Journal
SCIENCE CHINA-MATERIALS
Volume 64, Issue 5, Pages 1173-1181Publisher
SCIENCE PRESS
DOI: 10.1007/s40843-020-1522-y
Keywords
nitrogen reduction reaction; electrocatalysts; single-atom catalysts; density functional theory (DFT); black phosphorus
Categories
Funding
- National Natural Science Foundation of China [21525626, 21761132023]
- Program of Introducing Talents of Discipline to Universities [BP0618007]
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This study explores the performance trends and design principles of transition metal single-atom catalysts with P-based ligands in nitrogen reduction reaction. Results show that W@BP, Ta@BP, and Nb@BP are promising candidates for high selectivity and efficiency in NRR. Constructing a volcano plot reveals that a moderate positive charge on the metal center can enhance the catalytic performance of NRR.
Designing highly selective and efficient single-atom electrocatalysts is essential for ammonia production under ambient conditions. This paper describes a density functional theory study on exploring the performance trends of transition metal complexes with P-based ligands in nitrogen reduction reaction (NRR) and further develops a design principle for high-performance single-atom catalysts (SACs) of NRR. Among the explored catalysts, W@BP (0.40 eV), Ta@BP (0.47 eV), and Nb@BP (0.53 eV) are identified as remarkable candidates with low free energy change in the potential-limiting step, high stability and high electrical conductivity for NRR. It is worth noting that almost all SACs with P-based ligands exhibit high NRR selectivity, due to the fact that they adsorb *N-2 more strongly than *H. The adsorption free energy of *N2H can be considered as a descriptor for the intrinsic activity trends in NRR. Furthermore, by constructing a volcano plot of the activity against the electronic charge on metal centers, it is demonstrated that the metal center with a moderate amount of positive charge can promote the catalytic performance of NRR.
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