Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h−1 among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions.

As the electron transfer to CO2 is a critical step in the activation of CO2 , it is of significant importance to engineer the electronic properties of CO2 hydrogenation catalysts to enhance their activity. Herein, we prepared Pt3 Co nanocrystals with improved catalytic performance towards CO2 hydrogenation to methanol. Pt3 Co octapods, Pt3 Co nanocubes, Pt octapods, and Pt nanocubes were tested, and the Pt3 Co octapods achieved the best catalytic activity. Both the presence of multiple sharp tips and charge transfer between Pt and Co enabled the accumulation of negative charges on the Pt atoms in the vertices of the Pt3 Co octapods. Moreover, infrared reflection absorption spectroscopy confirmed that the high negative charge density at the Pt atoms in the vertices of the Pt3 Co octapods promotes the activation of CO2 and accordingly enhances the catalytic activity.

As the electron transfer to CO2 is a critical step in the activation of CO2, it is of significant importance to engineer the electronic properties of CO2 hydrogenation catalysts to enhance their activity. Herein, we prepared Pt3Co nanocrystals with improved catalytic performance towards CO2 hydrogenation to methanol. Pt3Co octapods, Pt3Co nanocubes, Pt octapods, and Pt nanocubes were tested, and the Pt3Co octapods achieved the best catalytic activity. Both the presence of multiple sharp tips and charge transfer between Pt and Co enabled the accumulation of negative charges on the Pt atoms in the vertices of the Pt3Co octapods. Moreover, infrared reflection absorption spectroscopy confirmed that the high negative charge density at the Pt atoms in the vertices of the Pt3Co octapods promotes the activation of CO2 and accordingly enhances the catalytic activity.

Marine heatwaves (MHWs) can cause various adverse effects on marine ecosystems associated with complicated social ramifications. It has been well established that the gradually rising sea surface temperature (SST) due to anthropogenic carbon emission will cause an increase of the MHW duration and intensity. However, for species with strong adaptation capacity or mobility, MHW changes due to the altered SST variability under greenhouse warming are more crucial but so far remain poorly assessed. Under the high carbon emission scenario, we show that the cumulative duration (intensity) of MHWs, with the effect of secular SST increase excluded, is projected to be 60% (100%) higher by the end of this century than in the 1990s due to an amplified SST seasonal cycle. This increase becomes more evident for stronger MHWs, reaching up to 8 (30) folds for the extreme MHW category. The amplified SST seasonal cycle also causes pronounced seasonality of MHWs, making them more active in summer-autumn than winter-spring. Our results suggest that MHWs are likely to have increasingly devastating impacts on a wide range of marine species in the future without taking effective steps for carbon emission reduction.