Carbon-coated nickel phosphide with enriched surface Niδ + sites enables an exceptionally high productivity of 2-methylfuran from biomass upgrading†

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-06-17 DOI:10.1039/d3cy01609a
Xu Yang , Wu Liu , Shuyi Su , Jinfeng Li , Xiaoyang Wang , Mengjie Lian , Lei Miao
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Abstract

In this study, we successfully synthesized a carbon-coated nickel phosphide composite catalyst (Ni2P@C) through a strategy of polyvinylpyrrolidone (PVP)-assisted pyrolysis and phosphidation of Ni-MOF. Thorough structural characterization revealed that the assistance of PVP significantly decreased the size of the nickel nanoparticles during pyrolysis, and the subsequent gas phosphidation transformed the metallic nickel into the Ni2P phase with strengthened Ni–P synergy. The resulting core–shell structured Ni2P@C possessed a substantial number of surface Niδ + sites with electron deficiency, which served as both a metal center to dissociate hydrogen and a Lewis acid to activate the C–O bond. Remarkably, under mild reaction conditions (120 °C and pH 2 of 2.0 MPa), the Ni2P@C composite demonstrated exceptional activity for hydrodeoxygenation of furfuryl alcohol, achieving an impressive 2-methylfuran productivity of 1.7 g2-MF gCata−1 h−1. These results surpass the performance of most non-noble metal catalysts currently reported. This study could provide valuable insights for the rational design of advanced carbon-coated Ni2P composite catalysts for hydrogenative biomass upgrading.

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表面富含 Niδ+ 位点的碳包覆磷化镍可实现生物质提纯 2-甲基呋喃的超高生产率
本研究采用聚乙烯吡咯烷酮(PVP)辅助热解和磷化 Ni-MOF 的策略,成功合成了碳包覆磷化镍复合催化剂(Ni2P@C)。透彻的结构表征显示,在 PVP 的辅助下,镍纳米颗粒的尺寸在热解过程中显著减小,随后的气体磷化将金属镍转化为 Ni2P 相,加强了 Ni-P 的协同作用。由此产生的核壳结构 Ni2P@C 具有大量缺电子的表面 Niδ+ 位点,既是离解氢的金属中心,又是激活 C-O 键的路易斯酸。值得注意的是,在温和的反应条件下(120 °C,pH2 为 2.0 兆帕),Ni2P@C 复合材料在糠醇的氢脱氧反应中表现出了卓越的活性,2-甲基呋喃的生产率达到了惊人的 1.7 g2-MF gCata-1 h-1。这些结果超过了目前报道的大多数非贵金属催化剂的性能。这项研究为合理设计先进的碳包覆 Ni2P 复合催化剂用于生物质加氢升级提供了宝贵的启示。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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