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沸石分子筛路易斯酸位点的构建、失活及稳定化研究进展OA

Research progress on construction,deactivation and stabilization of Lewis acid sites in zeolite molecular sieves

中文摘要英文摘要

精准构建沸石分子筛中的路易斯酸位点(Lewis acid sites,LAS)是提升其催化活性的重要策略之一.然而,在实际反应中,水诱导、中毒、积炭和骨架坍塌等问题会导致LAS被破坏从而催化剂失活.系统综述了LAS的构建方法、失活机制及稳定化策略.通过骨架脱铝(水热、酸碱处理)、金属离子掺杂和缺陷工程可有效构建LAS,其催化活性源于配位不饱和金属中心的缺电子特性.然而,LAS在反应过程中易与水分子配位饱和、发生高温羟基缩合、被积炭覆盖及溶出阳离子等,引起酸强度衰减及结构坍塌从而失活.当前LAS稳定化策略聚焦于:(1)疏水改性(增大硅铝比(物质的量比)、表面功能化)抑制水解反应;(2)结构强化(金属离子掺杂、物理防护层制备和高熵合金构建等)延缓铝物种迁移;(3)多级孔构建提升抗积炭性能;(4)LAS再生.以上策略对于稳定LAS发挥着重要作用.今后,随着表征技术和催化剂制备技术的不断发展,研究人员可精准解析LAS失活机制并构建原子层面抗失活位点.

Precise construction of Lewis acid sites(LAS)in zeolite molecular sieves is one of the important strategies to improve their catalytic activity.However,problems such as water induction,poisoning,carbon deposition and skeleton collapse in actual reactions can lead to the destruction and deactivation of LAS.The construction methods,deactivation mechanisms and stabilization strategies of LAS were systematically reviewed.LAS can be efficiently constructed by framework de-alumination(hydrothermal and acid treatment),metal ion doping and defect engineering,and their catalytic activity originates from the electron-deficient property of the coordinating unsaturated metal center.However,LAS are prone to coordination saturation with water molecules,high-temperature hydroxyl condensation,carbon deposition,and cation dissolution during the reaction process,leading to acid strength decay and structural collapse,resulting in deactivation.Current LAS stabilization strategies focus on:(1)Hydrophobic modification(increasing silica-aluminium ratio(molar ratio),surface functionalization)to inhibit hydrolysis;(2)Structural reinforcement(metal ion doping,preparation of physical protective layer and construction of high-entropy alloys)to delay the migration of aluminium species;(3)Hierarchical pore construction to enhance the anti carbon deposition performance;(4)LAS regeneration.Above strategies play an important role in stabilizing LAS.In the future,with the continuous development of characterization technologies and catalyst preparation technologies,researchers can accurately analyze the mechanisms of LAS deactivation and construct atomic level anti-deactivation sites.

贾伯阳;柳蒙蒙;岳宣宇;崔燕冉;陈亚松

中国长江三峡集团有限公司,湖北 武汉 430000中国长江三峡集团有限公司,湖北 武汉 430000浙江大学 生物系统工程与食品科学学院,浙江 杭州 310058浙江大学 生物系统工程与食品科学学院,浙江 杭州 310058中国长江三峡集团有限公司,湖北 武汉 430000

化学化工

沸石分子筛路易斯酸位点疏水改性结构强化多级孔构建

zeolite molecular sievesLewis acid siteshydrophobic modificationstructural reinforcementhierarchical pore construction

《低碳化学与化工》 2026 (4)

38-48,11

中国长江三峡集团有限公司科研项目资助(NBWL202200489)国家资助博士后研究人员计划(GZC20241500).

10.12434/j.issn.2097-2547.20250208

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