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| Open AccessUnderstanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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Article
| Open AccessExtreme Li-Mg selectivity via precise ion size differentiation of polyamide membrane
Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. Here the authors report the fabrication of polyamide NF membranes with ultra-high Li + /Mg2+ selectivity by modifying the interfacial polymerization process with an oil-soluble surfactant.
- Quan Peng
- , Ruoyu Wang
- & Lei Jiang
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Article
| Open AccessLiquid metals for boosting stability of zeolite catalysts in the conversion of methanol to hydrocarbons
For the methanol-to-hydrocarbons process, coke build can rapidly deactivate the zeolite catalyst. Here the authors show that the addition of liquid metal gallium can reduce coke deposition and increase catalyst lifetime.
- Yong Zhou
- , Sara Santos
- & Vitaly V. Ordomsky
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Article
| Open AccessCharging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction
The catalytic efficacy of covalent organic frameworks (COFs) is constrained by their restricted electro-transfer capability and weak binding affinities for reaction intermediates. Here the authors report COFs with various pyridinic-based units for tuning their catalytic activity towards oxygen reduction reaction.
- Xiubei Yang
- , Qizheng An
- & Gaofeng Zeng
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Article
| Open AccessRobust links in photoactive covalent organic frameworks enable effective photocatalytic reactions under harsh conditions
The development of heterogeneous photocatalysts applicable under harsh conditions is challenging. Here the authors report the conversion of imine linkages into quinoline groups in triphenylamine incorporated photosensitive covalent organic frameworks to develop robust heterogeneous photocatalysts for photocatalytic applications in harsh conditions.
- Jia-Rui Wang
- , Kepeng Song
- & Yanli Zhao
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Article
| Open AccessDistribution of Pt single atom coordination environments on anatase TiO2 supports controls reactivity
Elucidating structure-function relationships is crucial for developing efficient catalysts. Here, the authors elucidate Pt single atom coordination environments on anatase TiO2 and correlate active site structure with CO oxidation activity.
- Wenjie Zang
- , Jaeha Lee
- & Xiaoqing Pan
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Article
| Open AccessUnusual flexibility of transparent poly(methylsilsesquioxane) aerogels by surfactant-induced mesoscopic fiber-like assembly
Aerogels are mechanically friable despite their attractive properties such as visible-light transparency and low thermal conductivity. Here the authors show mechanically flexible, highly transparent aerogels based on fiber-like pore skeletons.
- Ryota Ueoka
- , Yosuke Hara
- & Kazuyoshi Kanamori
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Article
| Open AccessA micro-architectured material as a pressure vessel for green mobility
A shellular is a micro-architectured material, composed of a continuous smooth-curved thin shell in the form of a triply periodic minimal surface. Here, authors propose schellular designs applied to pressure vessels and demonstrate its competitive practical features against spherical and cylindrical vessels.
- Yoon Chang Jeong
- , Seung Chul Han
- & Kiju Kang
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Article
| Open AccessSolar-driven membrane separation for direct lithium extraction from artificial salt-lake brine
An efficient and cost-effective Mg/Li separation process is necessary for lithium extraction from Salt Lake brines. Inspired by the mangroves, authors developed a direct lithium extraction method from Salt Lake brines through the synergistic effect of an ion separation membrane and a solar evaporator.
- Shenxiang Zhang
- , Xian Wei
- & Jian Jin
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Article
| Open AccessCeramic thin-film composite membranes with tunable subnanometer pores for molecular sieving
Ceramic membranes are a promising alternative to polymeric membranes for selective separations, given their ability to operate under harsh chemical conditions. Here authors demonstrate a molecular-level design of ceramic membranes with tunable subnanometer pores.
- Xuechen Zhou
- , Rahul Shevate
- & Menachem Elimelech
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Article
| Open AccessImprovement of oxygen reduction activity and stability on a perovskite oxide surface by electrochemical potential
Solid oxide fuel and electrolysis cells suffer from surface instability which challenges their performance and durability. Here, the authors report that cathodic polarization improves the electrochemical activity by formation of Ruddlesden-Popper phase, exsolution of Co, and suppression of Sr segregation.
