Subsurface Hydrogen in a Alloy Hydrogenation Catalysis

催化剂是一种在不消耗自身的情况下提高反应速度的物质，它负责生产社会所依赖的许多化学品和材料。合金通常是比衍生它们的纯元素更有效的催化剂，因为它们的性质可以通过改变它们的元素组成来调节。然而，这种调整带来了一个具有挑战性的研究问题，因为它可能需要准备和测试数百种不同的成分来找到最佳催化剂。在化学催化项目的资助下，卡内基梅隆大学的安德鲁·盖尔曼博士正在开发和应用方法，通过同时测量许多合金成分上的催化反应来加速这类研究。这些数据有助于全面了解合金成分对催化反应速率和选择性的影响。此外，这些数据正被用于开发机器学习模型，以预测新合金的催化性能，并确定可能的候选对象，以进行进一步的测试和研究。盖尔曼博士积极参与本科研究，以鼓励年轻学生，特别是女性，追求更高的STEM学位和职业。在化学系化学催化计划的资助下，卡内基梅隆大学的安德鲁·盖尔曼博士正在综合使用表面分析工具、催化反应动力学和微动力学模型来研究催化表面化学。他的工具在成分扩散合金膜(CSFAF)上同时测量100种不同合金成分的催化反应动力学，提供了全面的数据集，作为了解合金催化中成分依赖趋势的基础。盖尔曼博士的工作是开发数据丰富的催化建模方法。他的工作使基本反应参数(如活化势垒)和催化剂特性(如d带能量)之间的相关性得到了实验证明；以前只有通过电子结构理论才能获得的相关性。这种方法被应用于乙烯(C2H4)和乙炔(C2H2)加氢反应。已有的关于Pd和Ni表面加氢反应的工作表明，表面下的氢可以在反应机理中发挥作用，并影响表面反应动力学。利用最近开发的动力学框架，其中包括机制中的地下氢，Gellman博士正在确定其在Pd和Pt合金上C2H4和C2H2氢化中的作用。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Catalysts, substances that increase reaction rates without themselves being consumed, are responsible for the production of many of the chemicals and materials on which society relies. Alloys are often more effective catalysts than the pure elements from which they are derived because their properties can be tuned by varying their elemental composition. However, this tuning poses a challenging research problem because it can require the preparation and testing of hundreds of different compositions to find the optimal catalyst. With funding from the Chemical Catalysis Program, Dr. Andrew Gellman at Carnegie Mellon University is developing and applying methods for the acceleration of such research by measuring catalytic reactions over many alloy compositions concurrently. These data are providing a comprehensive understanding of the influence of alloy composition on catalytic reaction rates and selectivities. In addition, these data are being used to develop machine learning models to predict the catalytic properties of new alloys and identify likely candidates for further testing and study. Dr. Gellman is actively involved in undergraduate research as a means of encouraging young students, especially women, to pursue advanced STEM degrees and careers.With funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. Andrew Gellman of Carnegie Mellon University is integrating the use of surface analysis tools, catalytic reaction kinetics, and microkinetic modelling to study catalytic surface chemistry. His tools for concurrent measurement of catalytic reaction kinetics at 100 different alloy compositions across a Composition Spread Alloy film (CSFAF) provide comprehensive datasets to serve as the basis for understanding composition dependent trends in alloy catalysis. Dr Gellman’s work is enabling development of data rich approaches to catalysis modeling. His work allows experimental demonstration of correlations between fundamental reaction parameters such as activation barriers and catalyst characteristics such as d-band energies; correlations that previously have been accessible only through electronic structure theory. This methodology is being applied to ethylene (C2H4) and acetylene (C2H2) hydrogenation reactions. Existing work on hydrogenation reactions on Pd and Ni surfaces has suggested that subsurface hydrogen can play a role in the mechanism and influence surface reaction kinetics. Using a recently developed kinetic framework that includes subsurface hydrogen in the mechanism, Dr. Gellman is determining its role in C2H4 and C2H2 hydrogenation on Pd and Pt alloys.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.