3. Results
3.1. Comparative Model Performance and Implementation Feasibility
Four distinct topic-modeling approaches were systematically implemented and evaluated in order to assess their practical feasibility for domain-expert teams operating under typical institutional resource constraints. The comparative analysis encompassed MalletLDA (18 topics), ProdLDA (22 topics), BERTopic+SciBERT (22 topics), and SciBERT-NVCTM (20 topics), with performance assessed across multiple quantitative and qualitative metrics through six independent runs per model (seeds 42, 123, 456, 789, 1024, 2048;
Table 1). The practical model-selection guidance distilled from this benchmark — matching pipeline choice to a team’s expertise, hardware, and time budget — is consolidated as a six-step implementation framework in
Figure 1.
No single pipeline dominated across the evaluation metrics. On the coherence-oriented metrics the strongest models were SciBERT-NVCTM and BERTopic+SciBERT, with semantic coherence of 0.633 ± 0.009 and 0.612 ± 0.005 respectively, domain specificity of 0.645 ± 0.004 and 0.621 ± 0.005, and domain-expert score of 0.795 ± 0.002 and 0.804 ± 0.028. Values are reported as mean ± SD over six seeds; the corresponding t-based 95% confidence intervals (df = 5) are, for semantic coherence, BERTopic+SciBERT [0.607, 0.618] and ProdLDA [0.318, 0.337]; for domain specificity, BERTopic+SciBERT [0.616, 0.625] and ProdLDA [0.386, 0.404]; for domain-expert score, BERTopic+SciBERT [0.774, 0.833], ProdLDA [0.585, 0.649], and MalletLDA [0.663, 0.708]; and for topic diversity, ProdLDA [0.937, 0.949], BERTopic+SciBERT [0.717, 0.752], and MalletLDA [0.540, 0.579]. For the SciBERT-NVCTM variant (n = 6 seeds) the corresponding t-based 95% confidence intervals are: semantic coherence [0.624, 0.643], domain specificity [0.640, 0.649], domain-expert score [0.793, 0.798], and C_v coherence [0.400, 0.427]. The model-metric intervals adopt the parametric Student-t method, appropriate for the mean of six continuous-valued seeds, whereas the LLM flag-rate intervals reported below adopt the bootstrap, appropriate for binary per-paper outcomes. ProdLDA (a paper-faithful re-implementation of Srivastava & Sutton [
7]) obtained intermediate coherence-oriented scores (C_v 0.408 ± 0.018, semantic coherence 0.327 ± 0.009, domain specificity 0.395 ± 0.008, domain-expert 0.617 ± 0.030), but achieved the highest topic diversity of all models (0.943 ± 0.006) and the highest field coverage (0.062 ± 0.001), at the lowest wall-clock among the neural pipelines (≈48 s per run). Pairwise Bonferroni-corrected comparisons confirmed these differences as highly significant for every metric (e.g., domain specificity ANOVA F = 6250.7, p < 0.001; topic diversity F = 1073.1, p < 0.001; see
Table 2). MalletLDA provided a stable, low-cost surface-term baseline (C_v 0.542 ± 0.009, domain-expert 0.686 ± 0.021) with the lowest semantic coherence (0.081 ± 0.009) and a low run-to-run variability (CV < 13% on most metrics). Custom corpus-derived vocabulary construction improved coherence and domain specificity relative to a generic vocabulary across all models.
Perplexity was computed for each pipeline but is not tabulated in the main text: the four architectures define their held-out likelihoods on different scales (Gibbs-sampled topic-word distributions for MalletLDA, variational bounds for ProdLDA and SciBERT-NVCTM, while no generative likelihood is defined for the c-TF-IDF representation of BERTopic+SciBERT), so cross-model perplexity comparisons are not meaningful; per-model values are reported, with this caveat, in Supplementary
Tables S2-S3. Perplexity is in any case treated as a secondary metric and is not used as a selection criterion, in agreement with the observation of Chang et al. [
21] that perplexity correlates poorly with human quality judgements in specialized scientific domains.
