The adsorption of adenine and thymine in komatiite and tonalite simulating the complexity of the primordial terrestrial crust
Adsorción de adenina y timina en komatiita y tonalita simulando la complejidad de la corteza terrestre primordial
Abigail Elvira Cruz-Hernández1
, María Colín-García2, Eva Mateo-Martí3
1 Posgrado en Ciencias de la Tierra, Universidad Nacional Autónoma de México. Circuito de Posgrados s/n, Ciudad Universitaria, Coyoacán, 04510, Ciudad de México, México.
2 Instituto de Geología, Universidad Nacional Autónoma de México. Circuito de la Investigación Científica, Ciudad Universitaria, 04510, Ciudad de México, México.
3 Centro de Astrobiología (CAB), Instituto Nacional de Técnica Aeroespacial (INTA), Consejo Superior de Investigaciones Científicas (CSIC). Ctra. Ajalvir Km 4, Torrejón de Ardoz, 28850, Madrid, España.
Corresponding author: (A. E. Cruz-Hernández) This email address is being protected from spambots. You need JavaScript enabled to view it.
How to cite this article:
Cruz-Hernández, A. E., Colín-García, M., & Mateo-Martí, E. (2026). The adsorption of adenine and thymine in komatiite and tonalite simulating the complexity of the primordial terrestrial crust: Boletín de la Sociedad Geológica Mexicana, 78(2), A170226. https://doi.org/10.18268/BSGM2026v78n2A170226
Manuscript received: December 10, 2025. Corrected manuscript received: February 12, 2026. Manuscript accepted: February 14, 2026.
ABSTRACT
Mineral surfaces may have played a fundamental role in the chemical processes that led to the origin of life by concentrating and transforming organic molecules into primitive aqueous environments. Hence, the adsorption potential of rocks representative of the primordial oceanic (komatiite) and continental (tonalite) crusts, as well as their main constituent minerals (lizardite and plagioclase), towards the nucleobases adenine and thymine was evaluated in this study. Batch adsorption experiments were performed in aqueous suspension at different time intervals, and the surfaces were characterized to determine their mineral and elemental composition, as well as their pore structure. The results showed that all studied surfaces adsorbed both molecules, with a higher affinity toward adenine. Thymine exhibited a bell-shaped kinetic trend for almost all surfaces (except komatiite and lizardite), possibly associated with conformational changes induced by silicate minerals. The differences observed between rocks and their constituent minerals are attributed to the heterogeneity of adsorption sites. These findings suggest that surface–molecule interactions involve different mechanisms and even catalytic sites that are dependent on surface composition. This work highlights the relevance of rock surfaces as potential concentrators of organic molecules in prebiotic scenarios.
Keywords: komatiite, tonalite, lizardite, plagioclase, adsorption, nucleobases.
RESUMEN
Las superficies minerales pudieron haber desempeñado un papel fundamental en los primeros pasos químicos que guiaron el origen de la vida, al concentrar y transformar moléculas orgánicas en ambientes acuosos primitivos. En este estudio se evaluó el potencial de rocas representativas de las cortezas primordiales, oceánica (komatiita) y continental (tonalita), así como de sus minerales principales (lizardita y plagioclasa), para adsorber las bases nitrogenadas adenina y timina. Se realizaron experimentos de adsorción en suspensión acuosa a diferentes intervalos de tiempo y se caracterizaron los sólidos para determinar su composición mineral, elemental, así como su estructura porosa. Los resultados mostraron que todas las superficies estudiadas adsorben ambas moléculas, con una afinidad mayor hacia la adenina. Por otro lado, la timina presentó una cinética en forma de campana para la mayoría de las superficies (excepto en la komatiita y lizardita), posiblemente asociada a cambios conformacionales inducidos por los silicatos. Las diferencias observadas entre rocas y minerales se atribuyen a la heterogeneidad de los sitios de adsorción. Estos hallazgos sugieren que las interacciones superficie-molécula involucran distintos mecanismos de adsorción e incluso sitios catalíticos que son dependientes de la composición de la superficie y destacan la relevancia de las superficies rocosas como potenciales concentradores de moléculas orgánicas en escenarios prebióticos.
Palabras clave: komatiita, tonalita, lizardita, plagioclasa, adsorción, bases nitrogenadas.
1. Introduction
The interaction of organic molecules with mineral surfaces is a process present on the planet since its formation; it is present in soil, sediments, and various marine and continental environments. Minerals are responsible for compartmentalizing and creating microsites where various processes occur, such as the adsorption and transformation of organic matter (Kleber et al., 2021). As it occurs currently, it has been proposed that in primitive environments, mineral surfaces acted as concentrators and catalysts of organic molecules, important for the first chemical steps that guided the origin of life (Bernal, 1951; Brucato and Fornaro, 2018; Hazen, 2006).
