Density functional theory (DFT) methods were used to enhance secondary-sphere interactions in catalysts for methane activation. Using formate (HCO2-) as a standard, more complex catalysts were designed through the addition of chemical groups to mimic peptide structures. The results indicated that the impact of hydrogen-bonding was substantial, and it was found that a modified version of a serine-glycine dipeptide yielded the lowest energy barriers with a ΔG‡ of 26.0 kcal/mol. A correlation between the energy barrier and bond lengths was elucidated, indicating that the length of C-H bonds have a more significant impact than the length of O-H bonds.