3.2. Thematic Structure Characterization and Topic Distribution Analysis
Each modeling approach generated a distinct thematic organization, reflecting different analytical strengths and implementation trade-offs that are relevant for domain-expert methodology selection. As quantified by the topic-diversity metric in
Table 1, the four pipelines differ systematically in thematic-separation quality, with direct implications for how readily a domain expert can tell topics apart: ProdLDA resolves the most distinct topics (diversity 0.943 ± 0.006) and, correspondingly, the lowest inter-topic vocabulary overlap, followed by BERTopic+SciBERT (0.734 ± 0.017) and MalletLDA (0.558 ± 0.011), whereas SciBERT-NVCTM yields the most overlapping topics (0.497 ± 0.015) — a trade-off in which its correlation-aware architecture favours thematically adjacent topics over maximally disjoint ones.
MalletLDA produced 18 clearly delineated topics with strong interpretability for exploratory analysis. The model effectively captured broad thematic categories with minimal computational overhead, which makes it accessible for an initial literature exploration by resource-constrained teams. Topic-by-year normalized relevance values exhibit extremes that are interpretable to domain experts but that we frame as descriptive proportions of the analyzed corpus rather than as evolutionary signal: Topic 0 (characterized by "fly ash, coal fly ash, process, carbonation efficiency") has its high-relevance assignments concentrated in 2013, with no high-relevance assignments thereafter, while Topic 17 ("ca_oh, crystal, calcite, calcium_carbonate") reaches its highest normalized relevance in 2025 (0.27). Given the temporal asymmetry of the corpus (19.9% pre-2017 vs 69.9% post-2020), we explicitly refrain from interpreting these extremes as causal evolutionary trajectories; the methodological observation is that MalletLDA produces topic-by-year distributions whose extremes are accessible to domain-expert reading, the substantive interpretation being left to the cluster-taxonomy analysis below, where the corpus-asymmetry caveat is operative throughout.
ProdLDA generated 22 topics with enhanced semantic granularity, effectively capturing nuanced thematic relationships beyond traditional keyword-clustering approaches. Because the paper-faithful re-implementation changes the topic indexing, individual ProdLDA topic_id references from earlier drafts are no longer used here; the model-level result that survives is the highest-in-benchmark topic diversity of ProdLDA (0.943 ± 0.006). ProdLDA also achieved the highest field coverage of the benchmark (0.062 ± 0.001), indicative of a comparatively even distribution across CO2 mineralization subfields. The increased topic granularity, however, created additional validation requirements for domain experts to distinguish meaningful themes from statistical artifacts.
BERTopic+SciBERT exploited its scientific-literature pre-training to produce 22 topics with superior technical-terminology recognition and methodological categorization. The transformer-based architecture excelled at differentiating research focused on experimental methodologies from application-oriented studies. Topics related to technical parameters and experimental conditions maintained a consistent presence across multiple temporal periods, indicative of the strength of the model in capturing fundamental concepts that remain central irrespective of temporal trends. BERTopic+SciBERT attained field-coverage scores of 0.052 ± 0.001, second only to ProdLDA (0.062 ± 0.001; the highest of the benchmark), although temporal-pattern analysis revealed a more sporadic evolution compared with the other approaches, possibly reflecting a sensitivity to lexical variation in scientific writing conventions.
SciBERT-NVCTM generated 20 topics with a distinctive emphasis on temporal research dynamics through neural variational correlation modeling. Notably, Topic 4 ("large scale, study we, energy intensive, mineralization") exhibited a systematic decline from an early high relevance (2013: 0.415) to a reduced prominence (2024: 0.086), whereas Topic 18 ("long term, mineralization which, pre-treatment, stability") emerged strongly in 2022 (0.113). These patterns may indicate potential transitions from conceptual large-scale discussions towards a practical implementation focus, although alternative explanations, including a methodological bias towards recent terminology, cannot be excluded.
3.3. Three Thematic Macro-Clusters in the Corpus
Topic-distribution analysis across all four models reveals three thematic macro-clusters that coexist in the analyzed corpus, each characterized by a distinct vocabulary, methodological orientation, and substrate focus. We deliberately frame these clusters as concurrent thematic strands rather than as a temporal sequence: the corpus exhibits a substantial temporal asymmetry (69.9% of documents from 2020–2025 vs 19.9% from 2013–2017) that prevents the reliable inference of evolutionary trajectories. The three clusters described below thus describe what the corpus contains, not how it has historically evolved.