Numerous studies have investigated the role that minerals may have played in processes contributing to the increase in molecular complexity on early Earth. These studies have shown that inorganic surfaces are capable of adsorbing organic molecules, there is a wealth of work with clays (Benetoli et al., 2007; Bhatt et al., 2022; Baú et al., 2020; Colín-García et al., 2024; Lailach et al., 1968; Lahav, 2001; Meléndez-López et al., 2021; Samulewski et al., 2021; Villafañe-Barajas et al., 2018); other minerals that have been used include zeolites and various oxides. The adsorption of organic molecules on complex surfaces has been recently addressed, and it is of particular interest to this research group (Cruz-Hernández et al., 2022). The use of solids such as rocks can better represent the complexity of dynamic systems in different early environments of both the oceanic and continental primitive crust.
The evidence indicates that, during the Hadean and Archean, the oceanic crust had a komatiitic composition (Korenaga, 2006; Meunier et al., 2010). Komatiites are ultramafic volcanic rocks with a high MgO content. These rocks have been found on Archean terraces and are considered important in the study of the evolution of the Earth’s mantle (Arndt and Lesher, 2004). Furthermore, komatiites provide evidence of early oceanic crust and mantle, and are considered the closest example of the hottest mantle plumes during the Archean (Smith and Morowitz, 2016). The unaltered composition of komatiites consists predominantly of olivine (40–80%), while the matrix usually has a variable composition, depending on the cooling rate. The presence of secondary minerals results from hydrological metamorphism, which alters olivine to serpentine (Arndt et al., 2008).
Tonalites are rocks that have been found in the oldest cratons of the Acasta gneiss, in Canada (Iizuka et al., 2007; Nutman et al., 1996). These cratons are the remnants of the continental crust in which the association of granitoid rocks TTG (Tonalite-Trondhjemite-Granodiorite) abounds (Chekulaev and Glebovitsky, 2017). Therefore, tonalites are considered representative rocks of the first continental crust. Furthermore, tonalitic magmas promote the formation of zircons, from which information has been obtained regarding both the age of these continental masses and the mechanisms that generated the primordial continental crust (Gargaud et al., 2006). The average composition of these granitoids is mainly plagioclase (45-55%), quartz (20-25%), biotite (10-20%), and microcline (5%) (Savko et al., 2018). Therefore, komatiites and tonalites represent key surfaces for prebiotic evolution studies (Nna-Mvondo and Martinez-Frias, 2007), as they may have acted as concentrators of diluted organics in primitive environments.
Nucleobases have been largely investigated, and their abiotic synthesis through different precursor molecules has been demonstrated (Oró, 1960; Ponnamperuma et al., 1963; Yuasa et al., 1984). These studies have shown the preferential synthesis of adenine, making it the most studied nitrogenous base, as well as its complementary base, thymine. Both molecules (Figure 1) are good representatives of the nucleobases and components of DNA.
The adsorption of adenine and thymine has been investigated in previous studies on non-clay mineral surfaces, including forsterite, magnetite, pyrite, pyrrhotite, quartz (Cohn et al., 2001; Plekan et al., 2007), natural graphite (Sowerby et al., 2001), rutile (Cleaves et al., 2010), magnesium oxide (Fornaro et al., 2013), and different types of zeolites (Anizelli et al., 2015, 2016; Baú et al., 2012). However, to our knowledge, no work has been done on complex and heterogeneous surfaces. Therefore, the objective of this work was to study the adsorption of adenine and thymine onto komatiite and tonalite, as well as their main minerals (plagioclase and lizardite), to understand their potential as concentrators in a neutral aqueous medium, simulating possible oceanic and continental prebiotic environments.
2. Materials and methods
The adenine and thymine reagents were obtained from Merck Sigma® in the highest purity available (99% in both cases). All the water used for the experiments was pure Milli-Q® grade water. The komatiite, tonalite, lizardite, and plagioclase samples were natural hand samples obtained by field collection.
2.1. PREPARATION OF GEOLOGICAL MATERIALS
The rock and mineral samples were broken into approximately one-centimeter pieces and then washed to remove all possible organic matter or contamination. The cleaning process was carried out according to the protocol detailed in Cruz-Hernández et al. (2022) using first an alkaline and later acidic solutions at low concentration. The samples were then ground by hand in an agate mortar until the powder passed through a 0.177 mm sieve. This was done to increase the surface area for the sorption experiments and to homogenize the materials. These same powders were used for characterization analyses.
