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@ARTICLE{Agharezaei:1024354,
      author       = {Agharezaei, Parastoo and Tomohiro, Noguchi Goroh and
                      Kobayashi, Hirokazu and Schlenz, Hartmut and Yamauchi, Miho
                      and Ghuman, Kulbir Kaur},
      title        = {{U}nraveling the {E}nhanced {N} 2 {A}ctivity on {C}u{N}i
                      {A}lloy {C}atalysts for {A}mmonia {P}roduction:
                      {E}xperiments, {DFT}, and {S}tatistical {A}nalysis},
      journal      = {The journal of physical chemistry / C},
      volume       = {128},
      number       = {9},
      issn         = {1932-7447},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {FZJ-2024-02110},
      pages        = {3703 - 3717},
      year         = {2024},
      abstract     = {One of the main challenges in designing catalysts for
                      ammonia synthesis is tocreate active sites on the surface of
                      the catalyst that prefers to reduce the strong N2
                      moleculedespite its highly stable structure. Binary alloys
                      have been demonstrated as potential ammoniasynthesis
                      catalysts in the literature. However, for binary alloys to
                      be commercially viable, oneneeds to improve their catalytic
                      activity for N2 reduction by strategically manipulating
                      theseveral unique active sites present on their surface.
                      Herein, by using computational tools, wecreated five
                      different compositions of CuxNi1−x (0.5 ≤ x ≤ 0.9)
                      alloys via special quasi-randomstructure (SQS) and genetic
                      algorithm (GA). The alloy with about $50\%$ of Cu and $50\%$
                      of Ni ispredicted to have the highest catalytic activity
                      based on the shift of the d-band center towardthe Fermi
                      level. We then synthesized MgO-supported Cu0.5Ni0.5
                      nanoparticles and comparedtheir activity for ammonia
                      synthesis with that of Ni/MgO and Cu/MgO. It was found that
                      theMgO-supported Cu0.5Ni0.5 alloy possesses 21 times higher
                      activity than Cu/MgO and 3 timeshigher than Ni/MgO for
                      ammonia synthesis, confirming the computational results.
                      Todemonstrate the impact of alloying on the catalytic
                      activity, we further investigated all thepossible unique
                      sites on the surface of the Cu0.5Ni0.5 alloy for nitrogen
                      reduction reaction (NRR) via density functional theory(DFT).
                      The investigation of the 96 unique active sites on the
                      Cu0.5Ni0.5 surface demonstrated that the position and
                      concentration ofNi atoms near each investigated adsorption
                      site have a linear correlation with the adsorption energy of
                      the N2. Along with thestructural and electronic properties
                      of the active sites modified by Ni, orientation of the N2
                      molecule also plays an important role indetermining the
                      activity of the CuNi catalyst. These findings not only
                      explained the notable increase in the activity of CuNi
                      catalystscompared to the pure metals for NH3 synthesis but
                      also offered critical insights required to tailor the
                      specific surface environment ofCuNi catalysts for NRR. This
                      knowledge can serve as a foundation for further developments
                      in designing binary alloy catalysts forsustainable ammonia
                      synthesis.},
      cin          = {IEK-1},
      ddc          = {530},
      cid          = {I:(DE-Juel1)IEK-1-20101013},
      pnm          = {1232 - Power-based Fuels and Chemicals (POF4-123)},
      pid          = {G:(DE-HGF)POF4-1232},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:001173697100001},
      doi          = {10.1021/acs.jpcc.3c06417},
      url          = {https://juser.fz-juelich.de/record/1024354},
}