Electrochemical reduction of CO2 provides an opportunity to produce fuels and chemicals in a carbon-neutral manner, assuming that CO2 can be captured from the atmosphere. To do so requires efficient, selective, and stable catalysts. In this study, we report a highly mesoporous metallic Cu catalyst prepared by electrochemical reduction of thermally nitrided Cu foil. Under aqueous saturated CO2 reduction conditions, the Cu3N-derived Cu electrocatalyst produces virtually no CH4, very little CO, and exhibits a faradaic efficiency of 68% in C2+ products (C2H4, C2H5OH, and C3H7OH) at a current density of ∼18.5 mA cm-2 and a cathode potential of -1.0 V versus the reversible hydrogen electrode. Under these conditions, the catalyst produces more oxygenated products than hydrocarbons. We show that surface roughness is a good descriptor of catalytic performance. The roughest surface reached 98% CO utilization efficiency for C2+ product formation from CO2 reduction and the ratio of oxygenated to hydrocarbon products correlates with the degree of surface roughness. These effects of surface roughness are attributed to the high population of undercoordinated sites as well as a high pH environment within the mesopores and adjacent to the surface of the catalyst.

We have investigated the role of surface roughening on the CO2 reduction reaction (CO2RR) over Cu. The activity and product selectivity of Cu surfaces roughened by plasma pretreatment in Ar, O2, or N2 were compared with that of electrochemically polished Cu samples. Differences in total and product current densities, the ratio of current densities for HER (the hydrogen evolution reaction) to CO2RR, and the ratio of current densities for C2+ to C1 products depend on the electrochemically active surface and are nearly independent of plasma composition. Theoretical analysis of an electropolished and roughened Cu surface reveals a higher fraction of undercoordinated Cu sites on the roughened surface, sites that bind CO preferentially. Roughened surfaces also contain square sites similar to those on a Cu(100) surface but with neighboring step sites, which adsorb OC-COH, a precursor to C2+ products. These findings explain the increases in the formation of oxygenates and hydrocarbons relative to CO and the ratio of oxygenates to hydrocarbons observed with increasing surface roughness.

Shifting electrochemical oxygen reduction towards 2e^- pathway to hydrogen peroxide (H₂O₂), instead of the traditional 4e^- to water, becomes increasingly important as a green method for H₂O₂ generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H₂O₂ catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm^-2 H₂O₂ current, and a high H₂O₂ selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e^-/4e^- ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e^-, are responsible for the H₂O₂ pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.

Electronic systems with flat bands are predicted to be a fertile ground for hosting emergent phenomena including unconventional magnetism and superconductivity 1–15 , but materials that manifest this feature are rare. Here, we use scanning tunnelling microscopy to elucidate the atomically resolved electronic states and their magnetic response in the kagome magnet Co 3 Sn 2 S 2 (refs. 16–20 ). We observe a pronounced peak at the Fermi level, which we identify as arising from the kinetically frustrated kagome flat band. On increasing the magnetic field up to ±8 T, this state exhibits an anomalous magnetization-polarized many-body Zeeman shift, dominated by an orbital moment that is opposite to the field direction. Such negative magnetism is induced by spin–orbit-coupling quantum phase effects 21–25 tied to non-trivial flat band systems. We image the flat band peak, resolve the associated negative magnetism and provide its connection to the Berry curvature field, showing that Co 3 Sn 2 S 2 is a rare example of a kagome magnet where the low-energy physics can be dominated by the spin–orbit-coupled flat band.