2.2. GEOCHEMICAL CHARACTERIZATION
Mineral composition was determined by X-ray diffraction (XRD) using an EMPYREAN diffractometer with a Ni filter, a fine-focus copper tube, a monochromator, and a PIXcel3D detector. Measurements were made in the 2θ angular range of 5° to 80° with a 0.003° step scan and an integration time of 40 seconds per step. It should be noted that the mineralogical composition of komatiite was reported in a previous work (Cruz-Hernández et al., 2022), and therefore, the data were taken from that study since it is the same sample.
X-ray fluorescence (XRF) was used to determine the elemental composition; the powders of all the materials were dried at 110 °C for two hours. Then, a 0.8 g fraction of each sample was taken to, which 7.8 g of Li2B4O7 was added to obtain a fusion bead. The analysis was performed using the Rigaku Primus II equipment, and the results were obtained as the percentage of the major oxide components of each geological material.
2.3. AREA AND POROSITY CHARACTERIZATION
The N2 adsorption and desorption isotherms Brunauer-Emmett-Teller (BET) method to determine the specific surface area (SSA) of each surface was used. Before analysis, samples were heat-treated in a muffle, and a gram of each sample was maintained at 200 °C for eight hours. With the isotherms, the values of specific surface area and total pore volume were calculated for each solid. SSA values are reported in m²/g and were used to interpret sorption behavior relative to surface availability.
2.4. ADSORPTION KINETICS EXPERIMENTS
For the adsorption experiments, a solution of adenine and thymine was prepared at concentrations of 1×10-4 mol·L-1 and 2×10-4 mol L-1, respectively. The suspensions were prepared in centrifuge tubes; 100 mg of material and 5 mL of solution of each nitrogenous base were added, for a proportion of 20 mg of surface area per milliliter of solution per tube. The tubes were placed on a shaking platform for different time lapses to determine the adsorption kinetics. Then, the samples were centrifuged at 10 000 rpm for 20 minutes to obtain the supernatant and to remove any remaining particles. Finally, the samples were filtered through 0.22-micron syringe filters. The adsorption experiments were performed at the natural pH of the solutions of adenine (6.48±0.14) and thymine (5.22±0.11) in pure water; a potentiometer OAKTON ION 700m was used, and five readings of different solutions were taken to obtain the average. Each sample was prepared in triplicate, and for each sample, a blank containing the solid suspended in pure water was prepared. This was used to calibrate the instrument with a blank measurement before analyzing the samples.
2.5. ANALYSIS AND QUANTIFICATION OF ADSORPTION
The supernatants were analyzed by UV spectroscopy to quantify the remaining molecules using a Jenway 7205 system. The maximum absorbance lengths of adenine (λ=261 nm) and thymine (λ=264 nm), as well as the linearity of the quantification, were determined using calibration curves. To calculate the percentage of adsorption, the remaining percentage (% Remaining) of molecules in the supernatant was first calculated (Equation 1), the average absorbance of the sample (Abs sample) and the absorbance of the standard (Abs sample) were used and that result was subtracted from the 100% corresponding to the standard, that is, the initial concentration.
The standard deviation of each point was calculated with the relative standard deviation (%RSD), in which the standard deviation and the average of each point are used (Equation 2).
3. Results and discussion
3.1. GEOCHEMICAL CHARACTERIZATION
As it was reported in a previous study (Cruz-Hernández et al., 2022), komatiite minerals are principally lizardite (29%) and plagioclase (26%), other mineral phases were identified in smaller quantities, such as phyllosilicates chlorite-type (21%), pyroxene diopside-type (14%), and olivine forsterite-type (10%). The mineral phases are detailed in Table 1.
The mineral phases found by XRD analysis reported in literature for the komatiite rock reported that the principal minerals are olivine (forsterite), clinopyroxene (diopside), and plagioclase with variable composition (Aitken and Echeverría, 1984). In the sample analyzed lizardite and chlorite were also found; those are secondary mineral products of the alteration of the original olivine and pyroxene. Due to the hydrothermal environmental formation, it is expected and common to find secondary minerals and transformation of the original composition of komatiite which is why they also agree with what has been reported in other works (Arndt et al., 2008; Nesbitt et al., 1979).
On the other hand, the results of the XRD analysis showed that tonalite is composed mainly of plagioclase of the andesine type (56%) and siderophyllite-typemica(19%); smallerpercentages of the minerals quartz (10%), amphibole (8%), and other chlorite-type phyllosilicates (7%) were found. A summary of the phases that compose tonalite is shown in Table 2.
