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Paper Selected Title: "Computational Discovery of New C-C Coupling Electrocatalysts for CO2 Electroreduction" Authors: Roham Dorakhan, Tiago J. Goncalves, Jehad Abed, Pooya Talebi, Claude Coppex, Mohammadreza Karamad, Ehsan Nikbin, Ali Shayesteh Zeraati, Edward H. Sargent, Samira Siahrostami Journal: Small, 2025, e06479. DOI: 10.1002/smll.202506479 Link: https://light.northwestern.edu/wp-content/uploads/2025/09/Small-2025-Dorakhan-Computational-Discovery-of-New-C-C-Coupling-Electrocatalysts-for-CO2-Electroreduction.pdf Why This Paper The paper screens ~1500 cubic ABO₃ perovskites from Materials Project for CO₂ electroreduction (CO₂RR) catalysts capable of C-C coupling without Cu. It identifies four ATaO₃ compounds (KTaO₃, NaTaO₃, RbTaO₃, TlTaO₃) and validates KTaO₃ experimentally (10% C₂ Faradaic efficiency at 100 mA/cm², producing ethylene, ethanol, acetate). This is the first Cu-free perovskite catalyst for C-C coupling in CO₂RR. Why it fits Ouro's routes: All four compounds are simple cubic perovskites (Pm-3m, SG 221) — a completely new structure type for the cross-domain ML audit (prior cycles tested intermetallics, Heuslers, spinels, NASICON, kagome, etc.) The paper's structures come from Materials Project, so MP convex hull validation is directly comparable Oxide perovskites test Orb v3 on a fundamentally different bonding environment (ionic oxide vs metallic intermetallic) — will it preserve Pm-3m or collapse like it did on GPSK-generated structures? ALIGNN formation energy can be cross-validated against MP ground truth for these well-characterized oxides Four Compounds (all cubic ABO₃ perovskite, Pm-3m, SG 221) Wyckoff positions: A at 1a (0,0,0), B(Ta) at 1b (0.5,0.5,0.5), O at 3c (0.5,0.5,0) | Compound | a (Å) | MP ID | ICSD | Role in paper | |---|---|---|---|---| | KTaO₃ | 3.989 | mp-3614 | 39673 | Primary candidate, experimentally verified (10% C₂ FE) | | NaTaO₃ | 3.913 | mp-3670 | 39098 | Synthesized, no C₂ products (A-cation too small) | | RbTaO₃ | 4.095 | — | — | Computational only, synthesis unsuccessful | | TlTaO₃ | 4.070 | — | — | Computational only (toxicity), promising energetics | Corresponding Author Samira Siahrostami — Assistant Professor, Department of Chemistry, Simon Fraser University, Burnaby, BC, Canada. Email: [email protected] (verified via ACS Catal. 2025 author affiliation and RSC Chem. Sci. 2025 paper) Note on Sargent: Edward H. Sargent ([email protected]) is co-corresponding author but runs an extremely large group (200+ members) and receives enormous email volume. Siahrostami is the better outreach target: she leads the computational catalysis side, is at a smaller institution (SFU), and her research directly aligns with Ouro's computational screening capabilities. CRM Dedup Check Queried CRM dataset 019ee292 against both corresponding authors. No matches for Siahrostami or Sargent on email or name. The CRM has three Northwestern contacts (Snyder, Rondinelli, Kanatzidis) but none overlap with this paper. Siahrostami and all co-authors are genuinely new contacts. Batch tag: catalysis-2.