Marked evolution of properties with minute changes in the doping level is a hallmark of the complex chemistry that governs copper oxide superconductivity as manifested in the celebrated superconducting domes and quantum criticality taking place at precise compositions^1-4. The strange-metal state, in which the resistivity varies linearly with temperature, has emerged as a central feature in the normal state of copper oxide superconductors^5-9. The ubiquity of this behaviour signals an intimate link between the scattering mechanism and superconductivity^10-12. However, a clear quantitative picture of the correlation has been lacking. Here we report the observation of precise quantitative scaling laws among the superconducting transition temperature (T_c), the linear-in-T scattering coefficient (A₁) and the doping level (x) in electron-doped copper oxide La_2-xCe_xCuO₄ (LCCO). High-resolution characterization of epitaxial composition-spread films, which encompass the entire overdoped range of LCCO, has enabled us to systematically map its structural and transport properties with unprecedented accuracy and with increments of Δx = 0.0015. We have uncovered the relations T_c ~ (x_c - x)^0.5 ~ (A₁^□)^0.5, where x_c is the critical doping in which superconductivity disappears and A₁^□ is the coefficient of the linear resistivity per CuO₂ plane. The striking similarity of the T_c versus A₁^□ relation among copper oxides, iron-based and organic superconductors may be an indication of a common mechanism of the strange-metal behaviour and unconventional superconductivity in these systems.

Superconducting materials exhibiting topological properties are emerging as an exciting platform to realize fundamentally new excitations from topological quantum states of matter. In this letter, we explore the possibility of a field-free platform for generating Majorana zero energy excitations by depositing magnetic Fe impurities on the surface of candidate topological superconductors, LiFeAs and PbTaSe2. We use scanning tunneling microscopy to probe localized states induced at the Fe adatoms on the atomic scale and at sub-Kelvin temperatures. We find that each Fe adatom generates a striking zero-energy bound state inside the superconducting gap, which do not split in magnetic fields up to 8 T, underlining a nontrivial topological origin. Our findings point to magnetic Fe adatoms evaporated on bulk superconductors with topological surface states for exploring Majorana zero modes and quantum information science under field-free conditions.

Kagome-nets, appearing in electronic, photonic and cold-atom systems, host frustrated fermionic and bosonic excitations. However, it is rare to find a system to study their fermion-boson many-body interplay. Here we use state-of-the-art scanning tunneling microscopy/spectroscopy to discover unusual electronic coupling to flat-band phonons in a layered kagome paramagnet, CoSn. We image the kagome structure with unprecedented atomic resolution and observe the striking bosonic mode interacting with dispersive kagome electrons near the Fermi surface. At this mode energy, the fermionic quasi-particle dispersion exhibits a pronounced renormalization, signaling a giant coupling to bosons. Through the self-energy analysis, first-principles calculation, and a lattice vibration model, we present evidence that this mode arises from the geometrically frustrated phonon flat-band, which is the lattice bosonic analog of the kagome electron flat-band. Our findings provide the first example of kagome bosonic mode (flat-band phonon) in electronic excitations and its strong interaction with fermionic degrees of freedom in kagome-net materials.

The mammalian central nervous system (CNS) is considered an immune privileged system as it is separated from the periphery by the blood brain barrier (BBB). Yet, immune functions have been postulated to heavily influence the functional state of the CNS, especially after injury or during neurodegeneration. There is controversy regarding whether adaptive immune responses are beneficial or detrimental to CNS injury repair. In this study, we utilized immunocompromised SCID mice and subjected them to spinal cord injury (SCI). We analyzed motor function, electrophysiology, histochemistry, and performed unbiased RNA-sequencing. SCID mice displayed improved CNS functional recovery compared to WT mice after SCI. Weighted gene-coexpression network analysis (WGCNA) of spinal cord transcriptomes revealed that SCID mice had reduced expression of immune function-related genes and heightened expression of neural transmission-related genes after SCI, which was confirmed by immunohistochemical analysis and was consistent with better functional recovery. Transcriptomic analyses also indicated heightened expression of neurotransmission-related genes before injury in SCID mice, suggesting that a steady state of immune-deficiency potentially led to CNS hyper-connectivity. Consequently, SCID mice without injury demonstrated worse performance in Morris water maze test. Taken together, not only reduced inflammation after injury but also dampened steady-state immune function without injury heightened the neurotransmission program, resulting in better or worse behavioral outcomes respectively. This study revealed the intricate relationship between immune and nervous systems, raising the possibility for therapeutic manipulation of neural function via immune modulation.