Conspectus Due to increasing worldwide fossil fuel consumption, carbon dioxide levels have increased in the atmosphere with increasingly important impacts on the environment. Renewable and clean sources of energy have been proposed, including wind and solar, but they are intermittent and require efficient and scalable energy storage technologies. Electrochemical CO2 reduction reaction (CO2RR) provides a valuable approach in this area. It combines solar- or wind-generated electrical production with energy storage in the chemical bonds of carbon-based fuels. It can provide ways to integrate carbon capture, utilization, and storage in energy cycles while maintaining controlled levels of atmospheric CO2. Electrochemistry allows for the utilization of an electrical input to drive chemical reactions. Because CO2 is kinetically inert, highly active catalysts are required to decrease reaction barriers sufficiently so that reaction rates can be achieved that are sufficient for electrochemical CO2 reduction. Given the reaction barriers associated with multiple electron–proton reduction of CO2 to CO, formaldehyde (HC­(O)­H), formic acid, or formate (HC­(O)­OH, HC­(O)­O–), or more highly reduced forms of carbon, there is also a demand for high selectivity in catalysis. Catalysts that have been explored include homogeneous catalysts in solution, catalysts immobilized on surfaces, and heterogeneous catalysts. In homogeneous catalysis, reduction occurs following diffusion of the catalyst to an electrode where multiple proton coupled electron transfer reduction occurs. Useful catalysts in this area are typically transition-metal complexes with organic ligands and electron transfer properties that utilize combinations of metal and ligand redox levels. As a way to limit the amount of catalyst, in device-like configurations, catalysts are added to the surfaces of conductive substrates by surface binding, in polymeric films, or on carbon electrode surfaces with molecular structures and electronic configurations related to catalysts in solution. Immobilized, homogeneous catalysts can suffer from performance losses and even decomposition during long-term CO2 reduction cycles, but they are amenable to detailed mechanistic investigations. In parallel efforts, heterogeneous nanocatalysts have been explored in detail with the development of facile synthetic procedures that can offer highly active catalytic surface areas. Their high activity and stability have attracted a significant level of investigation, including possible exploitation for large-scale applications. However, translation of catalytic reactivity to the surface creates a new reactivity environment and complicates the elucidation of mechanistic details and identification of the active site in exploring reaction pathways. Here, the results of previous studies based on transition-metal complex catalysts for CO2 electroreduction are summarized. Early studies showed that transition-metal complexes of Ru, Ir, Rh, and Os, with well-defined structures, are all capable of catalyzing...

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Abstract. The Scenario Model Intercomparison Project (ScenarioMIP) defines and coordinates the main set of future climate projections, based on concentration-driven simulations, within the Coupled Model Intercomparison Project phase 6 (CMIP6). This paper presents a range of its outcomes by synthesizing results from the participating global coupled Earth system models. We limit our scope to the analysis of strictly geophysical outcomes: mainly global averages and spatial patterns of change for surface air temperature and precipitation. We also compare CMIP6 projections to CMIP5 results, especially for those scenarios that were designed to provide continuity across the CMIP phases, at the same time highlighting important differences in forcing composition, as well as in results. The range of future temperature and precipitation changes by the end of the century (2081–2100) encompassing the Tier 1 experiments based on the Shared Socioeconomic Pathway (SSP) scenarios (SSP1-2.6, SSP2-4.5, SSP3-7.0 and SSP5-8.5) and SSP1-1.9 spans a larger range of outcomes compared to CMIP5, due to higher warming (by close to 1.5 ∘C) reached at the upper end of the 5 %–95 % envelope of the highest scenario (SSP5-8.5). This is due to both the wider range of radiative forcing that the new scenarios cover and the higher climate sensitivities in some of the new models compared to their CMIP5 predecessors. Spatial patterns of change for temperature and precipitation averaged over models and scenarios have familiar features, and an analysis of their variations confirms model structural differences to be the dominant source of uncertainty. Models also differ with respect to the size and evolution of internal variability as measured by individual models' initial condition ensemble spreads, according to a set of initial condition ensemble simulations available under SSP3-7.0. These experiments suggest a tendency for internal variability to decrease along the course of the century in this scenario, a result that will benefit from further analysis over a larger set of models. Benefits of mitigation, all else being equal in terms of societal drivers, appear clearly when comparing scenarios developed under the same SSP but to which different degrees of mitigation have been applied. It is also found that a mild overshoot in temperature of a few decades around mid-century, as represented in SSP5-3.4OS, does not affect the end outcome of temperature and precipitation changes by 2100, which return to the same levels as those reached by the gradually increasing SSP4-3.4 (not erasing the possibility, however, that other aspects of the system may not be as easily reversible). Central estimates of the time at which the ensemble means of the different scenarios reach a given warming level might be biased by the inclusion of models that have shown faster warming in the historical period than the observed. Those estimates show all scenarios reaching 1.5 ∘C of warming compared to the 1850–1900 baseline in the second half of the current decade, with the time span between slow and fast warming covering between 20 and 27 years from present. The warming level of 2 ∘C of warming is reached as early as 2039 by the ensemble mean under SSP5-8.5 but as late as the mid-2060s under SSP1-2.6. The highest warming level considered (5 ∘C) is reached by the ensemble mean only under SSP5-8.5 and not until the mid-2090s.

