Enhanced CO₂ Reduction on a Cu-Decorated Single-Atom Catalyst via an Inverse Sandwich M-Graphene-Cu Structure

Su, Jingnan1; Yu, Linke1,2; Han, Bing1,3; Li, Fengyu1; Chen, Zhongfang4; Zeng, Xiao Cheng5

2024-08-01

10.1021/acs.jpclett.4c01858

JOURNAL OF PHYSICAL CHEMISTRY LETTERS   影响因子和分区

1948-7185

The highly active and selective electrochemical CO2 reduction reaction (CO2RR) can be exploited to produce valuable chemicals and fuels and is also crucial for achieving clean energy goals and environmental remediation. Decorated single-atom catalysts (D-SACs), which feature synergistic interactions between the active metal site (M) and an axially decorated ligand, have been extensively explored for the CO2RR. Very recently, novel double-atom catalysts (DACs) featuring inverse sandwich structures were theoretically proposed and identified as promising CO2RR electrocatalysts. However, the experimental synthesis of DACs remains a challenge. To facilitate the fabrication and to realize the potential of these novel DACs, we designed a D-SAC system, denoted as M-1@gra+Cu-slab. This system features a graphene layer with a vacancy-anchored SAC, all stacked on a Cu(111) surface, thereby embodying a Cu slab-supported inverse sandwich M-graphene-Cu structure. Using density functional theory calculations, we evaluated the stability, selectivity, and activity of 27 M-1@gra+Cu-slab systems (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Ru, Rh, Pd, Ag, Cd, Hf, Ta, W, Re, Os, Ir, Pt, or Au) and showed five M-1@gra+Cu-slab (M = Co, Ni, Cu, Rh, or Pd) systems exhibit optimal characteristics for the CO2RR and can potentially outperform their SAC and DAC counterparts. This study offers a new strategy for developing highly efficient CO2RR D-SACs with an inverse sandwich structural moiety.

SCI ; EI

英语

其他

National Natural Science Foundation of China[12364038] ; Grassland Talents project of Inner Mongolia autonomous region[12000-12102613] ; Young science and technology talents cultivation project of Inner Mongolia University[21200-5223708] ; Department of Energy, Office of Basic Energy Sciences[DE-SC0023418] ; Hong Kong Global STEM Professor Scheme and a Guangdong Mianshang grant[2024A1515012307]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:001292276400001

AMER CHEMICAL SOC

Web of Science

1.Inner Mongolia Univ, Sch Phys Sci & Technol, Hohhot 010021, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518000, Peoples R China
3.Ordos Inst Appl Technol, Ordos 017000, Peoples R China
4.Univ Puerto Rico, Dept Chem, San Juan, PR 00931 USA
5.City Univ Hong Kong, Dept Mat Sci & Engn, Hong Kong 999077, Peoples R China

Su, Jingnan,Yu, Linke,Han, Bing,et al. Enhanced CO₂ Reduction on a Cu-Decorated Single-Atom Catalyst via an Inverse Sandwich M-Graphene-Cu Structure[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2024.

Su, Jingnan,Yu, Linke,Han, Bing,Li, Fengyu,Chen, Zhongfang,&Zeng, Xiao Cheng.(2024).Enhanced CO₂ Reduction on a Cu-Decorated Single-Atom Catalyst via an Inverse Sandwich M-Graphene-Cu Structure.JOURNAL OF PHYSICAL CHEMISTRY LETTERS.

Su, Jingnan,et al."Enhanced CO₂ Reduction on a Cu-Decorated Single-Atom Catalyst via an Inverse Sandwich M-Graphene-Cu Structure".JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2024).