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| Open AccessThe effect of enantioselective chiral covalent organic frameworks and cysteine sacrificial donors on photocatalytic hydrogen evolution
Chiral covalent organic frameworks are demonstrated to enable the docking of sacrificial electron donors via enantioselective combination, thereby improving oxidative half-reaction kinetics and boosting visible photocatalytic H2 production.
- Weijun Weng
- & Jia Guo
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Article
| Open AccessOscillating light engine realized by photothermal solvent evaporation
Developing an oscillating actuator that can directly convert solar energy into mechanical energy is highly desirable. Here, authors report a solvent-assisted light-driven oscillator by porous film that achieves excellent oscillating actuation performance and can even oscillate by carrying a load under light irradiation.
- Jingjing Li
- , Linlin Mou
- & Yongsheng Chen
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Article
| Open AccessElectronic modulation of metal-support interactions improves polypropylene hydrogenolysis over ruthenium catalysts
Catalytic pathways of plastic waste valorization to lubricants are attractive avenues to foster circular economy. Tuning of catalyst electronic properties allows to significantly improve its activity due to boosted hydrogen storage on the surface.
- Pavel A. Kots
- , Tianjun Xie
- & Dionisios G. Vlachos
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| Open AccessPrecursor engineering of hydrotalcite-derived redox sorbents for reversible and stable thermochemical oxygen storage
Thermochemical redox reactions of metal oxides are promising for CO2 capture, gas purification, air separation, and energy storage. Here, the authors report mixed metal oxides derived from layered double hydroxides precursors, and demonstrate their reversible and stable thermochemical oxygen storage.
- Michael High
- , Clemens F. Patzschke
- & Qilei Song
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| Open AccessUnderstanding the lithium–sulfur battery redox reactions via operando confocal Raman microscopy
The complex redox processes in lithium–sulfur batteries are not yet fully understood at the fundamental level. Here, the authors report operando confocal Raman microscopy measurements to provide mechanistic insights into polysulfide evolution and sulfur deposition during battery cycling.
- Shuangyan Lang
- , Seung-Ho Yu
- & Héctor D. Abruña
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| Open AccessLinking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O
A crystalline hetero-metallic cluster catalyst based on a covalent organic framework strategy is reported. The catalyst can facilitate both photocatalytic oxidative and reductive reactions leading to efficient production of HCOOH from CO2 and H2O.
- Jie Zhou
- , Jie Li
- & Ya-Qian Lan
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Article
| Open AccessCation-selective two-dimensional polyimine membranes for high-performance osmotic energy conversion
Two-dimensional (2D) membranes are emerging candidates for osmotic energy conversion but the trade-off between ion selectivity and conductivity remains the key bottleneck. Here, the authors demonstrate a fully crystalline imine-based 2D polymer membrane capable of combining excellent ionic conductivity and high selectivity for osmotic energy conversion.
- Zhen Zhang
- , Preeti Bhauriyal
- & Xinliang Feng
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| Open AccessDevelopment of efficient aqueous organic redox flow batteries using ion-sieving sulfonated polymer membranes
Aqueous organic redox flow batteries are promising for grid-scale energy storage, although their practical application is still limited. Here, the authors report highly ion-conductive and selective polymer membranes, which boost the battery’s efficiency and stability, offering cost-effective electricity storage.
- Chunchun Ye
- , Anqi Wang
- & Qilei Song
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Article
| Open AccessHighly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes
Catalytic hydrogenation of available nitroarenes is an environmentally benign and recyclable approach to synthesize value-added amines. Here, the authors design a RuNi single atom alloy with host-dopant synergistic effect, which exhibits outstanding performance toward nitroarenes hydrogenation.
- Wei Liu
- , Haisong Feng
- & Min Wei
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Article
| Open AccessModulating inherent lewis acidity at the intergrowth interface of mortise-tenon zeolite catalyst
The acid sites are important local structures to determine catalytic performances of zeolites. Here, the authors expand the interface engineering to the field of porous zeolites through the lattice mismatch of the intergrown zeolite to enrich the inherent Lewis acid sites at the interface of a mortise-tenon ZSM-5 catalyst.