Cluster A — Foundational mechanisms and reaction kinetics. Across models, this cluster aggregates topics characterized by terms such as dissolution kinetics, basaltic glass, hydromagnesite, divalent-cation chemistry, batch-reactor experiments, calcite and aragonite phase formation, and rock-fluid interaction. Representative topics include MalletLDA T15 (rates dissolution_rates dissolution), MalletLDA T8 (calcite basaltic_glass system), BERTopic+SciBERT T0 (hydromagnesite porosity mineralization mechanical), and SciBERT-NVCTM T1 (analysis process mineral temperature precipitation). This cluster represents the physico-chemical foundation of the field — fundamental investigations of carbonation pathways, thermodynamic and kinetic regimes, and primary mineral substrates.
Cluster B — Process engineering and industrial-residue valorization. This cluster aggregates topics characterized by terms such as carbonation efficiency, mine tailings, coal fly ash, steel slag, gas-solid reactors, leaching processes, and operational parameters. Representative topics include MalletLDA T9 (process carbonation mine_tailings), BERTopic+SciBERT T1 (CO2 mineralization, CO2 capture, processing, carbonation), ProdLDA T18 (cement kiln dust, concentration was measured, precipitation of secondary), and SciBERT-NVCTM T12 (gas solid, large scale, kinetics, thermal). It collects work translating fundamental knowledge into reproducible processing pathways and into the valorization of alkaline industrial residues, an area that has expanded rapidly within the available corpus.
Cluster C — Application-oriented and integrated systems. This cluster aggregates topics characterized by terms such as compressive strength, supplementary cementitious materials, membrane and electrochemical processes, brine and seawater treatment, pre-treatment integration, and long-term stability. Representative topics include MalletLDA T7 (carbonation compressive_strength hydration), BERTopic+SciBERT T6 (calcite, binder ratio, carbonation curing), ProdLDA T16 (CO2 mineralization plants, process, containing CO2), and SciBERT-NVCTM T18 (long term, mineralization which, pre-treatment, stability). It collects work on application contexts (cement industry, desalination water-carbon nexus) and on integrated multi-process systems combining mineralization with other capture or treatment steps.
Although the three clusters do exhibit different relative weights across the temporal periods sampled (
Figure 2) — Cluster A more prominent in pre-2017 papers (48.3% vs 40.9% in 2022-2025, four-pipeline mean), Cluster B expanding after 2016, and Cluster C increasing modestly toward 2022-2025, most markedly in MalletLDA — we explicitly refrain from claiming that this reflects a true historical evolution of the field, given the corpus temporal asymmetry. The relative-weight tables (top-3 topics per year for each model) are provided in the Supplementary Material as descriptive statistics rather than as evolutionary trajectories. The cluster taxonomy is stable across the four topic models — that is, each model independently partitions its topics into approximately the same three macro-areas — which supports the interpretation that the clusters are robust features of the corpus rather than artifacts of any single modeling approach. This robustness rests at the term level on well-separated underlying topics: as the within-model topic-similarity matrices in
Figure 3 make explicit, the pairwise Jaccard overlap of the top-15 topic terms stays below 0.15 for the large majority of topic pairs in every pipeline — sparsest for ProdLDA and BERTopic+SciBERT and densest for MalletLDA, in agreement with the topic-diversity ranking of
Table 1 — so the shared three-cluster taxonomy aggregates distinct topics rather than redundant ones.
3.4. Research Direction Discovery and Innovation Identification Methodologies
The integration of topic modeling with outlier-detection methodologies revealed distinct patterns of research innovation and emerging directions within the CO2 mineralization literature. Our ensemble approach, combining multiple anomaly-detection algorithms with semantic analysis, identified 9 documents (3.11% of the 289-document outlier-analysis corpus; 9/289 = 3.114%) exhibiting statistically distinctive characteristics suggestive of innovative research trajectories.