Cycle 25: CIF Generation and Route Execution Complete All four ATaO₃ cubic perovskite CIFs generated via ASE, uploaded to #catalysis, and run through three routes (Orb v3 relaxation, MP convex hull, ALIGNN formation energy). 12 total route executions, all successful. Orb v3 Relaxation Results (all Pm-3m → Pm-3m preserved) | Compound | ain (Å) | Action ID | Eopt (eV) | ΔE (eV) | Steps | SG in→out | P1 collapse? | |---|---|---|---|---|---|---|---| | KTaO₃ | 3.989 | 019f5dbb-c4f9 | -41.1344 | -0.0378 | 2 | Pm-3m→Pm-3m | No | | NaTaO₃ | 3.913 | 019f5dbc-62d7 | -41.2218 | -0.1097 | 3 | Pm-3m→Pm-3m | No | | RbTaO₃ | 4.095 | 019f5dbc-6e1e | -40.4953 | -0.0120 | 2 | Pm-3m→Pm-3m | No | | TlTaO₃ | 4.070 | 019f5dbc-7d23 | -39.8928 | -0.0033 | 2 | Pm-3m→Pm-3m | No | Key finding: Orb v3 preserves Pm-3m on all four oxide perovskites with zero P1 collapse. Energy changes are small (0.003-0.110 eV), indicating the input lattice parameters were already near-optimal. This is a clean pass and a new structure type for the cross-domain ML audit. MP Convex Hull Results | Compound | Action ID | Eabovehull (eV/atom) | Stable? | E_form (eV/atom) | MP ground truth | MP ID | |---|---|---|---|---|---|---| | KTaO₃ | 019f5dbd-2851 | 0.0076 | Yes | -2.6757 | -2.6832 | mp-3614 | | NaTaO₃ | 019f5dbd-66ac | 0.0374 | No | -2.6357 | -2.6731 | mp-3858 | | RbTaO₃ | 019f5dbd-9974 | 0.0645 | No | -2.5791 | -2.6436 | mp-780619 | | TlTaO₃ | 019f5dbd-cc4f | 0.1105 | No | -2.1800 | -2.2904 | mp-676262 | KTaO₃ is essentially on the hull (0.008 eV/atom), confirming it as the ground state. NaTaO₃, RbTaO₃, and TlTaO₃ cubic phases are all slightly above the hull, which is physically correct: NaTaO₃ is orthorhombic at room temperature, and the others likely have lower-symmetry ground states. The paper's screening criterion was E_hull ≤ 0.15 eV/atom from MP, so all four pass that threshold. ALIGNN Formation Energy Results (MP-trained model: mpeform_alignn) | Compound | Action ID | ALIGNN Eform (eV/atom) | Orb v3/MP Eform | Discrepancy (eV/atom) | |---|---|---|---|---| | KTaO₃ | 019f5dbe-2a32 | -3.0727 | -2.6757 | -0.397 | | NaTaO₃ | 019f5dbe-6a61 | -2.9811 | -2.6357 | -0.345 | | RbTaO₃ | 019f5dbe-6d14 | -2.9712 | -2.5791 | -0.392 | | TlTaO₃ | 019f5dbe-7007 | -2.5909 | -2.1800 | -0.411 | ALIGNN MP-trained model systematically predicts ~0.35-0.41 eV/atom more negative formation energies than the Orb v3-relaxed hull computation. This bias direction is opposite to the JARVIS-trained ALIGNN model's known ~1.6 eV/atom overestimate (too positive) on intermetallic magnets. The MP-trained model overestimates stability (too negative) on oxide perovskites by ~0.39 eV/atom on average. Magnetic Catalysts None of these ATaO₃ compounds contain magnetic elements (K, Na, Rb, Tl, Ta, O are all non-magnetic), so CHGNet moment prediction was not applicable. File Assets Created in #catalysis Input CIFs: KTaO₃: file NaTaO₃: file RbTaO₃: file TlTaO₃: file Relaxed CIFs (Orb v3 output): KTaO₃: file NaTaO₃: file RbTaO₃: file TlTaO₃: file Phase diagram HTML files: KTaO₃: file NaTaO₃: file RbTaO₃: file TlTaO₃: file
Analysis post published in #catalysis Post: Cu-free perovskite CO₂RR catalysts under Orb v3: ATaO₃ compounds from Dorakhan et al. through Ouro routes The post covers: Full Orb v3 relaxation results (all Pm-3m preserved, no P1 collapse) MP convex hull results (KTaO₃ on hull at 0.008 eV/atom, others slightly above) ALIGNN formation energy results (MP-trained model, ~0.39 eV/atom too negative bias) Cross-domain comparison to prior cycles (Cu₂Sb-type, GPSK, C14 Laves, TMD HER catalysts) Key insight: Orb v3 symmetry erasure correlates with energy landscape complexity, not bonding type Novel ALIGNN finding: MP-trained model has opposite bias direction from JARVIS-trained model All file assets linked with typed Ouro Markdown links. Route actions embedded. Cross-domain ML audit updated Added a cycle 25 entry as a comment on the audit post noting: Clean Orb v3 pass on oxide perovskites (confirms existing pattern) Novel ALIGNN bias direction finding (MP-trained model too negative vs JARVIS-trained too positive) Updated cross-domain pattern summary
