Displacement of methane by coadsorbed carbon dioxide is facilitated in narrow carbon nanopores

By using simulation methods, we studied the adsorption of binary CO2-CH4 mixtures on various CH4 preadsorbed carbonaceous materials (e.g., triply periodic carbon minimal surfaces, slit-shaped carbon micropores, and Harris's virtual porous carbons) at 293 K. Regardless of the different micropore geometry, two-stage mechanism of CH4 displacement from carbon nanospaces by coadsorbed CO2 has been proposed. In the first stage, the coadsorbed CO2 molecules induced the enhancement of CH4 adsorbed amount. In the second stage, the stronger affinity of CO2 to flat/curved graphitic surfaces as well as CO2-CO2 interactions cause the displacement of CH4 molecules from carbonaceous materials. The operating conditions of CO2-induced cleaning of the adsorbed phase from CH4 mixture component strongly depend on the size of the carbon micropores, but, in general, the enhanced adsorption field in narrow carbon ultramicropores facilitates the nonreactive displacement of CH4 by coadsorbed CO2. This is because in narrow carbon ultramicropores the equilibrium CO2/CH4 selectivity (i.e., preferential adsorption toward CO2) increased significantly. The adsorption field in wider micropores (i.e., the overall surface energy) for both CO2 and CH4 is very similar, which decreases the preferential CO2 adsorption. This suppresses the displacement of CH4 by coadsorbed CO2 and assists further adsorption of CH4 from the bulk mixture (i.e., CO2/CH4 mixing in adsorbed phase).

A Possible Change in Mass Balance of Greenland and Antarctic Ice Sheets in the Coming Century

A high-resolution GCM is found to simulate precipitation and surface energy balance of high latitudes with high accuracy. This opens new possibilities to investigate the future mass balance of polar glaciers and its effect on sea level. The surface mass balance of the Greenland and the Antarctic ice sheets is simulated using the ECHAM3 GCM with TI06 horizontal resolution. With this model, two 5-year integrations for the present and doubled carbon dioxide conditions based on the boundary conditions provided by the ECHAM1/T21 transient experiment have been conducted. A comparison of the two experiments over Greenland and Antarctica shows to what extent the effect of climate change on the mass balance on the two largest glaciers of the world can differ. On Greenland one sees a slight decrease in accumulation and a substantial increase in melt, while on Antarctica a large increase in accumulation without melt is projected. Translating the mass balances into terms of sea-level equivalent. the Greenland discharge causes a sea level rise of 1.1 mm yr−1, while the accumulation on Antarctica tends to lower it by 0.9 mm yr−1. The change in the combined mass balance of the two continents is almost zero. The sea level change of the next century can be affected more effectively by the thermal expansion of seawater and the mass balance of smaller glaciers outside of Greenland and Antarctica.

Impact of anthropogenic heat emissions on London's temperatures

We investigate the role of the anthropogenic heat flux on the urban heat island of London. To do this, the time-varying anthropogenic heat flux is added to an urban surface-energy balance parametrization, the Met Office–Reading Urban Surface Exchange Scheme (MORUSES), implemented in a 1 km resolution version of the UK Met Office Unified Model. The anthropogenic heat flux is derived from energy-demand data for London and is specified on the model's 1 km grid; it includes variations on diurnal and seasonal time-scales. We contrast a spring case with a winter case, to illustrate the effects of the larger anthropogenic heat flux in winter and the different roles played by thermodynamics in the different seasons. The surface-energy balance channels the anthropogenic heat into heating the urban surface, which warms slowly because of the large heat capacity of the urban surface. About one third of this additional warming goes into increasing the outgoing long-wave radiation and only about two thirds goes into increasing the sensible heat flux that warms the atmosphere. The anthropogenic heat flux has a larger effect on screen-level temperatures in the winter case, partly because the anthropogenic flux is larger then and partly because the boundary layer is shallower in winter. For the specific winter case studied here, the anthropogenic heat flux maintains a well-mixed boundary layer through the whole night over London, whereas the surrounding rural boundary layer becomes strongly stably stratified. This finding is likely to have important implications for air quality in winter. On the whole, inclusion of the anthropogenic heat flux improves the comparison between model simulations and measurements of screen-level temperature slightly and indicates that the anthropogenic heat flux is beginning to be an important factor in the London urban heat island.

