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| Open AccessRedox-tunable isoindigos for electrochemically mediated carbon capture
Electrochemically-mediated carbon capture has good energy efficiency and potential in carbon dioxide separation, but optimisation of these systems is challenging. Here, the authors report the use of isoindigo derivatives to give fine-tuned interactions with CO2 for carbon capture methods.
- Xing Li
- , Xunhua Zhao
- & Yayuan Liu
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Article
| Open AccessImpact of palladium/palladium hydride conversion on electrochemical CO2 reduction via in-situ transmission electron microscopy and diffraction
The evolution of Pd-based material during CO2 electroreduction requires further investigation. Here the authors use in-situ liquid-phase transmission electron microscopy and select area diffraction characterization techniques to visualize the morphological and phase structure evolution of the Pd/PdHx catalysts under CO2 electroreduction conditions.
- Ahmed M. Abdellah
- , Fatma Ismail
- & Drew Higgins
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Article
| Open AccessGas diffusion enhanced electrode with ultrathin superhydrophobic macropore structure for acidic CO2 electroreduction
Carbon dioxide electroreduction in acidic environments has been suboptimal. Here, the authors addressed this issue by designing a gas diffusion electrode with a special metal structure, which achieves efficient electroreduction while conducting a systematic investigation of the underlying mechanism.
- Mingxu Sun
- , Jiamin Cheng
- & Miho Yamauchi
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Article
| Open AccessVitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction
Efficiently producing multicarbon chemicals through electrochemical CO2 reduction is essential for achieving economically feasible carbon neutrality. Here, the authors present molecularly enhanced CO2-to-*CO conversion and *CO dimerization for high-rate ethylene production by nanoconfinement of ascorbic acid.
- Jongyoun Kim
- , Taemin Lee
- & Dae-Hyun Nam
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Article
| Open AccessEngineering a synthetic energy-efficient formaldehyde assimilation cycle in Escherichia coli
One-carbon substrates are attractive feedstocks for circular bioeconomy. Here, the authors design an erythrulose monophosphate (EuMP) cycle for formaldehyde assimilation, demonstrate the activity of the core reactions in E. coli, and show its integration with pathway reactions existed in pentose phosphate pathway and glycolysis.
- Tong Wu
- , Paul A. Gómez-Coronado
- & Hai He
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Article
| Open AccessA scalable membrane electrode assembly architecture for efficient electrochemical conversion of CO2 to formic acid
Electrochemical reduction of CO2 to formic acid is a promising and sustainable pathway for valuable chemical generation. However, direct production of formic acid rather than formate is challenging. Herein the authors report a zero-gap membrane electrode assembly architecture with perforated cation exchange membrane for the direct electrochemical synthesis of formic acid from CO2.
- Leiming Hu
- , Jacob A. Wrubel
- & K. C. Neyerlin
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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 AccessIntegrated urban water management by coupling iron salt production and application with biogas upgrading
Effective urban water management requires technological solutions that enable system-wide gains via a holistic approach. Here, authors propose an integrated system where an iron-oxidising electrochemical cell upgrades biogas while producing FeCO3 and subsequently uses the salt in wastewater treatment.
- Zhetai Hu
- , Lanqing Li
- & Zhiguo Yuan
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Matters Arising
| Open AccessReply to: The impact of thermodynamics when using a catalyst for conventional carbon capture solvent regeneration
- Masood S. Alivand
- , Geoffrey W. Stevens
- & Kathryn A. Mumford
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Matters Arising
| Open AccessThe impact of thermodynamics when using a catalyst for conventional carbon capture solvent regeneration
- Frédérick de Meyer
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Article
| Open AccessHow to make climate-neutral aviation fly
Europe’s aviation must reduce more than just flight CO2 emissions to achieve net-zero. Synthetic fuels and carbon capture and storage could help but decreasing air traffic is crucial due to non-CO2 climate impacts and resource constraints.
- Romain Sacchi
- , Viola Becattini
- & Marco Mazzotti
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Article
| Open AccessCu-based high-entropy two-dimensional oxide as stable and active photothermal catalyst
Synergistically enhancing catalytic stability and activity of Cu-based nanocatalysts is an ongoing challenge. Here the authors report Cu-based high-entropy two-dimensional oxide as stable and active catalyst for photothermal CO2 hydrogenation under ambient sunlight irradiation.
- Yaguang Li
- , Xianhua Bai
- & Jinhua Ye
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Article
| Open AccessAqueous phase conversion of CO2 into acetic acid over thermally transformed MIL-88B catalyst
Carbon dioxide conversion into chemicals is essential for carbon capture and utilization. Here, the authors present a novel iron-based catalyst, synthesized from the thermal treatment of a parent metal-organic framework (MIL-88B), to produce a dual-active site for carbon dioxide reduction into acetic acid.
