In this section, you can access to the latest technical information related to the FUTURE project topic.

Unveiling the mechanism of controllable CO2 hydrogenation by group VIB metal single atom anchored on N-doped graphite: A density functional theory study

CO2 hydrogenation has raised considerable interest due to concerns about climate change. Realizing low-temperature reverse water gas shift (rWGS) reaction remains a significant challenge in the context of coupling it with the C?C growth reactions to convert CO2 to C2+ fuels. We carried out systematic DFT simulations to unveil the underlying low-temperature mechanism for the selective hydrogenation of CO2 to produce CO, over a variety of metal-based single atom catalysts (SACs) supported on the nitrogen-doped graphite. Group VIB metal-based SACs outperformed other 15 metal candidates in terms of versatile capacities in both selective activation of CO2 molecule and facilitating escaping of CO and H2O. Mo1/N3-Gt was especially outstanding by giving rise to spontaneous production of CO and O? through an effective electron injection into the CO2 molecule. Water formation has been identified as the potential rate-controlling step in such a catalytic reaction over Mo1/N3-Gt with an energy barrier of 1.10?eV. Herein, the H migration played a pivotal role and had tight affinity to the charge of H? on the active site of catalyst. The dynamic coordination environment of Mo?+ was revealed to be the dominant factor affecting the surface H? charge, leading to a variety of hydrogenation behaviors. The electron-deficient ligands of CO2 and O? on Mo1/N3-Gt, as well as additional adsorbed H2, were effective in adjusting the 4d and 5s electronic structure of central Mo and consequently resulted in nearly electric neutral surface H?s, thus most benefiting the hydrogenation process. The optimal charge of the coordinated Mo for an outstanding selective hydrogenation performance in this scenario was found to be no less than +1.7e.

» Author: Jiajun Zhang, Bin Yang, Kai Hong Luo

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