Featured
-
-
Article
| Open AccessConfining H3PO4 network in covalent organic frameworks enables proton super flow
Development of porous proton-transporting materials combining stability and high performance has remained a challenge. Here, the authors report a stable covalent organic framework with excellent proton conductivity in which nitrogen sites on pore walls confine and stabilize a H3PO4 network in the channels via hydrogen-bonding interactions.
- Shanshan Tao
- , Lipeng Zhai
- & Donglin Jiang
-
Article
| Open AccessA solution-processable and ultra-permeable conjugated microporous thermoset for selective hydrogen separation
Rigidity, as seen in crosslinked polymers, and plastic processability are mutually exclusive properties. Here, the authors prepare a solution-processable conjugated microporous thermoset with permanent pores and demonstrate its application as a two-dimensional molecular sieving membrane for hydrogen separation.
- Wei Liu
- , Shu-Dong Jiang
- & Kian Ping Loh
-
Article
| Open AccessUnveiling reductant chemistry in fabricating noble metal aerogels for superior oxygen evolution and ethanol oxidation
Non-efficient gelation methods for noble metal particles limit the development of the corresponding gel materials. Here the authors describe the role of reductants, unlocking ligand chemistry, and largely expanding the composition space of noble metal aerogels for high-performance electrocatalysis.
- Ran Du
- , Jinying Wang
- & Alexander Eychmüller
-
Article
| Open AccessActivating low-temperature diesel oxidation by single-atom Pt on TiO2 nanowire array
Supported metal single-atom catalysts face challenges on both durability and practicality. Here, the authors demonstrate that a sustained 90% diesel oxidation conversion at ~160 oC is achieved by single-atom Pt on TiO2 nanowire-array integrated catalytic converter.
- Son Hoang
- , Yanbing Guo
- & Pu-Xian Gao
-
Article
| Open AccessMolecular elucidating of an unusual growth mechanism for polycyclic aromatic hydrocarbons in confined space
Coke-induced catalyst deactivation draws increasing concerns in industrially catalytic processes. Here the authors provide a strategy integrating advanced mass spectroscopy and isotope labeling to uncover a cage-passing molecular route of coking species in molecular sieve catalysts.
- Nan Wang
- , Yuchun Zhi
- & Zhongmin Liu
-
Article
| Open AccessNear 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation
Chemical looping methane partial oxidation is an effective technology to produce syngas with a minimal energy penalty. Here, the authors design and develop a mesoporous silica supported nanoparticle oxygen carrier that enables a near 100% CO generation with high recyclability and substantially lower operating temperature.
- Yan Liu
- , Lang Qin
- & Liang-Shih Fan
-
Article
| Open AccessVapour-phase-transport rearrangement technique for the synthesis of new zeolites
Assembly-Disassembly-Organization-Reassembly (ADOR) is a valuable method to prepare zeolites of predictable topologies, but has yet to be successfully applied on open framework zeolites. Here, the authors show that non-contact vapour-phase-transport rearrangement allows access to new zeolite topologies from open framework zeolites.
- Valeryia Kasneryk
- , Mariya Shamzhy
- & Maksym Opanasenko
-
Article
| Open AccessSpecific ion effects at graphitic interfaces
Understanding aqueous solutions at graphitic interfaces is critical in a wide variety of emerging technologies. Here, the authors unravel specific ion effects at the interface with graphene and within graphene slit-pores by coupling first-principles simulations and electrochemical measurements.
- Cheng Zhan
- , Maira R. Cerón
- & Patrick G. Campbell
-
Article
| Open AccessFast room temperature lability of aluminosilicate zeolites
While aluminosilicate zeolites are of interest for many applications, the affect of water on zeolite stability in mild aqueous conditions has yet to be established. Here, using ab initio calculations and NMR spectroscopy, the authors show that covalent bonds in the zeolite chabazite are labile when in contact with neutral liquid water.
- Christopher J. Heard
- , Lukas Grajciar
- & Russell E. Morris
-
Article
| Open AccessLinking synthesis and structure descriptors from a large collection of synthetic records of zeolite materials
Understanding zeolite synthesis-structure relationships remains challenging owing to the number of variables involved in their preparation. Here the authors analyze zeolite synthetic records from the literature via machine learning and find communities of synthetically related materials with previously overlooked similarities.