The data obtained from the tonalite sample showed results consistent with those reported for other tonalites from northern Mexico. In tonalite units from Baja California, the mineral composition was plagioclase, quartz, biotite, hornblende, and potassium feldspar (Duffield, 1968). Another study of tonalites from the same region reported that the components were anorthite-type plagioclases, which are randomly distributed throughout the rock (36-47%), and other types of plagioclases distributed in patches up to 17%. Other minerals found were hornblende, biotite, quartz, and magnetite (Tate et al., 1999). This indicates that the minerals that constitute tonalites are plagioclase, quartz, and amphibole; since they are sodic granitic rocks commonly associated with other granitoid rocks such as trondhjemite and granodiorite. The minerals chlorite-type and siderophyllite-type found in the sample of this work may be the result of the development of secondary phases resulting from alterations, coupled with the natural variability of the rocks themselves.
The elemental composition of the rocks and two minerals (lizardite and plagioclase) was analyzed by XRF. The results (Table 3) reveal that, for all four solids, the most abundant component is SiO2; the rest of the components are different for each solid. For the komatiite sample, in addition to the high SiO2 content (43.90%), MgO (16.1%), Fe2O3 (12.18%), and Al2O3 (11.61%) were the most abundant elements.
The results are similar to those reported for komatiites from the same area (Echeverría, 1980). As well, the analysis of lizardite revealed a high content of SiO2 (39.98%) and MgO (37.69%), characteristic of this mineral. This was also reported in other geochemical studies for natural lizardite samples (Votyakov et al., 2005).
On the other hand, for the tonalite sample, a high content of SiO2 (64.84%) and Al2O3 (17.44%) was observed; while in lower percentages, CaO (4.96%) and Na2O (4.33%) were found, which is consistent with the values obtained for other tonalite samples (Tate et al., 1999). Besides, high percentages of SiO2 (68.14%), Al2O3 (19.69%) and Na2O (11.48%) were also observed, which is why plagioclase was identified as a high-purity albite (Milam et al., 2010).
The surfaces with the highest silica contents were plagioclase and tonalite; thus, these materials contain a higher number of silanol groups (Si-O-H) compared to komatiite and lizardite. Silanol groups in contact with an aqueous phase can promote electrostatic interactions on the surface. This is because water molecules can be adsorbed by the silanol groups and act as an intermediate for the formation of hydrogen bonds with organic molecules, favoring their adsorption (Samrout et al., 2024). This means that we could expect greater adsorption in the tonalite and plagioclase through the silanol groups.
Among the major elements for komatiite and lizardite is MgO, which is a group with the ability to adsorb molecules because its O2- ions generate a basicity that has the potential to attract acid groups or molecules that behave as Brønsted acids (Fornaro et al., 2013).
3.2. SPECIFIC SURFACE AREA AND POROSITY CHARACTERIZATION
The BET results showed the SSA of all the solids studied (Table 4). Lizardite was the material with the highest area (30.53 m2/g); the second highest surface area was the komatiite (5.59 m2/g).
Tonalite and plagioclase were the solids with the minor SSA values, 0.46 and 0.20 m2/g, respectively. The SSA value is a parameter related to particle and porosity characteristics; smaller and spherical particles generally are associated with a higher SSA value (Lowell and Shields, 2013). In this study, all the solids were milled and sieved with the same process; this implies that the possible differences are related to the abundance and size of the porous, rather than particle dimensions. The mean pore diameter is shown in Table 4, along with the corresponding IUPAC classification for adsorbent materials based on pore size. Komatiite, lizardite, and tonalite can be classified as mesoporous materials, since their mean pore diameters are within the range of 2 and 50 nm. While plagioclase is considered a macroporous material because it has a pore size greater than 50 nm (Pourhakkak et al., 2021). According to these measurements, lizardite was the surface that showed the best characteristics to be a good adenine and thymine adsorbent, since it has the largest SSA of the four materials (30.53 m2/g), and a small APD (4.34 nm).
3.3. ADSORPTION EXPERIMENTS
3.3.1. KOMATIITE
The adsorption results for adenine and thymine on komatiite showed different behaviors as can be seen in Figure 2. Adenine was better adsorbed, with a tendency to increase its adsorption along with contact time; the maximum percentage observed was 29.85% after 112 h of contact. Thymine presented low sorption percentages throughout contact time, the maximum percentage of adsorption obtained being 8.12% at 71 h. The percentage of adsorption of adenine and thymine on komatiite were similar (4.81 and 5.51% respectively); however, adenine was found to have a greater affinity for the surface of komatiite than thymine. Adenine, having an exocyclic NH2 group, may be favoring the affinity for rock, unlike thymine, which does not possess exocyclic groups.