- Huiqiu Wang
- , Boyuan Shen
- & Weizhong Qian
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Article
| Open AccessDirect synthesis of highly stretchable ceramic nanofibrous aerogels via 3D reaction electrospinning
Ceramic aerogels are generally brittle and often tend to structurally collapse under large external tensile strain. Here the authors synthesize large-scale stretchable ceramic aerogels with interwoven crimped nanofibers by combining electrohydrodynamic method and 3D reaction electrospinning.
- Xiaota Cheng
- , Yi-Tao Liu
- & Bin Ding
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Article
| Open AccessHydrogen spillover assisted by oxygenate molecules over nonreducible oxides
Spontaneous migration of H-atoms from metal particles to a nonreducible oxide support is generally limited by thermodynamics. Here, small oxygenate molecules are found to act as effective H-carriers to promote this process and lead to much improved hydrodeoxygenation rates on Pt-Fe/SiO2 catalysts.
- Mingwu Tan
- , Yanling Yang
- & Yong Wang
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Article
| Open AccessControl of zeolite framework flexibility for ultra-selective carbon dioxide separation
All-silica zeolite membranes are highly desired for natural gas upgrading but the size-exclusion effect is compromised by defects generated during high-temperature detemplation. Here, the authors develop a strategy to fabricate ultra-selective DD3R zeolite membranes via tuning the zeolite flexibility under rapid template decomposition.
- Peng Du
- , Yuting Zhang
- & Xuehong Gu
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Article
| Open AccessReversible dehydrogenation and rehydrogenation of cyclohexane and methylcyclohexane by single-site platinum catalyst
Developing highly efficient and reversible hydrogenation-dehydrogenation catalysts shows great promise for hydrogen storage technologies. Here the authors develop a highly efficient and reversible de/rehydrogenation single-site platinum catalyst which exhibits great promise for hydrogen storage technologies with cyclic alkanes/aromatics as liquid organic hydrogen carriers.
- Luning Chen
- , Pragya Verma
- & Ji Su
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Article
| Open AccessAssembling covalent organic framework membranes with superior ion exchange capacity
Covalent organic framework-based membranes are highly tunable materials with potential use in a variety of applications. Here the authors report a dual-activation interfacial polymerization strategy to prepare ionic covalent organic framework membranes with high ion exchange capacity.
- Xiaoyao Wang
- , Benbing Shi
- & Zhongyi Jiang
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Article
| Open AccessDecoding reactive structures in dilute alloy catalysts
Rational catalyst design is crucial toward achieving more energy-efficient and sustainable catalytic processes. Here the authors report a data-driven approach for understanding catalytic reactions mechanisms in dilute bimetallic catalysts by combining X-ray absorption spectroscopy with activity studies and kinetic modeling.
- Nicholas Marcella
- , Jin Soo Lim
- & Anatoly I. Frenkel
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Article
| Open AccessDirect assessment of confinement effect in zeolite-encapsulated subnanometric metal species
Zeolite-encapsulated metal nanoparticles have important catalytic properties, but their effect on the zeolite local structure has been difficult to characterize. Here the authors, using DFT calculations and scanning transmission electron microscopy, characterize the local strain due to confinement effects in metal-zeolite catalysts.
- Lichen Liu
- , Miguel Lopez-Haro
- & Avelino Corma
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| Open AccessIntra-crystalline mesoporous zeolite encapsulation-derived thermally robust metal nanocatalyst in deep oxidation of light alkanes
Zeolite-confined metal nanoparticles (NPs) have attracted much attention owing to their superior sintering resistance and broad applications. Here the authors develop a facile in situ mesoporogen-free strategy to design and synthesize palladium NPs enveloped within a single-crystalline zeolite with intra-mesopores.
- Honggen Peng
- , Tao Dong
- & Sheng Dai
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| Open AccessFine pore engineering in a series of isoreticular metal-organic frameworks for efficient C2H2/CO2 separation
The separation of acetylene and carbon dioxide by porous materials requires delicate control over the pore size. Herein, the authors fine-tune the pore size at sub-nanometer scale in a series of isoreticular metal-organic frameworks to control the acetylene/carbon dioxide separation performance; subtle structural differences lead to remarkable performance enhancement.
- Jun Wang
- , Yan Zhang
- & Banglin Chen
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| Open AccessUltralow-temperature-driven water-based sorption refrigeration enabled by low-cost zeolite-like porous aluminophosphate
Thermally-driven water-sorption refrigeration is a promising environmentally friendly technology, but finding suitable porous materials is challenging. The authors report a very high coefficient of performance using a low-cost zeolite-like aluminophosphate as a water sorbent, suitable for use with low-grade thermal energy.