- Koki Muraoka
- , Yuki Sada
- & Tatsuya Okubo
-
Article
| Open AccessCarbon dioxide capture and efficient fixation in a dynamic porous coordination polymer
Porous coordination polymers that possess structural flexibility show great promise for gas adsorption and catalysis. Here the authors synthesize a dynamic porous coordination polymer with rotating ligands that permit effective CO2 trapping, and demonstrate subsequent CO2 cycloaddition to epoxides.
- Pengyan Wu
- , Yang Li
- & Susumu Kitagawa
-
Article
| Open AccessUprooting defects to enable high-performance III–V optoelectronic devices on silicon
The use of promising group III-V materials for optoelectronic applications is hindered by the high density of threading dislocations when integrated with silicon technology. Here, the authors present an electrochemical deep etching strategy to drastically reduce the the defect density.
- Youcef A. Bioud
- , Abderraouf Boucherif
- & Richard Arès
-
Article
| Open AccessTowards general network architecture design criteria for negative gas adsorption transitions in ultraporous frameworks
Porous framework material DUT-49 was recently demonstrated to exhibit a unique counterintuitive negative gas adsorption (NGA) behaviour. Here the authors identify framework DUT-50 as an additional pressure amplifying material that features distinct NGA transitions, and suggest structural design criteria to access other such materials.
- Simon Krause
- , Jack D. Evans
- & Stefan Kaskel
-
Article
| Open Access3D-structured supports create complete data sets for electron crystallography
3D electron crystallography enables structure determination of submicron-sized crystals, but obtaining complete data is difficult due to preferred orientations. Here the authors develop sample supports that allow sampling nanocrystals with full data completeness, and demonstrate this with ZSM-5 zeolites.
- Julian T. C. Wennmacher
- , Christian Zaubitzer
- & Tim Gruene
-
Article
| Open AccessA metal–organic framework for efficient water-based ultra-low-temperature-driven cooling
Ultra-low-temperature-actuated adsorption-driven chillers that rely on water as the cooling agent are desirable for energy-efficient and environmentally benign cooling devices. Here the authors show that the metal–organic framework of composition [Al(OH)(C6H2O4S)] displays high water uptake capacity, high stability, and driving temperatures as low as 60 °C.
- Dirk Lenzen
- , Jingjing Zhao
- & Norbert Stock
-
Article
| Open AccessSub-stoichiometric 2D covalent organic frameworks from tri- and tetratopic linkers
Using complementary linkers as building blocks in the design of 2D covalent organic frameworks (COFs) limits the formation of compositionally and structurally complex networks. Here, the authors demonstrate a COF with a bex topology by combining non-complementary triangular and rectangular linkers.
- Tanmay Banerjee
- , Frederik Haase
- & Bettina V. Lotsch
-
Article
| Open AccessForce-driven reversible liquid–gas phase transition mediated by elastic nanosponges
Conventional cooling systems rely on environmentally harmful halocarbons, while alternatives based on solid–solid transitions do not reach the required performance. Here the authors demonstrate using water and alcohol as refrigerants, through their confinement in nanosponges and their release by mechanical pressure.
- Keita Nomura
- , Hirotomo Nishihara
- & Takashi Kyotani
-
Article
| Open AccessMetal-organic framework crystal-glass composites
The formation of composite materials has been widely exploited to alter the chemical and physical properties of their components. Here the authors form metal–organic framework (MOF) crystal–glass composites in which a MOF glass matrix stabilises the open pore structure of MIL-53, leading to enhanced CO2 adsorption.
- Jingwei Hou
- , Christopher W. Ashling
- & Thomas D. Bennett
-
Article
| Open AccessTuning porosity in macroscopic monolithic metal-organic frameworks for exceptional natural gas storage
While metal–organic frameworks exhibit record-breaking gas storage capacities, their typically powdered form hinders their industrial applicability. Here, the authors engineer UiO-66 into centimetre-sized monoliths with optimal pore-size distributions, achieving benchmark volumetric working capacities for both CH4 and CO2.
- B. M. Connolly
- , M. Aragones-Anglada
- & D. Fairen-Jimenez
-
Article
| Open AccessIntegration of a (–Cu–S–)n plane in a metal–organic framework affords high electrical conductivity
Metal–organic frameworks that contain metal–sulfur chains have been demonstrated to exhibit good electrical conductivity. Here, the authors integrate a 2D metal–sulfur plane into a metal–organic framework, reporting a single crystal with a high conductivity of 10.96 S/cm.
