Oliver Christensen, Ana-Iulia Hutu, Henrik H. Kristoffersen, Jan Rossmeisl
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N2 dissociation on AuCoFeMoRu high-entropy alloys: Circumventing scaling relations and step dependencies
Finding a better catalyst for the reduction of nitrogen to ammonia would be of considerable use to the chemical industry, allowing for cheaper and possibly decentralized ammonia production. One approach to find a better catalyst is to explore the element component space continuously via the use of high-entropy alloys, uncovering as of yet untested multi-element catalysts and reaction sites to optimize reaction activity. Utilizing DFT calculations and microkinetic modeling, we use the AuCoFeMoRu high-entropy alloy as a discovery platform for N2 reduction catalysts. Testing both terrace and step sites, we find that high-entropy alloy terraces can reach as high activities as steps for the N2 reduction reaction, due to their heterogeneous surface structure. We also find that high-entropy alloys are able to circumvent the scaling relations to an extent, due to the decoupling of the transition state and final state structure of the reaction. We discover several promising high-entropy alloy reaction sites, with a roughly twofold improvement in activity over the best monometallic surface. However, significantly larger gains in activity seem to still be fundamentally limited by the scaling relations.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.