Trade-offs and responsiveness of the single-layer urban canopy parametrization in WRF: an offline evaluation using the MOSCEM optimization algorithm and field observations

For an increasing number of applications, mesoscale modelling systems now aim to better represent urban areas. The complexity of processes resolved by urban parametrization schemes varies with the application. The concept of fitness-for-purpose is therefore critical for both the choice of parametrizations and the way in which the scheme should be evaluated. A systematic and objective model response analysis procedure (Multiobjective Shuffled Complex Evolution Metropolis (MOSCEM) algorithm) is used to assess the fitness of the single-layer urban canopy parametrization implemented in the Weather Research and Forecasting (WRF) model. The scheme is evaluated regarding its ability to simulate observed surface energy fluxes and the sensitivity to input parameters. Recent amendments are described, focussing on features which improve its applicability to numerical weather prediction, such as a reduced and physically more meaningful list of input parameters. The study shows a high sensitivity of the scheme to parameters characterizing roof properties in contrast to a low response to road-related ones. Problems in partitioning of energy between turbulent sensible and latent heat fluxes are also emphasized. Some initial guidelines to prioritize efforts to obtain urban land-cover class characteristics in WRF are provided. Copyright © 2010 Royal Meteorological Society and Crown Copyright.

Modelling of urban sensible heat flux at multiple spatial scales : a demonstration using airborne hyperspectral imagery of Shanghai and a temperature–emissivity separation approach

Urbanization related alterations to the surface energy balance impact urban warming (‘heat islands’), the growth of the boundary layer, and many other biophysical processes. Traditionally, in situ heat flux measures have been used to quantify such processes, but these typically represent only a small local-scale area within the heterogeneous urban environment. For this reason, remote sensing approaches are very attractive for elucidating more spatially representative information. Here we use hyperspectral imagery from a new airborne sensor, the Operative Modular Imaging Spectrometer (OMIS), along with a survey map and meteorological data, to derive the land cover information and surface parameters required to map spatial variations in turbulent sensible heat flux (QH). The results from two spatially-explicit flux retrieval methods which use contrasting approaches and, to a large degree, different input data are compared for a central urban area of Shanghai, China: (1) the Local-scale Urban Meteorological Parameterization Scheme (LUMPS) and (2) an Aerodynamic Resistance Method (ARM). Sensible heat fluxes are determined at the full 6 m spatial resolution of the OMIS sensor, and at lower resolutions via pixel aggregation and spatial averaging. At the 6 m spatial resolution, the sensible heat flux of rooftop dominated pixels exceeds that of roads, water and vegetated areas, with values peaking at ∼ 350 W m− 2, whilst the storage heat flux is greatest for road dominated pixels (peaking at around 420 W m− 2). We investigate the use of both OMIS-derived land surface temperatures made using a Temperature–Emissivity Separation (TES) approach, and land surface temperatures estimated from air temperature measures. Sensible heat flux differences from the two approaches over the entire 2 × 2 km study area are less than 30 W m− 2, suggesting that methods employing either strategy maybe practica1 when operated using low spatial resolution (e.g. 1 km) data. Due to the differing methodologies, direct comparisons between results obtained with the LUMPS and ARM methods are most sensibly made at reduced spatial scales. At 30 m spatial resolution, both approaches produce similar results, with the smallest difference being less than 15 W m− 2 in mean QH averaged over the entire study area. This is encouraging given the differing architecture and data requirements of the LUMPS and ARM methods. Furthermore, in terms of mean study QH, the results obtained by averaging the original 6 m spatial resolution LUMPS-derived QH values to 30 and 90 m spatial resolution are within ∼ 5 W m− 2 of those derived from averaging the original surface parameter maps prior to input into LUMPS, suggesting that that use of much lower spatial resolution spaceborne imagery data, for example from Advanced Spaceborne Thermal Emission and Reflection Radiometer (ASTER) is likely to be a practical solution for heat flux determination in urban areas.