3.3.2. LIZARDITE
The adsorption of the nucleobases on the lizardite surface is shown in Figure 3. The adsorption of adenine remains at similar percentages over time, reaching an equilibrium after 48 hours of contact, the maximum adsorption was obtained at 72 h (15.56%). This indicates that the surface of lizardite becomes saturated with adenine molecules faster than in the case of komatiite. In this case, it was also observed that thymine was less adsorbed than adenine on lizardite; the maximum adsorption percentage obtained was 11.71% after 28 h of stirring the suspension. In the case of thymine, a decrease in adsorption was observed as contact time increased, showing that both the affinity and the interactions of thymine on plagioclase are weak, so the molecule desorbs back into solution.
3.3.3. TONALITE
Figure 4 presents the results of the adenine and thymine adsorption experiments on tonalite. The adenine adsorption trend is similar to that obtained on komatiite; the adsorption percentages increase over time; however, equilibrium is not reached, but rather a maximum point is reached after 112 h of contact, the adsorption was 28.78%. On the other hand, the adsorption of thymine on tonalite also showed a lower adsorption than adenine, and a bell-shaped trend, with the maximum adsorption at 45 h (11.12%). After this time, the adsorption decreased, as with the lizardite surface, due to the weak interactions that adsorb thymine, prolonged time on the surface does not favor adsorption but promotes the return of the molecule to the solution.
3.3.4. PLAGIOCLASE
Adenine and thymine showed low adsorption percentages on plagioclase (Figure 5); the adsorption trend was bell-shaped for both molecules. The maximum adsorption for adenine was 14.17% at 48 h, while for thymine it was 11.71% at 28 h of stirring. Specifically, adenine showed less affinity for the plagioclase surface compared to tonalite. In both cases, equilibrium was not reached, but adsorption decreased as the contact time increased. The interaction of both adenine and thymine was weak on the surface of plagioclase; their desorption at short contact times is due to this low affinity.
Table 1SM shows a summary of all the adsorption points obtained as well as their standard deviation, with which the adsorption kinetics for adenine and thymine were constructed.
3.4. BEHAVIOR ADSORPTION ANALYSIS
Elemental analysis of the surfaces showed a difference, mainly in the SiO2, Al2O3, and MgO content, between the mafic (komatiite and lizardite) and felsic (tonalite and plagioclase) materials.
The surfaces with the highest silica contents were plagioclase and tonalite; thus, these materials contain a higher number of silanol groups (Si-O-H) compared to komatiite and lizardite. Silanol groups in contact with an aqueous phase can promote electrostatic interactions on the surface. This is because water molecules can be adsorbed by the silanol groups and act as an intermediate for the formation of hydrogen bonds with organic molecules, favoring their adsorption (Samrout et al., 2024). This means that we could expect greater adsorption in the tonalite and plagioclase through the silanol groups. Likewise, tonalite and plagioclase showed a high Al2O3 content; the alumina groups are also capable of interacting with organic molecules either by physical adsorption or chemical adsorption. It has also been reported that Al from Al2O3 group can interact with N atoms of organic molecules to adsorb them (Ahmad and Martsinovich, 2022), so tonalite and plagioclase may be able to retain both nucleobases and amino acids.
MgO is among the major components for komatiite and lizardite, and this is a group with the ability to adsorb molecules, as O2- ions generate a basicity that has the potential to attract acid groups or molecules that behave as Brønsted acids (Fornaro et al., 2013).
On the other hand, the SSA and porosity characterization showed that lizardite and komatiite are the surfaces with larger surface area, compared to tonalite and plagioclase. If adsorption depended solely on the surface area of the solids, we would expect lizardite and komatiite to be the surfaces that presented the highest adsorption percentages for the two molecules studied. However, significant differences were observed in the adsorption behavior of the molecules on rocks compared to minerals. Furthermore, the adsorption for both molecules was different. The results can be discussed in two parts: first, the surface area and the porosity, both of which have a greater influence on the adsorption of molecules. Second, the physicochemical characteristics of molecules; adenine showed a better adsorption response compared to thymine; thus, the structure and characteristics of the molecule have a significant influence on the adsorption process.
3.4.1. ADSORPTION DIFFERENCES BETWEEN ROCKS AND MINERALS
Komatiite and tonalite rocks showed higher adenine adsorption percentages than isolated minerals (Figure 1SM). Furthermore, in lizardite and plagioclase, the adsorption of the nucleobases proved to reach a maximum point (equilibrium), and then it did not change. In the case of rocks, more contact time is required to reach equilibrium. This can be explained by the fact that heterogeneous solids hold different active sites and, therefore, different binding energies (Kumar et al., 2019). The heterogeneity of a material results in different adsorption and desorption behavior in each pore or active site; heterogeneous materials may have heterogeneous vacancies, functional groups, and pore sizes, which increases the complexity of the adsorption process, promoting interactions and the adsorption processes, as in the case here presented. Each site fits the adsorbed molecule with a different mechanism and, therefore, with a different equilibrium time (Chiang et al., 2018; Kumar et al., 2019).