- Zhangli Liu
- , Jiaxing Xu
- & Xiulan Huai
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Article
| Open AccessFacile construction of fully sp2-carbon conjugated two-dimensional covalent organic frameworks containing benzobisthiazole units
Synthesis of fully π-conjugated covalent organic frameworks (COFs) remains still challenging. Here, the authors propose a versatile synthesis method based on Knoevenagel polycondensation for the synthesis of vinylene-linked benzobisthiazole-based 2D COFs.
- Yuancheng Wang
- , Wenbo Hao
- & Yingjie Zhao
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Article
| Open AccessWater cluster in hydrophobic crystalline porous covalent organic frameworks
Research on water confinement in small hydrophobic pores remains scarce because of a preconception that small hydrophobic pores repulse water molecules. Here, the authors demonstrate water confinement across hydrophobic microporous channels in crystalline covalent organic frameworks.
- Ke Tian Tan
- , Shanshan Tao
- & Donglin Jiang
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Article
| Open AccessStrong metal-support interactions induced by an ultrafast laser
Constructing strong metal-support interactions (SMSI) is an effective means of regulating the interfacial properties of noble metal-based supported catalysts. Here, the authors propose a strategy of ultrafast laser-induced SMSI that can be constructed on a CeO2-supported Pt system by confining electric field in localized interface.
- Jian Zhang
- , Dezhi Zhu
- & Chang-An Wang
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Article
| Open AccessImmobilized covalent triazine frameworks films as effective photocatalysts for hydrogen evolution reaction
While covalent triazine frameworks are promising photocatalytic materials, it is challenging to prepare large-scale thin films. Here, authors report an interfacial polymerization method to prepare photocatalytic covalent triazine framework thin films with lateral sizes up to 250 cm2.
- Xunliang Hu
- , Zhen Zhan
- & Bien Tan
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Article
| Open AccessOne-step ethylene production from a four-component gas mixture by a single physisorbent
The purification of ethylene is an industrially relevant process. Here, the authors report the one-step separation of ethylene from quaternary gas mixtures of hydrocarbons and CO2 using a single metal–organic framework-based physisorbent.
- Jian-Wei Cao
- , Soumya Mukherjee
- & Kai-Jie Chen
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Article
| Open AccessThe origin of the particle-size-dependent selectivity in 1-butene isomerization and hydrogenation on Pd/Al2O3 catalysts
The selectivity of Pd catalysts in 1-butene hydrogenation and isomerization depends on nanoparticle size. Herein, the authors show by combining experiment and modeling that the type and specific properties of the contributing surface facets are decisive for the selectivity.
- Alexander Genest
- , Joaquín Silvestre-Albero
- & Günther Rupprechter
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Article
| Open AccessSelf-regeneration of supported transition metals by a high entropy-driven principle
Sintering of supported transition metal catalysts is problematic for high-temperature catalysis. Here the authors report entropy-driven, self-regeneration of high entropy oxide nanoparticles, promoting better stability and in situ reversible exsolution-dissolution process in multi-redox cycles.
- Shengtai Hou
- , Xuefeng Ma
- & Sheng Dai
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Article
| Open AccessIonic liquid facilitated melting of the metal-organic framework ZIF-8
The variety of hybrid glasses from metal-organic frameworks (MOFs) has remained strongly limited to only a handful of compounds. Here, the authors introduce a route to melt highly porous and non-meltable MOFs using ionic liquids in order to extend the range of MOF glasses.
- Vahid Nozari
- , Courtney Calahoo
- & Lothar Wondraczek
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| Open AccessDual metal nanoparticles within multicompartmentalized mesoporous organosilicas for efficient sequential hydrogenation
Controlling localization of multiple metal nanoparticles on a single support is at the cutting edge of designing innovatory cascade catalysts. Here, the authors report a multicompartmentalized mesoporous organosilica to spatially position different metal nanoparticles in intimate proximity for efficient sequential hydrogenation reactions.
