ABSTRACT The electrocatalytic ethanol oxidation reaction is bottlenecked by inefficient C─C bond cleavage. This challenge is epitomized at metal‐oxide heterointerfaces, where the active site identity and cleavage mechanism remain obscured. Here, we decoded this by atomically programming model PdO─Pt 3 Pd heterointerfaces. Through 18 O isotopic labeling, we identify the interfacial lattice oxygen (O Int ) in Pd 2+ ─O Int ─Pd alloy motif as the direct oxygen donor for C─C cleavage. The interfacial built‐in electric field activates O Int as a nucleophilic scalpel by upshifting its p‐band center, resulting in an ultralow cleavage barrier of 0.47 eV. Beyond a single site, we demonstrate that the interface functions as a reaction‐network architect. It creates a dominant O Int ‐mediated “non‐CO” C1 pathway at the PdO─Pt 3 Pd heterointerface while re‐engineering the traditional “CO” pathway on the adjacent Pt 3 Pd domain via threefold optimization: minimizing *CO source, suppressing acetate formation and ensuring rapid *CO removal. This dual‐path integration yields breakthrough performance with a mass activity of 9.09 A mg metal −1 and a C1‐pathway Faradaic efficiency of 75.6%. This work reports a paradigm shift from a passive “scavenger” model to an active “initial‐attack and system‐orchestration” mechanism, redefining heterointerfaces as atomically programmable reaction‐network architects. This paradigm offers a blueprint for mastering complex reaction networks, extending the frontier of rational catalyst design.

The development of energy-efficient amine-based absorbents is crucial for advancing industrial-scale CO2 capture. This study presents the alkylated ethylenediamine-based absorbents for CO2 capture and systematically investigates their structure–activity relationships. The findings reveal that increasing the degree of alkylation enhances the electron density around the primary amine groups, therefore strengthening their binding affinity towards CO2. Theoretical calculations further elucidate that functionalizing ethylenediamine with isopropyl groups can reduce the reaction energy barrier, consequently facilitating the CO2 absorption rate. Moreover, higher degrees of alkylation introduce stronger steric hindrance, promoting carbamate decomposition and enhancing CO2 cyclic capacity and desorption rates while reducing regeneration energy consumption. This work provides valuable insights into the structural design of amine absorbents with enhanced CO2 capture efficiency.

The separation of C2H4 from a ternary C2H2/C2H6/C2H4 mixture is critically important in the chemical industry, yet it remains a significant challenge because of their highly similar physical properties. In this work, we introduce a MOF-based adsorbent (Zn-BPT-BPDC) that incorporates synergistic electronegative and nonpolar adsorption sites to promote the efficient one-step separation of C2H4 from the ternary mixture. Zn-BPT-BPDC exhibits higher adsorption capacities for C2H2 and C2H6 than for C2H4, demonstrating superior competitive adsorption selectivity for both C2H2/C2H4 and C2H6/C2H4 mixtures. Dynamic breakthrough studies demonstrate its excellent performance in the one-step purification of C2H4 from the ternary gas mixture. Furthermore, theoretical calculations and molecular simulations elucidate that the enhanced binding affinities for C2H2 and C2H6 arise from the synergistic interactions with the tailored electronegative and nonpolar sites within the framework of Zn-BPT-BPDC. This adsorbent demonstrates considerable promise for industrial use in the separation of C2H4 from gas mixtures.

Antimony selenosulfide (Sb2(S,Se)3) demonstrates strong potential for thin-film solar cells owing to its tunable bandgap, low toxicity, and high stability. However, conventional fabrication methods often yield films with small grain sizes and random orientations, which hinder device performance. Herein, an in situ polymerization-assisted grain growth (iPAGG) strategy was developed, specifically enabling the oriented growth of Sb2(S,Se)3 on Cd-free TiO2 substrates, by introducing acrylic acid (AA) into the chemical bath deposition process. The carboxylate groups from AA coordinate with Sb3+ ions, promoting oriented growth of Sb2(S,Se)3 film. This approach yields films with enlarged grains, reduced defect densities, and strengthened [hk1] preferred orientation. As a result, Cd-free Sb2(S,Se)3 solar cells employing the optimized AA concentration yielded a champion power conversion efficiency (PCE) of 7.24%, outperforming the control device (6.70%). Further interfacial modification with poly (acrylic acid)-modified SnO2 boosts the PCE to 7.55%. This work offers an effective way toward the fabrication of high-performance and environmentally friendly Sb2(S,Se)3 photovoltaics.

