced graphene oxide (GO) as a support matrix, a high-efficiency noble-metal-free hybrid for oxygen reduction reaction (ORR) consisting of Co3S4 nanoparticles encapsulated in porous sulfur doped graphene (referred as Co3S4–S/G) was fabricated. The catalyst obtained at 800 °C (Co3S4–S/G-800) manifests excellent oxygen reduction activity. Of note, the Co3S4–S/G-800 hybrids also exhibited prominent ORR activity with high selectivity (mainly 4e– reaction process) and very low H2O2 yield in acidic electrolyte. The optimal Co3S4–S/G-800 hybrid displayed much greater tolerance to methanol and higher stability than that of Pt/C. These admirable performances endorse Co3S4–S/G-800 electrocatalyst holding great potential for fuel cells. Meanwhile, this work also provides a simple and practical method to fabricate cobalt chalcogenides by using the cost-effective and easily synthesized S4-chelate complex.
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