Synergistic magnetic Cu-Fe catalysts on N-doped biochar for efficient alkali lignin catalytic depolymerization into monophenols

IF 5.6 1区 农林科学 Q1 AGRICULTURAL ENGINEERING
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Abstract

Alkali lignin, a major by-product of papermaking, poses disposal challenges, hindering the full valorization of lignocellulose in sustainable biorefineries. One-pot lignin catalytic depolymerization (LDP) in water offers a promising route for producing valuable phenolic compounds. This study reports the successful synthesis of in-situ N-doped biochar supported CuxFey catalysts (CuxFey/N-BC) via a one-step carbothermal reduction method, enabling LDP in water without the need for external hydrogen, additives, alcohol solvent, or co-catalysts. Notably, the Cu5Fe1/N-BC could achieve remarkable catalytic performance under mild reaction conditions (280 °C, 6 h, 18 mL water), yielding 80.84±2.23 mg/g of monophenol, 56.17±1.32 % of bio-oil, and a lignin conversion rate of 80.66±0.73 %. This significantly surpassed the performance of monometallic catalysts and bare biochar. The synergistic effects of intermetallic interactions and nitrogen doping were proposed to create abundant active sites and rich pore structures, promoting efficient LDP reactions. Furthermore, the Cu5Fe1/N-BC exhibited excellent recyclability, with minimal activity loss (2.79 %) per cycle, due to its strong magnetism and favorable interactions. Mechanism investigation revealed that the Cu5Fe1/N-BC efficiently cleaved the C-O and C-C bonds in lignin, and led to the targeted production of guaiacyl phenols. This study provides valuable insights and practical strategy for valorizing lignin into valuable chemicals, advancing its utilization in various applications.

掺杂 N 的生物炭上的协同磁性 Cu-Fe 催化剂用于将碱木质素催化解聚为单酚
碱木素是造纸过程中产生的一种主要副产品,它的处理带来了挑战,阻碍了木质纤维素在可持续生物炼制过程中的充分发挥价值。水中单锅木质素催化解聚(LDP)为生产有价值的酚类化合物提供了一条前景广阔的途径。本研究报告通过一步碳热还原法成功合成了原位掺杂 N 的生物炭支撑 CuxFey 催化剂(CuxFey/N-BC),从而实现了水中木质素催化解聚,无需外加氢气、添加剂、醇溶剂或助催化剂。值得注意的是,Cu5Fe1/N-BC 在温和的反应条件下(280 °C、6 小时、18 mL 水)可实现显著的催化性能,可获得 80.84±2.23 mg/g 的单酚、56.17±1.32 % 的生物油和 80.66±0.73 % 的木质素转化率。这大大超过了单金属催化剂和裸生物炭的性能。金属间相互作用和氮掺杂的协同效应被认为创造了丰富的活性位点和孔隙结构,促进了高效的 LDP 反应。此外,Cu5Fe1/N-BC 由于其强磁性和有利的相互作用,表现出极佳的可回收性,每次循环的活性损失极小(2.79%)。机理研究表明,Cu5Fe1/N-BC 能高效地裂解木质素中的 C-O 和 C-C 键,从而定向生产愈创木酚。这项研究为将木质素转化为有价值的化学品提供了宝贵的见解和实用的策略,推动了木质素在各种应用领域的利用。
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来源期刊
Industrial Crops and Products
Industrial Crops and Products 农林科学-农业工程
CiteScore
9.50
自引率
8.50%
发文量
1518
审稿时长
43 days
期刊介绍: Industrial Crops and Products is an International Journal publishing academic and industrial research on industrial (defined as non-food/non-feed) crops and products. Papers concern both crop-oriented and bio-based materials from crops-oriented research, and should be of interest to an international audience, hypothesis driven, and where comparisons are made statistics performed.
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