- Houbing Zou
- , Jinyu Dai
- & Hengquan Yang
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| Open AccessAtomically dispersed Pb ionic sites in PbCdSe quantum dot gels enhance room-temperature NO2 sensing
Quantum dot-based NO2 sensors often suffer from low sensitivity or long recovery times. Here, the authors report that bimetallic PbCdSe quantum dot gels containing atomically dispersed Pb ionic sites enable ultra-sensitive and fast NO2 sensing.
- Xin Geng
- , Shuwei Li
- & Long Luo
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| Open AccessQuantification of critical particle distance for mitigating catalyst sintering
Deactivation of supported metal catalysts via thermally induced sintering is a major concern in the catalysis community. Here, the authors demonstrate that enlarging particle distance to over the critical distance could suppress the particle coalescence greatly up to 900 °C.
- Peng Yin
- , Sulei Hu
- & Hai-Wei Liang
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Article
| Open Access17O-EPR determination of the structure and dynamics of copper single-metal sites in zeolites
The identification of catalytically active sites with atomic-scale precision occupies a central place in the theory and practice of heterogeneous catalysis. Here the authors assess the nature of the copper-oxygen bond in a Cu-CHA zeolite and recover the microscopic structure of single-metal sites.
- Paolo Cleto Bruzzese
- , Enrico Salvadori
- & Mario Chiesa
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| Open AccessEncapsulate α-MnO2 nanofiber within graphene layer to tune surface electronic structure for efficient ozone decomposition
Ozone is a major air pollutant, but its elimination is challenging. Here the authors encapsulate defective α-MnO2 nanofiber within ultrathin graphene shells to construct a hierarchical MnO2@graphene catalyst for ozone decomposition that possesses high activity and stability under humid conditions.
- Guoxiang Zhu
- , Wei Zhu
- & Yongfa Zhu
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Article
| Open AccessFrustrated flexibility in metal-organic frameworks
Responsiveness in metal-organic frameworks involving amorphous phases remains poorly understood. Here, the authors demonstrate MOFs that reversibly switch between well-defined crystalline and structurally degenerate amorphous states mediated by competing intra-framework forces.
- Roman Pallach
- , Julian Keupp
- & Sebastian Henke
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| Open AccessDesign of carbon supports for metal-catalyzed acetylene hydrochlorination
Carbons are indispensable as supports for metal-based catalysts in polyvinyl chloride manufacture via acetylene hydrochlorination. In this work, the acetylene interaction, tunable through adjusting microporosity and oxygen sites is identified as central activity and stability descriptor.
- Selina K. Kaiser
- , Ivan Surin
- & Javier Pérez-Ramírez
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| Open AccessPEG-stabilized coaxial stacking of two-dimensional covalent organic frameworks for enhanced photocatalytic hydrogen evolution
Two-dimensional covalent organic frameworks are expected to boost photocatalytic H2 evolution from water splitting, but are not stable in photocatalysis. Here, authors demonstrate that photocatalytic performances can be enhanced by stabilizing layered stacking via a polymer-infiltration strategy.
- Ting Zhou
- , Lei Wang
- & Jia Guo
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Article
| Open AccessThe origin of the high electrochemical activity of pseudo-amorphous iridium oxides
The origins of the superior catalytic activity of poorly crystallized Ir-based oxide material for the OER in acid is still under debate. Here, authors synthesize porous IrMo oxides to deconvolute the effect of Ir oxidation state from short-range ordering and show the latter to be a key factor.
- Marine Elmaalouf
- , Mateusz Odziomek
- & Jennifer Peron
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| Open AccessHydrogen spillover-driven synthesis of high-entropy alloy nanoparticles as a robust catalyst for CO2 hydrogenation
Facile fabrication of high-entropy alloys (HEAs) nanoparticles (NPs) on conventional catalyst supports remains challenging. Here the authors show TiO2 is a promising platform for the low-temperature synthesis of supported CoNiCuRuPd HEA NPs with excellent activity and durability in CO2 hydrogenation.
- Kohsuke Mori
- , Naoki Hashimoto
- & Hiromi Yamashita
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Article
| Open AccessSulfur stabilizing metal nanoclusters on carbon at high temperatures
The sulfur is a documented poison reagent for metal catalysts. Here the authors show when doped in a carbon matrix, sulfur can enhance the adhesion strength and eventually suppress the metal sintering, which improve the performance of propane dehydrogenation by strong chemical/electronic interactions.
