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大连化物所实现甲醇与一氧化碳高选择性耦合制取芳烃

2018-09-29 11:16:01    央广网

央广网大连9月29日消息(记者张四清 贾铁生 通讯员倪友明)芳烃(苯、甲苯、二甲苯)是重要的基础化工原料,其产量和规模仅次于乙烯和丙烯。目前,芳烃的大规模工业生产是通过石脑油为原料的芳烃联合装置实现。近年来,我国聚酯工业高速发展,芳烃消费量快速上升,供应缺口逐年加大。因此,加快芳烃生产、发展芳烃新技术对于我国聚酯业的健康发展至关重要。

由于我国石油资源短缺,煤炭丰富,能源及化学品的清洁高效供应已成为国家发展中亟须解决的问题。发展煤经甲醇制芳烃等化学品技术,对于降低原油对外依存度和保障国家能源安全意义重大,且市场前景广阔。甲醇制芳烃反应常选用具有择形性的ZSM-5分子筛作为催化剂。因为氢转移反应存在,生成芳烃的同时会伴随着烷烃生成,芳烃选择性有待进一步提高。

近日,中科院大连化物所甲醇制烯烃国家工程实验室刘中民院士、朱文良研究员团队,发现在无金属改性的纯H-ZSM-5分子筛上,甲醇与一氧化碳能够发生耦合反应,获得约80%芳烃选择性。另外,该团队还提出了一种全新的芳构化机理:甲醇与一氧化碳在H-ZSM-5上发生羰化反应生成羰化物中间体,然后与烯烃反应生成环戊烯酮类中间体,经脱水得到芳烃。通过13C核磁与同位素示踪等方法,证明了一氧化碳的碳能进入到芳烃以及环戊烯酮类中间体中。由于一氧化碳中的碳部分进入到芳烃中,相对甲醇直接制芳烃,能提升芳烃的产量,有利于提高工业化过程的经济性。该研究以通讯形式发表在《德国应用化学》(Angew. Chem. Int. Ed. 2018, 57, 12549-12553)上。该论文还被评为热点论文(Hot Paper)。

上述研究工作得到国家自然科学基金的支持。

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