Subiao Liu

Navigating the vast compositional landscape of polynary oxide electrocatalysts is traditionally limited by funnel-style screening paradigms that treat high-fidelity data as binary gates rather than informative training signals. Here, we present an expert-guided multiscale framework for Pr–Sr–Co-Fe perovskites. By integrating atomic descriptors, experimental structural features, and mechanism-informed electronic features, this framework addresses these limitations within a descriptor-accessible polynary perovskite space. By implementing a “Nearest Grid Interpolation” strategy, the computational cost of high-fidelity density functional theory calculations is reduced by nearly 2 orders of magnitude within the search space. Two rounds of active learning surge the discovery efficiency of high-performance candidates (η@10 mA cm–2 < 370 mV) from an initial 4.4% to 60.0%. Integrated with human-in-the-loop expertise, this workflow identifies a localized synergistic optimum at Pr0.01Sr0.99Co0.66Fe0.34O3−δ (PSC0.66F), which exhibits a low overpotential of 338 mV at 10 mA cm–2. Symbolic regression reveals that the intrinsic activity is closely associated with a nexus of O 2p-band center, its bandwidth, and Fe eg orbital filling within this local region. Experimental validation confirms that this optimized electronic configuration promotes highly efficient lattice oxygen mechanism (LOM) kinetics, supported by accelerated bulk oxygen diffusion and dynamic surface reconstruction. This multiscale and expert-guided strategy provides a practical and extensible framework for descriptor-accessible complex materials systems, transforming fragmented data tiers into a cohesive, learnable predictive landscape.

Construction of a strong metal‐oxide heterointerface via perovskite in situ exsolution synchronously generates oxygen vacancies (Vö) and B‐site cation defects. However, their individual contributions are often conflated and overshadowed by the overall high performance toward CO ₂ electrolysis in solid‐state electrolyzers, obscuring their specific roles in modulating perovskite properties. Here we designed a series of Sr ₂ Fe _1.35 Mo _0.45 Ni _0.2 O _6−δ (SFMN) with different levels of B‐site Fe/Ni defects and Vö. Cross‐scale experimental and theoretical results revealed that increased B‐site Fe/Ni defects and Vö strengthened Fe 3d−O 2p orbital hybridization, thereby enhancing electrical conductivity, but this trend reversed beyond a certain threshold. Then, in situ topotactic exsolution was performed for SFMN to refill B‐site cation defects while maintaining Vö concentration intact. The resulting sample without B‐site cation defects exhibited a faster oxygen‐ion transport capability than conventionally exsolved SFMN with rich B‐site defects, achieving a high current density of 2.40 A cm ⁻² at 1.5 V and 850°C, while avoiding SrCO ₃ formation. Theoretical calculations demonstrated that refilling B‐site cation defects in exsolved SFMN thermodynamically accelerated CO ₂ adsorption and activation, as well as suppressed Sr segregation. This study unravels the crucial impact of B‐site defects on perovskite properties and provides insights for the future development of robust perovskite electrocatalysts.

Faced with global energy and environmental challenges, seawater electrolysis has emerged as a promising route for marine resource utilization. However, its efficiency is limited by impurities and slow reaction kinetics. Although noble metal catalysts show high activity, their high cost and insufficient durability drive the search for alternatives. Perovskite oxides (ABO ₃ ) have gained attention due to their tunable structures, excellent stability, and outstanding catalytic activity. This review systematically explores the roles of perovskite oxides in seawater electrolysis, focusing on their design and function at each electrode. At the cathode, they are tailored to catalyze the hydrogen evolution reaction (HER) by improving electron transfer and adsorption. At the anode, the ABO ₃ structure enables both oxygen evolution reaction (OER) and chlorine evolution reaction (CER). The selectivity between OER and CER depends on lattice oxygen stability and the metal’s relative affinity for oxygen and chlorine. In addition, this review covers the compositional flexibility, synthesis methods, and electrocatalytic performance of perovskite oxides in seawater electrolysis. Furthermore, modification strategies aimed at enhancing the activity, selectivity, and durability of perovskite oxides in seawater electrolytes are also discussed. Finally, we present the current challenges and propose future research directions.

Metallic interatomic spacing emerges as a key activity descriptor in electrocatalysis, yet achieving angstrom‐level precision in its dynamic modulation and establishing definitive structure–activity correlations persist as critical bottlenecks. Here, we developed a phase‐controlled strategy enabling continuous interatomic spacing modulation in a library of hexagonal Pd‐Te nanoplates (NPs), where various atomically ordered intermetallic phases from cubic Pd ₄ Te to rhombohedral Pd ₂₀ Te ₇ /Pd ₈ Te ₃ and hexagonal PdTe ₂ were synthesized, realizing precise tuning of adjacent Pd‐Pd distances (d _Pd‐a‐Pd ) from 2.75 to 4.07 Å. The proof‐of‐concept electrochemical CO ₂ reduction (ECR) for CO formation displayed a volcano‐shaped dependence on d _Pd‐a‐Pd , where Pd ₂₀ Te ₇ NPs with a d _Pd‐a‐Pd of 2.88 Å exhibited a maximal CO Faraday efficiency (FE _CO ) of 99.9%, and preserved FE _CO over 90% at ∼120 mA cm ⁻² during long‐term stability. Integrated in situ spectra and theoretical calculations confirmed the dominated distance effect over electronic effect, and revealed that increasing d _Pd‐a‐Pd upshifted d ‐band center toward the Fermi level while altering *CO adsorption configuration from strongly bound *CO _T to weakly bound *CO _L , resulting in exceptional ECR activity and CO anti‐poisoning capacity on Pd ₂₀ Te ₇ NPs owing to the optimally balanced *COOH adsorption and *CO desorption. This study underscores the pivotal role of interatomic spacing in regulating intermediate adsorption configurations for electrocatalysis.

Metallic interatomic spacing emerges as a key activity descriptor in electrocatalysis, yet achieving angstrom‐level precision in its dynamic modulation and establishing definitive structure–activity correlations persist as critical bottlenecks. Here, we developed a phase‐controlled strategy enabling continuous interatomic spacing modulation in a library of hexagonal Pd‐Te nanoplates (NPs), where various atomically ordered intermetallic phases from cubic Pd ₄ Te to rhombohedral Pd ₂₀ Te ₇ /Pd ₈ Te ₃ and hexagonal PdTe ₂ were synthesized, realizing precise tuning of adjacent Pd‐Pd distances (d _Pd‐a‐Pd ) from 2.75 to 4.07 Å. The proof‐of‐concept electrochemical CO ₂ reduction (ECR) for CO formation displayed a volcano‐shaped dependence on d _Pd‐a‐Pd , where Pd ₂₀ Te ₇ NPs with a d _Pd‐a‐Pd of 2.88 Å exhibited a maximal CO Faraday efficiency (FE _CO ) of 99.9%, and preserved FE _CO over 90% at ∼120 mA cm ⁻² during long‐term stability. Integrated in situ spectra and theoretical calculations confirmed the dominated distance effect over electronic effect, and revealed that increasing d _Pd‐a‐Pd upshifted d ‐band center toward the Fermi level while altering *CO adsorption configuration from strongly bound *CO _T to weakly bound *CO _L , resulting in exceptional ECR activity and CO anti‐poisoning capacity on Pd ₂₀ Te ₇ NPs owing to the optimally balanced *COOH adsorption and *CO desorption. This study underscores the pivotal role of interatomic spacing in regulating intermediate adsorption configurations for electrocatalysis.