- Sanaz Koohfar
- , Masoud Ghasemi
- & Bilge Yildiz
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Article
| Open AccessMg-incorporated sorbent for efficient removal of trace CO from H2 gas
The challenge of trace CO removal from H2 remains at the forefront of the hydrogen economy. Here, the authors demonstrated exceptional CO removal using a highly stable, hierarchically structured sorbent bead, Mg13CuCeOx. Mechanistic analysis showed the pivotal role of Mg in enhancing CO sorption.
- Gina Bang
- , Seongmin Jin
- & Chang-Ha Lee
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Article
| Open AccessDirect prediction of gas adsorption via spatial atom interaction learning
Accurate end-to-end deep learning models for adsorption prediction in porous materials would help its discovery. Here, the authors present DeepSorption, a spatial atom interaction learning network to predict structure-adsorption from atomic coordinates and chemical element types.
- Jiyu Cui
- , Fang Wu
- & Huabin Xing
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Article
| Open AccessPhotocatalytic CO2 reduction to syngas using metallosalen covalent organic frameworks
Here, the authors report a gram-scale, one-step synthesis of metallosalen-covalent organic frameworks (M(salen)-COFs) without vacuum evacuation. M(salen)-COFs exhibit good crystallinity and adjustable activities in CO2 photoreduction to syngas.
- Wei Zhou
- , Xiao Wang
- & Wei-Qiao Deng
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Article
| Open AccessEfficient photocatalytic production of hydrogen peroxide using dispersible and photoactive porous polymers
Current industrial production of hydrogen peroxide suffers from hefty energy penalties and toxic byproducts. Here, the authors report efficient photocatalytic production of hydrogen peroxide by protonation-induced dispersible porous polymers with good charge-carrier transport properties.
- Shengdong Wang
- , Zhipeng Xie
- & Cheng Gu
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Article
| Open AccessTwistedly hydrophobic basis with suitable aromatic metrics in covalent organic networks govern micropollutant decontamination
The synergetic regulation of the electronic structure and interfacial reaction of covalent organic frameworks (COF) for water purification remains a challenge. Here the authors propose that COFs materials possessing molecular interfaces with ordered π skeletons, suitable pore size, and hydrophilic/hydrophobic channels synergically break through the adsorption energy barrier achieving high removal rates for micropollutants.
- Chencheng Qin
- , Yi Yang
- & Hou Wang
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Article
| Open AccessPhotoelectric responsive ionic channel for sustainable energy harvesting
Artificial ion channels with multiple functions provide exciting opportunities to emulate natural processes and enhance energy conversion. Here, the authors introduce a family of photoelectrically responsive ionic covalent organic frameworks membranes for solar energy and salinity gradient energy conversion.
- Qing Guo
- , Zhuozhi Lai
- & Qi Sun
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Article
| Open AccessAtmospheric-moisture-induced polyacrylate hydrogels for hybrid passive cooling
Gan et al. have developed sodium polyacrylate-based films for passive radiative cooling that can be fabricated using atmospheric moisture alone, offering radiative and evaporative cooling, reducing temperatures by up to 5 °C under partly cloudy skies.
- Roisul Hasan Galib
- , Yanpei Tian
- & Qiaoqiang Gan
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Article
| Open AccessIncorporation of multiple supramolecular binding sites into a robust MOF for benchmark one-step ethylene purification
One-step separation of C2H4 from ternary C2 hydrocarbon mixtures remains a challenge for current physisorbents. Here, the authors reported a strategy of designing multiple supramolecular binding sites in a robust and scalable MOF for highly efficient one-step C2H4 purification from ternary mixtures.
- Enyu Wu
- , Xiao-Wen Gu
- & Bin Li
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Article
| Open Access3D covalent organic framework membrane with fast and selective ion transport
3D ionic covalent organic frameworks (iCOF) are used in the fabrication of membranes breaking the trade-off between ion conductivity and ion selectivity is challenging. Here, the authors report the fabrication of a 3D sulfonic acid-functionalized iCOF membrane for efficient and selective ion transport, using dual acid-mediated interfacial polymerization
- Tianhao Zhu
- , Yan Kong
- & Zhongyi Jiang
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Article
| Open AccessDual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis
In this study, benzotrithiophene-based covalent organic frameworks with spatially separated oxidative and reductive reaction centers are rationally designed for photocatalytic production of H2O2 from water and oxygen without sacrificial agents.
