Impact of interannual and multidecadal trends on methane-climate feedbacks and sensitivity.

We estimate the causal contributions of spatiotemporal changes in temperature (T) and precipitation (Pr) to changes in Earth's atmospheric methane concentration (CCH4) and its isotope ratio δ13CH4 over the last four decades. We identify oscillations between positive and negative feedbacks, showing that both contribute to increasing CCH4. Interannually, increased emissions via positive feedbacks (e.g. wetland emissions and wildfires) with higher land surface air temperature (LSAT) are often followed by increasing CCH4 due to weakened methane sink via atmospheric •OH, via negative feedbacks with lowered sea surface temperatures (SST), especially in the tropics. Over decadal time scales, we find alternating rate-limiting factors for methane oxidation: when CCH4 is limiting, positive methane-climate feedback via direct oceanic emissions dominates; when •OH is limiting, negative feedback is favoured. Incorporating the interannually increasing CCH4 via negative feedbacks gives historical methane-climate feedback sensitivity ≈ 0.08 W m-2 °C-1, much higher than the IPCC AR6 estimate.

Pt-decorated PdFe nanoparticles as methanol-tolerant oxygen reduction electrocatalyst.

The activity and selectivity of carbon-supported Pt-decorated PdFe nanoparticles in the oxygen reduction reaction (ORR) were investigated in the presence and absence of methanol. The Pt-decorated PdFe nanoparticles, which consist of a PdPt surface and a PdFe interior, were prepared by the galvanic reaction between PdFe/C alloy nanoparticles and PtCl4(2-) in aqueous solution. The presence of a Pt-enriched surface after the replacement reaction was independently confirmed by several microstructural characterization techniques and cyclic voltammetry. The catalyst with such heterogeneous architecture is catalytically more active than a bulk PdFePt alloy catalyst with the same overall composition. The observed enhancements in catalyst performance can be attributed to the lattice strain effect between the shell and core components. The Pt-decorated PdFe (PdFe@PdPt/C) catalyst also compares favorably with a commercial Pt/C catalyst with four times as much Pt in terms of ORR activity, cost, and methanol tolerance.