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Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation
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Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation
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Journal Article
Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation
2020
Overview
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.
Developing non-noble-metal heterogeneous catalysts with high efficiency in HCOOH dehydrogenation is significant for the acquisition of hydrogen, but remains a great challenge. Here, the authors modulate oxygen coverage of Ti
3
C
2
T
x
MXenes to boost the catalytic activity toward HCOOH dehydrogenation.