Waste rock wool (RW) is transformed into a multifunctional composite material by modifying RW fibers with silver nanoparticles (AgNPs) and polydimethylsiloxane (PDMS). The resulting composite exhibits excellent electrical conductivity, electromagnetic interference (EMI) shielding effectiveness, water repellency, self-cleaning properties, and flame retardancy. Silver nanoparticles not only impart conductivity to the composite material but also improve surface roughness. This enables them to work with PDMS, enhancing the composite's hydrophobicity. The composite exhibited an EMI shielding effectiveness of 31.04 ± 0.87 dB in the X-band and a water contact angle (WCA) of 153.53° ± 0.59°, demonstrating superhydrophobicity. In addition, due to its inorganic nature, the composite showed impressive flame-retardant performance. This work demonstrates that, by carefully considering structural features and meticulously designing modification strategies, waste can be successfully converted into valuable composites through a simple approach.

The separation of CH4 from natural gas is an industrially significant yet challenging task. In this study, we rationally designed metal-organic framework (MOF)-based adsorbents with polar-nonpolar synergistic sites to enhance the efficient separation of CH4 from natural gas. Our study demonstrates that the adsorbents exhibit superior adsorption capacity for C3H8 and C2H6 compared to CH4, as well as high separation selectivity for C3H8/CH4 (1336) and C2H6/CH4 (46), effectively overcoming the trade-off between adsorption capacity and selectivity. Breakthrough experiments further confirm the exceptional dynamic separation performance of the adsorbents for the C3H8/C2H6/CH4 ternary mixture under various operating conditions, achieving >99.99% CH4 purity and a yield of 11.27 mmol & centerdot;g(-1). Molecular simulations and theoretical calculations elucidate that the incorporated polar and nonpolar sites in the adsorbents provide multiple strong interactions, which significantly enhance the separation of CH4 from the C3H8/C2H6/CH4 mixture.

This study employs biodegradable polymer PBAT as the matrix and talc as a reinforcing filler, utilizing a gradient modification approach with silane coupling agent KH560, tannic acid (TA), and calcium ions (Ca2⁺) as modifiers. Through a three-step surface functionalization process of “KH560 grafting + TA coating + Ca2⁺ chelation” on talc, combined with melt blending, twin-screw extrusion granulation, and blow molding techniques, PBAT/Talc composite films were fabricated. With 10% talc loading, 3% TA, and 2% Ca2⁺ content, the composite film exhibited tensile strength of 33.73 MPa, and elongation at break of 612%. Additionally, the film showed improved melt index and enhanced thermal stability, with char residue at 600 °C increasing from 5.69% to 14.72% and crystallization temperature rising from 49.08 °C to 95.18 °C, achieving synergistic optimization of strength, toughness, processability, and thermal stability. The gradient modification with KH560, TA, and Ca2⁺ establishes multi-scale interfacial interactions through covalent bonding, hydrogen bonding, and coordination bonding. This enables precise regulation of talc’s surface hydrophilicity/hydrophobicity, effectively improving interfacial compatibility between talc and PBAT matrix while enhancing talc dispersion uniformity. Furthermore, the modified talc acts as a heterogeneous nucleating agent optimizing PBAT crystallization behavior, facilitating uniform stress transfer through strengthened interfacial interactions.

Artificial solid electrolyte interphase (SEI) represents a promising strategy for stabilizing Zn electrodes by suppressing dendrite formation and parasitic reactions. However, conventional SEI designs suffer from sluggish Zn2+ transport kinetics and mechanical instability during cycling. Herein, we construct a thin chitosan@alginate (CS@SA, similar to 1.5 lm) bilayer SEI on Zn electrodes via electrodeposition. Mutually activated functional groups (-COOH in outer SA and -NH2 in inner CS) synergistically (1) facilitate the desolvation of [Zn(H2O)6]2+ , (2) block reactive H2O contact with the Zn surface, and (3) establish polymer-chain-accelerated Zn2+ transport pathways. Hydrogen-bond reconfiguration endows the CS@SA bilayer with in-situ self-healing and anti-detachment features, dynamically maintaining interfacial integrity. These merits simultaneously enhance the Zn electrode stability and Zn2+ migration kinetics. Consequently, the Zn@CS@SA electrode demonstrates a high average Coulombic efficiency (CE) of 99.74% over 1000 cycles at 2 mA cm-2 and 1 mAh cm-2 in the asymmetric cell. The Zn@CS@SA//MnO2 demonstrates a four-fold capacity of Zn//MnO2 after 1000 cycles at 2 A g-1. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Amine-scrubbing-based chemical absorption is an effective and industrialized technology for CO2 capture, but the challenge lies in developing efficient and energy-saving absorbents. Here we present a rationally designed amine absorbent, N-(2-hydroxypropyl)-N-ethylethylenediamine (HPEEDA), featuring simultaneous functionalized ethyl and hydroxypropyl groups on a tertiary amine. Experimental results demonstrate that HPEEDA exhibits high efficiency in both CO2 absorption and desorption, while offering great energy-saving advantages during regeneration. The structure-activity relationship between HPEEDA and CO2 capture is revealed through the systematic examination of the disassembled HPEEDA blends. Quantitative experiments and theoretical calculations elucidate the CO2 capture mechanism of HPEEDA, highlighting the critical role of intermolecular proton transfer in promoting CO2 capture. This rationally designed amine absorbent that breaks the CO2 absorption-desorption trade-off is expected to advance underway efforts toward large-scale CO2 capture.