- Abhishek Pathak
- , Jing-Wen Shen
- & Kuang-Lieh Lu
-
Article
| Open AccessControllable ion transport by surface-charged graphene oxide membrane
Graphene oxide membranes have great potential in separation processes, but small ions rejection needs improvement for large scale applications. Here the authors manipulate the membrane’s surface charge to control selective ion transport, achieving high rejection for A2B and AB2 type salts and maintaining high water permeance.
- Mengchen Zhang
- , Kecheng Guan
- & Nanping Xu
-
Article
| Open AccessStructural dynamics of a metal–organic framework induced by CO2 migration in its non-uniform porous structure
Metal–organic frameworks that undergo structural transitions in response to external stimuli are promising for gas storage, but the mechanisms of such dynamics are poorly understood. Here the authors show that the structural transformation of ZIF-7 is induced by CO2 migration through its non-uniform porous structure.
- Pu Zhao
- , Hong Fang
- & Simon A. T. Redfern
-
Article
| Open AccessBlock copolymer derived uniform mesopores enable ultrafast electron and ion transport at high mass loadings
High mass loading and fast charge transport are two crucial but often mutually exclusive characteristics of pseudocapacitors. Here, the authors address this challenge by making use of block copolymer phase separation in the synthesis of porous carbon fibres as carbon supports for pseudocapacitors.
- Tianyu Liu
- , Zhengping Zhou
- & Guoliang Liu
-
Article
| Open AccessPorous hypercrosslinked polymer-TiO2-graphene composite photocatalysts for visible-light-driven CO2 conversion
Renewable CO2 conversion to useful products presents a sustainable, carbon-neutral method to limit climate change, yet few materials can perform this complex chemistry. Here, authors prepare a polymer-TiO2-graphene composite that can take up CO2 and convert it to CH4 using light and water.
- Shaolei Wang
- , Min Xu
- & Bien Tan
-
Article
| Open AccessPermanent porous hydrogen-bonded frameworks with two types of Brønsted acid sites for heterogeneous asymmetric catalysis
The search for porous materials with strong Brønsted acid sites for challenging chemical reactions has been of significant interest, but remains challenging. Here the authors report a cage extension strategy to construct chiral permanent porous hydrogen-bonded frameworks with strong Brønsted acid groups for heterogeneous asymmetric catalysis.
- Wei Gong
- , Dandan Chu
- & Yan Liu
-
Article
| Open AccessPorous supraparticle assembly through self-lubricating evaporating colloidal ouzo drops
Mass fabrication of supraparticles is essential for their applications, but it is not easy. Tan et al. produce porous supraparticles with tunable shapes by drying colloidal particles in water-ethanol-oil ternary drops, where the pining effect at drop edges is alleviated by the formation of oil rings.
- Huanshu Tan
- , Sanghyuk Wooh
- & Detlef Lohse
-
Article
| Open AccessCooperative adsorption of carbon disulfide in diamine-appended metal–organic frameworks
The large-scale production of CS2 presents both environmental and biological hazards, yet adsorbents capable of CS2 capture remain scarcely explored. Here, Long and colleagues demonstrate that CS2 is adsorbed in diamine-appended metal–organic frameworks through a cooperative and chemically specific insertion process.
- C. Michael McGuirk
- , Rebecca L. Siegelman
- & Jeffrey R. Long
-
Article
| Open AccessMetal-organic framework glasses with permanent accessible porosity
Metal–organic framework glasses have emerged as a new family of melt-quenched glass, but have yet to display the accessible porosity of their crystalline counterparts. Here, Bennett and colleagues report that glasses derived from ZIF-76 parent materials possess 4 – 8 Å pores and exhibit reversible gas adsorption.
- Chao Zhou
- , Louis Longley
- & Thomas D. Bennett
-
Article
| Open AccessA robust zirconium amino acid metal-organic framework for proton conduction
Metal-organic frameworks are promising materials for proton exchange membrane fuel cells, but cumbersome ligand preparation and use of toxic metals or solvents hinders their application. Here, the authors report the green synthesis of a zirconium, amino acid-based MOF that displays high proton conductivity and excellent stability.
- Sujing Wang
- , Mohammad Wahiduzzaman
- & Christian Serre
-
Article
| Open AccessContinuous negative-to-positive tuning of thermal expansion achieved by controlled gas sorption in porous coordination frameworks
Achieving control over the thermomechanical properties of functional materials is desirable, yet remains highly challenging. Here, the authors demonstrate continuous negative-to-positive tuning of thermal expansion in two Prussian blue analogues, by varying the concentration of adsorbed CO2.
