Efficient Hydrogen Production from Ethylene Glycol Steam Reforming Catalyzed by Na-Promoted Pt/γ-Mo2N

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Xuan Liang, Zirui Gao, Xingjie Peng, Maolin Wang, Yao Xu, Jie Zhang, Shuheng Tian, Chengyu Li, Xuetao Qin, Rongli Mi, Zhaohua Wang, Wu Zhou, Meng Wang* and Ding Ma*, 
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Abstract

Ethylene glycol (EG) derived from biomass and plastic wastes can serve as a sustainable H2 resource through steam reforming (HOCH2CH2OH + 2H2O ⇄ 5H2 + 2CO2). However, achieving high activity in H2 production with good selectivity toward CO2 under mild conditions poses a challenge. A thoughtful understanding of the active sites that accelerate the cleavage of the C–C bond rather than the C–O bond and the activation of the water molecule is still lacking. In this study, we developed a PtNa/γ-Mo2N catalyst that efficiently enables hydrogen production from ethylene glycol steam reforming (EGSR) reactions. This catalyst achieved outstanding H2 productivity, reaching 6000 molH2·molPt–1·h–1 at 250 °C under 10 bar with high CO2 selectivity (89%) and low CO selectivity (1%) in carbon-containing products. Comprehensive characterizations revealed the crucial role of the interface between highly dispersed Pt species and Mo2N in activating ethylene glycol and water. Additionally, sodium (Na) was found to block acidic sites, preventing the formation of side products from C–O bond cleavage, and to modulate Pt sites, enhancing the reforming process by accelerating the water gas shift reaction.

Abstract Image

Abstract Image

na促进Pt/γ-Mo2N催化乙二醇蒸汽重整高效制氢
从生物质和塑料废物中提取的乙二醇(EG)可以通过蒸汽重整成为可持续的H2资源(HOCH2CH2OH + 2H2O)。然而,如何在温和条件下实现高活性的产氢和对CO2的良好选择性是一个挑战。对加速C-C键而不是C-O键的裂解和水分子活化的活性位点的深入了解仍然缺乏。在这项研究中,我们开发了一种PtNa/γ-Mo2N催化剂,可以有效地实现乙二醇蒸汽重整(EGSR)反应的制氢。该催化剂具有优异的H2产率,在250℃、10 bar条件下可达到6000 molH2·molPt-1·h-1,在含碳产物中具有高的CO2选择性(89%)和低的CO选择性(1%)。综合表征揭示了高度分散的Pt和Mo2N之间的界面在活化乙二醇和水方面的关键作用。此外,钠(Na)被发现阻断酸性位点,防止C-O键裂解产生副产物,并调节Pt位点,通过加速水气转移反应加速重整过程。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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