The low structural stability of hydrogen-bonded organic frameworks (HOFs) is a thorny issue retarding the development HOFs. A rational design approach now proposed for construction stable HOF. resultant HOF (PFC-1) exhibits high surface area 2122 m2 g-1 and excellent chemical (intact in concentrated HCl at least 117 days). new method acid-assisted crystalline redemption used to readily cure thermal damage PFC-1. With periodic integration photoactive pyrene robust framework, PFC-1 can...

The recombination of electron–hole pairs severely detracts from the efficiency photocatalysts. This issue could be addressed in metal–organic frameworks (MOFs) through optimization charge-transfer kinetics via rational design structures at atomic level. Herein, a pyrazolyl porphyrinic Ni-MOF (PCN-601), integrating light harvesters, active catalytic sites, and high surface areas, has been demonstrated as superior durable photocatalyst for visible-light-driven overall CO2 reduction with H2O...

Abstract The electrocatalytic conversion of CO 2 into value‐added chemicals is a promising approach to realize carbon‐energy balance. However, low current density still limits the application electroreduction reaction (CO RR). Metal–organic frameworks (MOFs) are one class alternatives for RR due their periodically arranged isolated metal active sites. poor conductivity traditional MOFs usually results in RR. We have prepared conductive two‐dimensional (2D) phthalocyanine‐based MOF (NiPc‐NiO...

Hydrogen-bonded organic frameworks (HOFs) show great potential in many applications, but few structure-property correlations have been explored this field. In work, we report that self-assembly of a rigid and planar ligand gives rise to flat hexagonal honeycomb motifs which are extended into undulated two-dimensional (2D) layers finally generate three polycatenated HOFs with record complexity. This kind undulation is absent the 2D built from very similar nonplanar ligand, indicating slight...

Abstract The unique applications of porous metal–organic framework (MOF) liquids with permanent porosity and fluidity have attracted significant attention. However, fabrication MOF remains challenging because the easy intermolecular self‐filling cavity or rapid settlement hosts in hindered solvents that cannot enter their pores. Herein, we report a facile strategy for liquid (Im‐UiO‐PL) by surface ionization an imidazolium‐functionalized sterically poly(ethylene glycol) sulfonate (PEGS)...

Under topological guidance, the self-assembly process based on a tetratopic porphyrin synthon results in hydrogen-bonded organic framework (HOF) with predicted square layers topology (sql) but unsatisfied stability. Strikingly, simply introducing transition metal center does not change network drastically causes noticeable noncovalent interaction, orbital overlap, and molecular geometry, therefore ultimately giving rise to series of metalloporphyrinic HOFs high surface area, excellent...

The pursuit of selective two-electron oxygen reduction reaction to H

Abstract The low structural stability of hydrogen‐bonded organic frameworks (HOFs) is a thorny issue retarding the development HOFs. A rational design approach now proposed for construction stable HOF. resultant HOF (PFC‐1) exhibits high surface area 2122 m 2 g −1 and excellent chemical (intact in concentrated HCl at least 117 days). new method acid‐assisted crystalline redemption used to readily cure thermal damage PFC‐1. With periodic integration photoactive pyrene robust framework, PFC‐1...

Abstract Three tetrahedral organic cages have been obtained by condensing a triamino linker with set of three ostensibly analogous triformyl precursors. Despite the large number imine bonds formed, corresponding were in exceptionally high yields. Both theory and experimental results demonstrate that intramolecular CH⋅⋅⋅π interactions within all cage frameworks play an important role abetting condensations contributing to near‐quantitative synthetic The this study exhibit thermodynamic...

Although many ionic metal-organic frameworks (MOFs) have been reported, little is known about how the charge of skeleton affects properties MOF materials. Herein we report chemical stability MOFs can be substantially improved through embedding electrostatic interactions in structure. A with a cationic impervious to extremely acidic, oxidative, reductive, and high strength conditions, such as 12 m HCl (301 days), aqua regia (86 H2 O2 (30 seawater which unprecedented for MOFs. DFT calculations...

This study reports a photocatalyst based on hydrogen-bonded organic framework exhibiting high H₂ evolution rate and easy recyclability. The ordered arrangement of photosensitizers is proved to play vital role in the photocatalytic activity.