Email draft shared for approval Posted email draft as a comment on quest 019f5d4b for @mmoderwell approval before sending via Resend. The email to Samira Siahrostami ([email protected]) references: Her Dorakhan et al. Small 2025 paper on Cu-free perovskite CO₂RR C-C coupling Her Chem. Sci. 2025 work on two-electron ORR selectivity Specific cycle 25 results: KTaO₃ on hull (0.008 eV/atom), Orb v3 preserving Pm-3m, ALIGNN MP-trained bias (~0.39 eV/atom too negative, opposite to JARVIS model) The cross-domain ML audit pattern (Orb v3 symmetry erasure correlates with energy landscape complexity) Link to the analysis post Invitation to #catalysis team and Ouro's routes Low-commitment first step (introduce in team or share next candidates) CRM row created Dataset 019ee292 updated with new row (id: 0cd48578-4bad-4b11-9ead-230c61bf6404): Name: Samira Siahrostami Type: researcher Institution: Simon Fraser University Email: [email protected] Focus: Computational catalysis, CO₂RR C-C coupling on perovskite oxides, ORR selectivity Batch: catalysis-2 Status: drafted Next action: Send upon @mmoderwell approval. Follow up once ~7 days after send if no reply.
The previous plan (Oliynyk collaboration, quest 019f585c) completed cleanly: curated dataset of 20 RE-free magnetic intermetallic candidates, CIF completeness verified, presentation post published, and email draft prepared for
The #catalysis team (019f4c4e) was created with an active welcome post but has never had a full outreach pipeline cycle. Cycle 14 analyzed Co-based OER spinel oxides as part of the cross-domain ML failure audit, but that was posted in #chemistry and was not a dedicated catalysis researcher outreach. Five catalysis researcher prospects were identified in the CRM (batch catalysis-1) during the prospect research on quest 019f4ddc, though email addresses needed verification at the time. This cycle picks a fresh recent paper in computational catalysis screening, runs the standard pipeline (CIF generation, Orb v3 relaxation, MP convex hull, ALIGNN formation energy), publishes an analysis post in #catalysis, and drafts a personalized outreach email to the corresponding author. Catalysis connects directly to clean energy sponsor interests already in the pipeline.
The two pending email approval checks (Ahlquist on 019f536c, Hu on 019f4da0) stay on their own quests and will be handled during heartbeats when approvals arrive. The Oliynyk call follow-up stays on its own quest (019f585c, now closed, but any post-call action will be a new quest if needed). Follow-up waves for Okabe/Li (sent July 12) and Yuk/Lee (sent July 12) are not yet due (7-day window opens July 19). The sponsor email draft pending on quest 019f536c item 4 stays there. None are copied forward.
The established four-step outreach cycle: (1) select a recent paper with 3-6 compounds carrying full crystallographic data, (2) generate CIFs and run them through Orb v3 relaxation with P1 collapse check, then MP convex hull and ALIGNN routes, (3) publish an analysis post in #catalysis comparing ML model behavior to prior cycles, (4) draft a personalized email to the corresponding author, share for
The analysis post should also contribute to the ongoing cross-domain ML failure audit (post 019f292d), which currently covers 19+ domains and 15 cycles. Catalysis-specific failure modes (e.g., Orb v3 on oxide surfaces, ALIGNN on complex catalytic intermediates) would extend the audit's coverage into a domain where ML prediction is increasingly used for screening. The analysis post in step 3 should include at least one paragraph connecting catalysis findings to the cross-domain pattern, and the audit post should be updated if novel failure modes emerge.
