Atomistic Mechanisms For Catalytic Transformations Of NO To NH3 ...

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Peiping Yu, Yu Wu, Hao Yang, Miao Xie, William A. Goddard Ⅲ, Tao Cheng. Atomistic Mechanisms for Catalytic Transformations of NO to NH3, N2O, and N2 by PdJ. Chinese Journal of Chemical Physics , 2023, 36(1): 94-102. DOI: 10.1063/1674-0068/cjcp2109153

Citation:

Peiping Yu, Yu Wu, Hao Yang, Miao Xie, William A. Goddard Ⅲ, Tao Cheng. Atomistic Mechanisms for Catalytic Transformations of NO to NH3, N2O, and N2 by PdJ. Chinese Journal of Chemical Physics , 2023, 36(1): 94-102. DOI: 10.1063/1674-0068/cjcp2109153

Peiping Yu, Yu Wu, Hao Yang, Miao Xie, William A. Goddard Ⅲ, Tao Cheng. Atomistic Mechanisms for Catalytic Transformations of NO to NH3, N2O, and N2 by PdJ. Chinese Journal of Chemical Physics , 2023, 36(1): 94-102. DOI: 10.1063/1674-0068/cjcp2109153

Citation:

Peiping Yu, Yu Wu, Hao Yang, Miao Xie, William A. Goddard Ⅲ, Tao Cheng. Atomistic Mechanisms for Catalytic Transformations of NO to NH3, N2O, and N2 by PdJ. Chinese Journal of Chemical Physics , 2023, 36(1): 94-102. DOI: 10.1063/1674-0068/cjcp2109153

Atomistic Mechanisms for Catalytic Transformations of NO to NH3, N2O, and N2 by Pd

• Peiping Yu,
• Yu Wu,
• Hao Yang,
• Miao Xie,
• William A. Goddard Ⅲ,
• Tao Cheng

Abstract

• Abstract

  The industrial pollutant NO is a potential threat to the environment and to human health. Thus, selective catalytic reduction of NO into harmless N_2, NH_3, and/or N_2O gas is of great interest. Among many catalysts, metal Pd has been demonstrated to be most efficient for selectivity of reducing NO to N_2. However, the reduction mechanism of NO on Pd, especially the route of N-N bond formation, remains unclear, impeding the development of new, improved catalysts. We report here the elementary reaction steps in the reaction pathway of reducing NO to NH_3, N_2O, and N_2, based on density functional theory (DFT)-based quantum mechanics calculations. We show that the formation of N_2O proceeds through an Eley-Rideal (E-R) reaction pathway that couples one adsorbed NO^* with one non-adsorbed NO from the solvent or gas phase. This reaction requires high NO^* surface coverage, leading first to the formation of the trans-(NO)_2^* intermediate with a low N-N coupling barrier (0.58 eV). Notably, trans-(NO)_2^* will continue to react with NO in the solvent to form N_2O, that has not been reported. With the consumption of NO and the formation of N_2O^* in the solvent, the Langmuir-Hinshelwood (L-H) mechanism will dominate at this time, and N_2O^* will be reduced by hydrogenation at a low chemical barrier (0.42 eV) to form N_2. In contrast, NH_3 is completely formed by the L-H reaction, which has a higher chemical barrier (0.87 eV). Our predicted E-R reaction has not previously been reported, but it explains some existing experimental observations. In addition, we examine how catalyst activity might be improved by doping a single metal atom (M) at the NO^* adsorption site to form M/Pd and show its influence on the barrier for forming the N-N bond to provide control over the product distribution.
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