Proton-Coupled Electron Transfer on Cu(2)O/Ti(3)C(2)T(x) MXene for Propane (C(3)H(8)) Synthesis from Electrochemical CO(2) Reduction

利用Cu₂O/Ti₃C₂Tₓ MXene上的质子耦合电子转移,通过电化学CO₂还原合成丙烷(C₃H₈)

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Abstract

Electrochemical CO(2) reduction reaction (CO(2)RR) to produce value-added multi-carbon chemicals has been an appealing approach to achieving environmentally friendly carbon neutrality in recent years. Despite extensive research focusing on the use of CO(2) to produce high-value chemicals like high-energy-density hydrocarbons, there have been few reports on the production of propane (C(3)H(8)), which requires carbon chain elongation and protonation. A rationally designed 0D/2D hybrid Cu(2)O anchored-Ti(3)C(2)T(x) MXene catalyst (Cu(2)O/MXene) is demonstrated with efficient CO(2)RR activity in an aqueous electrolyte to produce C(3)H(8). As a result, a significantly high Faradaic efficiency (FE) of 3.3% is achieved for the synthesis of C(3)H(8) via the CO(2)RR with Cu(2)O/MXene, which is ≈26 times higher than that of Cu/MXene prepared by the same hydrothermal process without NH(4)OH solution. Based on in-situ attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR) and density functional theory (DFT) calculations, it is proposed that the significant electrocatalytic conversion originated from the synergistic behavior of the Cu(2)O nanoparticles, which bound the *C(2) intermediates, and the MXene that bound the *CO coupling to the C(3) intermediate. The results disclose that the rationally designed MXene-based hybrid catalyst facilitates multi-carbon coupling as well as protonation, thereby manipulating the CO(2)RR pathway.

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