Rationally tailoring the surface/interface structures of noble metal nanostructures emerges as a highly efficient method for improving their electrocatalytic activity, selectivity, and long-term stability. Recently, hydrogen evolution reaction is attracting more and more attention due to the energy crisis and environment pollution. Herein, we successfully synthesize polyallylamine-functionalized rhodium nanosheet nanoassemblies-carbon nanotube nanohybrids via a facile one-pot hydrothermal method. Three-dimensionally branched rhodium nanosheet nanoassemblies are consisted of two dimensionally atomically thick ultrathin rhodium nanosheets. The as-prepared polyallylamine-functionalized rhodium nanosheet nanoassemblies-carbon nanotube nanohybrids show the excellent electrocatalytic activity for the hydrogen evolution reaction in acidic media, with a low onset reduction potential of −1 mV, a small overpotential of 5 mV at 10 mA cm⁻², which is much superior to commercial platinum nanocrystals. Two dimensionally ultrathin morphology of rhodium nanosheet, particular rhodium-polyallylamine interface, and three-dimensionally networks induced by carbon nanotube are the key factors for the excellent hydrogen evolution reaction activity in acidic media.

合理地定制贵金属纳米结构的表面/界面结构是一种提高其电催化活性，选择性和长期稳定性的高效方法。近年来，由于能源危机和环境污染，析氢反应越来越受到关注。在这里，我们成功地通过简便的一锅水热法合成了聚烯丙胺官能化的铑纳米片纳米组件-碳纳米管纳米杂化物。三维支化的铑纳米片纳米组件由两个原子上原子厚的超薄铑纳米片组成。制备的聚烯丙胺官能化的铑纳米片纳米组件-碳纳米管纳米杂化物在酸性介质中显示出优异的电催化活性，用于氢的分解反应，^-2，比市售的铂纳米晶体优越得多。铑纳米片的二维超薄形态，特别是铑-聚烯丙胺界面，以及碳纳米管诱导的三维网络，是在酸性介质中优异的析氢反应活性的关键因素。