Towards improved stability of transition metal nitrides in aqueous solutions

IF 9.1 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Progress in Solid State Chemistry Pub Date : 2024-07-15 DOI:10.1016/j.progsolidstchem.2024.100474
Xiang Li , Anna Bergljót Gunnarsdóttir , Valery Pershina , Árni Björn Höskuldsson , Marc Francis Hidalgo , Egill Skúlason , Helga Dögg Flosadóttir , Cristina Giordano
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Abstract

Transition metal nitrides (TMNs), in some cases referred as metallic ceramics, have unique physical and chemical properties, thanks to their ceramic-metallic nature, and are considered an attractive alternative to noble metals for electrochemical processes. In particular, theoretical work predicts TMNs as promising electrocatalysts towards the nitrogen reduction reaction (NRR). However, recent experimental studies under realistic conditions, have shown the release of lattice nitride to ammonia in a noncatalytic process, suggesting inherent instability of these materials. TMNs stability can be increased by the incorporation of a second metal in the lattice, to form bimetallic systems. Herein, we present a robust approach to prepare nonprecious transition multi-metallic nitride nano-catalysts, followed by a comprehensive study on their stability. The stability of the as-prepared catalysts was tested in electrolytes relevant for electrocatalysis, showing a higher chemical resistance of the bimetallic catalysts over the monometallic ones. This study suggests a novel approach to matching electrolyte pH and catalyst to ensure chemical stability in the electrochemical environment.

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提高过渡金属氮化物在水溶液中的稳定性
过渡金属氮化物(TMNs)在某些情况下被称为金属陶瓷,由于其陶瓷-金属性质而具有独特的物理和化学特性,被认为是电化学过程中贵金属的一种有吸引力的替代品。特别是,理论研究预测 TMNs 是氮还原反应 (NRR) 的理想电催化剂。然而,最近在现实条件下进行的实验研究表明,在非催化过程中,氮化晶格会释放出氨气,这表明这些材料具有固有的不稳定性。通过在晶格中加入第二种金属,形成双金属系统,可以提高 TMN 的稳定性。在此,我们提出了一种制备非贵金属过渡多金属氮化物纳米催化剂的可靠方法,并随后对其稳定性进行了全面研究。在与电催化相关的电解质中测试了所制备催化剂的稳定性,结果表明双金属催化剂的耐化学性高于单金属催化剂。这项研究提出了一种匹配电解质 pH 值和催化剂的新方法,以确保在电化学环境中的化学稳定性。
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来源期刊
Progress in Solid State Chemistry
Progress in Solid State Chemistry 化学-无机化学与核化学
CiteScore
14.10
自引率
3.30%
发文量
12
期刊介绍: Progress in Solid State Chemistry offers critical reviews and specialized articles written by leading experts in the field, providing a comprehensive view of solid-state chemistry. It addresses the challenge of dispersed literature by offering up-to-date assessments of research progress and recent developments. Emphasis is placed on the relationship between physical properties and structural chemistry, particularly imperfections like vacancies and dislocations. The reviews published in Progress in Solid State Chemistry emphasize critical evaluation of the field, along with indications of current problems and future directions. Papers are not intended to be bibliographic in nature but rather to inform a broad range of readers in an inherently multidisciplinary field by providing expert treatises oriented both towards specialists in different areas of the solid state and towards nonspecialists. The authorship is international, and the subject matter will be of interest to chemists, materials scientists, physicists, metallurgists, crystallographers, ceramists, and engineers interested in the solid state.
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