Local-scale urban meteorological parameterization scheme (LUMPS): longwave radiation parameterization and seasonality-related developments

Recent developments to the Local-scale Urban Meteorological Parameterization Scheme (LUMPS), a simple model able to simulate the urban energy balance, are presented. The major development is the coupling of LUMPS to the Net All-Wave Radiation Parameterization (NARP). Other enhancements include that the model now accounts for the changing availability of water at the surface, seasonal variations of active vegetation, and the anthropogenic heat flux, while maintaining the need for only commonly available meteorological observations and basic surface characteristics. The incoming component of the longwave radiation (L↓) in NARP is improved through a simple relation derived using cloud cover observations from a ceilometer collected in central London, England. The new L↓ formulation is evaluated with two independent multiyear datasets (Łódź, Poland, and Baltimore, Maryland) and compared with alternatives that include the original NARP and a simpler one using the National Climatic Data Center cloud observation database as input. The performance for the surface energy balance fluxes is assessed using a 2-yr dataset (Łódź). Results have an overall RMSE < 34 W m−2 for all surface energy balance fluxes over the 2-yr period when

Observations of urban boundary layer structure during a strong urban heat island event

It has long been known that the urban surface energy balance is different to that of a rural surface, and that heating of the urban surface after sunset gives rise to the Urban Heat Island (UHI). Less well known is how flow and turbulence structure above the urban surface are changed during different phases of the urban boundary layer (UBL). This paper presents new observations above both an urban and rural surface and investigates how much UBL structure deviates from classical behaviour. A 5-day, low wind, cloudless, high pressure period over London, UK, was chosen for analysis, during which there was a strong UHI. Boundary layer evolution for both sites was determined by the diurnal cycle in sensible heat flux, with an extended decay period of approximately 4 h for the convective UBL. This is referred to as the “Urban Convective Island” as the surrounding rural area was already stable at this time. Mixing height magnitude depended on the combination of regional temperature profiles and surface temperature. Given the daytime UHI intensity of 1.5∘C, combined with multiple inversions in the temperature profile, urban and rural mixing heights underwent opposite trends over the period, resulting in a factor of three height difference by the fifth day. Nocturnal jets undergoing inertial oscillations were observed aloft in the urban wind profile as soon as the rural boundary layer became stable: clear jet maxima over the urban surface only emerged once the UBL had become stable. This was due to mixing during the Urban Convective Island reducing shear. Analysis of turbulent moments (variance, skewness and kurtosis) showed “upside-down” boundary layer characteristics on some mornings during initial rapid growth of the convective UBL. During the “Urban Convective Island” phase, turbulence structure still resembled a classical convective boundary layer but with some influence from shear aloft, depending on jet strength. These results demonstrate that appropriate choice of Doppler lidar scan patterns can give detailed profiles of UBL flow. Insights drawn from the observations have implications for accuracy of boundary conditions when simulating urban flow and dispersion, as the UBL is clearly the result of processes driven not only by local surface conditions but also regional atmospheric structure.

Progress in observing and modelling the urban boundary layer

The urban boundary layer (UBL) is the part of the atmosphere in which most of the planet’s population now lives, and is one of the most complex and least understood microclimates. Given potential climate change impacts and the requirement to develop cities sustainably, the need for sound modelling and observational tools becomes pressing. This review paper considers progress made in studies of the UBL in terms of a conceptual framework spanning microscale to mesoscale determinants of UBL structure and evolution. Considerable progress in observing and modelling the urban surface energy balance has been made. The urban roughness sub-layer is an important region requiring attention as assumptions about atmospheric turbulence break down in this layer and it may dominate coupling of the surface to the UBL due to its considerable depth. The upper 90% of the UBL (mixed and residual layers) remains under-researched but new remote sensing methods and high resolution modelling tools now permit rapid progress. Surface heterogeneity dominates from neighbourhood to regional scales and should be more strongly considered in future studies. Specific research priorities include humidity within the UBL, high-rise urban canopies and the development of long-term, spatially extensive measurement networks coupled strongly to model development.

Global analysis of radiative forcing from fire-induced shortwave albedo change

Land surface albedo, a key parameter to derive Earth's surface energy balance, is used in the parameterization of numerical weather prediction, climate monitoring and climate change impact assessments. Changes in albedo due to fire have not been fully investigated on a continental and global scale. The main goal of this study, therefore, is to quantify the changes in instantaneous shortwave albedo produced by biomass burning activities and their associated radiative forcing. The study relies on the MODerate-resolution Imaging Spectroradiometer (MODIS) MCD64A1 burned-area product to create an annual composite of areas affected by fire and the MCD43C2 bidirectional reflectance distribution function (BRDF) albedo snow-free product to compute a bihemispherical reflectance time series. The approximate day of burning is used to calculate the instantaneous change in shortwave albedo. Using the corresponding National Centers for Environmental Prediction (NCEP) monthly mean downward solar radiation flux at the surface, the global radiative forcing associated with fire was computed. The analysis reveals a mean decrease in shortwave albedo of −0.014 (1σ = 0.017), causing a mean positive radiative forcing of 3.99 Wm−2 (1σ = 4.89) over the 2002–20012 time period in areas affected by fire. The greatest drop in mean shortwave albedo change occurs in 2002, which corresponds to the highest total area burned (378 Mha) observed in the same year and produces the highest mean radiative forcing (4.5 Wm−2). Africa is the main contributor in terms of burned area, but forests globally give the highest radiative forcing per unit area and thus give detectable changes in shortwave albedo. The global mean radiative forcing for the whole period studied (~0.0275 Wm−2) shows that the contribution of fires to the Earth system is not insignificant.

