Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation

Tingting Hou, Qiquan Luo, Qi Li, Hualu Zu, Peixin Cui, Siwei Chen, Yue Lin (), Jiajia Chen, Xusheng Zheng, Wenkun Zhu, Shuquan Liang, Jinlong Yang () and Liangbing Wang ()
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Tingting Hou: Central South University
Qiquan Luo: Anhui University
Qi Li: Central South University
Hualu Zu: Central South University
Peixin Cui: the Chinese Academy of Sciences
Siwei Chen: Central South University
Yue Lin: University of Science and Technology of China
Jiajia Chen: University of Science and Technology of China
Xusheng Zheng: University of Science and Technology of China
Wenkun Zhu: Southwest University of Science and Technology
Shuquan Liang: Central South University
Jinlong Yang: University of Science and Technology of China
Liangbing Wang: Central South University

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract 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 Ti3C2Tx MXenes to boost the catalytic activity toward HCOOH dehydrogenation. Impressively, Ti3C2Tx MXenes after treating with air at 250 °C (Ti3C2Tx-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 H2 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 Ti3C2Tx MXenes with different coverages of surface oxygen atoms. Increasing the oxygen coverage on the surface of Ti3C2Tx MXenes not only promotes the conversion from HCOO* to CO2* by lowering the energy barrier, but also weakens the adsorption energy of CO2 and H2, thus accelerating the dehydrogenation of HCOOH.

Date: 2020
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DOI: 10.1038/s41467-020-18091-7

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