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Thermodynamic Analysis of Catalyst Stability in Hydrothermal Reaction Media
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2018-06-20 , DOI: 10.1021/acs.iecr.8b01334 Jennifer N. Jocz 1 , Phillip E. Savage 1, 2 , Levi T. Thompson 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2018-06-20 , DOI: 10.1021/acs.iecr.8b01334 Jennifer N. Jocz 1 , Phillip E. Savage 1, 2 , Levi T. Thompson 1
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Hydrothermal solutions are important media for the conversion of biomass-derived species to useful chemicals and the destruction of environmental pollutants. These solutions are aggressive and can degrade heterogeneous catalysts. This article describes a framework for understanding the hydrothermal stability of heterogeneous catalyst materials with respect to oxidation and dissolution. We applied the revised Helgeson–Kirkham–Flowers thermodynamic equation of state to determine the oxidation states and solubilities of metals and oxides in water at 150–550 °C and 22–50 MPa. Design criteria for catalyst compositions were determined through correlations between metal solubility and electronegativity and between oxide solubility and cation electronegativity, ionic–covalent parameter, and polarizing power. Design criteria for aqueous solution compositions were determined by constructing oxygen fugacity–pH diagrams, which illustrate material phase changes in response to changes in pH and the oxidative or reductive strength of the solution. Combined, these criteria facilitate design of stable catalytic materials for hydrothermal reactions.
中文翻译：
水热反应介质中催化剂稳定性的热力学分析
热液解决方案是将生物质来源的物种转化为有用的化学品以及破坏环境污染物的重要介质。这些溶液具有腐蚀性，会降解多相催化剂。本文介绍了一个框架，用于了解非均相催化剂材料在氧化和溶解方面的水热稳定性。我们应用修正的Helgeson–Kirkham–Flowers热力学状态方程来确定150–550°C和22–50 MPa下水中金属和氧化物的氧化态以及溶解度。催化剂组成的设计标准是通过金属溶解度和电负性之间的关系以及氧化物溶解度和阳离子电负性，离子共价参数和极化能力之间的相关性来确定的。水溶液组成的设计标准是通过构建氧气逸度-pH图确定的，该图说明了材料相随pH的变化以及溶液的氧化或还原强度而发生的变化。这些标准相结合，有助于设计用于水热反应的稳定催化材料。
更新日期：2018-06-20
中文翻译：
水热反应介质中催化剂稳定性的热力学分析
热液解决方案是将生物质来源的物种转化为有用的化学品以及破坏环境污染物的重要介质。这些溶液具有腐蚀性，会降解多相催化剂。本文介绍了一个框架，用于了解非均相催化剂材料在氧化和溶解方面的水热稳定性。我们应用修正的Helgeson–Kirkham–Flowers热力学状态方程来确定150–550°C和22–50 MPa下水中金属和氧化物的氧化态以及溶解度。催化剂组成的设计标准是通过金属溶解度和电负性之间的关系以及氧化物溶解度和阳离子电负性，离子共价参数和极化能力之间的相关性来确定的。水溶液组成的设计标准是通过构建氧气逸度-pH图确定的，该图说明了材料相随pH的变化以及溶液的氧化或还原强度而发生的变化。这些标准相结合，有助于设计用于水热反应的稳定催化材料。
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