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Summary
Quantificationin the driving patterns of activity descriptorson structure-activity relationships and reaction mechanismsover heterogeneous catalysts is still a great challenge and needsto be addressed urgently. Herein, with the example of typical Mn-basedcatalysts, based on the activity regularity and many characterizations,the chemisorbed oxygen density (& rho;O& beta; ) and particle size (d TEM) have beenproposed as the two-dimensional descriptors for selective catalyticreduction of NO, whose role is in quantifying the contents of vacancydefects and the amounts of active sites located on terraces or interfaces,respectively. They can be utilized to construct and quantify the drivingpatterns for the structure-activity relationships and reactionmechanisms of NO reduction. As a consequence, a complementary modulationfor E a by & rho;O& beta; and d TEM is described quantitativelyin terms of the fitted functions. Moreover, based on the structure-activityrelationships and the quantification laws of in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS),the reaction efficiency (RE) of the specific combined NO x -intermediate is identified as the trigger to drivethe Langmuir-Hinshelwood mechanism and modulated by the descriptorscomplementally and collaboratively following the fitted quantificationfunctions. Either of the two descriptors at its lower values playsa dominant role in regulating E a and RE,and the dominant factor evolves progressively: d TEM & LRARR; coupling d TEM with & rho;O& beta; & LRARR; & rho;O& beta; , when the dependency of E a andRE on the descriptors is adopted to identify the dominant factor anddomains. Therefore, this work has quantitatively accounted for theessence of activity modulation and may provide insight into the quantitativedriving patterns for reaction activity and mechanism.
