Liquid Gallium Nanoislands on Zeolite: A Dynamic Confinement Strategy to Break the Catalytic Trade-Off in Hydrodeoxygenation

IF 13.6 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2026-10-21 DOI:10.1021/acscatal.6c05041

Mingkun Gao,Wenli Bao,Cailing Chen,Chenzhu Wang,Kai Liu,Zhuangzhuang Ren,Qiang Zhang,Guoju Yang,Ziyi Zhao,Donghai Mei,Jihong Yu

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Abstract

Breaking the pervasive activity–selectivity–stability trade-off in catalytic hydrodeoxygenation (HDO) remains a formidable challenge. Herein, we report a bifunctional nanoisland catalyst (GaNPs-Pt/Beta) that overcomes this limitation by utilizing liquid gallium nanodroplets anchored on Beta zeolite as mobile nanoislands. These islands effectively restrict platinum single-atom migration and agglomeration. Concurrently, Brønsted acid sites provided by the zeolite sea facilitate the dehydration-etherification process. This synergy enables highly efficient transfer hydrogenation at the gallium–platinum interface, achieving selective C–O bond cleavage while preserving C═C bonds under mild conditions. Benefiting from this island-sea architecture, the GaNPs-Pt/Beta catalyst delivers high catalytic activity, achieving >99% cinnamyl alcohol conversion and 93.8% β-methylstyrene selectivity within 6 h at 160 °C, with recyclability demonstrated over nine cycles involving intercycle regeneration. This strategy is scalable to diverse α,β-unsaturated aldehyde/alcohol chemicals, demonstrating that zeolite-based liquid metal nanoislands provide a versatile platform for the sustainable synthesis of high-value chemicals.

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沸石上的液态镓纳米岛：打破氢脱氧催化权衡的动态约束策略

打破催化加氢脱氧（HDO）中普遍存在的活性-选择性-稳定性权衡仍然是一个艰巨的挑战。在此，我们报道了一种双功能纳米岛催化剂（GaNPs-Pt/Beta），它通过利用锚定在Beta沸石上的液态镓纳米液滴作为移动纳米岛来克服这一限制。这些孤岛有效地限制了铂的单原子迁移和团聚。同时，沸石海提供的Brønsted酸位促进了脱水-醚化过程。这种协同作用使镓-铂界面上的高效转移氢化成为可能，在温和条件下实现选择性C - o键裂解，同时保留C = C键。得益于这种岛海结构，GaNPs-Pt/Beta催化剂具有很高的催化活性，在160°C下，6小时内实现了bbbb99 %的肉桂醇转化率和93.8%的β-甲基苯乙烯选择性，并且经过9个循环（包括循环间再生）证明了可回收性。该策略可扩展到多种α，β-不饱和醛/醇化学品，表明基于沸石的液态金属纳米岛为高价值化学品的可持续合成提供了一个多功能平台。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.