Catalytic performance of low loading palladium-carbon catalyst in rosin disproportionation: Characterization, process enhancement, and reaction pathway

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-02-05 Epub Date: 2024-12-15 DOI:10.1016/j.apcata.2024.120077
Yifan Niu , Siyu Gong , Jinhao Zheng , Xian Zhou , Ziyu Song , Shaohua Ju , Yongwan Gu
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Abstract

This study introduces an efficient Pd/C catalyst for the rosin disproportionation (RD) reaction, a key biomass conversion process. The low-loaded Pd/C catalysts, with 3–6 nm Pd nanoparticles, were synthesized via deposition-precipitation and characterized for their high dispersion of metallic Pd on activated carbon. Optimized using the Box-Behnken design of response surface methodology, the catalyst achieved a 71.36 % maximum DAA yield under optimal conditions (280 °C, 150 min, 0.04 wt% catalyst, 3.00 wt% Pd), surpassing commercial catalysts by 1.27 times with reduced Pd usage. Key factors for catalytic activity included Pd loading, dispersion, particle size, and metallic Pd content. Kinetic studies showed an activation energy of 21.52 kJ/mol for the conversion of abietic acid to dehydroabietic acid, highlighting the superior potential in the RD reaction. Ultraviolet-visible absorption spectra and gas chromatography-mass spectrometry analyses elucidated the reaction pathway and mechanism, providing a practical approach to developing high-activity catalysts for industrial RD applications.
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低负载钯碳催化剂在松香歧化中的催化性能:表征、工艺改进和反应途径
介绍了一种高效Pd/C催化剂用于松香歧化反应,这是生物质转化的关键过程。采用沉积沉淀法合成了3-6 nm 纳米钯纳米颗粒的低负载钯/碳催化剂,其特点是金属钯在活性炭上的高度分散。使用响应面法的Box-Behnken设计进行优化,在最佳条件下(280 °C, 150 min, 0.04 wt%催化剂,3.00 wt% Pd),催化剂的DAA产率达到71.36 %,比减少Pd用量的商业催化剂高出1.27倍。催化活性的关键因素包括钯负载、分散、颗粒大小和金属钯含量。动力学研究表明,松木酸转化为脱氢松木酸的活化能为21.52 kJ/mol,表明该反应具有较好的发展潜力。紫外-可见吸收光谱和气相色谱-质谱分析分析阐明了反应途径和机理,为工业研发开发高活性催化剂提供了切实可行的途径。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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