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Fundamental Insights into High-Temperature Water Electrolysis Using Ni-Based Electrocatalysts
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-11-18 00:00:00 , DOI: 10.1021/acs.jpcc.5b07814 Xiang-Kui Gu 1 , Eranda Nikolla 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-11-18 00:00:00 , DOI: 10.1021/acs.jpcc.5b07814 Xiang-Kui Gu 1 , Eranda Nikolla 1
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Hydrogen production from water electrolysis using solid oxide electrolysis cells (SOECs) has attracted considerable attention because of favorable kinetics and thermodynamics associated with operation at elevated temperatures. In the present work, we employ density functional theory calculations combined with microkinetic modeling to investigate the factors that govern this process on Ni and Ni-based alloy electrocatalysts. Our studies show that H2O dissociation is the rate-limiting step on Ni(111) and Ni(211), with Ni(211) exhibiting the lowest barrier for this step. The effect of alloying Ni with another metal on the energetics associated with this process is also investigated. Our studies show that the binding energies of the most abundant intermediates, OH and O, become gradually weaker, and the barriers for water dissociation become gradually higher as Ni is alloyed with metals from left to right in the periodic table. A volcano-type relationship between the calculated electrochemical rates and the binding energies of O is found, with the Ni/Fe alloy exhibiting the highest rate among the Ni alloys considered. These predictions are consistent with the reported experimental results, suggesting that these structure/performance relationships can be used to guide the design of heterogeneous electrocatalysts for high-temperature water electrolysis.
中文翻译：
使用镍基电催化剂进行高温水电解的基本原理
使用固体氧化物电解池（SOEC）进行水电解制氢，由于在高温下运行具有良好的动力学和热力学特性，因此引起了人们的极大关注。在当前的工作中，我们采用密度泛函理论计算与微动力学建模相结合的方法来研究控制Ni和Ni基合金电催化剂上这一过程的因素。我们的研究表明H 2O解离是Ni（111）和Ni（211）上的限速步骤，其中Ni（211）显示出最低的势垒。还研究了镍与另一种金属合金化对与此过程相关的高能学的影响。我们的研究表明，随着元素周期表中镍从左到右与金属合金化，最丰富的中间体OH和O的结合能逐渐变弱，水离解的势垒也逐渐变高。发现计算出的电化学速率与O的结合能之间的火山类型关系，其中所考虑的Ni合金中Ni / Fe合金的速率最高。这些预测与所报告的实验结果一致，
更新日期：2015-11-18
中文翻译：
使用镍基电催化剂进行高温水电解的基本原理
使用固体氧化物电解池（SOEC）进行水电解制氢，由于在高温下运行具有良好的动力学和热力学特性，因此引起了人们的极大关注。在当前的工作中，我们采用密度泛函理论计算与微动力学建模相结合的方法来研究控制Ni和Ni基合金电催化剂上这一过程的因素。我们的研究表明H 2O解离是Ni（111）和Ni（211）上的限速步骤，其中Ni（211）显示出最低的势垒。还研究了镍与另一种金属合金化对与此过程相关的高能学的影响。我们的研究表明，随着元素周期表中镍从左到右与金属合金化，最丰富的中间体OH和O的结合能逐渐变弱，水离解的势垒也逐渐变高。发现计算出的电化学速率与O的结合能之间的火山类型关系，其中所考虑的Ni合金中Ni / Fe合金的速率最高。这些预测与所报告的实验结果一致，
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