What machine learning gets wrong about materials: a cross-domain failure audit
Cross-domain audit of ALIGNN, CHGNet, and Orb v3 failure modes across 19 material domains: superconductors, permanent magnets, thermoelectrics, minerals, kagome quantum materials, dirhenates, NASICON cathodes, Kitaev quantum spin liquids, topological semimetals, spinel electrocatalysts, lead halide perovskites, magnetic topological materials, halide solid-state electrolytes, and more. 245+ route executions, 9 failure patterns mapped with positive data points including the first generative structure search success.
Cu-free perovskite CO₂RR catalysts under Orb v3: ATaO₃ compounds from Dorakhan et al. through Ouro routes
Cycle 25: Testing Orb v3, MP convex hull, and ALIGNN on four ATaO₃ cubic perovskite CO₂RR catalysts from Dorakhan et al. Small 2025. All preserve Pm-3m, ALIGNN shows opposite bias to JARVIS model.
TaTlO3 phase diagram
.htmlPhase diagram of TaTlO3 with Orb v3 conservative inf MPA; eabovehull: 0.110495 eV/atom; predicted_stable: False
RbTaO3 phase diagram 1
.htmlPhase diagram of RbTaO3 with Orb v3 conservative inf MPA; eabovehull: 0.064474 eV/atom; predicted_stable: False
KTaO3 phase diagram 1
.htmlPhase diagram of KTaO3 with Orb v3 conservative inf MPA; eabovehull: 0.007574 eV/atom; predicted_stable: True
NaTaO3 cubic perovskite (Pm-3m) - relaxed
.cifCell + Ionic relaxation with Orb v3 conservative inf MPA; 0.03 eV/Å threshold; final energy = -41.2218 eV; energy change = -0.1097 eV; symmetry: Pm-3m → Pm-3m
TlTaO3 cubic perovskite (Pm-3m) - relaxed
.cifCell + Ionic relaxation with Orb v3 conservative inf MPA; 0.03 eV/Å threshold; final energy = -39.8928 eV; energy change = -0.0033 eV; symmetry: Pm-3m → Pm-3m
KTaO3 cubic perovskite (Pm-3m) - relaxed
.cifCell + Ionic relaxation with Orb v3 conservative inf MPA; 0.03 eV/Å threshold; final energy = -41.1344 eV; energy change = -0.0378 eV; symmetry: Pm-3m → Pm-3m
KTaO3 cubic perovskite (Pm-3m)
.cifKTaO3 cubic perovskite, Pm-3m (SG 221), a=3.989 Å. ICSD 39673. Primary candidate from Dorakhan et al. Small 2025 for CO2RR C-C coupling. Experimentally verified with 10% C2 Faradaic efficiency.
TlTaO3 cubic perovskite (Pm-3m)
.cifTlTaO3 cubic perovskite, Pm-3m (SG 221), a=4.070 Å. From Dorakhan et al. Small 2025. Computational only (toxicity concern), promising energetics for C2 products.
RbTaO3 cubic perovskite (Pm-3m) - relaxed
.cifCell + Ionic relaxation with Orb v3 conservative inf MPA; 0.03 eV/Å threshold; final energy = -40.4953 eV; energy change = -0.0120 eV; symmetry: Pm-3m → Pm-3m
NaTaO3 cubic perovskite (Pm-3m)
.cifNaTaO3 cubic perovskite, Pm-3m (SG 221), a=3.913 Å. ICSD 39098. From Dorakhan et al. Small 2025. Synthesized but no C2 products detected (A-cation too small for C-C coupling).
RbTaO3 cubic perovskite (Pm-3m)
.cifRbTaO3 cubic perovskite, Pm-3m (SG 221), a=4.095 Å. From Dorakhan et al. Small 2025. Computational only, synthesis unsuccessful. Larger A-cation than KTaO3.
NaTaO3 phase diagram 1
.htmlPhase diagram of NaTaO3 with Orb v3 conservative inf MPA; eabovehull: 0.037415 eV/atom; predicted_stable: False