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[Display omitted] • Single-atom catalysts M 1 /2DMs could presented high 1,3-butadiene conversions. • Single-atom catalysts M 1 /2DMs could presented high 1-butene selectivity. • Ni 1 /GR and Ni 1 /BN are the ideal catalysts for 1,3-butadiene hydrogenation. Selective hydrogenating 1,3-butadiene to butene is an important tool for the removal of 1,3-butadiene which is a by-product of olefin production. Traditional noble metal catalysts are expensive and relatively low selective for 1-butene. In order to decrease the catalyst cost and improve the 1-butene selective, single-atom catalysts were designed by doping non-noble metals single atom (Pd, Ru, Fe, Co, Ni) on two-dimensional material carriers, hexagonal BN and graphene. It is found that 1,3-butadiene tends to be dominated by mono-π-adsorption on single-atom catalysts, resulting in dissociated H atom preferentially attack the one end C C bond of 1,3-butadiene. Unlike the metallic nanomaterials, low energy barriers for the hydrogenation of 1,3-butadiene to 1-butene were obtained (Ru 1 /BN: 0.20 eV, Fe 1 /GR: 0.23 eV, Co 1 /BN: 0.36 eV, Ru 1 /GR: 0.44 eV, Co 1 /GR: 0.59 eV, Ni 1 /GR: 0.61 eV, Ni 1 /BN: 0.62 eV). The 1-butene desorption energies are smaller than the further hydrogenation energy barriers on the Pd 1 /GR, Ni 1 /GR, Pd 1 /BN Co 1 /BN and Ni 1 /BN surfaces, which indicated better selectivity on these catalysts' surfaces. By contrast, Ni 1 /GR and Ni 1 /BN single-atom catalysts would be the best catalysts among all the studied catalyst in terms of adsorption energies of feed gas, dissociation ability of H 2 , hydrogenation energy barrier and 1-butene desorption energy. [ABSTRACT FROM AUTHOR]

[Display omitted] • The introduction of Ni/Cu lower the 1,3-butadiene hydrogenation energy barriers. • Higher butene selectivity could obtained on AgCuPd 2 and Ag 2 NiPd surfaces. • Cu is benefit of forming 2-butene and Ni is favorable of generating 1-butene. Selective hydrogenation of 1,3-butadiene to form butene is an important tool for the removal of 1,3-butadiene which is a by-product of olefin production. AgPd bimetallic catalysts improved the butene selective, but its expensive cost is still an urgent problem. In this study, we introduced a third inexpensive metal Ni or Cu to replace part of the noble metal Pd or Ag in a common AgPd catalyst and studied the influence of the introduction on the hydrogenation reaction by DFT. Compared with the Ag 3 Pd and AgPd 3 alloys, AgCuPd 2 and Ag 2 NiPd hardly changed the adsorption energy of 1,3-butadiene and hydrogen but lowered the butene adsorption energy, which indicates that the addition of Cu or Ni metals can improve the butene selectivity. By calculating the reaction pathways, it was found that the energy barriers of 1,3-butadiene hydrogenation to butene on AgCuPd 2 and Ag 2 NiPd was lower than that of Ag 3 Pd and AgPd 3 alloys, while the energy barriers of butene further hydrogenation to butane was much larger than the desorption energy of butene. The partial replacement of Ag or Pd atom of AgPd alloys with Cu or Ni not only reduces the catalyst cost but also improves the conversion and selectivity of the hydrogenation reaction. [ABSTRACT FROM AUTHOR]