- Chencheng Qin
- , Xiaodong Wu
- & Hou Wang
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Article
| Open AccessImaging the dynamic influence of functional groups on metal-organic frameworks
Here authors use iDPC-STEM to directly image the rotation of linkers in MOFs, demonstrating an approach to study the local flexibility. They show that the dynamic properties of UiO-66-X are likely correlated to their macroscopic properties of CO2 uptake.
- Boyang Liu
- , Xiao Chen
- & Tiefeng Wang
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Article
| Open AccessMachine-learning-assisted material discovery of oxygen-rich highly porous carbon active materials for aqueous supercapacitors
Machine-learning technology provides a data-driven approach to find the critical features for ideal carbon-based supercapacitors. Here, the authors report machine-Learning assisted discovery of oxygen rich highly porous carbons that exhibits a high specific capacitance.
- Tao Wang
- , Runtong Pan
- & Sheng Dai
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Article
| Open AccessBreathing porous liquids based on responsive metal-organic framework particles
Responsive liquid systems which exhibit a breathing behaviour and show step-shaped gas sorption isotherms, akin to the distinct oxygen saturation curve of haemoglobin in blood have been developed. Their breathing behaviour upon sorption of industrially relevant gases is demonstrated.
- Athanasios Koutsianos
- , Roman Pallach
- & Sebastian Henke
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Article
| Open AccessPost-synthetic modification of covalent organic frameworks for CO2 electroreduction
Covalent organic frameworks constructed with ionic skeletons and C-N linkages by multilevel post-synthetic modification. These frameworks achieved high activity and stability for electrocatalytic CO2 reduction.
- Minghao Liu
- , Shuai Yang
- & Gaofeng Zeng
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Article
| Open AccessGreen synthesis of stable hybrid biocatalyst using a hydrogen-bonded, π-π-stacking supramolecular assembly for electrochemical immunosensor
Integration of nanomaterials and enzymes has potential in the development of robust biocatalysts, but preparation can still be technically challenging. Here, the authors report the preparation of a hydrogen-bonded organic framework biocatalyst and its use as an immunosensor.
- Wei Huang
- , Haitao Yuan
- & Gangfeng Ouyang
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Article
| Open AccessComputation-based regulation of excitonic effects in donor-acceptor covalent organic frameworks for enhanced photocatalysis
The donor-acceptor (D-A) interaction and exciton binding energy have been investigated for a series of D-A pairs by DFT calculations. Here, the authors synthesize the corresponding D-A COFs, and demonstrate that their photocatalytic hydrogen production activities match well with the calculation results.
- Yunyang Qian
- , Yulan Han
- & Hai-Long Jiang
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Article
| Open AccessScalable-produced 3D elastic thermoelectric network for body heat harvesting
Flexible thermoelectric generators can use body heat to power electronic wearables but are often limited by a trade-off between flexibility and output performance. Here, authors demonstrate a scalable, lightweight, elastic, and high-performing network-based Ag2Se thermoelectric generator.
- Yijie Liu
- , Xiaodong Wang
- & Feng Cao
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Article
| Open AccessOxidative cleavage and ammoxidation of organosulfur compounds via synergistic Co-Nx sites and Co nanoparticles catalysis
The cleavage and functionalization of C-S bonds has become a hot topic. Here the authors report a novel and efficient protocol that enables direct oxidative cleavage and ammoxidation of organosulfur compounds by heterogeneous nonprecious-metal Co-N-C catalyst comprising graphene encapsulated Co nanoparticles and Co-Nx sites.
- Huihui Luo
- , Shuainan Tian
- & Wen Dai
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Article
| Open AccessRecovery of homogeneous photocatalysts by covalent organic framework membranes
Transition metal-based homogenous photocatalysts are important in organic synthesis, but the metals used can be rare and immobilization of the catalysts for recycling is challenging. Here, the authors report the recovery of such catalysts using covalent organic framework membranes with tuneable pore sizes.