3.5. Outlier Detection Performance and Validation
The multi-method ensemble approach achieved a robust performance in identifying semantically distinctive documents within our corpus constraints. The detection framework combined Isolation Forest (weight: 0.3), Local Outlier Factor (0.3), distance-based metrics (0.2), and semantic-diversity measures (0.2), producing ensemble scores ranging from 0.722 to 0.816 for the identified outliers. Statistical validation confirmed a significant semantic distance between outlier and mainstream documents (p < 0.001, Cohen's d = 1.24), with outliers showing 42% higher lexical diversity (measured as type-token ratio, TTR, on the title+abstract text after pre-processing; see Methods, Evaluation Metrics) and 38% more cross-domain terminology (operationalized as the fraction of terms in each document that fall outside the top-95% frequency band of the corpus vocabulary, i.e., terms occurring in fewer than 5% of corpus documents).
The temporal distribution of the identified outliers revealed concentrated innovation periods, with 66.7% occurring between 2021 and 2023. This pattern co-occurs with the cross-temporal proportions of the three macro-clusters described above (Cluster A more prominent in pre-2017 papers, Cluster C increasing modestly toward 2022-2025), and is consistent with the substantial temporal asymmetry of the corpus (69.9% post-2020). We deliberately refrain from interpreting this co-occurrence as a convergent demonstration of an evolutionary trajectory: as noted in the cluster section, the corpus temporal asymmetry prevents reliable causal-temporal inference, and the apparent temporal alignment between outlier dates and cluster prominence reflects, in part, the underlying sampling distribution.
3.6. Characterization of Research Innovation Patterns
The identified outliers fall into three distinct innovation categories, each representing a different mechanism of scientific advancement within CO2 mineralization research.
Cross-domain integration (33.3% of outliers): documents introducing concepts from adjacent fields showed the highest outlier scores. Xie et al. [
22] (score: 0.816) pioneered electricity generation through CO2 mineralization cells, representing the strongest deviation from conventional approaches. Similarly, Luong, Veyret & Boily [
23] (score: 0.754) introduced nanotechnology through MgO nanocubes in nanometric water films, demonstrating a successful integration of materials-science innovations. These cross-domain outliers consistently exhibited unique terminology clusters absent from the mainstream corpus.
Methodological innovation (44.4% of outliers): novel experimental or analytical approaches characterized the largest outlier category. Coppola et al. [
24] (score: 0.798) introduced direct dry carbonation in fluidized beds, eliminating traditional wet-processing steps. Strunge, Renforth & Van der Spek [
25] (score: 0.739) applied uncertainty-quantification frameworks to techno-economic analysis, introducing risk-assessment methodologies uncommon in the field. Semantic analysis revealed that these papers introduced an average of 12.3 unique technical terms per document, compared with 3.2 for mainstream publications ("unique technical terms" defined as tokens in the document title+abstract that do not appear in the corpus-wide top-90% frequency band of the custom CO2-mineralization vocabulary; the difference was tested through a Welch's two-sample t-test on the per-document term counts, n_outliers = 9 vs n_mainstream = 277, t = 6.84, p < 0.001).
Application-domain extension (22.2% of outliers): documents extending CO2 mineralization to novel application contexts formed a distinct cluster. Callagon La Plante et al. [
26] (score: 0.756) explored gigatonne-scale saline-water mineralization pathways, whereas Moon et al. [
27] (score: 0.731) applied computational fluid dynamics to cement-industry applications. These outliers retained the core mineralization concepts while introducing domain-specific adaptations.
3.7. Validation Within Corpus Constraints
Acknowledging our corpus limitations (286 documents, 69.9% post-2020, English-only), we validated the outlier-detection methodology through multiple approaches rather than claiming an absolute innovation identification. Stability analysis across five independent runs showed an 88.9% consistency in outlier identification (8 of 9 documents consistently flagged across all 5 runs; non-parametric bootstrap 95% CI for the per-document consistency rate on the n = 45 binary observations: [78.5%, 96.3%]), indicative of robust detection despite the stochastic elements in the algorithms. Expert assessment of the top 5 outliers confirmed their substantive methodological or conceptual divergence from mainstream approaches, although we cannot claim that these represent all global innovations in CO2 mineralization.
The conservative detection threshold (targeting 5%, achieving 3.11%) minimized false positives while potentially missing some innovative work. The 5% target was set as the upper percentile of the calibrated ensemble-score distribution; the achieved rate of 3.11% (9/289) reflects the additional constraint that the four base detectors (Isolation Forest, LOF, distance-based, semantic-diversity) jointly assigned scores above their respective per-method thresholds. This trade-off was intentional, prioritizing precision over recall given the exploratory nature of innovation identification. The strong correlation between ensemble scores and expert innovation ratings (r = 0.76, p < 0.01) suggests that the automated approach successfully captures human judgements of research novelty within the available corpus.
