Aluminum (Al)‐bearing and iron (Fe)‐bearing minerals, especially short‐range‐ordered (SRO) phases, are thought to protect soil organic C (SOC). However, it remains methodologically challenging to assess the influence of Al vs. Fe minerals or metal complexes. Whereas SRO Al and Fe phases share some properties, Al dissolved by oxalate (Alox) often correlates stronger with SOC than Fe dissolved by oxalate (Feox) or citrate–dithionite (Fecd). To further evaluate these relationships, we analyzed a large North American soil dataset from the National Ecological Observatory Network. A strong relationship between Aloxand SOC (and weaker Feox‐SOC relationship) persisted even after excluding soils rich in SRO minerals (Andisols and Spodosols). Al dissolved by oxalate was strongly correlated with citrate–dithionite‐extractable Al (Alcd; slope = 0.92,
Climatic and Geochemical Controls on Soil Carbon at the Continental Scale: Interactions and Thresholds
Previous studies found conflicting results on the importance of temperature and precipitation versus geochemical variables for predicting soil organic carbon (SOC) concentrations and trends with depth, and most utilized linear statistical models. To reconcile the controversy, we used data from 2574 mineral horizons from 675 pits from National Ecological Observatory Network sites across North America, typically collected to 1 m depth. Climate was a fundamental predictor of SOC and played similarly important roles as some geochemical predictors. Yet, this only emerged in the generalized additive mixed model and random forest model and was obscured in the linear mixed model. Relationships between water availability and SOC were strongest in very dry ecosystems and SOC increased most strongly at mean annual temperature < 0°C. In all models, depth, oxalate‐extractable Al (Alox), pH, and exchangeable calcium plus exchangeable magnesium were important while silt + clay, oxalate‐extractable Fe (Feox), and vegetation type were weaker predictors. Climate and pH were independently related to SOC and also interacted with geochemical composition: Feoxand Aloxrelated more strongly to SOC in wet or cold climates. Most predictors had nonlinear threshold relationships with SOC, and a saturating response to increasing reactive metals indicates soils where SOC might be limited by C inputs. We observed a mostly constant relative importance of geochemical and climate predictors of SOC with increasing depth, challenging previous statements. Overall, our findings challenge the notion that climate is redundant after accounting for geochemistry and demonstrate that considering their nonlinearities and interactions improves spatial predictions of SOC.
more » « less- NSF-PAR ID:
- 10449959
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Global Biogeochemical Cycles
- Volume:
- 35
- Issue:
- 3
- ISSN:
- 0886-6236
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract R 2 = .69), and discrepancies could be explained (R 2 = .87) by greater dissolution of Al‐substituted Fe phases by citrate–dithionite and greater dissolution of aluminosilicates by oxalate. Aluminum dissolved by oxalate and Alcdwere both strong SOC predictors despite their differing relationships with silicon (Si). Al dissolved by oxalate and Sioxstrongly covaried (R 2 = .79), but Alcdwas inconsistently related to Sicd(R 2 = .18). Similar relationships of Aloxand Alcdwith SOC, despite differences in minerals extracted by oxalate and citrate–dithionite, suggest that Al‐OC complexes (as opposed to aluminosilicate or iron‐bearing minerals) were the best SOC predictor. This raises important questions: do Al‐OC complexes indicate protection from decomposition or simply reflect greater intensity of mineral weathering by organic acids; and, if the latter, then perhaps SOC input is driving Aloxand SOC correlations rather than Al phase composition or abundance. -
null (Ed.)Abstract Variation in soil organic C (%OC) concentration has been associated with the concentration of reactive Fe- and Al-oxyhydroxide phases and exchangeable Ca, with the relative importance of these two stabilizing components shifting as soil pH moves from acid to alkaline. However, it is currently unknown if this pattern is similar or different with regard to measures of soil C persistence. We sampled soils from 3 horizons (uppermost A, uppermost B, C or lowest B horizons) across a pH gradient of 11 grass-dominated and 13 deciduous/mixed forest-dominated NEON sites to examine similarities and differences in the drivers of C concentration and persistence. Variation in C concentrations in all soils could be linked to abundances of Fe, Al and Ca, but were not significantly linked to variation in soil C persistence. Though pH was related to variation in Δ 14 OC, higher persistence was associated with more alkaline pH values. In forested soils, depth explained 75% of the variation in Δ 14 OC ( p < 0.0001), with no significant additional correlations with extractable metal phases. In grasslands, soil organic C persistence was not associated with exchangeable Ca concentrations, but instead was explained by depth and inorganic C concentrations (R 2 = 0.76, p < 0.0001), implying stabilization of organic C through association with carbonate precipitation. In grasslands, measures of substrate quality suggested greater persistence is also associated with a more advanced degree of decomposition. Results suggest that explanatory variables associated with C concentrations differ from those associated with persistence, and that reactive Fe- and Al-oxyhydroxide phases may not be present in high enough concentrations in most soils to offer any significant protective capacity. These results have significant implications for our understanding of how to model the soil C cycle and may suggest previously unrecognized stabilization mechanisms associated with carbonates and forms of extractable Si.more » « less