Simulation of long-term thermal characteristics of three Estonian lakes

A one-dimensional surface energy-balance lake model, coupled to a thermodynamic model of lake ice, is used to simulate variations in the temperature of and evaporation from three Estonian lakes: Karujärv, Viljandi and Kirjaku. The model is driven by daily climate data, derived by cubic-spline interpolation from monthly mean data, and was run for periods of 8 years (Kirjaku) up to 30 years (Viljandi). Simulated surface water temperature is in good agreement with observations: mean differences between simulated and observed temperatures are from −0.8°C to +0.1°C. The simulated duration of snow and ice cover is comparable with observed. However, the model generally underpredicts ice thickness and overpredicts snow depth. Sensitivity analyses suggest that the model results are robust across a wide range (0.1–2.0 m−1) of lake extinction coefficient: surface temperature differs by less than 0.5°C between extreme values of the extinction coefficient. The model results are more sensitive to snow and ice albedos. However, changing the snow (0.2–0.9) and ice (0.15–0.55) albedos within realistic ranges does not improve the simulations of snow depth and ice thickness. The underestimation of ice thickness is correlated with the overestimation of snow cover, since a thick snow layer insulates the ice and limits ice formation. The overestimation of snow cover results from the assumption that all the simulated winter precipitation occurs as snow, a direct consequence of using daily climate data derived by interpolation from mean monthly data.

Observational constraints on atmospheric and oceanic cross-equatorial heat transports: revisiting the precipitation asymmetry problem in climate models

Satellite based top-of-atmosphere (TOA) and surface radiation budget observations are combined with mass corrected vertically integrated atmospheric energy divergence and tendency from reanalysis to infer the regional distribution of the TOA, atmospheric and surface energy budget terms over the globe. Hemispheric contrasts in the energy budget terms are used to determine the radiative and combined sensible and latent heat contributions to the cross-equatorial heat transports in the atmosphere (AHT_EQ) and ocean (OHT_EQ). The contrast in net atmospheric radiation implies an AHT_EQ from the northern hemisphere (NH) to the southern hemisphere (SH) (0.75 PW), while the hemispheric difference in sensible and latent heat implies an AHT_EQ in the opposite direction (0.51 PW), resulting in a net NH to SH AHT_EQ (0.24 PW). At the surface, the hemispheric contrast in the radiative component (0.95 PW) dominates, implying a 0.44 PW SH to NH OHT_EQ. Coupled model intercomparison project phase 5 (CMIP5) models with excessive net downward surface radiation and surface-to-atmosphere sensible and latent heat transport in the SH relative to the NH exhibit anomalous northward AHT_EQ and overestimate SH tropical precipitation. The hemispheric bias in net surface radiative flux is due to too much longwave surface radiative cooling in the NH tropics in both clear and all-sky conditions and excessive shortwave surface radiation in the SH subtropics and extratropics due to an underestimation in reflection by clouds.

Quantifying polynya ice production in the Laptev Sea with the COSMO model

Arctic flaw polynyas are considered to be highly productive areas for the formation of sea-ice throughout the winter season. Most estimates of sea-ice production are based on the surface energy balance equation and use global reanalyses as atmospheric forcing, which are too coarse to take into account the impact of polynyas on the atmosphere. Additional errors in the estimates of polynya ice production may result from the methods of calculating atmospheric energy fluxes and the assumption of a thin-ice distribution within polynyas. The present study uses simulations using the mesoscale weather prediction model of the Consortium for Small-scale Modelling (COSMO), where polynya area is prescribed from satellite data. The polynya area is either assumed to be ice-free or to be covered with thin ice of 10 cm. Simulations have been performed for two winter periods (2007/08 and 2008/09). When using a realistic thin-ice thickness of 10 cm, sea-ice production in Laptev polynyas amount to 30 km3 and 73 km3 for the winters 2007/08 and 2008/09, respectively. The higher turbulent energy fluxes of open-water polynyas result in a 50-70% increase in sea-ice production (49 km3 in 2007/08 and 123 km3 in 2008/09). Our results suggest that previous studies have overestimated ice production in the Laptev Sea.

