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Ni-Co 和 Ni-Cu 催化剂介导的木质素解聚为酚类物质与异丙醇供氢溶剂中的活性和产物分布。

Activity and product distribution in Ni-Co and Ni-Cu catalyst-mediated lignin depolymerization into phenolic substances with isopropanol H-donating solvent.

机构信息

School of Chemical Engineering, Universiti Sains Malaysia, Nibong Tebal, 14300, Seberang Perai, Penang, Malaysia.

出版信息

Environ Sci Pollut Res Int. 2024 Aug;31(37):49727-49743. doi: 10.1007/s11356-024-34504-2. Epub 2024 Jul 30.

Abstract

Lignin, a vital renewable biopolymer, serves as the Earth's primary source of aromatics and carbon. Its depolymerization presents significant potential for producing phenolic fine chemicals. This study assesses promoted Ni-based bimetallic catalysts (Ni-Co/C and Ni-Cu/C) supported on activated carbon in isopropanol for lignin depolymerization, compared to monometallic counterparts. BET, SEM, EDX, and XPS analyses highlight their physicochemical properties and promotional effects, enhancing hydrogenolysis activity and hydrogen transformation. Reaction parameter exploration elucidates the influence on lignin depolymerization, with cobalt and copper as promoters notably increasing conversion and monomer yield. Ni-Co/C exhibits the highest lignin conversion (94.2%) and maximum monomer yield (53.1 wt%) under specified conditions, with lower activation energy (36.1 kJ/mol) and higher turnover frequency (31.6 h) compared to Ni/C. FT-IR, GPC, GC-FID, and GC-MS analyses confirm effective depolymerization, identifying 20 monomer products. Proposed reaction mechanisms underscore the potential of Ni-based bimetallic catalysts for lignin valorization, offering insights into developing efficient catalytic systems for lignin hydrogenolysis. This research enhances understanding and facilitates the development of selective catalytic processes for lignin valorization.

摘要

木质素是一种重要的可再生生物聚合物,是地球上芳香族化合物和碳的主要来源。其解聚为生产酚类精细化学品提供了巨大的潜力。本研究评估了负载在活性炭上的促进型 Ni 基双金属催化剂(Ni-Co/C 和 Ni-Cu/C)在异丙醇中对木质素解聚的作用,与单金属催化剂相比。BET、SEM、EDX 和 XPS 分析突出了它们的物理化学性质和促进作用,提高了氢解活性和氢转化。反应参数的探索阐明了其对木质素解聚的影响,钴和铜作为促进剂显著提高了转化率和单体收率。在特定条件下,Ni-Co/C 表现出最高的木质素转化率(94.2%)和最大的单体收率(53.1wt%),其活化能(36.1kJ/mol)较低,转化频率(31.6h)较高,而 Ni/C 则较低。FT-IR、GPC、GC-FID 和 GC-MS 分析证实了有效的解聚作用,鉴定出 20 种单体产物。提出的反应机制强调了 Ni 基双金属催化剂在木质素增值方面的潜力,为开发木质素氢解的高效催化体系提供了思路。本研究增强了对木质素增值的选择性催化过程的理解和促进。

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