Catalytic Reduction Of NO Without NH3 On Mn Embedded Graphene: A Density Of Functional Theory Study

Abstract

Nitrogen oxide (NO) is an important air pollutant that occurs as a result of burning fossil fuels. Through NO reduction reactions on catalytically selective catalysts, its detrimental effects can be significantly reduced. Mn-doped graphene systems can be synthesized experimentally, and due to the use of relatively few Mn (manganese) atoms, it is anticipated that they will cost much less than single-atom crystal surfaces over time. In this study, NO reduction reaction on Mn doped graphene surface was investigated by density functional theory. The structural properties of the Mn-doped graphene surface were analyzed by bader charge analysis and electron density difference map. For the reduction of NO, two different reaction paths were considered according to the different adsorption conditions of NO molecules. Our calculation results showed that, on the first reaction path, the reaction takes place at the end of two transition states with energy barriers of 0.27 eV and 0.59 eV, while the other reaction path takes place directly with an energy barrier of 0.42 eV. These results showed that the Mn doped graphene catalyst has high catalytic activity on both reaction paths. This information can be used to develop different strategies on graphene-based materials for NO removal.

Keywords

• NO reduction reaction
• Mn embedded grafen
• Adsorption
• Density functional theory.

Mn Katkılı Grafen Yüzey Üzerinde NH3 Olmadan NO’nun Katalitik İndirgenmesi: Bir Yoğunluk Fonksiyonel Teorisi Çalışması

Öz

Nitrojen oksit (NO) fosil yakıtların yanması sonucunda ortaya çıkan önemli bir hava kirleticisidir. Katalitik olarak seçici katalizörler üzerinde NO indirgenme reaksiyonları yoluyla onun zararlı etkileri önemli ölçütlerde azaltılabilir. Mn katkılı grafen sistemler deneysel olarak sentezlenebilir ve nispeten az sayıda Mn (manganez) atomu kullanımı nedeniyle ilerleyen zaman içerisinde tek atom kristal yüzeylerine göre çok daha düşük maliyetli olması ön görülmektedir. Bu çalışmada Mn katkılı grafen yüzey üzerinde NO indirgenme reaksiyonu yoğunluk fonksiyonel teorisi yoluyla incelenmiştir. Mn katkılı grafen yüzeyin yapısal özellikleri bader yük analizi ve elektron yoğunluğu farkı haritası ile analiz edildi. NO indirgenmesi için, NO moleküllerinin farklı adsorpsiyon durumlarına göre iki farklı reaksiyon yolu düşünüldü. Bizim hesaplama sonuçlarımız göstermiştir ki, birinci reaksiyonu yolu üzerinde reaksiyon 0.27 eV ve 0.59 eV enerji bariyerleri ile iki geçiş durumu sonunda gerçekleşirken, diğer reaksiyon yolu 0.42 eV enerji bariyeri ile direkt olarak gerçekleşmektedir. Bu sonuçlar, her iki reaksiyon yolu üzerinde Mn katkılı grafen katalizörün yüksek katalitik aktiviteye sahip olduğunu göstermiştir. Bu bilgiler, NO’nun uzaklaştırılması için grafen tabanlı malzemeler üzerinde farklı stratejiler geliştirmek için kullanılabilir. 

Anahtar Kelimeler

• NO indirgenme reaksiyonu
• Mn katkılı grafen
• Adsorpsiyon
• Yoğunluk fonksiyonel teorisi

Kaynakça

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