Rational synthesis of hydrogen-bonded organic frameworks (HOFs) with predicted structure has been a long-term challenge. Herein, by using the efficient, simple, low-cost, and scalable mechanosynthesis, we demonstrate that reticular chemistry is applicable to HOF assemblies based on building blocks different geometry, connectivity, functionality. The obtained crystalline HOFs show uniform nano-sized morphology, which challenging or unachievable for conventional solution-based methods....

Structural self-assembly enables the hydrogen-bonded organic frameworks (HOFs) with facile synthesis, self-repair structures, and intriguing optoelectronic attributes. Herein, we report a strategy that directly employs HOF monomer for efficient photoredox catalysis without involving catalyst prefabrication. Remarkably, this simplified mode was equally effective as prefabricated catalysts, verified high activity, selectivity, generality in photocatalytic sulfide oxygenation. The complementary...

Herein we construct a novel three-dimension (3D) hydrogen-bonded organic framework (PFC-2) with hierarchical meso-microporous structure, which possesses the largest open channels relative to all known HOFs and exhibits highly selective separation of acetylene ethylene versus methane at ambient atmosphere. Comparison on adsorption behaviors PFC-2 an analogue structure PFC-1 clearly shows that extensively existed unpaired hydrogen bond acceptor C═O groups in dramatically increase affinity...

Abstract The unique applications of porous metal–organic framework (MOF) liquids with permanent porosity and fluidity have attracted significant attention. However, fabrication MOF remains challenging because the easy intermolecular self‐filling cavity or rapid settlement hosts in hindered solvents that cannot enter their pores. Herein, we report a facile strategy for liquid (Im‐UiO‐PL) by surface ionization an imidazolium‐functionalized sterically poly(ethylene glycol) sulfonate (PEGS)...

Abstract The electrocatalytic conversion of CO 2 into value‐added chemicals is a promising approach to realize carbon‐energy balance. However, low current density still limits the application electroreduction reaction (CO RR). Metal–organic frameworks (MOFs) are one class alternatives for RR due their periodically arranged isolated metal active sites. poor conductivity traditional MOFs usually results in RR. We have prepared conductive two‐dimensional (2D) phthalocyanine‐based MOF (NiPc‐NiO...

Three cationic capsule-shaped Zr-based metal–organic polyhedra (MOPs) with different cavity sizes were successfully constructed through the self-assembly of trinuclear zirconocene clusters and imidazolium-functionalized dicarboxylic ligands. Owing to imidazolium groups in MOPs, they show good CO2 adsorption uptake. Moreover, halogen anions Brønsted acid sites (−OH) knots are close proximity, making these MOPs able catalyze synergistically cycloaddition reaction epoxides into cyclic...

A microporous porphyrin-based hydrogen-bonded organic framework, named PFC-5, was precisely designed and successfully constructed. Because of the present multiple hydrogen bondings π–π interactions between porphyrinic ligands, PFC-5 possesses a robust framework with excellent water, thermal, chemical stability. CO2 sorption isotherm demonstrated that permanent microporosity after activation. The obtained material has been explored for highly selective C2 light hydrocarbons/CH4 separations at...

As a ubiquitous aspect of modern information technology, data compression has wide range applications. Therefore, quantum autoencoder which can compress into low-dimensional space is fundamentally important to achieve automatic in the field information. Such be implemented through training parameters device using classical optimization algorithms. In this paper, we demonstrate condition achieving perfect and theoretically prove that losslessly high-dimensional (also called latent space) if...

Herein, we developed a strategy of rational constructing bimetallic metal–organic frameworks (MOFs) and at the same time embedding charges on backbones. Based Pearson's hard/soft acid/base (HSAB) principle, soft base (azolate) hard (carboxylate) were simultaneously implanted in one building block for MOF construction, which can preferentially coordinate with relative acid Cu2+ Zr4+ (or Hf4+), respectively. This combination during self-assembly process not only generates robust coordination...

Proton transport channels in biological systems are constructed by the specific amino acid residues with hanging carboxylic groups acting as proton donors and acceptors, enabling rapid conduction via Grotthuss mechanism. Hydrogen‐bonded organic frameworks (HOFs) promising candidates for artificially simulating due to their designable structure abundant sources network. However, these protons were usually immobilized within hydrogen bonds between two building blocks, which require a high...