Using a novel approach to characterize the surface reactivities of silica-rich ferrihydrite and biogenic cyanobacteria-ferrihydrite aggregates and the implications for Archean ocean geochemistry
Notice bibliographique
Résumé
Precambrian banded iron formations (BIF) are iron- and silica-rich chemical sedimentary rocks that are commonly used as paleo-redox proxies for Archean and Paleoproterozoic seawater geochemistry. At the onset of the Great Oxidation Event (herein GOE) around 2.4 Ga, cyanobacteria flourished with increasing nutrient fluxes due to oxidative weathering on land. In turn, this led to increased primary productivity that facilitated the permanent shift from a reducing Earth atmosphere to an oxidizing one. Interestingly, the duration of GOE also overlapped with one of the most prolific periods of BIF deposition.It is widely accepted that cyanobacteria were likely responsible for BIF formation during the GOE. Oxidation of dissolved Fe(II) by oxygen produced from cyanobacteria forms a metastable and amorphous mineral phase ferrihydrite, Fe(OH) 3 . As an essential component in both ancient BIF deposits and various modern ecosystems, the surface reactivity of ferrihydrite has been extensively studied under different conditions (i.e., pH and ionic strengths). Not only are the highly reactive surfaces of ferrihydrite particles important shuttles for trace element transport from the water column to the sediment pile, but previous studies have also demonstrated that cyanobacterial cells and ferrihydrite tend to aggregate at seawater pH. This means that ferrihydrite was also a vector for the transport of organic carbon to the seafloor. However, a complicating issue is how co-ions affect the surface reactivity of ferrihydrite, specifically dissolved silica which was abundant in ancient seawater. Although previous studies have demonstrated that silica can passivate the surface reactivity of ferrihydrite, what remains unclear is how silica impacts ferrihydrite-biomass aggregation. To fill this knowledge gap, we formed both silica-spiked ferrihydrite and cyanobacteria-ferrihydrite aggregates in situ and subsequently conducted empirical potentiometric acid-base titrations and Cd adsorption experiments on the fresh aggregate samples at three different ionic strengths (0.56 M, 0.1 M and 0.01 M). We minimized sample processing (i.e., drying and powdering) to a simple washing step, in which the aggregate pellets remained hydrated to avoid any mineral transformation thus altering their true surface reactivity in seawater. Experimental results were then fitted with non-electrostatic model to predict both surface charges and metal-adsorption behavior of ferrihydrite aggregates. Different from previous surface-complexation modelling studies, here we used a novel and more powerful modelling program called Phreefit. It utilizes the global optimization algorithms instead of more commonly used Newton-Raphson method in FITEQL program, which is often too limited for precisely modelling complex systems such as the two samples in this study. Furthermore, we also measured the surface charges of both samples over the pH range from 3 to 9 on a Malvern Zetasizer and characterized the surface functional groups through Fourier-Transform Infrared Spectroscopy to help with our interpretation of the experimental data.Preliminary results show that cyanobacteria-ferrihydrite aggregates formed primarily due to ionic bridging. Cyanobacterial cells likely facilitated the precipitation of dissolved silica. Findings from titration and Cd adsorption experiments indicate that the surface reactivity and capacity of both silica-rich ferrihydrite cyanobacteria-ferrihydrite aggregates to adsorb trace elements differ from their individual components, likely due to site blockage. This distinction is particularly prominent when considering the expected Archean seawater pH from 6 to 8. This disparity implies that the biogenic ferrihydrite aggregates do not exhibit an additive surface reactivity, which is in agreement with similar previous studies. Our combined results are crucial to accurately predict the adsorption of trace elements onto the aggregate surface and, ultimately, comprehend the archive of trace elements in sedimentary rocks used to reconstruct Precambrian ocean chemistry.
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Comment cette classification a été obtenuedéplier
Prédiction distillée sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Apprise à partir de 10 348 étiquettes directes de Codex et de 10 348 étiquettes directes de Gemma. Le mode candidate est l'union des têtes enseignantes seuillées; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont ni des étiquettes humaines ni des étiquettes directes de modèles de pointe.
Scores Codex et Gemma par catégorie
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,001 | 0,000 |
| Méta-épidémiologie (sens strict) | 0,000 | 0,000 |
| Méta-épidémiologie (sens large) | 0,000 | 0,000 |
| Bibliométrie | 0,000 | 0,000 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,000 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,000 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,000 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découleClassification
machine, non validéePrédiction automatique; un appel candidat d’une seule tête enseignante, pas un consensus.
Le détail, modèle par modèle et score par score, se trouve en fin de page sous « Comment cette classification a été obtenue ».