反应性挤出技术制备碳基乙炔氢氯化催化剂
Synthesis of Carbon-Based Catalysts for Acetylene Hydrochlorination Using Reactive Extrusion Technology
杜盛郁 1牛强 2张鹏飞3
作者信息
- 1. 上海交通大学 化学化工学院,上海 200240
- 2. 内蒙古鄂尔多斯电力冶金集团股份有限公司 国家企业技术中心,内蒙古 鄂尔多斯 016064
- 3. 上海交通大学 化学化工学院,上海 200240;宁夏大学 化学化工学院,宁夏 银川 750021
- 折叠
摘要
Au催化剂是乙炔氢氯化反应的重要无汞催化剂之一,如何增强Au催化剂的稳定性成为当前研究的热点和难点.设计新型载体材料是增强Au催化剂稳定性的优选策略.反应性挤出技术可精准控制反应条件,将材料合成与加工成型二合一,可实现连续生产.用反应性挤出技术制备碳基材料,可极大提高反应的合成效率.以瓜尔胶为主要前驱体,采用反应性挤出技术合成多种异质元素掺杂的碳基材料,将碳基材料负载氯金酸并用于乙炔氢氯化反应.实验结果表明,以N掺杂的多孔碳为载体的Au催化剂Au/G‒N具有优异的催化稳定性.在乙炔空速为180 h-1,反应温度为180 ˚C的条件下,Au/G‒N催化的乙炔转化率为83%,反应3 600 min后乙炔的转化率仅下降3%.这主要归因于载体中N与Au物种的相互作用,提高了Au的分散度,减少了氧化态Au被还原并发生团聚的情况.同时N的引入有效抑制了催化剂的积碳行为,避免了催化剂表面的活性位点因被覆盖而导致催化剂失活.
Abstract
Au catalysts are crucial for the mercury-free acetylene hydrochlorination reaction.Enhancing their sta-bility is a key and challenging research focus.Developing novel support materials is a preferred strategy to improve the stability of Au catalysts.Reactive extrusion technology allows precise control of reaction condi-tions,combining material synthesis and shaping into a single process,enabling continuous production and signif-icantly enhancing synthesis efficiency when preparing carbon-based materials.Guar gum was used as the pri-mary precursor to synthesize carbon-based materials doped with diverse heterogeneous elements through reac-tive extrusion technology.These carbon-based materials were then impregnated with chloroauric acid for the acetylene hydrochlorination reaction.Experimental results reveal that the Au catalyst Au/G-N,with nitrogen-doped porous carbon as the carrier,exhibits excellent catalytic stability.The acetylene conversion rate catalyzed by Au/G-N was 83% at a volumetric airspeed of 180 h-1 and a reaction temperature of 180℃,with only a 3% decrease in conversion rate after 3 600 minutes of reaction.This is primarily attributed to the interaction between nitrogen atoms and Au species in the carrier,enhancing Au dispersion and reducing the aggregation of oxidized Au after reduction.Additionally,nitrogen introduction effectively suppresses carbon deposition on the catalyst,preventing catalyst deactivation due to the coverage of active sites.
关键词
Au催化剂/稳定性/反应性挤出技术/多孔碳基材料Key words
Au catalysts/stability/reactive extrusion technology/porous carbon-based materials引用本文复制引用
基金项目
国家重点研发计划基金资助项目(2020YFB0606400)
内蒙古重点研发计划基金资助项目(2021ZD0042)
出版年
2024
国家科技期刊平台
NSTL
万方数据