3.8. Integration with Topic Evolution Patterns
Cross-referencing the outliers with the topic-modeling results revealed systematic relationships between thematic structure and innovation emergence. Outliers predominantly aligned with emerging or declining topics rather than with stable mainstream themes: peripheral and emerging topics showed a stronger correlation with recent outliers, whereas traditional carbonation topics showed an inverse correlation with outlier status (specific ProdLDA topic_id references are omitted here because the paper-faithful re-implementation changes the topic indexing). This pattern suggests that innovations often emerge at thematic boundaries or during topic-transition periods, in agreement with theoretical frameworks of scientific innovation occurring at disciplinary interfaces.
Network analysis of the topic relationships further illuminated innovation pathways, with outlier documents serving as bridges between previously disconnected thematic clusters. Documents with a high betweenness centrality in the topic network showed a 3.2 times higher probability of being classified as outliers, which confirms their role in connecting disparate research areas. This finding provides actionable guidance for the identification of future innovation opportunities at the intersection of established research themes.
3.9. Domain-Specific Findings on CO2 Mineralization Research
While the primary contribution of the present study is methodological, the four-pipeline benchmark and the LLM-augmented analysis also surface domain-specific findings of direct relevance to the CO2 mineralization research community, which we summarize here and document in full in the Supplementary Material (Section S9). Topic-distribution analysis across the four classical pipelines and the LLM-generated descriptive labels converge on three coexisting thematic macro-clusters — foundational mechanisms and reaction kinetics (Cluster A), process engineering and industrial-residue valorization (Cluster B), and application-oriented and integrated systems (Cluster C) — whose vocabulary signatures and representative topics are reported in
Supplementary Tables S4–S7. Method triangulation (calibrated statistical ensemble, high-recall LLM screen R4, high-precision LLM filter R3) further identifies a set of 13 LLM-identified, partially expert-validated innovation-landmark papers, of which 5 are jointly confirmed by the statistical ensemble and at least one LLM mode and 8 are flagged by R3 self-reflection only, the latter corresponding to historical or pioneering field landmarks whose embedding-space distinctiveness is moderate but whose conceptual-narrative novelty is articulable. The full landmark list with bibliographic details cross-validated against Crossref and Web of Science, together with the high-betweenness bridge-term analysis of interdisciplinary integration opportunities, is provided in Supplementary Section S9. We emphasize that these findings are bounded by the corpus characteristics (286 papers, 69.9% post-2020, English-only) and should be interpreted as descriptive of the analyzed corpus rather than as exhaustive characterizations of the field at large; a focused follow-up analysis dedicated entirely to the CO2 mineralization research landscape, using the methodology validated here, is in preparation.
3.10. LLM Zero-Shot Baseline and Calibration Ablation
In order to address the question of whether large-language-model approaches can substitute the calibrated statistical ensembles described above, we performed a controlled four-level ablation of Claude Haiku 4.5 zero-shot topic extraction over the same 286-paper corpus. The LLM ablation operates on the 286-paper text corpus, whereas the statistical outlier ensemble operates on a 289-document set that additionally includes three records carried by the detection pipeline; the two denominators are reported as such rather than forced to a common value, and the ~3.11% ensemble rate corresponds to 9/289 = 3.114%. The four runs differed only in the calibration mechanism applied to the innovation-flag (is_outlier_candidate) decision: (R1) naïve zero-shot with no calibration anchor; (R2) qualitative-strict prompt requiring outlier flags to be grounded in one of five pre-defined novelty dimensions (mechanism, material, cross-domain, magnitude, application context) and to list at least two established alternatives; (R3) self-reflection multi-pass, in which Haiku critically rereads its own R1 outputs and either confirms or downgrades each flag against the strict criteria; and (R4) a unified one-shot prompt that fuses the R2 criteria with the ten-year-citation thought experiment used in R3 within a single inference pass. The total cost across the four runs was USD 5.40 and the total runtime 115 minutes, on consumer hardware (Mac Mini M2, 16 GB RAM) and without fine-tuning, retrieval augmentation, or specialized infrastructure.
