CoZn/N-Doped porous carbon derived from bimetallic zeolite imidazolate framework/g-C3N4 for efficient hydrodeoxygenation of vanillin,Catalysis Science & Technology

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CoZn/N-Doped porous carbon derived from bimetallic zeolite imidazolate framework/g-C3N4 for efficient hydrodeoxygenation of vanillin
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2022-07-08 , DOI: 10.1039/d2cy00642a
Zegang Qiu ₁ , Xiaoxia He ₁ , Zhiqin Li ₁ , Qichen Guan ₂ , Liang Ding ₁ , Yanan Zhu ₁ , Yueling Cao _{2,

3}

Affiliation

The development of non-noble metal catalysts with high efficiency for the hydrodeoxygenation (HDO) of bio-oil is of great importance for the utilization of lignin biomass resources. As a crucial lignin-based platform chemical, vanillin is a promising candidate for the production of fine chemicals and polymers. Here, a promising non-noble Co–Zn/NPC catalyst (NPC: nitrogen-doped porous carbon materials) for the HDO of vanillin was prepared by pyrolysis of Co–Zn zeolite imidazolate framework/graphitic carbon nitride (Co–Zn-ZIF/g-C₃N₄) composites. Full vanillin conversion with 99% MMP (2-methoxy-4-methylphenol) selectivity could be achieved at 100 °C and 1 MPa H₂ over 4Co–1Zn/NPC. Characterization results indicate that the presence of g-C₃N₄ promotes the formation of mesopores, which is beneficial for fast mass transfer. Additionally, the introduction of Zn downsizes the size of Co nanoparticles, and lowers the electron density around the Co atoms in Co–Zn/NPC catalysts, which can accelerate the hydrogenation of vanillin. More importantly, the Zn introduced in the catalyst may function as a basic site to facilitate the conversion of the intermediate HMP (4-hydroxy-3-methoxybenzyl alcohol) into MMP, thus enhancing the MMP selectivity. Moreover, Co–Zn/NPC presents excellent stability in the HDO reaction of vanillin. This work provides some useful insights into the design of novel non-noble metal catalysts with high efficiency for HDO of bio-oil.

中文翻译：

由双金属沸石咪唑骨架/g-C3N4衍生的CoZn/N掺杂多孔碳用于香草醛的高效加氢脱氧

开发用于生物油加氢脱氧（HDO）的高效非贵金属催化剂对于木质素生物质资源的利用具有重要意义。作为一种重要的基于木质素的平台化学品，香草醛是生产精细化学品和聚合物的有希望的候选者。在这里，通过热解 Co-Zn 沸石咪唑酸盐骨架/石墨氮化碳 (Co-Zn-ZIF/ gC ₃ N ₄ ) 复合材料。_{在 100 °C 和 1 MPa H 2}超过 4Co–1Zn/NPC 条件下，可以实现具有 99% MMP（2-甲氧基-4-甲基苯酚）选择性的完全香草醛转化。表征结果表明，gC _3的存在N ₄促进中孔的形成，有利于快速传质。此外，Zn 的引入减小了 Co 纳米颗粒的尺寸，并降低了 Co-Zn/NPC 催化剂中 Co 原子周围的电子密度，这可以加速香兰素的氢化。更重要的是，催化剂中引入的 Zn 可以作为碱性位点促进中间体 HMP（4-羟基-3-甲氧基苯甲醇）转化为 MMP，从而提高 MMP 的选择性。此外，Co-Zn/NPC 在香草醛的 HDO 反应中表现出优异的稳定性。这项工作为设计用于生物油 HDO 的高效新型非贵金属催化剂提供了一些有用的见解。

更新日期：2022-07-08

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