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The use of Compressed Natural Gas (CNG) has demonstrated the potential to decrease Particulate Matter (PM) and nitrogen oxide (NOx) emissions simultaneously when used in a dual-fuel application with diesel fuel functioning as the ignition source. However, some authors do find that NOx emissions can increase. One postulation is that the conflicting results in the literature may be due to the difference in composition of natural gas around the world. Therefore, in order to investigate if CNG composition influences combustion performance and emissions, four unique mixtures of CNG were tested (i.e., 87% to 96% methane) while minimizing the combined difference of the density, heating value, and constant pressure specific heat of each mixture. This was accomplished at moderate energy substitution ratios (up to 40%) in a single cylinder engine operating at various loads.