论文标题

Octapod形的CDSE纳米晶体托有具有高质量活性的氢进化反应的PT

Octapod-shaped CdSe nanocrystals hosting Pt with high-mass activity for the hydrogen evolution reaction

论文作者

Najafi, Leyla, Bellani, Sebastiano, Castelli, Andrea, Arciniegas, Milena P., Brescia, Rosaria, Oropesa-Nuñez, Reinier, Martín-García, Beatriz, Serri, Michele, Drago, Filippo, Manna, Liberato, Bonaccorso, Francesco

论文摘要

用最少的贵金属量的电化学水分裂的有效电催化剂的设计对于获得可再生和可持续的能量转换至关重要。在这里,我们报告了由CDSE核心和八个CDSE POD(所谓的Octapods)制成的CDSE分支胶体纳米晶网络的使用,能够在其PODS PT颗粒上托管,从而催化水分分裂反应。多亏了OctApod形状,由此产生的PT托管网络被机械地捕获到碳纳米管BuckyPaper上,提供机械柔性和无粘合剂电极。我们发现,这种层次结构可最大程度地提高氢进化反应(HER)的质量活性和利用效率。在-0.15 V与可逆的氢电极的电势下,基于PT/OCTAPOD网络的电极在酸性和碱性培养基中分别在166 A MG-1和42 A MG-1上显示出PT质量活性。这些值分别对应于168 S-1和42 S-1的周转频率,与市售的PT/C基准相比,该频率在该顺序高14和21倍。 PT和OCTAPOD表面之间的强大化学和机械相互作用,以及PT/Octapod网络对Buckypaper的POD辅助粘附,在两种介质中都导致了长期耐用性(> 20 h)。这些结果在实验上证明了我们对托管Pt颗粒的分支纳米晶体网络的开发可以规避催化剂的耐用性问题,同时采用超低PT载荷或基准测试碳支持的PT纳米晶体。我们的工作为使用由分支纳米晶体制成的多孔网络作为具有超高量金属和受控催化特性的催化剂的前景。

The design of efficient electrocatalysts for electrochemical water splitting with minimal amount of precious metal is crucial to attain renewable and sustainable energy conversion. Here, we report the use of a network of CdSe branched colloidal nanocrystals, made of a CdSe core and eight CdSe pods (so-called octapods), able to host on their pods Pt particles, and thus catalyzing water splitting reactions. Thanks to the octapod shape, the resulting Pt-hosting network is mechanically trapped onto carbon nanotube buckypaper, providing mechanically flexible and binder-free electrodes. We found that such hierarchical configuration maximizes the mass activity and the utilization efficiency of Pt for the hydrogen evolution reaction (HER). At a potential of -0.15 V vs. reversible hydrogen electrode, the Pt/octapod network-based electrodes display a Pt mass activity on the HER of 166 A mg-1 and 42 A mg-1 in acidic and alkaline media, respectively. These values correspond to turnover frequencies of 168 s-1 and 42 s-1, respectively, which are in that order 14 and 21 times higher compared to commercially available Pt/C benchmarks. The strong chemical and mechanical interactions between the Pt and the octapod surface, along with pod-aided adhesion of the Pt/octapod network to the buckypaper, result in a long-term durability (>20 h) of the HER-activity in both media. These results experimentally prove that the exploitation of our network of branched nanocrystals hosting Pt particles can circumvent the durability issues of the catalysts while adopting either ultralow Pt loadings or benchmarking carbon-supported Pt nanocrystals. Our work opens up prospects for using porous networks made by branched nanocrystals as catalysts with ultralow amount of noble metals and controlled catalytic properties.

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