The difference between adsorption on homogeneous and heterogeneous surfaces is that the diversity and variability of active sites (available on heterogeneous materials) affect their adsorption behavior; each site contributes individually to the total adsorption of the system, making it more complex to study. On homogeneous surfaces, however, the sites are uniform, and therefore, their adsorption energy remains unchanged, and their behavior is more predictable (Babatunde et al., 2022).
Due to this complexity, to our knowledge, there are few studies that use heterogeneous surfaces to adsorb organics, in this case adenine or thymine. Worthy of mention is the study by El Amri et al. (2004), who studied adenine adsorption on two meteoritic materials with heterogeneous mineral composition, Zagami and Murchison. The Murchison meteorite is composed mostly (97.5% w/w) of pyroxene, enstatite, serpentine, olivine, and iron oxides, while the Martian Zagami meteorite is composed of pyroxene-rich basalt, glass, plagioclase, oxides, sulfates, phosphates, and amphibole-containing melt zones. In this study, adenine adsorption was observed in both meteorites, but the Murchison meteorite showed a greater affinity for the nitrogenous base, which was attributed to the amount of organic matter contained in this carbonaceous chondrite (2.5% w/w). This organic matter, possibly rich in amino and imino groups, functions as an active site for adenine retention. In contrast, the Zagami meteorite, which does not have organic matter, exhibits less adenine retention. This reinforces the idea that the composition of heterogeneous solids has a significant influence on their ability to adsorb organic molecules, as it influences the type, number, and distribution of active sites to retain the molecules.
Lizardite and plagioclase showed lower molecular adsorption percentages (Figure 1SM), but the kinetics are closer to equilibrium, which may be related to greater homogeneity in the surface sites of each mineral where adenine adsorbs. There are some studies on the adsorption of organic molecules on serpentine, for example, Colín-García et al. (2010) studied the adsorption of HCN on different minerals, including serpentine (which is the mineral group to which lizardite belongs). In this study, HCN was adsorbed at 32%, which was lower compared to other minerals used, such as zeolite and dolomite, in which the authors obtained higher adsorption rates, of 70% and 61% respectively. More recently, Percot et al. (2024) established that the maximum amount of adenine adsorbed on serpentinite is 10%; they performed experiments simulating extraterrestrial dust, and determined the amount of adenine adsorbed previously to test the effectivity of SERS (Surface-Enhanced Raman Spectroscopy) as a detection technique. It is worth noting that for the mentioned work, a lizardite with an SSA of 8 m2/g was used, while the one used in this study had an SSA of 30.53 m2/g; therefore, a lizardite with a higher SSA can adsorb more, which agrees with the results obtained in this work. However, even though it shows greater molecular adsorption due to its higher SSA, it still shows less molecular adsorption than both komatiite and tonalite.
The values of the highest adsorption for each system are shown in Table 1SM. For adenine adsorption mesoporous surfaces exhibit the highest percentages: komatiite (29.85%), tonalite (28.78%), and lizardite (15.56%). Plagioclase (14.17%), which was the only mineral with a macroporous surface, showed the lowest maximum value among the measured parameters.
In the case of thymine, lizardite (11.71%), plagioclase (11.71%), and tonalite (11.12%) recorded the highest maximum adsorption values among the studies samples; meanwhile, komatiite (8.12%) exhibited the lowest maximum percentages observed during the experiments. This suggests that the adsorption of thymine follows different behavior, potentially governed by one or more mechanisms not related to the porosity of the solids showing that the chemical structure of each molecule also has a notable influence on the adsorption process and the affinity for the substrate (mineral or rock).
3.4.2. DIFFERENTIAL ADSORPTION OF ADENINE AND THYMINE
The adsorption of adenine has been previously studied; it is adsorbed in greater quantities than other nucleobases. Different surfaces have been tested, such as pyrite, quartz, pyrrhotite, magnetite, forsterite (Cohn et al., 2001), pyrite, silicon dioxide (Plekan et al., 2007), rutile (Cleaves et al., 2010), montmorillonite (Carneiro et al., 2011), magnesium oxide (Fornaro et al., 2013), natural zeolites (Anizelli et al., 2015), ferrihydrite (Canhisares-Filho et al., 2015), and artificial zeolites (Anizelli et al., 2016). This is consistent with the results obtained in this study, as adenine showed higher percentages of adsorption than thymine. Adenine is less soluble than thymine; in general, purines are less soluble than pyrimidines (Cleaves, 2018). Less soluble molecules are more likely to be adsorbed because the repulsive forces with water molecules cause the organic molecules to move first to the interface and then to the surface of minerals or rocks (Weber, 2021); this occurs to adenine. The preferential adsorption of adenine related to thymine can also be attributed to: i) the exocyclic amino group that the molecule possesses and ii) to its planar arrangement, which gives it a greater affinity for surfaces (Cleaves et al., 2010; Anizelli et al., 2016).
