Ab Initio Thermodynamic Stability of Carbide Catalysts under Electrochemical Conditions,ACS Catalysis

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Ab Initio Thermodynamic Stability of Carbide Catalysts under Electrochemical Conditions
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-08-10 , DOI: 10.1021/acscatal.2c01732
Haobo Li _{1,

2} , Karsten Reuter ₁

Affiliation

Transition metal carbides (TMCs) are considered as promising electrocatalysts to break adsorption energy scaling relations that limit the catalytic function of the parent transition metals. Yet, their stability under electrochemical conditions is uncertain, with at least hexagonal Mo₂C in an aqueous electrolyte known to form a surface oxide layer already at very negative potentials. Here, we use ab initio thermodynamics to systematically investigate the stability of all low-index facets of a series of TMCs (TM = Ti, Zr, V, Nb, Cr, and Mo) with different metal/carbon ratios. The deduced electrochemical stability window indeed challenges an intended use of TMCs as CO₂ reduction catalysts. Only MoC and CrC are found to stably exhibit facets with accessible, methanol-selective C-rich active sites.

中文翻译：

电化学条件下碳化物催化剂的从头算热力学稳定性

过渡金属碳化物（TMCs）被认为是有前途的电催化剂，可以打破限制母体过渡金属催化功能的吸附能标度关系。然而，它们在电化学条件下的稳定性是不确定的，至少六方 Mo ₂ C 在水性电解质中已知会在非常负的电势下形成表面氧化物层。在这里，我们使用从头算热力学系统地研究了一系列具有不同金属/碳比的 TMC（TM = Ti、Zr、V、Nb、Cr 和 Mo）的所有低指数晶面的稳定性。推导出的电化学稳定性窗口确实挑战了 TMC 作为 CO _{2的预期用途}还原催化剂。只有 MoC 和 CrC 被发现稳定地表现出具有可访问的、甲醇选择性的富 C 活性位点的刻面。

更新日期：2022-08-10

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