Angew.Chem.南京工业徐乐/华东师范大学吴鹏、庹杰/四川大学王岩: 整合氢解离-溢流位点于限域Pt/SAPO-34实现CO₂高效转化为轻质烷烃!

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The depressing of atmospheric CO₂ concentration necessitates sustainable chemical conversion strategies by direct hydrogenation to light alkanes (C₂⁰-C₄⁰) over oxide/zeolite (OXZEO) bifunctional catalyst. Prior studies demonstrated that SSZ-13 aluminosilicate with strong acidity as zeolite component promotes hydrogen transfer to yield alkanes but also accelerates coking/deactivation, while SAPO-34 silicoaluminophosphate with moderate acidity greatly improves the catalytic stability but yields insufficient alkane selectivity. Herein, we designed a new OXZEO bifunctional catalytic system based on trace Platinum species (0.11 wt.%) confined within SAPO-34 coupling with ZnZrOx solid solution (ZnZrOx/Pt@SAPO-34), achieving a high CO₂ conversion (46.1%) with C₂⁰-C₄⁰ selectivity (94.1%), and giving a superior stable lifetime over 200 h. The excellent catalytic performance is attributed to the confined hydrogen spillover mechanism over Pt species in SAPO-34 that suppresses carbon deposition and enables efficient H₂ dissociation and spillover to significantly promote light olefin hydrogenation to corresponding alkanes.

KEYWORDS: bifunctional catalyst, CO₂ hydrogenation, light alkanes, zeolite

       降低大气CO₂浓度需发展可持续化学转化策略，通过氧化物/沸石（OXZEO）双功能催化剂可将CO₂直接加氢转化为C₂⁰-C₄⁰链烷烃。先前研究表明，采用酸性较强的SSZ-13硅铝沸石作为沸石组分可促进氢转移生成烷烃，但也会加速积炭/失活；而酸性适中的SAPO-34硅磷铝分子筛虽显著提高了催化稳定性，却无法获得足够的烷烃选择性。

要点1. 本文设计了一种基于痕量Pt物种（0.11 wt.%）限域于SAPO-34中并与ZnZrOx固溶体耦合的新型OXZEO双功能催化体系（ZnZrOx/Pt@SAPO-34），实现了46.1%的CO₂转化率与94.1%的C₂⁰-C₄⁰选择性，且具有超过200小时的优异稳定寿命。

要点2. 其出色的催化性能归因于SAPO-34中Pt物种的限域氢溢流机制，该机制抑制了积炭，并实现高效的H₂解离与溢流，从而显著促进轻质烯烃加氢生成相应的烷烃。

要点3. 本研究通过借鉴成熟的烷烃脱氢催化技术，为将CO₂转化为高价值烃类提供了一条可行且稳定的技术路径。

Jinsong Cui,Han Jiang, Jie Tuo*, Hongwei Guo, Ming-Ao Sun, Jilong Wang, Yan Wang*, Xudong Tian, Jiaqing Zhu, Jian Li, Peng Wu*, Le Xu*. Integrating Hydrogen Dissociation and Spillover Sites Into Platinum Confined SAPO-34 Zeolite Unlocks Efficient CO₂ Hydrogenation to Light Alkanes. Angew. Chem. Int. Ed. 2026, e2445993.

DOI: 10.1002/ange.2445993

https://doi.org/10.1002/ange.2445993

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