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作 者:辛宗武 马占玲 秦绍杰 黄玉红 Xin Zongwu;Ma Zhanling;Qin Shaojie;Huang Yuhong(Longzihu New Energy Laboratory,Zhengzhou Institute of Emerging Industrial Technology,Zhengzhou 450000,Henan,China;Beijing Key Laboratory of Ionic Liquids Clean Process,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China)
机构地区:[1]龙子湖新能源实验室,郑州中科新兴产业技术研究院,河南郑州450000 [2]中国科学院过程工程研究所,离子液体清洁过程北京市重点实验室,北京海淀区100190
出 处:《工业催化》2024年第7期66-72,共7页Industrial Catalysis
基 金:国家自然科学基金项目(22208326,22078346);河南省重点研发与推广专项(科技攻关)项目(232102231063,231111232600);中科豫能化绿色过程联合研发中心项目(ZKYN2022005)。
摘 要:戊二胺是生物基尼龙56的核心单体,以廉价且产能过剩的L-赖氨酸为原料,通过一步多相催化脱羧合成戊二胺,实现绿色高值化利用。L-赖氨酸脱羧需在强酸体系下进行,提高Ru基催化剂稳定性是共性科学难题之一。采用原位水热合成方法,设计制备双蛋壳包裹的钌催化剂,首先利用FAU孔道实现Ru纳米颗粒的高分散,其次在外层原位生长硅壳silicate-1(S-1),提高催化剂在酸体系下的稳定性。表征结果显示,双蛋壳包裹的Ru/FAU@S-1催化剂外层硅元素明显富集。在戊二胺合成反应中,Ru/FAU@S-1催化活性很高,L-赖氨酸转化率高达81.5%,戊二胺选择性65.8%,循环使用5次后催化效果无明显下降,催化剂稳定性得到显著改善。Cadaverine is a prime important monomer for development of bio-based nylon 56.The synthesis of cadaverine from low-cost and overcapacity L-lysine is a green and high-value pathway.Efficient and stable catalyst is the key to the chemo-catalytic heterogeneous process for cadaverine.In this work,high dispersion of Ru nanoparticles encapsulated in FAU was synthesized for high catalytic activity.Then,Ru/FAU@S-1 with a shell of the silicalite-1 was synthesized by in situ hydrothermal method to improve stability of catalyst in decarboxylation of L-lysine to cadaverine.In addition,the Ru/FAU encapsulated in all silicon shell had moderate acidity,which was beneficial for the decarboxylation of L-lysine to cadaverine.Finally,the conversion of L-lysine reached 81.5%,and the selectivity of cadaverine reached 65.8%.And,after 5 cycles,there was no significant decrease in catalytic performance of Ru/FAU@S-1.The stability of the catalyst was significantly improved.
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