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Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction

Yang Li, Jun Li, Hao Yang, Bo Zhang, Zhiwen Zhou

Among all CO2 electroreduction products, methane (CH4) and ethylene (C2H4) are two typical and valuable hydrocarbon products which are formed in two different pathways: hydrogenation and dimerization reactions of the same CO intermediate. Theoretical studies show that the adsorption configurations of CO intermediate determine the reaction pathways towards CH4/C2H4. However, it is challenging to experimentally control the CO adsorption configurations at the catalyst surface, and thus the hydrocarbon selectivity is still limited. Herein, we seek to synthesize two well-defined copper nanocatalysts with controllable surface structures. The two model catalysts exhibit a high hydrocarbon selectivity toward either CH4 (83%) or C2H4 (93%) under identical reduction conditions. Scanning transmission electron microscopy and X-ray absorption spectroscopy characterizations reveal the low-coordination Cu-0 sites and local Cu-0/Cu+ sites of the two catalysts, respectively. CO-temperature programed desorption, in-situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory studies unveil that the bridge-adsorbed CO (COB) on the low-coordination Cu-0 sites is apt to be hydrogenated to CH4, whereas the bridge-adsorbed CO plus linear-adsorbed CO (COB + COL) on the local Cu-0/Cu+ sites are apt to be coupled to C2H4. Our findings pave a new way to design catalysts with controllable CO adsorption configurations for high hydrocarbon product selectivity. (C) 2020 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.

ELSEVIER2021

Evidence of a coupled electron-phonon liquid in NbGe2

Philip Johannes Walter Moll, Mathieu François Padlewski, Matthias Carsten Putzke, Hao Yang

Whereas electron-phonon scattering relaxes the electron's momentum in metals, a perpetual exchange of momentum between phonons and electrons may conserve total momentum and lead to a coupled electron-phonon liquid. Such a phase of matter could be a platform for observing electron hydrodynamics. Here we present evidence of an electron-phonon liquid in the transition metal ditetrelide, NbGe2, from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe2 with weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and standard Fermi liquid calculations. Third, Raman scattering shows anomalous temperature dependences of the phonon linewidths that fit an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential design principles for materials with coupled electron-phonon liquid. It was predicted that in the regime of strong electron-phonon interactions, electrons and phonons can form a coupled non-equilibrium state, characterized by the conservation of the total momentum and by hydrodynamic transport. Here, the authors report experimental evidence for such a coupled electron-phonon liquid in NbGe2.

NATURE PORTFOLIO2021

Quantum oscillations in the type-II Dirac semi-metal candidate PtSe2

Philip Johannes Walter Moll, Hao Yang

Three-dimensional topological semi-metals carry quasiparticle states that mimic massless relativistic Dirac fermions, elusive particles that have never been observed in nature. As they appear in the solid body, they are not bound to the usual symmetries of space-time and thus new types of fermionic excitations that explicitly violate Lorentz-invariance have been proposed, the so-called type-II Dirac fermions. We investigate the electronic spectrum of the transition-metal dichalcogenide PtSe2 by means of quantum oscillation measurements in fields up to 65 T. The observed Fermi surfaces agree well with the expectations from band structure calculations, that recently predicted a type-II Dirac node to occur in this material. A hole- and an electron-like Fermi surface dominate the semi-metal at the Fermi level. The quasiparticle mass is significantly enhanced over the bare band mass value, likely by phonon renormalization. Our work is consistent with the existence of type-II Dirac nodes in PtSe2, yet the Dirac node is too far below the Fermi level to support free Dirac-fermion excitations.

2018