The four LLM modes produced markedly different outlier-flag rates (
Table 3): R1 flagged 203/286 papers (71.0%, an over-attribution factor of 22.8× relative to the 3.11% identified by the calibrated ensemble), R2 reduced this to 76/286 (26.6%, 8.5×), R4 to 80/286 (28.0%, 9.0×), and R3 to 10/286 (3.5%, 1.1×). The bootstrap 95% confidence intervals (10,000 resamples) for these rates are R1 [65.7%, 76.2%], R2 [21.7%, 31.8%], R4 [23.1%, 33.2%], and R3 [1.4%, 5.6%]; the calibrated statistical ensemble rate (3.11%) falls within the R3 interval, and the R2 and R4 intervals overlap substantially, consistent with a shared prompt-level floor near 28% rather than with two distinct rates. Two findings stand out. First, R2 and R4 — two structurally distinct prompts that both impose strict qualitative criteria — converge on nearly identical flag rates, which indicates that prompt-level calibration encounters a natural floor at approximately 28% that cannot be reduced further by prompt sophistication alone. Second, R3 self-reflection achieves convergence with the statistical ensemble (3.5% vs 3.11%) and, importantly, the 10 papers flagged by R3 are a strict subset of the 80 flagged by R4 (R3 ⊂ R4, Jaccard 0.125 against the larger R4 pool). This subset relationship excludes the interpretive concern that the model is merely deferring to authority under a stricter prompt frame: R3 applies an internally consistent discriminative criterion that identifies the most defensible candidates from a pre-screened pool rather than declassing randomly.
Topic agreement between Haiku R1 and the four classic models, measured by Jaccard plus soft overlap on the per-paper top-1 topic assignment and reported under three calibrations to control for vocabulary heterogeneity, was: MalletLDA 33.2%, ProdLDA 24.1%, BERTopic+SciBERT 29.0%, and SciBERT-NVCTM 27.3% (Z-score > μ+0.5σ rate). The four classic models converge with the LLM on the central themes of CO2 mineralization (basalt in-situ sequestration, fly-ash and slag carbonation, brine-based pathways) but diverge on peripheral or methodological themes — a pattern consistent with complementary roles, the LLM capturing semantic intent in a single pass and the statistical models revealing distributional regularities that may be semantically diffuse.
The pick-level overlap between the LLM modes and the calibrated ensemble's declared outliers further characterizes the complementarity. Of the nine declared outliers from the classic ensemble that are uniquely identifiable in our corpus by author-year, R4 captures five (Callagon La Plante et al. [
26], Coppola et al. [
24], Luong et al. [
23], Strunge et al. [
25], Moon et al. [
27]), whereas R3 captures only two (Callagon La Plante et al. [
26], Luong et al. [
23]). The eight R3 outliers absent from the classic list — Alqahtani et al. [
28] (cation exchange in zeolites), Myers & Nakagaki [
29] and Myers et al. [
30] (gas-solid mineralization framework, brine processing), Gislason & Oelkers [
31] (basalt rapid trapping), Matter et al. [
32] (CarbFix pilot), Sharifian et al. [
33] (bipolar-membrane electrodialysis of seawater), Sigfusson et al. [
34] (first full-scale dissolved-CO2 injection), and Pogge von Strandmann et al. [
35] (calcium-isotope quantification of in-situ rates) — represent field landmarks identifiable from domain-narrative cues that the embedding-based statistical detector did not surface. The two LLM modes (R3 high-precision, R4 high-recall) and the classic ensemble thus detect different signal types in the corpus, which supports triangulation rather than substitution. A methodologically important observation emerged during the verification of the R3 output: while accurate in identifying conceptually distinctive papers, R3 self-reflection returned bibliographic metadata (authors, year, journal) with a non-negligible error rate. Six of the thirteen initial R3 candidates contained one or more metadata errors — ranging from an incorrect year and an incorrect journal to fabricated publication dates — which required systematic cross-validation against Crossref and Web of Science prior to inclusion. This observation directly motivates the fourth verification layer of the triangulated workflow described below (see Calibration Regimes of LLM-Based Innovation Detection), and is itself a non-trivial finding on the operational use of LLM self-reflection for innovation-landmark identification.