Water-lean CO2 phase change absorbents (CPCAs) have attracted considerable attention for their energy-saving potential. This study constructed a novel water-lean CPCA via a rapid screening method based on differences in hydrophilicity/hydrophobicity (Δlog P). The system employs piperazine (PZ) as the amine absorbent, diethylene glycol butyl ether (DB) as the phase separator, and ethylene glycol (EG) as the organic solvent. The system exhibits a high CO2 enrichment rate of 97.3% and a low viscosity of 40.8 mPa·s. Thermodynamic analysis reveals that its regeneration energy consumption can be reduced to 1.89 GJ·t−1 CO2, which is 57.4% lower than the PZ/H2O system. Mechanistic studies confirm that the polarity difference among components after CO2 absorption is the fundamental driver for phase separation. Overall, the PZ/DB/EG/H2O CPCA system developed in this study demonstrates significant potential for industrial CO2 capture applications.

Direct ethanol fuel cells are hindered by the ethanol oxidation reaction (EOR) that favors the low-efficiency C2 pathway over the desirable C1 pathway. Here, we report a catalyst design integrating an ultrathin Turing-type nanonet with a Pd-based crystalline/amorphous (C/A) heterointerface, achieving a near-complete C1-pathway selectivity of 97.1% for alkaline EOR, which is the highest reported to date. Inspired by spatially decoupling C─C cleavage and CO oxidation, we engineer two intimately integrated phases: strained interstitial-carbon-doped PdO (Cint-PdO) enriched with oxygen vacancies and defective amorphous PdCx (a-PdCx). This heterostructure is realized via a "carbon engineering" strategy combining salt-melt templating with secondary annealing. Atomic-resolution studies confirm atomically sharp C/A interfaces and the highly unsaturated a-PdCx phase. In situ Fourier-transform infrared spectroscopy (FTIR) directly visualizes CO2 emergence at ultralow overpotentials, while high-performance liquid chromatography (HPLC) verifies the near-complete C1 pathway. Density functional theory (DFT) reveals a dual-cooperative mechanism: Cint-PdO steers the EOR toward C1 pathway by facilitating CH3CO* dehydrogenation and subsequent C─C cleavage via CH2CO*, thereby suppressing acetate formation; concurrently, a-PdCx dramatically accelerates CO oxidation and may also contribute to C─C cleavage via an alternative direct CH3CO* pathway. This work establishes carbon-engineered C/A heterointerfaces as a powerful platform for overcoming the EOR selectivity bottleneck.

Interface engineering with a CC spacer and 1-fold Au–S coordination in a helicene-based single-molecule junction enables reversible photoswitching between non-spin-polarized transport (closed form) and 99.67% spin-polarized transport (open form).

While Zn2+ exhibits enhanced stability in organic solvents, which facilitates improved redox reversibility and coulombic efficiency while mitigating the formation of passivation byproducts commonly encountered in aqueous systems, the inherent flammability of organic electrolytes poses substantial safety hazards. Herein, we propose a novel multifunctional organic electrolyte system composed of trimethyl phosphate (TMP) and acetonitrile (AN), which integrates synergistic anti-freezing capability and wide-temperature adaptability (-20 to 40 degrees C). Mechanistic investigations reveal that the coordinated interactions among TMP, AN, and OTF- anions promote the formation of an organic-inorganic hybrid solid electrolyte interphase (SEI) on Zn anodes. Theoretical simulations demonstrate that TMP molecules preferentially adsorb onto the Zn (002) crystallographic planes to guide spatially homogeneous Zn2+ plating, and their unique molecular configuration significantly reduces the Zn2+ desolvation energy barrier. Consequently, Zn||Zn symmetric cells achieve ultralong cycling stability exceeding 3000 h at 5 mA cm-2/1 mAh cm-2 and 2000 h at 10 mA cm-2/1 mAh cm-2. The NHVO|| A2T1||Zn full cell delivers exceptional cyclability with 88.7 % capacity retention after 3000 cycles at 2 A g-1, and it maintains stable operation over the wide temperature range of -20-40 degrees C. This work exemplifies the rational design of multifunctional organic electrolytes, as it addresses critical challenges in Zn metal batteries through the integration of low-temperature compatibility and interface engineering to accelerate their practical implementation.