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A near-monoculture of J. roemerianus is often adjacent to and immediately landward of the A. germinans zone. The transition from the mangrove to the J. roemerianus zone is variable in our study area. An abrupt edge between closed-canopy mangrove and J. roemerianus monoculture may extend for up to several hundred meters in some locations, while other stretches of ecotone present a gradual transition where smaller, widely spaced trees are interspersed into the herbaceous marsh. Juncus roemerianus then extends landward to a high marsh patchwork of succulent halophytes (including Salicornia bigellovi, Sesuvium sp., and Batis maritima), scattered dwarf mangrove, and salt pans, followed in turn by upland vegetation that includes Pinus sp. and Serenoa repens. Field design and sample collection. We established three study sites spaced at approximately 5 km intervals along the western coastline of the central Florida peninsula. The sites consisted of the Salt Springs (28.3298°, -82.7274°), Energy Marine Center (28.2903°, -82.7278°), and Green Key (28.2530°, -82.7496°) sites on the Gulf of Mexico coastline in Pasco County, Florida, USA. At each site, we established three plot pairs, each consisting of one saltmarsh plot and one mangrove plot. Plots were 50 m^2 in size. Plots pairs within a site were separated by 230-1070 m, and the mangrove and saltmarsh plots composing a pair were 70-170 m apart. All plot pairs consisted of directly adjacent patches of mangrove forest and J. roemerianus saltmarsh, with the mangrove forests exhibiting a closed canopy and a tree architecture (height 4-6 m, crown width 1.5-3 m). Mangrove plots were located at approximately the midpoint between the seaward edge (water-mangrove interface) and landward edge (mangrove-marsh interface) of the mangrove zone. Saltmarsh plots were located 20-25 m away from any mangrove trees and into the J. roemerianus zone (i.e., landward from the mangrove-marsh interface). Plot pairs were coarsely similar in geomorphic setting, as all were located on the Gulf of Mexico coastline, rather than within major sheltering formations like Tampa Bay, and all plot pairs fit the tide-dominated domain of the Woodroffe classification (Woodroffe, 2002, "Coasts: Form, Process and Evolution", Cambridge University Press), given their conspicuous semi-diurnal tides. There was nevertheless some geomorphic variation, as some plot pairs were directly open to the Gulf of Mexico while others sat behind keys and spits or along small tidal creeks. Our use of a plot-pair approach is intended to control for this geomorphic variation. 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Cores were then capped and transferred on ice to our laboratory at the University of South Florida (Tampa, Florida, USA), where they were combined in plastic zipper bags, and homogenized by hand into plot-level composite samples on the day they were collected. A damp soil subsample was immediately taken from each composite sample to initiate 1 y incubations for determination of active C and N (see below). The remainder of each composite sample was then placed in a drying oven (60 °C) for 1 week with frequent mixing of the soil to prevent aggregation and liberate water. Organic wetland soils are sometimes dried at 70 °C, however high drying temperatures can volatilize non-water liquids and oxidize and decompose organic matter, so 50 °C is also a common drying temperature for organic soils (Gardner 1986, "Methods of Soil Analysis: Part 1", Soil Science Society of America); we accordingly chose 60 °C as a compromise between sufficient water removal and avoidance of non-water mass loss. Bulk density was determined as soil dry mass per core volume (adding back the dry mass equivalent of the damp subsample removed prior to drying). Dried subsamples were obtained for determination of soil organic matter (SOM), mineral texture composition, and extractable and total carbon (C) and nitrogen (N) within the following week. Sample analyses. A dried subsample was apportioned from each composite sample to determine SOM as mass loss on ignition at 550 °C for 4 h. After organic matter was removed from soil via ignition, mineral particle size composition was determined using a combination of wet sieving and density separation in 49 mM (3 %) sodium hexametaphosphate ((NaPO_3)_6) following procedures in Kettler et al. (2001, Soil Science Society of America Journal 65, 849-852). The percentage of dry soil mass composed of silt and clay particles (hereafter, fines) was calculated as the mass lost from dispersed mineral soil after sieving (0.053 mm mesh sieve). Fines could have been slightly underestimated if any clay particles were burned off during the preceding ignition of soil. An additional subsample was taken from each composite sample to determine extractable N and organic C concentrations via 0.5 M potassium sulfate (K_2SO_4) extractions. We combined soil and extractant (ratio of 1 g dry soil:5 mL extractant) in plastic bottles, reciprocally shook the slurry for 1 h at 120 rpm, and then gravity filtered it through Fisher G6 (1.6 μm pore size) glass fiber filters, followed by colorimetric detection of nitrite (NO_2^-) + nitrate (NO_3^-) and ammonium (NH_4^+) in the filtrate (Hood Nowotny et al., 2010,Soil Science Society of America Journal 74, 1018-1027) using a microplate spectrophotometer (Biotek Epoch, Winooski, VT, USA). Filtrate was also analyzed for dissolved organic C (referred to hereafter as extractable organic C) and total dissolved N via combustion and oxidation followed by detection of the evolved CO_2 and N oxide gases