- Hao Yang
- , Jinhui Xu
- & Dan Zhao
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Article
| Open AccessSelective conversion of CO2 to isobutane-enriched C4 alkanes over InZrOx-Beta composite catalyst
Direct conversion of CO2 to a specific hydrocarbon with high selectivity is attractive but challenging. Here the authors report a highly active InZrOx-Beta tandem catalyst for CO2 hydrogenation to butane and develop a surface silica protection strategy to inhibit the migration of indium species, greatly improving catalytic stability.
- Han Wang
- , Sheng Fan
- & Jianguo Wang
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Article
| Open AccessRegulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation
The interaction among single sites in densely populated single-atom catalysts (SACs) has received much attention. Here the authors report a general and facile strategy for the synthesis of several densely populated SACs and decipher the influence of density on regulating their electronic structure and catalytic performance in alkene epoxidation.
- Hongqiang Jin
- , Kaixin Zhou
- & Changyan Cao
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Article
| Open AccessRegulation of molecular transport in polymer membranes with voltage-controlled pore size at the angstrom scale
The ability to regulate membrane pore size as needed has been a topic of active research for developing next-generation stimuli-responsive smart membranes. Herein, the authors report the observation of operando regulation of the pore size of A membrane based on electro-osmotic swelling.
- Yuzhang Zhu
- , Liangliang Gui
- & Jian Jin
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Article
| Open AccessAchieving volatile potassium promoted ammonia synthesis via mechanochemistry
Potassium oxide is used as a promotor in industrial ammonia synthesis, although metallic potassium is better in theory. Here, the authors demonstrate metallic potassium, an unstable metal that easily volatilizes at high temperature, can be used as a promotor for ammonia synthesis.
- Jong-Hoon Kim
- , Tian-Yi Dai
- & Jong-Beom Baek
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Article
| Open AccessInterfacial engineered superelastic metal-organic framework aerogels with van-der-Waals barrier channels for nerve agents decomposition
Personal protective equipment used to prevent exposure to chemical warfare agents are devoid of detoxifying activity. Here, the authors report MOF aerogels via a hydrogen bonding-assisted interfacial engineering strategy for nerve agent decomposition.
- Zishuo Yan
- , Xiaoyan Liu
- & Yang Si
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Article
| Open AccessStaggered circular nanoporous graphene converts electromagnetic waves into electricity
The electromagnetic (EM) energy released by electronic devices in the environment is largely wasted and contributes to EM pollution. Here, the authors report the synthesis of staggered circular nanoporous graphene enabling the absorption and conversion of EM waves into electricity via the thermoelectric effect.
- Hualiang Lv
- , Yuxing Yao
- & Xiaoguang Wang
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Article
| Open AccessLamella-heterostructured nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride electrodes as stable catalysts for oxygen evolution
Developing stable catalysts for industrial-scale current densities is challenging. Here, the authors report self-supported laminate electrodes composed of nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride hybrid that can catalyze the oxygen evolution reaction at high current densities.
- Shu-Pei Zeng
- , Hang Shi
- & Qing Jiang
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Article
| Open AccessAcidic graphene organocatalyst for the superior transformation of wastes into high-added-value chemicals
Upcycling glycerol can substantially contribute to circular carbon economy. Here, an amino acid-functionalized graphene organocatalyst with high acidity converts glycerol and biooil wastes into high-value chemicals and fuels, even at low temperatures, advancing the state-of-the-art in sustainable carbon valorization technologies and circular economy.
- Aby Cheruvathoor Poulose
- , Miroslav Medveď
- & Radek Zbořil
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Article
| Open AccessTunable hybrid zeolites prepared by partial interconversion
Hybrid zeolites, which are materials made of building units from various zeolites, have been prepared by partial interzeolite transformation. The relative proportion of the various zeolites can be conveniently tuned to optimize their catalytic performance simply by interrupting the interconversion at different times.
- Monica J. Mendoza-Castro
- , Zhipeng Qie
- & Javier García-Martínez
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Article
| Open AccessProbing sub-5 Ångstrom micropores in carbon for precise light olefin/paraffin separation
Achieving highly selective separation of olefin/paraffin is a significant challenge in the chemical industry. Here the authors present polydopamine-derived carbons with tailorable sub-5 Å micropores probed by a series of gas molecules that can realize precise size-sieving of olefin from paraffin.
