In:
Nature Communications, Springer Science and Business Media LLC, Vol. 11, No. 1 ( 2020-08-25)
Kurzfassung:
As a promising hydrogen carrier, formic acid (HCOOH) is renewable, safe and nontoxic. Although noble-metal-based catalysts have exhibited excellent activity in HCOOH dehydrogenation, developing non-noble-metal heterogeneous catalysts with high efficiency remains a great challenge. Here, we modulate oxygen coverage on the surface of Ti 3 C 2 T x MXenes to boost the catalytic activity toward HCOOH dehydrogenation. Impressively, Ti 3 C 2 T x MXenes after treating with air at 250 °C (Ti 3 C 2 T x -250) significantly increase the amount of surface oxygen atoms without the change of crystalline structure, exhibiting a mass activity of 365 mmol·g −1 ·h −1 with 100% of selectivity for H 2 at 80 °C, which is 2.2 and 2.0 times that of commercial Pd/C and Pt/C, respectively. Further mechanistic studies demonstrate that HCOO* is the intermediate in HCOOH dehydrogenation over Ti 3 C 2 T x MXenes with different coverages of surface oxygen atoms. Increasing the oxygen coverage on the surface of Ti 3 C 2 T x MXenes not only promotes the conversion from HCOO* to CO 2 * by lowering the energy barrier, but also weakens the adsorption energy of CO 2 and H 2 , thus accelerating the dehydrogenation of HCOOH.
Materialart:
Online-Ressource
ISSN:
2041-1723
DOI:
10.1038/s41467-020-18091-7
Sprache:
Englisch
Verlag:
Springer Science and Business Media LLC
Publikationsdatum:
2020
ZDB Id:
2553671-0
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