Ruthenium Nanoparticles Anchored on Cobalt Oxide Married with Nitrogen and Phosphorus Co-Doped Carbon for Hydrolytic Dehydrogenation of Ammonia Borane

氨硼烷 脱氢 催化作用 无机化学 氧化钴 碳纤维 化学 纳米颗粒 氮气 硼烷 水解 材料科学 纳米技术 有机化学 复合数 复合材料
作者
Yutong Li,Haoyue Huang,Qiuhong Wei,Shujun Qiu,Yongpeng Xia,Fen Xu,Lixian Sun,Hailiang Chu
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:15 (11): 9158-9170 被引量:26
标识
DOI:10.1021/acscatal.5c01378
摘要

The development of cost-effective and high-efficiency catalysts for hydrogen generation through ammonia borane (AB) hydrolysis remains a significant challenge in the field of clean energy production. Controlled introduction of dopants into catalysts offers a promising strategy to enhance the intrinsic activity of noble metals, such as ruthenium (Ru), by tuning their electronic energy levels. Herein, we explored the interactions between cobalt oxide and Ru nanoparticles (NPs) supported on N and P co-doped carbon-based nanostructures. Notably, the N, P co-doping uniquely modulates the electronic structures, simultaneously tuning the electronic properties of carbon support and cobalt oxide. Therefore, this composite catalyst demonstrates the distinctly enhanced metal–support interactions, achieving a 3.5-fold increase in turnover frequency (TOF) to 1429 molH2·molRu–1·min–1 at 25 °C, compared to the undoped counterparts. Moreover, the catalyst retains over 90% of its initial activity after five cycles of reuse. Experimental and theoretical analyses attribute the superior catalytic activity of Ru@CoOx/NPC to the optimized electronic configuration of CoOx and the downward shift in its d-band center induced by N and P doping. This microstructural alteration further modifies the electronic state of Ru, enhancing H2O adsorption and dissociation. These findings offer a pragmatic tactic for electronic structure modulation to design highly active and selective noble-metal-based catalysts for AB hydrolysis.
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