DOI: 10.1021/jacs.6c16356 ISSN: 0002-7863

Dynamic Extraction of Internal Active Species in Liquid Metal-Based Biphasic Catalyst

Yixiao Zou, Zanyu Chen, Wenda Chen, Chen Zhang, Jiajun Wang, Xin Wang, Sheng Zhao, Kang Liao, Peng Cui, Jinfeng Zhang, Jia Ding, Wenbin Hu, Xiaopeng Han

Abstract

Catalyst development is pivotal for industrial and energy advancements, yet it is fundamentally challenged by the static nature of the conventional solid catalysts. Their active sites, locked within rigid frameworks, are neither dynamically responsive nor regenerable, leading to an irreversible consumption during reaction cycles. Herein, we report an electrocapillary-enhanced dynamic extraction process to design a liquid metal-based biphasic catalyst (LMBC), enabling precise population control and in situ regeneration of active species. We establish two key thermodynamic criteria for the dynamic extraction mechanism to guide the LMBC development: alloying energy, which governs the tendency of active elements to form solid active alloys within the liquid metal matrix (gallium, Ga), and surface energy, which drives the dynamic extraction and surface exposure of internal active alloys. Through this mechanism, the quantity of exposed active species becomes adaptively adjustable, allowing fine-tuned control over the catalytic activity. Moreover, deactivated species can be replenished in situ from the liquid metal interior. This LMBC platform demonstrates universality and scalability in the alloy composition across diverse catalysis systems. Overall, this work provides a novel strategy for designing adaptive renewable catalytic systems.

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