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Controllable synthesis of grain boundary-enriched Pt nanoworms decorated on graphitic carbon nanosheets for ultrahigh methanol oxidation catalytic activity
Journal of Energy Chemistry ( IF 13.1 ) Pub Date : 2020-09-08 , DOI: 10.1016/j.jechem.2020.08.063
Huajie Huang , Yujie Wei , Ying Yang , Minmin Yan , Haiyan He , Quanguo Jiang , Xiaofei Yang , Jixin Zhu

Although one-dimensional Pt nanocrystals have long been regarded as ideal electrode catalysts for fuel cells, the synthetic techniques commonly involve the use of various complicated templates or surfactants, which have largely hampered their large-scale industrial application. Herein, we present a convenient and cost-effective approach to the stereoassembly of quasi-one-dimensional grain boundary-enriched Pt nanoworms on nitrogen-doped low-defect graphitic carbon nanosheets (Pt NWs/NL-CNS). Benefiting from its numerous catalytically active grain boundaries as well as optimized electronic structure, the as-derived Pt NWs/NL-CNS catalyst possesses exceptionally good electrocatalytic properties for methanol oxidation, including an ultrahigh mass activity of 1949.5 mA mg-1, reliable long-term durability, and strong poison tolerance, affording one of the most active Pt-based electrocatalysts for methanol oxidation reaction. Density functional theory calculation further reveals that the formation of worm-shape Pt morphology is attributed to the modified electronic structure as well as controllable defect density of the carbon matrix, which could also weaken the adsorption ability of Pt towards CO molecule and meanwhile synergistically promotes the catalytic reaction kinetics.



中文翻译:

可控合成石墨碳纳米片上富集晶界富集的Pt纳米蠕虫,具有超高的甲醇氧化催化活性

尽管一维Pt纳米晶体长期以来一直被认为是燃料电池的理想电极催化剂,但合成技术通常涉及使用各种复杂的模板或表面活性剂,这在很大程度上阻碍了其大规模工业应用。在这里,我们提出了一种方便且具有成本效益的方法,用于在氮掺杂的低缺陷石墨碳纳米片(Pt NWs / NL-CNS)上立体组装准一维富晶界的Pt纳米蠕虫。得益于其众多的催化活性晶界以及优化的电子结构,这种衍生的Pt NWs / NL-CNS催化剂具有出色的甲醇氧化电催化性能,包括1949.5 mA mg -1的超高质量活性,可靠的长期耐用性和强大的毒物耐受性,是甲醇氧化反应中活性最高的基于Pt的电催化剂之一。密度泛函理论计算进一步表明,蠕虫状Pt形态的形成归因于修饰的电子结构以及碳基体的可控缺陷密度,这也可能削弱了Pt对CO分子的吸附能力,同时协同促进了Pt对CO分子的吸附。催化反应动力学。

更新日期:2020-09-09
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