ゼオライト触媒設計を革新する新モデル(New Model Revolutionizes Zeolite Catalyst Design for Enhanced Stability)

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2025-05-29 中国科学院(CAS)

中国科学院大連化学物理研究所と福州大学の研究チームは、ゼオライト内部における金属クラスターの移動と凝集を定量的に記述する初の理論モデルを構築しました。シリカライト-1(S-1)ゼオライト中での白金(Pt)クラスターの動きを第一原理計算で解析し、結晶サイズがその挙動に与える影響を明らかにしました。特にb軸長が2μmを超えるとPtが凝集し安定化する現象を発見し、この知見を基に高安定性を持つプロパン脱水素用Pt-Sn@MFI触媒を開発。触媒設計の新たな理論基盤を提供しました。

<関連情報>

安定したプロパン脱水素触媒のためのゼオライト中の白金移動ロックアップ Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst

Zhikang Xu,Mingbin Gao,Yao Wei,Yuanyuan Yue,Zhengshuai Bai,Pei Yuan,Paolo Fornasiero,Jean-Marie Basset,Bingbao Mei,Zhongmin Liu,Haibo Zhu,Mao Ye & Xiaojun Bao
Nature  Published:28 May 2025
DOI:https://doi.org/10.1038/s41586-025-09168-8

We are providing an unedited version of this manuscript to give early access to its findings. Before final publication, the manuscript will undergo further editing. Please note there may be errors present which affect the content, and all legal disclaimers apply.

Abstract

The shale gas revolution has shifted propylene production from naphtha cracking to on-purpose production with propane dehydrogenation (PDH) as the dominant technology1-9. Because PDH is endothermic and requires high temperatures that favour sintering and coking, the challenge is to develop active and stable catalysts1-3 that are sufficiently stable10,11. Zeolite-supported Pt-Sn catalysts have been developed to balance activity, selectivity and stability12,13, and more recent work documented a PDH catalyst based on zeolite-anchored single rhodium atoms with exceptional performance and stability14. Here we show for silicalite-1 (S-1) that migration of encapsulated Pt-Sn2 clusters and hence agglomeration and anchoring within the zeolite versus agglomeration on the external surface can be controlled by adjusting the length of the S-1 crystals’ b-axis. We find that when this axis is longer than 2.00 μm, migration of Pt-Sn2 monomers during PDH results in intra-crystalline formation of (Pt-Sn2)2 dimers that are securely locked in the channels of S-1 and capable of converting pure propane feed to propylene at 550 °C for more than 6 months with 98.3% selectivity at 91% equilibrium conversion. This performance exceeds that of other Pt-based PDH catalysts and approaches that of the Rh-based catalyst. While synthesis requirements and cost are currently prohibitive for industrial use, we anticipate that our approach to controlling the migration and lockup of metals in zeolites may enable to development of other noble metal catalysts that offer extended service lifetimes in industrial applications15-17.

0505化学装置及び設備
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