Impact of Laptev Sea flaw polynyas on the atmospheric boundary layer and ice production using idealized mesoscale simulations

The interaction between polynyas and the atmospheric boundary layer is examined in the Laptev Sea using the regional, non-hydrostatic Consortium for Small-scale Modelling (COSMO) atmosphere model. A thermodynamic sea-ice model is used to consider the response of sea-ice surface temperature to idealized atmospheric forcing. The idealized regimes represent atmospheric conditions that are typical for the Laptev Sea region. Cold wintertime conditions are investigated with sea-ice–ocean temperature differences of up to 40 K. The Laptev Sea flaw polynyas strongly modify the atmospheric boundary layer. Convectively mixed layers reach heights of up to 1200 m above the polynyas with temperature anomalies of more than 5 K. Horizontal transport of heat expands to areas more than 500 km downstream of the polynyas. Strong wind regimes lead to a more shallow mixed layer with strong near-surface modifications, while weaker wind regimes show a deeper, well-mixed convective boundary layer. Shallow mesoscale circulations occur in the vicinity of ice-free and thin-ice covered polynyas. They are forced by large turbulent and radiative heat fluxes from the surface of up to 789 W m−2, strong low-level thermally induced convergence and cold air flow from the orographic structure of the Taimyr Peninsula in the western Laptev Sea region. Based on the surface energy balance we derive potential sea-ice production rates between 8 and 25 cm d−1. These production rates are mainly determined by whether the polynyas are ice-free or covered by thin ice and by the wind strength.

The role of CO2 and dynamic vegetation on the impact of temperate land use change in the HadCM3 coupled climate model

Human induced land-use change (LUC) alters the biogeophysical characteristics of the land surface influencing the surface energy balance. The level of atmospheric CO2 is expected to increase in the coming century and beyond, modifying temperature and precipitation patterns and altering the distribution and physiology of natural vegetation. It is important to constrain how CO2-induced climate and vegetation change may influence the regional extent to which LUC alters climate. This sensitivity study uses the HadCM3 coupled climate model under a range of equilibrium forcings to show that the impact of LUC declines under increasing atmospheric CO2, specifically in temperate and boreal regions. A surface energy balance analysis is used to diagnose how these changes occur. In Northern Hemisphere winter this pattern is attributed in part to the decline in winter snow cover and in the summer due to a reduction in latent cooling with higher levels of CO2. The CO2-induced change in natural vegetation distribution is also shown to play a significant role. Simulations run at elevated CO2 yet present day vegetation show a significantly increased sensitivity to LUC, driven in part by an increase in latent cooling. This study shows that modelling the impact of LUC needs to accurately simulate CO2 driven changes in precipitation and snowfall, and incorporate accurate, dynamic vegetation distribution.

How do green roofs mitigate urban thermal stress under heat waves?

As the climate warms, heat waves (HW) are projected to be more intense and to last longer, with serious implications for public health. Urban residents face higher health risks because urban heat islands (UHIs) exacerbate HW conditions. One strategy to mitigate negative impacts of urban thermal stress is the installation of green roofs (GRs) given their evaporative cooling effect. However, the effectiveness of GRs and the mechanisms by which they have an effect at the scale of entire cities are still largely unknown. The Greater Beijing Region (GBR) is modeled for a HW scenario with the Weather Research and Forecasting (WRF) model coupled with a state-of-the-art urban canopy model (PUCM) to examine the effectiveness of GRs. The results suggest GR would decrease near-surface air temperature (ΔT2max = 2.5 K) and wind speed (ΔUV10max = 1.0 m s-1) but increase atmospheric humidity (ΔQ2max = 1.3 g kg-1). GRs are simulated to lessen the overall thermal stress as indicated by apparent temperature (ΔAT2max = 1.7 °C). The modifications by GRs scale almost linearly with the fraction of the surface they cover. Investigation of the surface-atmosphere interactions indicate that GRs with plentiful soil moisture dissipate more of the surface energy as latent heat flux and subsequently inhibit the development of the daytime planetary boundary layer (PBL). This causes the atmospheric heating through entrainment at the PBL top to be decreased. Additionally, urban GRs modify regional circulation regimes leading to decreased advective heating under HW.