Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study

Ali, Sajjad2,5; Iqbal, Rashid1; Khan, Azim2; Rehman, Shafiq Ur3; Haneef, Muhammad4; Yin, Lichang2

2021-07-23

10.1021/acsanm.1c00959

ACS Applied Nano Materials   影响因子和分区

2574-0970

As an essential component of single-atom catalysts, support materials determine the dispersion, utilization, and stability of single metal atoms. Here, we reported the potential of defective and doped graphene as a single-atom catalyst (SAC) support for CO2 conversion to formic acid by hydrogenation. The support effect was screened based on the stability of a single-metal atom. Our calculation revealed that Cu, Pd, and Ru supported on defective graphene with monovacancy (m-VacG) have higher adsorption energy than the cohesive energy of their bulk counterparts; therefore we selected Cu, Pd, and Ru supported on m-VacG as potential SACs to examine the catalytic reaction. The stability and reactivity of SACs/ m-VacG were uncovered by molecular dynamics (MD) simulations, migration barrier calculation, and electronic structure analysis. The reaction of CO2 hydrogenation proceeds through two pathways starting from different initial states, i.e., the coadsorption of H-2 and CO2 on SACs/m-VacG (path A) and H-2 adsorption on SACs/m-VacG (path B). From the reaction pathways analysis, it is found that path B dominates the entire reaction thermodynamically with lower energy barrier compared with path A. Moreover, Pd supported on m-VacG is predicted to be the highest active SAC with the lowest energy barrier along the reaction path.

single-atom catalysts doped and defective carbon CO2 hydrogenation formic acid density functional theory

SCI ; EI

英语

通讯

National Natural Science Foundation of China (NSFC)[51972312]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000677582900040

AMER CHEMICAL SOC

20212910656689

Atoms ; Calculations ; Carbon dioxide ; Catalysis ; Catalysts ; Defects ; Electronic structure ; Energy barriers ; Formic acid ; Graphene ; Hydrogenation ; Molecular dynamics ; Ruthenium ; Stability

Precious Metals:547.1 ; Nanotechnology:761 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Mathematics:921 ; Atomic and Molecular Physics:931.3 ; Materials Science:951

Web of Science

1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Hazara Univ, Dept Phys, Mansehra 21300, Pakistan
5.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China

Ali, Sajjad,Iqbal, Rashid,Khan, Azim,et al. Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study[J]. ACS Applied Nano Materials,2021,4(7):6893-6902.

Ali, Sajjad,Iqbal, Rashid,Khan, Azim,Rehman, Shafiq Ur,Haneef, Muhammad,&Yin, Lichang.(2021).Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study.ACS Applied Nano Materials,4(7),6893-6902.

Ali, Sajjad,et al."Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study".ACS Applied Nano Materials 4.7(2021):6893-6902.