In this study, the effect of the tropical North Atlantic (TNA) sea surface temperature (SST) variation in inducing the circulation anomaly in the Indo-East Asian monsoon (IEAM) region is investigated through the observational analysis and numerical modeling. The observational analysis shows that the TNA summer SST is positively correlated with the preceding winter Niño3 SST and is simultaneously correlated with the circulation in the IEAM region. The simultaneous circulation pattern resembles that of the ENSO-decaying summer. The positive correlation between the TNA SST and the Niño3 region SST is primarily ascribed to the surface latent heat flux and short wave radiation anomalies induced by the ENSO teleconnection. Coupled general circulation model experiments show that, while including the air-sea coupling in the Atlantic, the model can reproduce the main features of the IEAM circulation, such as an anomalous anticyclone over the western North Pacific (WNP) and southerly anomalies over southeast China. While the climatological Atlantic SST is prescribed, the circulation over the WNP displays a significantly different pattern, with an eastward migration of the WNP anticyclone and the associated northerly anomalies over southeast China. It is argued that anticyclonic shear and Ekman divergence associated with the atmospheric Kelvin wave response to the TNA warm SSTA forcing is the primary mechanism for the generation of the anomalous anticyclone in WNP. The results presented in this study provide a teleconnection pattern between TNA and short-term climate variability in IEAM region. ENSO, Indian monsoon, East Asian monsoon, western North Pacific anticyclone, Atlantic Citation:Rong X Y, Zhang R H, Li T. Impacts of Atlantic sea surface temperature anomalies on Indo-East Asian summer monsoon-ENSO relationship.

The amplitude asymmetry between El Niñ o and La Niñ a is investigated by diagnosing the mixed-layer heat budget during the ENSO developing phase by using the three ocean assimilation products: Simple Ocean Data Assimilation (SODA) 2.0.2, SODA 1.4.2, and the Global Ocean Data Assimilation System (GODAS). It is found that the nonlinear zonal and meridional ocean temperature advections are essential to cause the asymmetry in the far eastern Pacific, whereas the vertical nonlinear advection has the opposite effect. The zonal current anomaly is dominated by the geostrophic current in association with the thermocline depth variation. The meridional current anomaly is primarily attributed to the Ekman current driven by wind stress forcing. The resulting induced anomalous horizontal currents lead to warm nonlinear advection during both El Niñ o and La Niñ a episodes and thus strengthen (weaken) the El Niñ o (La Niñ a) amplitude. The convergence (divergence) of the anomalous geostrophic mixed-layer currents during El Niñ o (La Niñ a) results in anomalous downwelling (upwelling) in the far eastern equatorial Pacific, which leads to a cold nonlinear vertical advection in both warm and cold episodes.

A theory is developed in a stochastic climate model for understanding the general features of the seasonal predictability barrier (PB), which is characterized by a band of maximum decline in autocorrelation function phase-locked to a particular season. Our theory determines the forcing threshold, timing, and intensity of the seasonal PB as a function of the damping rate and seasonal forcing. A seasonal PB is found to be an intrinsic feature of a stochastic climate system forced by either seasonal growth rate or seasonal noise forcing. A PB is generated when the seasonal forcing, relative to the damping rate, exceeds a modest threshold. Once generated, all the PBs occur in the same calendar month, forming a seasonal PB. The PB season is determined by the decline of the seasonal forcing as well as the delayed response associated with damping. As such, for a realistic weak damping, the PB season is locked close to the minimum SST variance under the seasonal growth-rate forcing, but after the minimum SST variance under the seasonal noise forcing. The intensity of the PB is determined mainly by the amplitude of the seasonal forcing. The theory is able to explain the general features of the seasonal PB of the observed SST variability over the world. In the tropics, a seasonal PB is generated mainly by a strong seasonal growth rate, whereas in the extratropics a seasonal PB is generated mainly by a strong seasonal noise forcing. Our theory provides a general framework for the understanding of the seasonal PB of climate variability.

Electrification is a potential approach to decarbonizing the chemical industry. Electrochemical processes, when they are powered by renewable electricity, have lower carbon footprints in comparison to conventional thermochemical routes. In this Perspective, we discuss the potential electrochemical routes for chemical production and provide our views on how electrochemical processes can be matured in academic research laboratories for future industrial applications. We first analyze the CO 2 emission in the manufacturing industry and conduct a survey of state of the art electrosynthesis methods in the three most emission-intensive areas: petrochemical production, nitrogen compound production, and metal smelting. Then, we identify the technical bottlenecks in electrifying chemical productions from both chemistry and engineering perspectives and propose potential strategies to tackle these issues. Finally, we provide our views on how electrochemical manufacturing can reduce carbon emissions in the chemical industry with the hope to inspire more research efforts in electrifying chemical manufacturing.

Electrifying chemical manufacturing using renewable energy is an attractive approach to reduce the dependence on fossil energy sources in chemical industries. Primary amines are important organic building blocks; however, the synthesis is often hindered by the poor selectivity because of the formation of secondary and tertiary amine byproducts. Herein, we report an electrocatalytic route to produce ethylamine selectively through an electroreduction of acetonitrile at ambient temperature and pressure. Among all the electrocatalysts, Cu nanoparticles exhibit the highest ethylamine Faradaic efficiency (~96%) at −0.29 V versus reversible hydrogen electrode. Under optimal conditions, we achieve an ethylamine partial current density of 846 mA cm−2. A 20-hour stable performance is demonstrated on Cu at 100 mA cm−2 with an 86% ethylamine Faradaic efficiency. Moreover, the reaction mechanism is investigated by computational study, which suggests the high ethylamine selectivity on Cu is due to the moderate binding affinity for the reaction intermediates.