DataVXACS Energy LettersPaper
journal article·2022-12-09

Identification of Active Sites for Ammonia Electrosynthesis on Ruthenium

Lin Hu, Hemanth Somarajan Pillai, Corbin Feit, Kaige Shi, Zhengning Gao, Parag Banerjee, Hongliang Xin, Xiaofeng Feng

ACS Energy Letters· Volume 7· Issue 12
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Source abstract

Abstract

Electrochemical N2 reduction reaction (NRR) provides an attractive approach toward sustainable NH3 production, while the design of electrocatalysts for NRR is hindered by the lack of knowledge of the structure–activity relationships and active sites. Here we report a prominent size-dependent activity for the NRR on Ru nanoparticles prepared by atomic layer deposition. As the Ru particle size increased from 2.1 to 8.4 nm, the mass activity and Faradaic efficiency for NH3 production both decreased monotonically, while the specific (Ru-surface-area-normalized) activity reached the highest value on 3.8 nm Ru nanoparticles but declined by 5-fold on 8.4 nm Ru nanoparticles. Density functional theory (DFT) calculations and free energy analysis of elementary steps revealed the Ru D5 step site, with its maximal population at ∼4 nm particles, as the active site for the NRR on Ru, because it favors the adsorption of the *N2H intermediate compared to other surface sites while not getting poisoned by the *NH2 intermediate.
Source: openalex_inverted_index · Quality: baseline

Research context

NanomaterialsCatalysis & surfacesMaterials processing

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Advanced Photocatalysis Techniques · Nanomaterials for catalytic reactions

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States

Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, Virginia24061, United States

Department of Physics, University of Central Florida, Orlando, Florida32816, United States

Renewable Energy and Chemical Transformations (REACT) Cluster, University of Central Florida, Orlando, Florida32816, United States

NanoScience and Technology Center, University of Central Florida, Orlando, Florida32816, United States

Florida Solar Energy Center, University of Central Florida, Orlando, Florida32816, United States

Department of Chemistry, University of Central Florida, Orlando, Florida32816, United States

Funding

Division of Chemistry · Division of Electrical, Communications and Cyber Systems · Division of Chemical, Bioengineering, Environmental, and Transport Systems

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