Blended amines have attracted considerable research interest due to their potential for high CO2 capture efficiency. This study systematically investigates blended alcoholamine solutions containing alkylated-secondary and tertiary amine structures for CO2 capture. The experimental results indicate that a higher degree of alkylation in secondary amines, attributed to the electron-donating effect, correlates with enhanced absorption capacity. Additionally, an increased alkylation degree in secondary amines, due to steric hindrance, improves CO2 desorption while reducing the absorption rate. Particularly, N-ethylethanolamine (EAE) exhibits superior capture performance, owing to the synergistic effects of the electron-donating and steric hindrance properties of the ethyl group. The blended amine system composed of EAE and 3-(diethylamino)-1-propanol (3DEA1P) demonstrates exceptional capture efficiency and low regeneration energy requirements (2.11 GJ & sdot;t-1 CO2). This work provides critical insights for developing high-efficiency, low-energy blended amine systems for CO2 capture.

Biological ion channels exemplify nature's high-efficiency ion selectivity filters, yet replicating their functional architectures in synthetic membranes remains a fundamental challenge. Here, we report an ultramicroporous hydrogen-bonded organic framework membrane that structurally emulates the CLC chloride filter. Its channels exhibit size adaptability to anions and incorporate hydrogen-bond donors that provide "low-viscosity" compensatory interactions, thereby alleviating anion dehydration energy penalties. By leveraging differential dehydration and energy compensation between Cl- and larger anions such as SO42-, this bioinspired design achieves an exceptional Cl-/SO42- selectivity of over 400-several tens of times higher than those of existing counterparts-while maintaining a high Cl- permeation rate double that of the commercial Neosepta® ACS membrane, setting a new benchmark for advanced anion-sieving membranes. In electrodialysis (ED) for high-salinity wastewater valorization, our membrane enables higher NaCl product purity (99.62 wt% vs. 72.86 wt%) with 28.7% lower energy consumption than the Neosepta® ACS membrane. This work establishes a biomimetic design principle of biological anion channels that is potentially extendable to a wide range of selective and conductive membranes.

Achieving precise control over reaction pathways is central to selectivity breakthroughs in heterogeneous catalysis. Here, we demonstrate that Zn incorporation into a Cu-based catalyst induces a programmable electronic switch that fundamentally redirects the dominant methanol steam reforming (MSR) pathway. A seaurchin-like CuZn-Cu2O/SiO2 catalyst with hierarchical porous architecture is constructed via a combined hydrothermal-impregnation strategy. Comprehensive characterization confirms the formation of a CuZn alloy phase, which selectively withdraws electron density from Cu0, creating electron-deficient yet highly polarizable Cu0/Cu+ interfaces while leaving Cu+ electronically stable. The catalyst achieves complete methanol conversion with 100% CO2 selectivity in the 180-240 degrees C range, a high H2 production rate, and significantly enhanced stability. In situ FTIR spectroscopy provides definitive evidence of a complete pathway switch: the CO-pathway is completely suppressed on the Zn-modified catalyst, and the reaction proceeds exclusively via the formate (HCOO)-pathway. This work establishes a direct causal link from atomic-scale electronic modulation to macroscopic reaction pathway control, offering a new design principle for high-selectivity catalysts in clean energy applications.

This study develops an indole-functionalized zirconium-based metal-organic cage (Zr-MOC-Indole) for efficient iodine capture. The material exhibits high iodine vapor uptake and effective iodine removal from solution. Experimental and theoretical analyses reveal a synergistic adsorption mechanism involving charge transfer and hydrogen bonding, stabilizing polyiodides within the structure.

Nonaqueous amine absorbents have received considerable attention currently due to their energy efficiency and noncorrosiveness for CO2 capture. In this study, the new nonaqueous amine absorbents were developed by dissolving 2-hydroxypropyl-diethylenetriamine (HPDETA) in various organic solvents. The experimental results demonstrated that the obtained HPDETA-based nonaqueous amine absorbents have improved efficiency for CO2 capture compared to HPDETA in H2O, especially in terms of CO2 cyclic capability, reusability, and thermal stability. Moreover, the regeneration energy consumption of the optimal nonaqueous amine absorbent, HPDETA in diethylene glycol (HPDETA/DEG), can be reduced to as low as 2.00 GJ center dot t(-1) CO2. Importantly, HPDETA/DEG demonstrated near noncorrosiveness to 20# carbon steel during CO2 capture, which is significantly superior to that of DETA and HPDETA in H2O. Overall, the HPDETA-based nonaqueous amine absorbents will be the promising candidates for practical CO2 capture application.