吴敏雅,刘明华,刘以凡,吕源财.过渡金属硫酸盐协同Pd/C高效定向降解木质素的研究[J].中国造纸学报,2021,(1):6-12 本文二维码信息
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过渡金属硫酸盐协同Pd/C高效定向降解木质素的研究
Efficient and Product-controlled Degradation of Lignin Using Transition Metal Sulfates Cooperated with Pd/C
投稿时间:2019-12-05  
DOI:10.11981/j.issn.1000-6842.2021.01.06
中文关键词:  过渡金属硫酸盐  Pd/C  木质素  定向降解  酚类化合物
Key Words:transition metal sulfate  Pd/C  lignin  product-controlled degradation  phenolic compound
基金项目:福建省高校产学合作项目(2019H6008)。
作者单位邮编
吴敏雅 福州大学环境与资源学院福建福州350116 350116
刘明华 福州大学环境与资源学院福建福州350116
福建省农村废弃物绿色循环技术工程研究中心福建福州350116 
350116
刘以凡 福州大学环境与资源学院福建福州350116
福建省农村废弃物绿色循环技术工程研究中心福建福州350116 
350116
吕源财 福州大学环境与资源学院福建福州350116
福建省农村废弃物绿色循环技术工程研究中心福建福州350116 
350116
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中文摘要:
      以改善当前木质素催化降解存在的降解产物可控性较差、小分子化合物总收率较低、均一化程度不足、难以进一步开发利用等问题为目标,采用过渡金属硫酸盐NiSO4·6H2O协同Pd/C催化降解玉米芯酶解木质素,考察了过渡金属离子、反应温度、反应时间、NiSO4·6H2O与Pd/C协同作用等对木质素降解率的影响,并分析了降解产物的分布和催化作用机理。结果表明,NiSO4·6H2O可有效提高Pd/C对木质素的催化降解效率,如木质素降解率相较于单独使用Pd/C催化降解时提高14.5%,小分子化合物总收率提高39.9%,其中,酚类化合物的得率提高88.6%,且产物的均一化程度提高了35.8%;分析表明,由于NiSO4·6H2O的路易斯酸特性和镍离子的高电负性,木质素的醚键可有效地在Pd/C和NiSO4·6H2O酸性催化中心上发生裂解,并通过加氢反应,定向生成以酚类为主体的中间产物。
Abstract:
      In order to overcome several obstacles which limit the further development and utilization of degradation products existing in lignin catalytic degradation at present, such as poor product-controlled property, low yield of small molecule compounds, insufficient degree of uniformity, and difficulty for further utilization. NiSO4·6H2O cooperated with Pd/C was used to catalyze the degradation of corncob lignin in this study. The effects of transition metal ions, reaction temperature, reaction time, and synergistic effect of NiSO4·6H2O and Pd/C on lignin degradation ratio were investigated. Meantime, the degradation products and mechanism were analyzed. The results showed that NiSO4·6H2O cooperated with Pd/C could effectively improve the lignin degradation ratio. The degradation ratio was increased by 14.5%, and the yield of small molecules was improved by 39.9%. Especially, the yield of phenolic compounds was increased by 88.6% and the products uniformity was upgraded by 35.8% as well. Due to the properties of Lewis acid and the high electronegativity of Ni2+ in NiSO4·6H2O, the ether bonds of lignin could be cleaved on the acidic catalytic centers of Pd/C and NiSO4·6H2O effectively, and phenolic compounds were formed through the hydrogenation reaction.
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