In this work, we found that, as reported by other authors, thymine was less adsorbed, but the adsorption of this nitrogenous base showed a bell shape (except for lizardite surface). This behavior may be related to the keto-enol tautomerization (Figure 6). In the case of thymine, as with other nucleobases, the two tautomeric forms interconvert with the movement of a hydrogen atom, that goes from a carbonyl group (in the keto form) to a hydroxyl group (in the enol form) (Vinje et al., 2017). This change in the structure of the molecule plays an important role in adsorption (Zhang et al., 2022). In neutral aqueous solutions, the predominant form of thymine is the keto form, and this enantiomer is also the most stable (Vinje et al., 2017). The first part of the kinetics observed in the bell-shaped adsorption of thymine may be related to the adsorption of the molecule in its keto form. The second part of the bell, in an apparent desorption, may be related to a change of thymine to its enol tautomer. This keto-enol change of thymine can be caused by the solids themselves, as observed by Zhang et al. (2022). The authors noticed that the keto-enol tautomerization of thymine can be induced by the reactivity of a Si (111) surface, due to the delocalization of electrons in the aromatic ring of the molecule. To corroborate this proposal, more detailed analyses and a more detailed study of the adsorption system are necessary, which is beyond the scope of this work, and raises the need to continue studying geological surfaces and their role not only as concentration mechanisms, but as important agents in chemical evolution.
Finally, calculations were performed to verify a fit with the experimental adsorption data for pseudo-first and pseudo-second order kinetics (Simonin, 2016). This was done to compare the adsorption of adenine and thymine on the different surfaces. The parameters obtained are shown in Table 2SM, and it can be observed that the adenine systems showed the best fit to the pseudo-second-order model. Although the fit was not perfect, these data help to corroborate that adenine adsorbs to the surfaces more strongly than thymine. This differential adsorption, as previously stated, can be attributed to the molecular structure of adenine, since its exocyclic amino and imidazole groups may be forming complexes with the metal atoms of the surfaces, especially komatiite and lizardite, which contain a higher amount of Mg (Mastropietro et al., 2007; Verma et al., 2010).
This, in turn, helps to understand the adsorption response of thymine. The fact that no good fit was obtained for any of the models indicates that the interactions of this nitrogenous base are governed by weak electrostatic forces. Furthermore, its desorption with increasing contact time reinforces the suggested enantiomeric changes, which require further analysis.
3.5. IMPLICATIONS IN PREBIOTIC CHEMISTRY STUDIES
It has been proposed that the origin of life depended on the interactions between the ocean, the primitive atmosphere, and rocks and minerals during the Archean. Hazen (2005) proposed four elementary steps for the emergence of living systems: i) the synthesis of biomolecules, ii) the formation of macromolecular systems, iii) the emergence of self-replicating cycles, and iv) the emergence of molecular evolution by natural selection. Geological surfaces may have played a role in all these steps, acting as key agents in facilitating the chemical processes that guided the transition from inorganic matter to living systems (Hazen, 2005, 2006). The results obtained in this work support the idea that rocks must have played an important role as surfaces concentrating adenine and thymine in prebiotic environments.
The superior adsorption of adenine over thymine, as demonstrated experimentally here, could support the importance of this molecule in different processes in living organisms today.
Considering that adenine is concentrated in greater quantities by geological surfaces may have allowed adenine to be more available for other reactions, which resulted in addition to being naturally important in nucleic acids, it is a molecule that is present in other fundamental biochemical processes such as the structure of enzymes as a cofactor, is present in second messengers such as NAD+, FADH2, and cAMP, all molecules essential for metabolic catalysis, and there is a fraction of adenine that plays a catalytic role at the ribosomal peptidyltransferase center (Verma et al., 2010). Additionally, it is present in molecules such as ATP, which is the source of energy for use and storage by the cell, as well as ADP and AMP, which are important molecules in energy transfer during metabolism (Dunn and Grider, 2020).
