Rational design of metal single-site embedded porous graphitic carbon nitride (P-g-C3N4) nanostructures exploiting maximum atom utilization is warranted to enhance the thermal CO oxidation (COOx) reaction. Herein, a facile, green, one-pot, and template-free approach is developed to fabricate the hierarchical porous P-g-C3N4-crumpled ultrathin nanosheets atomically doped with copper single atoms (Cu-P-g-C3N4). Mechanistically, the quick protonation of melamine and pyridine under acidic conditions induces deamination to form melem, which is polycondensed under heating. The interconnected pores, high surface area (240 m2g-1), and maximized exposed isolated Cu atomic active sites (1.8 wt %) coordinated with nitrogen atom P-g-C3N4 are the salient features of Cu- P-g-C3N4 that endowed complete conversion to CO2 at 184 °C. In contrast, P-g-C3N4 only converted 3.8% of CO even at 350 °C, implying the electronic effect of Cu single atoms. The abundant Cu-nitrogen moieties can drastically weaken the binding affinity of the CO-oxidation (COOx) intermediates and products, thus accelerating the reaction kinetics at a low temperature. This study may promote the fabrication of P-g-C3N4 doped with various single atoms for the oxidation of CO.

Center for Advanced Materials Qatar University Doha 2713 Qatar

Gas Processing Center College of Engineering Qatar University Doha 2713 Qatar

Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute Palacky University Slechtitelu 27 Olomouc 783 71 Czech Republic

SESAME Synchrotron King Hussein Bin Talal St Box 7 Allan 19252 Jordan

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