- Josie E. Auckett
- , Arnold A. Barkhordarian
- & Cameron J. Kepert
-
Article
| Open AccessMetal-organic framework patterns and membranes with heterogeneous pores for flow-assisted switchable separations
Tailoring MOFs to allow access of complex and large molecules is a challenging task due to their inherent microporous nature. Here the authors engineer meso- and macroporous MOF patterns and membranes via a mild decarboxylation applicable to different substrates, demonstrating their potential in macromolecule separations.
- Guan-Young Jeong
- , Ajay K. Singh
- & Dong-Pyo Kim
-
Article
| Open AccessControl of coordinatively unsaturated Zr sites in ZrO2 for efficient C–H bond activation
Identifying active sites and designing rationally heterogeneous catalysts are not inherently straightforward due to their complexity. Here, the authors reveal the nature of active sites for efficient C–H bond activation in C1-C4 alkanes over bare ZrO2 and provide fundamentals for controlling their concentration.
- Yaoyuan Zhang
- , Yun Zhao
- & Evgenii V. Kondratenko
-
Article
| Open AccessCreating solvation environments in heterogeneous catalysts for efficient biomass conversion
Solvents play important roles in chemical transformations, but isolating products from solvents is cumbersome and energy-consuming. Here, the authors develop promising alternatives by anchoring the solvent moieties onto porous materials for creating solvation environments in heterogeneous catalysts for efficient biomass conversion.
- Qi Sun
- , Sai Wang
- & Feng-Shou Xiao
-
Article
| Open AccessA dynamic and multi-responsive porous flexible metal–organic material
Stimuli-responsive porous materials are attractive for a range of applications, but each material typically exhibits only one type of transformation. Here, the authors report on a metal–organic material that exhibits six distinct phases as a result of four types of structural transformation in response to different stimuli.
- Mohana Shivanna
- , Qing-Yuan Yang
- & Michael J. Zaworotko
-
Article
| Open AccessFacile transformation of imine covalent organic frameworks into ultrastable crystalline porous aromatic frameworks
Despite recent success in developing new covalent organic frameworks (COFs) materials, synthesis of chemically stable COFs still remains challenging. Here the authors demonstrate a facile strategy that transforms imine-linked COFs into robust porous aromatic frameworks by kinetically fixing the reversible imine linkage via an aza-Diels-Alder cycloaddition reaction.
- Xinle Li
- , Changlin Zhang
- & Yi Liu
-
Article
| Open AccessSelf-assembly of metal–organic polyhedra into supramolecular polymers with intrinsic microporosity
Porosity in metal–organic materials typically relies on highly ordered crystalline networks, which hinders material processing and morphological control. Here, the authors use metal–organic polyhedra as porous monomers in supramolecular polymerization to produce colloidal spheres and gels with intrinsic microporosity.
- Arnau Carné-Sánchez
- , Gavin A. Craig
- & Shuhei Furukawa
-
Article
| Open AccessSingle-layer graphene membranes by crack-free transfer for gas mixture separation
Graphene shows great promise for gas separation applications, but obtaining large membranes that are free of cracks and tears remains highly challenging. Here, the authors realize monolayer, crack-free, millimeter-scale graphene membranes that exhibit selective gas permeation solely thanks to their intrinsic defects
- Shiqi Huang
- , Mostapha Dakhchoune
- & Kumar Varoon Agrawal
-
Article
| Open AccessTransient modes of zeolite surface growth from 3D gel-like islands to 2D single layers
While zeolites are industrially relevant as molecular sieves and catalysts, their growth mechanisms remain widely debated. Here, Rimer and colleagues probe the crystallization pathway of zeolite LTA with spatiotemporal resolution, identifying a distinctive nonclassical pathway, and demonstrating that growth is highly dependent on synthetic conditions.
- Manjesh Kumar
- , Madhuresh K. Choudhary
- & Jeffrey D. Rimer
-
Article
| Open AccessSelf-activated surface dynamics in gold catalysts under reaction environments
Nanoporous gold (NPG) has gained significant attention, but its catalytically active structure has not yet been clarified. Here, the authors identify the catalytically active and dynamic structure in NPG by combining atomic-scale and microsecond-resolution environmental transmission electron microscopy with ab initio calculations.