On the other hand, the nonlinear adsorption of thymine suggests that nucleic bases respond differently, and surfaces may have played a crucial role in configurational changes of molecules by modulating the stability or reactivity of organics. Reactivity, especially in carbon chemistry, must have been crucial for self-organization and the formation of reaction networks of organic molecules in complex systems that guided the origin of life. Likewise, stability, and especially dynamic stability, which is the property of prebiotic molecules to remain unchanged for a certain period also must have been fundamental for increasing the diversity of reaction pathways and subsequently organizing them at the macromolecular level in prebiotic scenarios (Pascal, 2025). For this to happen, the molecules need a place to stay safe from degradation caused by heat or other energy sources that could break them down; geological surfaces could have fulfilled this need.
Komatiites and serpentines like lizardite are important surfaces that have been attributed with relevant roles in chemical evolution. Serpentines are minerals that form under hydrothermal conditions through the alteration of ultramafic rocks rich in olivine and pyroxene. It has been proposed that the serpentinization process could have served as a source of metabolic chemical energy in primitive organisms, as it creates strongly reducing conditions and H2-rich fluids. In this scenario, the primitive rocks as komatiites could have provided an environment that favored the reactions necessary for the emergence of a primitive form of metabolism, raising the possibility that other bodies in the solar system with ultramafic rocks, such as Mars, Titan, Europa, and other moons of Jupiter, may also contain signs of past or present life (Gomes and Rautureau, 2021).
Also it has been observed that geological surfaces, and specifically tonalites and komatiites, are capable of promoting the formation of lipid vesicles through the surface concentration of fatty acids and catalyzing its self-assembly (Sahai et al., 2017). This reaffirms that the geological surfaces present on early Earth must have played an important role in the concentration and catalysis not only of organic molecules but also of pre-cellular elements. Because they are porous surfaces and adsorb molecules in these cavities, they can also protect molecules from direct contact with the environment and from degradation due to energy sources such as heat or UV rays, pH variations, or the presence of reactive chemical species.
Additionally, it has been proposed that the chemical composition of the solutions resulting from the weathering of komatiites and tonalites could be a determining factor for the availability of fundamental elements in the synthesis of ribonucleotide and the stability of protocells (Sahai et al., 2022). Therefore, studying rock surfaces and their interaction with the atmosphere and water is relevant to understanding the early planet’s geochemistry that allowed the formation of key molecular systems for the origin of life.
Taken together, these considerations underscore the importance of geological surfaces as concentrators and raise the possibility that they may have played more active roles during the formation of more complex molecular systems on early Earth. The adsorption responses observed in this study reinforce the proposal that mineral-organic interactions were key drivers of chemical evolution. Therefore, it is necessary to expand research on these complex systems in prebiotic chemistry to encompass the inherent complexity of heterogeneous surfaces, which can offer more realistic scenarios of early Earth and potentially other planetary bodies.
Conclusions
The results obtained show that more complex geological surfaces, such as rocks, are also capable of adsorbing organic molecules, like the nucleobases adenine and thymine. Kinetic behavior demonstrated that adenine adsorbs in greater amounts than thymine for all four surfaces. It was also observed that nucleobases adsorb through different mechanisms. As adenine adsorbed progressively over time, thymine tended to adsorb in a bell-shaped pattern for komatiite, tonalite, and plagioclase. Further research is needed to determine the specific mechanisms. However, the molecular structure and chemical characteristics of each surface in an aqueous medium may be mainly responsible for differential adsorption. This implies that the employed solids: komatiite, lizardite, tonalite, and plagioclase, chosen as representative components of early terrestrial crusts, might have influenced the adsorption of organic molecules, concentrating different prebiotic environments. Future studies are needed to better understand the role of complex surfaces on early Earth; they have to incorporate physicochemical changes in the environment, such as pH, salinity, and other nucleobases.
Contributions of authors
(1) Conceptualization: MCG; (2) Data analysis or acquisition: AECH, MCG; (3) Methodological development: AECH; (4) Drafting of the original manuscript: MCG, AECH; (5) Drafting of the revised and edited manuscript: AECH, MCG, EMM; (6) Interpretation: AECH, MCG, EMM; (8) Funding: MCG, EMM.
Funding
This research was partially supported by SECIHITI (A1-S-25341), DGAPA (IN218323), and PID2022-140180OB-C22 of the Spanish Ministry of Science and Innovation projects. AECH wants to acknowledge SECIHITI for the grant (738714) for Ph.D. studies.
Acknowledgments
The authors would like to thank Fernando Ortega, Antoni Camprubí, and Luca Ferrari for donating the rocks and mineral samples for this work. Additionally, Ulises Loredo Jaso, Rufino Lozano, and Luciano Antonio Gómez Cortés are acknowledged for their invaluable technical support.
Conflicts of interest
The authors declare that there is no conflict of interest, between themselves and other authors or institutions.
Handling editor
Alexander Correa.
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