Abstract Developing highly efficient and cost-effective catalysts for the hydrogen evolution reaction (HER) is of paramount importance to solve the problems arising from the depletion of non-renewable fossil fuels and increasing air pollution issues. Herein, an in-situ heterogeneous catalytic synthesis approach is developed for constructing hierarchical Ni/carbon hybrids via grafting nitrogen-doped-carbon (NC) nanotubes with Ni encapsulation onto the metal-organic framework (MOF)-derived carbon matrix. Following the “nanotube tip-growth model” involved in the in-situ catalytic synthesis process, the morphology and size of the nanotubes and encapsulated particles of the as-prepared hierarchical Ni-based carbon hybrids can be controlled by regulating the conditions during the thermal decomposition of the Ni-MOF in the presence of melamine. The grafting and decoration of the Ni-encapsulated carbon nanotubes on the MOF-derived architecture rapidly enhance the HER electrocatalytic performance of the bare thermally decomposed Ni/N-doped carbon composite. Due to the synergistic effects of the stable metallic Ni active sites and the N-doped carbon support, the optimized Ni@NC6-600 sample exhibits stable and high catalytic activity, only requiring an overpotential of 181 mV to drive 10 mA/cm2 towards the HER in alkaline media.

中文翻译：

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将含 Ni 包封的 N 掺杂碳纳米管原位接枝到 MOF 衍生的分层杂化物上，以实现高效的电催化析氢

摘要 开发高效、经济的析氢反应（HER）催化剂对于解决不可再生化石燃料枯竭和日益严重的空气污染问题至关重要。在此，开发了一种原位多相催化合成方法，通过将具有 Ni 封装的氮掺杂碳 (NC) 纳米管接枝到金属有机框架 (MOF) 衍生的碳基质上来构建分层 Ni/碳杂化物。遵循原位催化合成过程中涉及的“纳米管尖端生长模型”，可以通过调节热过程中的条件来控制所制备的分层 Ni 基碳杂化物的纳米管和包封颗粒的形态和尺寸。在三聚氰胺存在下 Ni-MOF 的分解。在 MOF 衍生的结构上接枝和装饰 Ni 包封的碳纳米管，迅速提高了裸热分解 Ni/N 掺杂碳复合材料的 HER 电催化性能。由于稳定的金属 Ni 活性位点和 N 掺杂的碳载体的协同作用，优化后的 Ni@NC6-600 样品表现出稳定且高的催化活性，只需要 181 mV 的过电位即可驱动 10 mA/cm2碱性介质中的 HER。