- Naoto Kamiuchi
- , Keju Sun
- & Seiji Takeda
-
Article
| Open AccessTopologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers
The separation of C6 alkane isomers is crucial to the petroleum refining industry, but the distillation methods in place are energy intensive. Here, the authors design a series of topologically-guided zirconium-based metal-organic frameworks with optimized pore structures for efficient C6 alkane isomer separations.
- Hao Wang
- , Xinglong Dong
- & Jing Li
-
Article
| Open AccessChemical diversity in a metal–organic framework revealed by fluorescence lifetime imaging
Metal-organic frameworks are typically characterized by a variety of techniques, but most only provide information on properties as an average of a bulk sample. Here, Wuttke and colleagues demonstrate that fluorescence imaging and lifetime analysis allows access to local information on defects and functional groups.
- Waldemar Schrimpf
- , Juncong Jiang
- & Stefan Wuttke
-
Article
| Open AccessA phase transformable ultrastable titanium-carboxylate framework for photoconduction
Porous TiO2 materials are attractive for energy-related applications owing to their accessible active sites, but suffer from poor stability. Here the authors synthesize a highly stable and porous metal–organic framework containing polymeric 1D Ti–O subunits, which displays a high condensation degree and high photoconductivity.
- Sujing Wang
- , Takashi Kitao
- & Christian Serre
-
Article
| Open AccessBio-inspired nano-traps for uranium extraction from seawater and recovery from nuclear waste
Uranium extraction is important for both uranium recovery and nuclear waste management. Here, inspired by the high sensitivity of proteins towards specific metal ions, Ma and colleagues demonstrate that introducing secondary coordination spheres into amidoxime-functionalized porous polymers can enhance their uranyl chelating abilities.
- Qi Sun
- , Briana Aguila
- & Shengqian Ma
-
Article
| Open AccessThe effect of crystallite size on pressure amplification in switchable porous solids
Pressure amplification phenomena have recently been observed in ordered mesoporous solids, but little is understood about this counter-intuitive behaviour. Here, Kaskel and colleagues demonstrate that crystal size can play an important role in modulating pressure amplification in metal-organic frameworks.
- Simon Krause
- , Volodymyr Bon
- & Stefan Kaskel
-
Article
| Open AccessHighly stable graphene-oxide-based membranes with superior permeability
Graphene oxide membranes show great potential for water filtering, but improving their performance and stability remains difficult. Here, the authors use theanine amino acid and tannic acid to reduce and cross-link graphene oxide membranes with remarkably high permeability and stability in aqueous solution.
- Khalid Hussain Thebo
- , Xitang Qian
- & Wencai Ren
-
Article
| Open AccessUnderstanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling
Understanding host–guest interactions and structural changes within porous materials is crucial for enhancing gas storage properties. Here, the authors combine cryogenic loading of gases with high pressure crystallography and computational techniques to obtain atomistic detail of adsorption-induced structural and energetic changes in ZIF-8.
- Claire L. Hobday
- , Christopher H. Woodall
- & Stephen A. Moggach
-
Article
| Open AccessA non-invasive method to directly quantify surface heterogeneity of porous materials
Surface heterogeneity significantly influences the properties of porous materials, but remains extremely difficult to characterize. Here, the authors extend Porod’s scattering law from homogeneous to heterogeneous porous materials, allowing for surface variation to be non-invasively probed.
- Wei-Shan Chiang
- , Daniel Georgi
- & Yun Liu
-
Article
| Open AccessOxidation-stable amine-containing adsorbents for carbon dioxide capture
Amine-containing solids are promising adsorbents for CO2 capture, but their low oxidative stability has hindered their application. Here, Choi and colleagues develop a strategy to poison the metal impurities present in poly(ethyleneimine)/silica adsorbents, significantly improving their stability towards oxidation.
- Kyungmin Min
- , Woosung Choi
- & Minkee Choi
-
Article
| Open AccessA general soft-enveloping strategy in the templating synthesis of mesoporous metal nanostructures
Metal species are highly mobile within mesoporous silica, making it difficult to template growth of metallic nanocrystals inside the channels. Here, the authors introduce a solid-liquid-solution interfacial strategy to suppress migration of the metal species, achieving control over a variety of mesostructured nanomaterials.
- Jixiang Fang
- , Lingling Zhang
- & Hongjun You