- Peng Yin
- , Xiao Luo
- & Hai-Wei Liang
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Article
| Open AccessResolving atomic SAPO-34/18 intergrowth architectures for methanol conversion by identifying light atoms and bonds
The micro-structures of zeolite catalysts affect their macroarchitectures and catalytic performances. Here, the different SAPO-34/18 intergrowth catalysts are atomically resolved, and the correlation between synthesis conditions and zeolite structures is revealed to further enhance their performances in methanol conversion.
- Boyuan Shen
- , Xiao Chen
- & Fei Wei
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Article
| Open AccessOperando high-pressure investigation of size-controlled CuZn catalysts for the methanol synthesis reaction
The nature of the active species over Cu/ZnO catalysts for methanol synthesis remains elusive. Here, the authors shed light on the evolution of the nanoparticle/support interface and correlate its structural and chemical transformations with changes in the catalytic performance.
- Núria J. Divins
- , David Kordus
- & Beatriz Roldan Cuenya
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Article
| Open AccessNanoengineered chiral Pt-Ir alloys for high-performance enantioselective electrosynthesis
Tremendous efforts have been made over the past decades regarding the development of materials with enantioselective properties. Here, the authors present a nanostructured chiral imprinted metal alloy that exhibits high enantioselectivity and stability for the electrosynthesis of chiral molecules.
- Sopon Butcha
- , Sunpet Assavapanumat
- & Alexander Kuhn
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Article
| Open AccessSimple physical mixing of zeolite prevents sulfur deactivation of vanadia catalysts for NOx removal
V-based NOx abatement systems are limited in operating at low-temperatures due to the formation of ammonium bisulfate that blocks active sites of catalysts. Here, the authors report that physically mixed zeolites trap ammonium bisulfate in their micropores, thereby protecting the catalysts.
- Inhak Song
- , Hwangho Lee
- & Do Heui Kim
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Article
| Open AccessTime-resolved in situ visualization of the structural response of zeolites during catalysis
Study of structural inhomogeneities in zeolites is important but limited by conventional techniques. Here the authors employ in situ free-electron-laser-based time-resolved coherent X-ray diffraction imaging to visualize the effect of these inhomogeneities during catalytic deoxygenation of NOx.
- Jinback Kang
- , Jerome Carnis
- & Hyunjung Kim
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Article
| Open AccessSelf-templated synthesis of uniform hollow spheres based on highly conjugated three-dimensional covalent organic frameworks
Covalent organic frameworks (COFs) are promising porous crystalline materials but controllable synthesis of COFs with uniform morphology remains challenging. Here, the authors report a self-templated synthesis of uniform and unique hollow spheres based on highly conjugated three-dimensional COFs.
- Yuan-Yuan Liu
- , Xiang-Chun Li
- & Wei Huang
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Article
| Open AccessEfficient separation of xylene isomers by a guest-responsive metal–organic framework with rotational anionic sites
The separation of xylene isomers remains a great challenge in industry due to their similar molecular structure and physical properties. Here the authors demonstrate adaptively molecular discrimination of xylene isomers by employing a NbOF52−-pillared metal–organic framework with rotational anionic sites.
- Xili Cui
- , Zheng Niu
- & Huabin Xing
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Comment
| Open AccessPorous organic materials offer vast future opportunities
In light of the surging research on porous organic materials, we herein discuss the key issues of their porous structures, surface properties, and end functions. We also present an outlook on emerging opportunities, new applications, and data science-assisted materials discovery.
- Tianyu Liu
- & Guoliang Liu
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Comment
| Open AccessMuch ado about nothing – a decade of porous materials research
Research on porous materials has produced intriguing novel materials in terms of composition, porosity and structures recently. This perspective aims to provide a short overview on some of the highlights reported within the last decade in this field.
- Arne Thomas
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Article
| Open AccessCatalytic nanosponges of acidic aluminosilicates for plastic degradation and CO2 to fuel conversion
The synthesis of solid acids with strong zeolite-like acidity and textural properties like amorphous aluminosilicates (ASAs) is still a challenge. Here the authors synthesized “acidic amorphous aluminosilicates”, with Brønsted acidic sites like in zeolites and textural properties like ASAs for catalyzing various reactions.
- Ayan Maity
- , Sachin Chaudhari
- & Vivek Polshettiwar