- Shengjun Du
- , Jiawu Huang
- & Banglin Chen
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Article
| Open AccessLarge-scale physically accurate modelling of real proton exchange membrane fuel cell with deep learning
Accurate liquid water modelling is challenging. Here the authors use X-ray micro-computed tomography, deep learned super-resolution, multi-label segmentation, and direct multiphase simulation to simulate fuel cell and guide fuel cell design.
- Ying Da Wang
- , Quentin Meyer
- & Ryan T. Armstrong
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Article
| Open AccessCOx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5
A series of materials containing Mo-S clusters confined in zeolitic cages of ZSM-5 are reported and shown to be efficient for CO2 or CO hydrogenation with >98% selectivity to methanol, stable over 1000 h, or C2 and C3 hydrocarbons, stable over 100 h.
- Gui Liu
- , Pengfei Liu
- & Weiping Ding
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Article
| Open AccessSelective hydrogenation via precise hydrogen bond interactions on catalytic scaffolds
Weak interactions between substrates and the active site environment have been known to be vital in enzyme catalysis. Inspired by this, the authors synthesize hyper-crosslinked porous polymer-based catalysts with different H-bonds to enhance adsorption and modify the interfacial sites and reactivity.
- Song Shi
- , Piaoping Yang
- & Dionisios G. Vlachos
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Article
| Open AccessStructure sensitivity in gas sorption and conversion on metal-organic frameworks
Probing gas sorption on defects and facets of porous materials at the nanoscale is challenging. Here, we visualize nano-domains of preferred formaldehyde sorption on (defective) ZIF-8 microcrystals using in situ Photo-induced Force Microscopy (PiFM).
- Guusje Delen
- , Matteo Monai
- & Bert M. Weckhuysen
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Article
| Open AccessThe electric field cavity array effect of 2D nano-sieves
Nanocomposites are promising dielectric candidates due to their nano-modification effect. Here authors report homogeneous nano-sieves of different pore sizes and incorporate them uniformly into P(VDF-HFP)-based films with extremely low dopings.
- Fan Xu
- , Yuke Li
- & Yu Wang
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Article
| Open AccessMagnesium hexacyanoferrate nanocatalysts attenuate chemodrug-induced cardiotoxicity through an anti-apoptosis mechanism driven by modulation of ferrous iron
Doxorubicin is commonly used in cancer chemotherapy, but its cardiotoxicity from iron overload is one of the severe side effects. Here, the authors prepare magnesium hexacyanoferrate nanocatalysts to capture excess ferrous species and eliminate cytotoxic radical species in vitro and in vivo.
- Minfeng Huo
- , Zhimin Tang
- & Jianlin Shi
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Article
| Open AccessRevealing carbon capture chemistry with 17-oxygen NMR spectroscopy
A hurdle for designing improved capture materials is the lack of adequate tools to characterise how carbon dioxide adsorbs. Here the authors developed a method to understand how carbon dioxide is captured by materials. Their 17O solid-state NMR spectroscopy reveals clear signatures for different capture products.
- Astrid H. Berge
- , Suzi M. Pugh
- & Alexander C. Forse
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Article
| Open AccessQuantification of gas-accessible microporosity in metal-organic framework glasses
Glasses derived from meltable metal-organic frameworks (MOFs) offer great potential for gas separation and solid state ionics. Here, the authors quantify the porosity of a series of MOF glasses by cryogenic carbon dioxide gas sorption and propose design principles for rational tuning the glasses‘ pore size and pore volume.
- Louis Frentzel-Beyme
- , Pascal Kolodzeiski
- & Sebastian Henke
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Article
| Open Access4D printing of MXene hydrogels for high-efficiency pseudocapacitive energy storage
2D MXene hydrogels are promising for diverse applications. Here, the authors report a universal 4D printing technology to manufacture MXene hydrogels with customizable geometry, high conductivity, and efficient pseudocapacitive energy storage ability.
- Ke Li
- , Juan Zhao
- & Valeria Nicolosi