Hydrogenolysis of guaiacol and lignin to phenols over Ni/Nb2O5HZSM-5 catalyst

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-09-21 DOI:10.1016/j.mcat.2024.114559
Xiaohong Ren, Zeming Rong, Xiaoqiang Yu
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Abstract

Selective hydrogenolysis of CAr-O bonds in lignin to produce aromatic compounds typically necessitates severe conditions. We developed a Ni/Nb2O5HZSM-5 catalyst that facilitates direct cleavage of guaiacol's aryl ether bonds at reduced temperatures (200 °C) and pressure (0.1 MPa H2), achieving a conversion of 89.5 % with the selectivity of phenol at 81.7 %, while retaining its activity after five cycles. The Ni/Nb2O5HZSM-5 exhibits a higher yield of phenol (49.1 mmolphenol·gNi−1·h−1), currently achieving the highest phenol yield among Ni-based catalysts. The addition of Nb2O5 enhances the dispersion of Ni and augments the effective surface area. In addition, the strong interaction of Nb with the HZSM-5 changed the electronic state of Nb and enhanced the resistance of the catalyst to high temperature and mechanical stress. Employing this catalyst for lignin depolymerization in an aqueous medium led to a 17.0 wt% yield of alkyl phenolic compounds. This approach represents an advancement in biomass resource conversion, circumventing the dependency on high-pressure and precious-metal catalysts, and signaling a new trajectory for sustainable biomass utilization in scientific research.

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在 Ni/Nb2O5HZSM-5 催化剂上将愈创木酚和木质素加氢水解为苯酚
选择性氢解木质素中的 CAr-O 键以生成芳香族化合物通常需要苛刻的条件。我们开发了一种 Ni/Nb2O5HZSM-5 催化剂,可在较低温度(200 °C)和压力(0.1 兆帕 H2)下促进愈创木酚芳基醚键的直接裂解,转化率达到 89.5%,苯酚的选择性为 81.7%,同时在五个循环后仍能保持其活性。Ni/Nb2O5HZSM-5 表现出更高的苯酚产率(49.1 mmolphenol-gNi-1-h-1),是目前镍基催化剂中苯酚产率最高的催化剂。Nb2O5 的加入提高了镍的分散性,增加了有效表面积。此外,铌与 HZSM-5 的强烈相互作用改变了铌的电子状态,增强了催化剂的耐高温和耐机械应力性能。利用这种催化剂在水介质中进行木质素解聚,可获得 17.0 wt% 的烷基酚化合物。这种方法代表了生物质资源转化领域的一大进步,避免了对高压和贵金属催化剂的依赖,标志着生物质可持续利用在科学研究中迈出了新的步伐。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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