富含 Co-N 中心的氮掺杂碳负载的钴纳米颗粒及催化甲酸制氢性能

Co-N-Rich Nitrogen-doped Carbon-supported Cobalt Nanoparticles for Hydrogen Production from Formic Acid

摘要

采用蔗糖为碳源、 尿素为氮源、 硝酸钴为前驱体, 经研磨混合后利用高温焙烧法制备了一种氮掺杂碳负载的钴纳米颗粒非贵金属催化剂, 并将其用于液相甲酸脱氢反应. 在100 ℃下, 性能最佳的Co@NC-Co_0.1-Ur_2.3 催化剂的制氢速率可以达到350 mL·g⁻¹·h⁻¹, 超过部分贵金属(Pd, Pt)催化剂及非贵金属催化剂（如单原子钴）的性能. 此外，该催化剂循环多次后仍能保持较高活性. 表征结果显示, 丰富的孔结构和比表面积有利于反应过程中HCOO^*等活性物种吸附, 而Co-N位点可能是该反应的催化活性位.

Abstract

Using sucrose as the carbon source, urea as the nitrogen source, and cobalt nitrate as the precursor, a nitrogen-doped carbon-supported cobalt nanoparticle catalyst was prepared via a grinding-mixing and high-temperature calcination method. The as-synthesized catalyst was applied for hydrogen production from formic acid in the liquid phase. At 100 ℃, Co@NC-Co_0.1-Ur_2.3 catalyst achieved a hydrogen generation rate of 350 mL·g⁻¹·h⁻¹, exceeding the performance of some noble metal (Pd, Pt) catalysts and non-noble catalysts such as single-atom cobalt. Furthermore, the catalyst remains highly activity even after multiple recycles. Characterization results revealed that the abundant porous structure and high specific surface area might facilitate the adsorption of active species such as HCOO^* during the reaction, while the Co-N moieties are proposed as the catalytic active sites.

关键词

甲酸制氢 / Co-N中心 / 氮掺杂碳 / 钴纳米颗粒

Key words

Formic acid dehydrogenation / Co-N center / N-doped carbon / Co nanoparticle

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基金资助

国家重点研发计划项目(2022YFE0116000)