Abstract

Nitrogen-doped carbon materials have attracted enormous interest in catalysis owing to their outstanding catalytic performance. In this work, nitrogen-doped carbonaceous catalysts (NCC) supported on inexpensive and naturally abundant halloysite nanotubes were successfully synthesized via precipitation polymerization, calcination, and sulfonation processes. The physical and chemical properties of the obtained catalysts were systematically characterized by different methods. The results indicated that NCC catalysts had mesoporous structures, excellent thermostability and acid-base bi-functional active sites. One-pot synthesis of 5-hydroxymethylfurfural (HMF) from glucose was performed to investigate the synthesized NCC catalysts. Benefiting from the synergistic effects of the acid-base bi-functional active sites, the highest HMF yield (62.8%) was achieved in an isopropanol-mediated DMSO system under optimal conditions. Moderate to excellent yields of HMF were also obtained from one-pot conversions of other carbohydrates, including inulin, sucrose, cellobiose, maltose and starch, with our developed catalytic system. The one-pot production of HMF from cellulose was also smoothly processed by the NCC bi-functional catalyst in an IL-based system. This work has developed a versatile strategy for designing nitrogen-doped carbonaceous catalysts that can be employed for the direct transformation of renewable carbohydrates to platform chemicals.

中文翻译：

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在埃洛石纳米管上负载的酸碱双功能碳质催化剂上由碳水化合物一锅合成HMF

摘要

氮掺杂碳材料由于其出色的催化性能而引起了人们极大的兴趣。在这项工作中，通过沉淀聚合，煅烧和磺化工艺成功合成了负载在廉价且天然丰富的埃洛石纳米管上的氮掺杂碳质催化剂（NCC）。用不同的方法对得到的催化剂的物理和化学性质进行了系统的表征。结果表明，NCC催化剂具有介孔结构，优异的热稳定性和酸碱双功能活性位。由葡萄糖一锅合成5-羟甲基糠醛（HMF），以研究合成的NCC催化剂。受益于酸碱双功能活性位点的协同作用，HMF产量最高（62。在最佳条件下，由异丙醇介导的DMSO系统可达到8％的效果。使用我们开发的催化系统，通过一锅转化其他糖类（包括菊粉，蔗糖，纤维二糖，麦芽糖和淀粉），也可以得到中等至极好的HMF收率。由NCC双功能催化剂在基于IL的系统中也顺利地处理了由纤维素一锅生产HMF的问题。这项工作为设计氮掺杂的碳质催化剂开发了一种通用策略，该催化剂可用于将可再生碳水化合物直接转化为平台化学品。用我们开发的催化系统。由NCC双功能催化剂在基于IL的系统中也顺利地处理了由纤维素一锅生产HMF的问题。这项工作为设计氮掺杂的碳质催化剂开发了一种通用策略，该催化剂可用于将可再生碳水化合物直接转化为平台化学品。用我们开发的催化系统。由NCC双功能催化剂在基于IL的系统中也顺利地处理了由纤维素一锅生产HMF的问题。这项工作为设计氮掺杂的碳质催化剂开发了一种通用策略，该催化剂可用于将可再生碳水化合物直接转化为平台化学品。