CO₂ valorization has been recognized as a pivotal process in reducing carbon sequestration costs. While metal–organic frameworks (MOFs) exhibit remarkable CO₂ capture performance, their photocatalytic CO₂ reduction activity is often constrained by factors, such as insufficient active sites and frequent charge carrier recombination. In this work, an innovative strategy tailoring MOF surface architecture was developed. By tuning the concentration of highly supersaturated synthesis solutions, nonclassical secondary crystallization was facilitated, constructing abundant surface protrusions on the classic UiO-66 for the first time. These ultrasmall crystalline structures featuring high-index facets and missing-linker defects markedly increased both the amount and Lewis acid strength of exposed Zr sites, enhancing CO₂ adsorption capacity and kinetics. Concurrently, the surface architecture induced an interfacial homojunction with a supporting built-in electric field, precisely delivering the photogenerated electrons to adsorbed CO₂. Collectively, these upgrades synergistically boosted the critical surface reactions of the engineered catalyst, resulting in a sixfold increase in its CO yield relative to the pristine seeds. With its versatility, this strategy enriches the methodologies for addressing the intrinsic limitations of MOFs and enables the a priori design of efficient photocatalysts for low-concentration CO₂.

Separating/capturing SF₆, having the strongest global warming potential, from exhaust gas with low concentration (1%–10%) in the power industry is significant for both greenhouse gas emission control and SF₆ recycling and reutilization. In this study, we achieved highly efficient SF₆/N₂ separation under different SF₆ concentrations (1% and 10%) using two homologous metal-organic frameworks, Ni-bpz and Zn-bpz. This outcome underscores the effectiveness of rational nano-traps distribution engineering for targeted separation applications. The molecular simulation suggests that an SF₆ molecule interacts with a single nano-trap in Zn-bpz. At the same time, it is efficiently confined by two adjacent nano-traps in the parallel distribution of Ni-bpz. Consequently, exceptional SF₆/N₂ selectivity for 1/99 and 10/90 mixtures have been respectively achieved in Ni-bpz (516, SF₆/N₂ = 1/99) and Zn-bpz (608, SF₆/N₂ = 10/90) at 298 K and 1 bar. In dynamic breakthrough experiments, Ni-bpz exhibits a record pure N₂ (≥ 99.99%) productivity (1496 mL/g) for an SF₆/N₂ (1/99) gas mixture. Moreover, both MOFs demonstrate excellent water resistance across multiple cycles, suggesting their high promise for practical application.

Green synthesis of metal-organic frameworks (MOFs) in water with alleviated environmental influence and reduced cost is an essential step to transfer laboratory MOFs research to industrial application. Switching from the commonly used organic solvents to pure water encounters challenges of the poor solubility of organic linkers, slow reaction kinetics, and the formation of polymorphic products. So far, a universal MOFs synthetic strategy in water system has yet to be developed. This study reports the seed-aided synthesis of eleven MOFs with diverse compositions and structures while pure water serving as solvent. The corresponding reaction temperature and time of using this new strategy were reduced compared with original synthetic approaches, while the products maintain porous structure and high crystallinity. The success of this strategy relies on the addition of parent MOFs as seeds which could promote crystallization process by skipping the time-consuming induction period and avoiding the formation of polymorphic impurities.

The illegal usage of antibiotics as veterinary drugs is an increasing threat for human health. The specific sensing of antibiotics with different toxicity levels is of high challenge, and mainly relies on expensive, time-consuming, and complex instruments. To realize specific sensing by rapid and handy optical sensors, a metal-organic framework (MOF) based dual sensor system is herein developed using two MOF materials BUT-128 and BUT-129 with high sensing selectivity and sensitivity. BUT-128 and BUT-129 exhibit the lowest limit of detection (LOD) towards chloramphenicol and furazolidone among reported MOF sensors. The corresponding dual sensor system with enriched signal readouts realized specific sensing of the strictly forbidden antibiotics (chloramphenicol and nitrofurans) from other regulated veterinary drugs including thiamphenicol, a structural analog of chloramphenicol. Besides, the strategy of this work is expected to flourish the development of optical sensors with high specificity for environment and food safety purposes.

Enhancing electrocatalytic water splitting performance by modulating the intrinsic electronic structure is of great importance. Here, porous bimetallic oxide and chalcogenide nanosheets grown on carbon paper denoted as NiCo₂X₄/CP (X = O, S, and Se) are prepared to demonstrate how the anion components affect the electronic structures and thereby disclose the correlation between their intermediates interaction and catalytic activities. The experimental characterization and theoretical calculation demonstrate that Se and S substitution can promote the ratio of Co³⁺/Co²⁺ and thereby modulate the electronic structure accompanied with the upshift of d band centers, which not only enhance the inner conductivity but also regulate the interaction between the catalyst surface and intermediates, especially for the adsorption of absorbed H and hydroperoxy intermediates towards respective hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As a result, a full alkaline electrolyzer using NiCo₂Se₄/CP and NiCo₂S₄/CP as cathode and anode delivers a low voltage of 1.51 V at 10 mA·cm^-2, which is comparable even superior to most transition metal-based electrolyzers.

Photocatalytic CO₂ reduction to convert solar energy to clean energy remains a critical challenge in exploring efficient catalysts. Herein, a hierarchical structured BiVO₄@Au@UiO-66-NH₂ with high photocatalytic activity was fabricated. The theoretical calculations revealed that the metal–organic framework (MOF) with relative higher conduction band (CB) and UiO-66-NH₂ with relative lower valence band (VB) could absorb full light spectrum, combining Au nanoparticle with suitable Fermi level into a particulate tandem heterojunction. This configuration can not only lower the activation barrier of CO₂ reduction using the rich active site of MOF, but also improve the selectivity toward CO by optimizing the reaction pathway. Notably, the experimental evaluation proved that BiVO₄@Au@UiO-66-NH₂ displays a producing rate of 232.7 μmol h⁻¹ g⁻¹ for CO and a selectivity of 97.2%. The investigation reveals that elaborately integrating multiple functional components into such a hierarchical structure enables optimizing crucial processes in photocatalytic CO₂ conversion and enhancing selectivity via synergistic catalysis.