Highly stable biochar-encapsulated CoTi@BC nanocatalysts for lignin hydrogenolysis

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-02-01 DOI:10.1016/j.jcat.2024.115914
Bowen Luo , Zhipeng Tian , Riyang Shu , Chao Wang , Ying Chen , Jianping Liu , Yuhe Liao
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Abstract

Valorization of renewable lignin toward value-added fuels and chemicals can improve the economies of biorefinery. However, maintaining catalyst stability and preventing metal aggregation under the certain conditions of lignin hydrogenolysis remains a key challenge. Herein, hydrogenolysis of corncob enzymatic lignin was investigated using biochar-encapsulated CoTi@BC catalysts at reaction temperature of 250 °C. Co1Ti0.5@BC catalyst with the addition of Ti species outperformed Co@BC catalyst, resulting in 82.5 % lignin liquefaction degree and 23.7 wt% yield of monophenols. Besides, the catalytic stability of Co1Ti0.5@BC catalyst was outstanding in the lignin hydrogenolysis, where almost no activity loss was observed after four recycle runs. Catalyst characterization suggests that the addition of moderate amounts of Ti species changed the reduction temperature of Co species and the interaction between metal sites and carbon layer. The uniform distribution of Ti species improved the dispersion of Co metal particles, and the carbon layer can protect the surface of metal nanoparticles from oxidation, thus maintaining the stability and the activity of Co metal sites. Furthermore, the mechanism of lignin hydrogenolysis with CoTi@BC catalysts was investigated based on the results of benzyloxyphenol hydrogenolysis. These findings demonstrate the unique advantages of biochar-encapsulated metal particles for efficient C-O bond cleavage and offer valuable insights for advancing lignin valorization and sustainable biorefinery development.

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用于木质素氢解的高稳定性生物炭包封 CoTi@BC 纳米催化剂
可再生木质素向增值燃料和化学品的增值可以提高生物炼制的经济性。然而,在一定条件下保持催化剂稳定性和防止金属聚集仍然是木质素氢解的关键挑战。在250 ℃的反应温度下,采用生物炭包封CoTi@BC催化剂对玉米芯酶解木质素进行了氢解研究。添加Ti的Co1Ti0.5@BC催化剂优于Co@BC催化剂,木质素液化度为82.5 %,单酚收率为23.7 wt%。此外,Co1Ti0.5@BC催化剂在木质素氢解反应中的催化稳定性较好,经过4次循环后几乎没有活性损失。催化剂表征表明,适量Ti的加入改变了Co的还原温度以及金属位与碳层之间的相互作用。Ti的均匀分布提高了Co金属颗粒的分散性,碳层可以保护金属纳米颗粒表面不被氧化,从而保持Co金属位点的稳定性和活性。在苯氧酚氢解的基础上,研究了CoTi@BC催化剂对木质素氢解的机理。这些发现证明了生物炭包封金属颗粒在高效裂解C-O键方面的独特优势,为推进木质素增值和可持续生物炼制发展提供了有价值的见解。
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文献相关原料
公司名称
产品信息
麦克林
cobalt nitrate hexahydrate
麦克林
H<sub>2</sub>O<sub>2</sub>
麦克林
cellulose
麦克林
Cobalt nitrate hexahydrate (Co(NO3)2·6H2O)
麦克林
H2O2
麦克林
Cellulose
阿拉丁
ethanol
阿拉丁
Butyl titanate
阿拉丁
Ethanol
阿拉丁
Butyl titanate
来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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