Uniting activity design principles of anode catalysts for direct liquid fuel cells†

EES catalysis Pub Date : 2024-08-02 DOI:10.1039/D4EY00100A
Daniel J. Zheng, Jiayu Peng, Kaylee McCormack, Hongbin Xu, Jin Soo Kang, Zhenshu Wang, Zhichu Ren, Ju Li, Yuriy Román-Leshkov and Yang Shao-Horn
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Abstract

Direct liquid fuel cells have advantages over hydrogen-based fuel cells and lithium-ion batteries for portable and mobile applications due to their high volumetric energy density and the convenient storage or refueling of liquid fuels. Unfortunately, the electrochemical oxidation of liquid fuels (such as methanol, ethanol, and formic acid) currently corresponds to ∼50% of the energy losses of these devices at operating conditions. Moreover, state-of-the-art catalysts for such critical reactions are generally composed of precious metals such as Pt and Pd, hindering the cost-effective implementation of these technologies. The development of novel catalyst design principles for electrochemical liquid fuel oxidation has been constrained by its complex, structure-sensitive reaction energetics that can involve multiple parallel, competitive reaction intermediates and pathways. In this review, we aim to dissect and bridge the understanding of fundamental energetics and the materials engineering of novel catalysts for the electrochemical oxidation of various liquid fuels. By deconvoluting these reactions into the energetics of different critical elementary steps, we define essential descriptors that govern the activity and selectivity of electrochemical liquid fuel oxidation. Several universal and fundamental design principles are proposed to optimize the catalytic performance of state-to-the-art and emerging electrocatalysts by tuning the chemistry and electronic structure of active sites. This review aims to provide a unique perspective connecting the electro-oxidation energetics of different liquid fuels with mechanistic and materials-centric studies to provide a holistic picture connecting the fundamental surface science with materials engineering for the rational design of electrocatalysts for liquid fuel oxidation.

Abstract Image

Abstract Image

统一直接液体燃料电池阳极催化剂的活性设计原则
与氢基燃料电池和锂离子电池相比,直接液体燃料电池在便携式和移动式应用中具有体积能量密度高、液体燃料储存或补充方便等优势。遗憾的是,液体燃料(如甲醇、乙醇和甲酸)的电化学氧化目前相当于这些设备在工作条件下能量损失的 50%。此外,用于此类关键反应的最先进催化剂通常由铂和钯等贵金属组成,阻碍了这些技术的成本效益实施。电化学液体燃料氧化的新型催化剂设计原则的开发一直受限于其复杂、结构敏感的反应能量学,其中可能涉及多个并行、竞争性的反应中间体和途径。在本综述中,我们旨在剖析各种液体燃料电化学氧化过程中新型催化剂的基本能量学和材料工程学,并在两者之间架起一座桥梁。通过将这些反应分解为不同关键基本步骤的能量学,我们定义了支配电化学液体燃料氧化的活性和选择性的基本描述符。通过调整活性位点的化学和电子结构,我们提出了几项通用的基本设计原则,以优化最先进和新兴电催化剂的催化性能。本综述旨在提供一个独特的视角,将不同液体燃料的电氧化能量学与机理研究和以材料为中心的研究联系起来,为合理设计液体燃料氧化电催化剂提供一个将基础表面科学与材料工程学联系起来的整体图景。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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