The CatMath: an online predictive platform for thermal + electrocatalysis

The catalytic volcano activity models are the quantified and visualized tools of the Sabatier principle for heterogeneous catalysis, which can depict the intrinsic activity optima and trends of a catalytic reaction as a function of the reaction descriptors, i.e., the bonding strengths of key reaction species. These models can be derived by microkinetic modeling and/or free energy changes in combination with the scaling relations among the reaction intermediates. Herein, we introduce the CatMath—an online platform for generating a variety of common and industrially important thermal + electrocatalysis. With the CatMath, users can request the volcano models for available reactions and analyze their materials of interests as potential catalysts. Besides, the CatMath provides the function of the online generation of Surface Pourbaix Diagram for surface state analysis under electrocatalytic conditions, which is an essential step before analyzing the activity of an electrocatalytic surface. All the model generation and analysis processes are realized by cloud computing via a user-friendly interface.

Axial coordination regulation of MOF-based single-atom Ni catalysts by halogen atoms for enhanced CO_(2) electroreduction

Single-atom catalysts(SACs),with the utmost atom utilization,have attracted extensive interests for various catalytic applications.The coordination environment of SACs has been recognized to play a vital role in catalysis while their precise regulation at atomic level remains an immense challenge.Herein,a post metal halide modification(PMHM)strategy has been developed to construct Ni-N4 sites with axially coordinated halogen atoms,named Ni1-N-C(X)(X=CI,Br,and I),on pre-synthetic nitrogen-doped carbon derived from metal-organic frameworks.The axial halogen atoms with distinct electronegativity can break the symmetric charge distribution of planar Ni-N4 sites and regulate the electronic states of central Ni atoms in Ni1-N-C(X)(X=Cl,Br,and I).Significantly,the Ni1-N-C(CI)catalyst,decorated with the most electronegative Cl atoms,exhibits Faradaic efficiency of CO up to 94.7%in electrocatalytic CO_(2) reduction,outperforming Ni1-N-C(Br)and Ni1-N-C(I)catalysts.Moreover,Ni1-N-C(CI)also presents superb performance in Zn-CO_(2) battery with ultrahigh CO selectivity and great durability.Theoretical calculations reveal that the axially coordinated Cl atom remarkably facilitates*COOH intermediate formation on single-atom Ni sites,thereby boosting the CO_(2) reduction performance of Ni1-N-C(CI).This work offers a facile strategy to tailor the axial coordination environments of SACs at atomic level and manifests the crucial role of axial coordination microenvironments in catalysis.