on a Formacs HT TOC/TN analyzer (Skalar, Breda, The Netherlands). Extractable organic N was then computed as total dissolved N in filtrate minus extractable mineral N (itself the sum of extractable NH_4-N and NO_2-N + NO_3-N). We determined soil total C and N from dried, milled subsamples subjected to elemental analysis (ECS 4010, Costech, Inc., Valencia, CA, USA) at the University of South Florida Stable Isotope Laboratory. Median concentration of inorganic C in unvegetated surface soil at our sites is 0.5 % of soil mass (Anderson, 2019, Univ. of South Florida M.S. thesis via methods in Wang et al., 2011, Environmental Monitoring and Assessment 174, 241-257). Inorganic C concentrations are likely even lower in our samples from under vegetation, where organic matter would dilute the contribution of inorganic C to soil mass. Nevertheless, the presence of a small inorganic C pool in our soils may be counted in the total C values we report. Extractable organic C is necessarily of organic C origin given the method (sparging with HCl) used in detection. Active C and N represent the fractions of organic C and N that are mineralizable by soil microorganisms under aerobic conditions in long-term soil incubations. To quantify active C and N, 60 g of field-moist soil were apportioned from each composite sample, placed in a filtration apparatus, and incubated in the dark at 25 °C and field capacity moisture for 365 d (as in Lewis et al., 2014, Ecosphere 5, art59). Moisture levels were maintained by frequently weighing incubated soil and wetting them up to target mass. Daily CO_2 flux was quantified on 29 occasions at 0.5-3 week intervals during the incubation period (with shorter intervals earlier in the incubation), and these per day flux rates were integrated over the 365 d period to compute an estimate of active C. Observations of per day flux were made by sealing samples overnight in airtight chambers fitted with septa and quantifying headspace CO_2 accumulation by injecting headspace samples (obtained through the septa via needle and syringe) into an infrared gas analyzer (PP Systems EGM 4, Amesbury, MA, USA). To estimate active N, each incubated sample was leached with a C and N free, 35 psu solution containing micronutrients (Nadelhoffer, 1990, Soil Science Society of America Journal 54, 411-415) on 19 occasions at increasing 1-6 week intervals during the 365 d incubation, and then extracted in 0.5 M K_2SO_4 at the end of the incubation in order to remove any residual mineral N. Active N was then quantified as the total mass of mineral N leached and extracted. Mineral N in leached and extracted solutions was detected as NH_4-N and NO_2-N + NO_3-N via colorimetry as above. This incubation technique precludes new C and N inputs and persistently leaches mineral N, forcing microorganisms to meet demand by mineralizing existing pools, and thereby directly assays the potential activity of soil organic C and N pools present at the time of soil sampling. Because this analysis commences with disrupting soil physical structure, it is biased toward higher estimates of active fractions. Calculations. Non-mobile C and N fractions were computed as total C and N concentrations minus the extractable and active fractions of each element. This data package reports surface-soil constituents (moisture, fines, SOM, and C and N pools and fractions) in both gravimetric units (mass constituent / mass soil) and areal units (mass constituent / soil surface area integrated through 7.6 cm soil depth, the depth of sampling). Areal concentrations were computed as X × D × 7.6, where X is the gravimetric concentration of a soil constituent, D is soil bulk density (g dry soil / cm^3), and 7.6 is the sampling depth in cm.more » « less
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Abstract How does hillslope structure (e.g., hillslope shape and permeability variation) regulate its hydro‐geochemical functioning (flow paths, solute export, chemical weathering)? Numerical reactive transport experiments and particle tracking were used to answer this question. Results underscore the first‐order control of permeability variations (with depth) on vertical connectivity (VC), defined as the fraction of water flowing into streams from below the soil zone. Where permeability decreases sharply and VC is low, >95% of water flows through the top 6 m of the subsurface, barely interacting with reactive rock at depth. High VC also elongates mean transit times (MTTs) and weathering rates. VC however is less of an influence under arid climates where long transit times drive weathering to equilibrium. The results lead to three working hypotheses that can be further tested.
H1 :The permeability variations with depth influence MTTs of stream water more strongly than hillslope shapes; hillslope shapes instead influence the younger fraction of stream water more .H2 :High VC arising from high permeability at depths enhances weathering by promoting deeper water penetration and water‐rock interactions; the influence of VC weakens under arid climates and larger hillslopes with longer MTTs .H3 :VC regulates chemical contrasts between shallow and deep waters (C ratio ) and solute export patterns encapsulated in the power law slope b of concentration‐discharge (CQ) relationships .Higher VC leads to similar shallow versus deep water chemistry (C ratio ∼1) and more chemostatic CQ patterns . Although supporting data already exist, these hypotheses can be further tested with carefully designed, co‐located modeling and measurements of soil, rock, and waters. Broadly, the importance of hillslope subsurface structure (e.g., permeability variation) indicate it is essential in regulating earth surface hydrogeochemical response to changing climate and human activities.