- Waqar Ahmad
- , Paramita Koley
- & Akshat Tanksale
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Article
| Open AccessScalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis
Scalable fabrication of coordinatively unsaturated metal-nitrogen is challenging. Here the authors report a general method for synthesize such material for CO2 electrochemical conversion at a high catalytic current of 10 A for more than 60 h stability using a 100 cm2 membrane flow cell.
- Ji Wei Sun
- , Xuefeng Wu
- & Hua Gui Yang
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Article
| Open AccessSustainable methane utilization technology via photocatalytic halogenation with alkali halides
A sustainable photocatalytic methane halogenation strategy is developed for methyl halide production using low-cost alkali halides over Cu-doped TiO2 nanostructures. Copper sites ultimately stabilize *CH3 to promote reaction with Cl− to form CH3Cl.
- Jun Ma
- , Can Zhu
- & Yujie Xiong
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Article
| Open AccessBenchmark single-step ethylene purification from ternary mixtures by a customized fluorinated anion-embedded MOF
Ethylene (C2H4) purification from multi-component mixtures by physical adsorption is a great challenge in the chemical industry. Here authors present a GeF62- anion embedded MOF ZNU-6 with customized pore structure and pore chemistry for benchmark one-step C2H4 recovery from C2H2 and CO2 with record C2H4 productivity.
- Yunjia Jiang,
- , Yongqi Hu,
- & Yuanbin Zhang
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Article
| Open AccessElectrochemical direct air capture of CO2 using neutral red as reversible redox-active material
Electrochemical direct air capture (DAC) of CO2 requires air-stable redox-active materials. Here, the authors present an electrochemical DAC using air-stable redox couple of neutral red with a minimum energy requirement of 65 kJe/molCO2.
- Hyowon Seo
- & T. Alan Hatton
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Article
| Open AccessToward economical application of carbon capture and utilization technology with near-zero carbon emission
Carbon capture, utilization and storage technology is limited by the need for a separate CO2 capture step. Here, the authors propose a strategy and economic analysis for simultaneous dilute CO2 capture from flue gas and direct electrochemical reduction to synthesis gas via reaction swing absorption.
- Kezia Megagita Gerby Langie
- , Kyungjae Tak
- & Ung Lee
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Article
| Open AccessFast light-switchable polymeric carbon nitride membranes for tunable gas separation
Simuli-responsive separation membranes often suffer from slow response times or require high energy input for switching to occur. Here authors demonstrate light-switchable gas separation membranes based on polymeric carbon nitride with fast switching times for the efficient separation of gases with higher polarizabilities.
- Timur Ashirov
- , Julya Stein Siena
- & Ali Coskun
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Article
| Open AccessEnergy comparison of sequential and integrated CO2 capture and electrochemical conversion
Coupling CO2 capture and electrolysis offers new opportunities to reduce energy cost. Here, the authors identify that the integrated electrolyser must show similar performance to the gas-fed electrolyser to ensure an energy benefit of up to 44% versus sequential capture and conversion processes.
- Mengran Li
- , Erdem Irtem
- & Thomas Burdyny
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Article
| 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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Article
| Open AccessBipolar membrane electrolyzers enable high single-pass CO2 electroreduction to multicarbon products
In the carbon dioxide (CO2) to multicarbon electrolysis, the crossover CO2 to the oxygen-rich anodic gas stream add a further energy-intensive chemical separation step. Here, the authors demonstrate a bipolar membrane-based electrolyzer design that eliminates the crossover CO2.
- Ke Xie
- , Rui Kai Miao
- & Edward H. Sargent
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Article
| Open AccessEliminating the need for anodic gas separation in CO2 electroreduction systems via liquid-to-liquid anodic upgrading
In the electrified conversion of CO2 to multicarbon products, CO2 crossover to the O2-rich anodic stream adds a further, energy-intensive, chemical separation step. Here, the authors demonstrate a strategy that eliminates the separation requirement.
- Ke Xie
- , Adnan Ozden
- & Edward H. Sargent
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Article
| Open AccessLow energy carbon capture via electrochemically induced pH swing with electrochemical rebalancing
This work demonstrates a safe and scalable electrochemical CO2 separation method that allows promisingly low (62 kJ/molCO2) energetic cost at a high current density, and it can be used for direct air capture when a suitable molecule is used.
- Shijian Jin
- , Min Wu
- & Michael J. Aziz
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Article
| Open AccessEngineered assembly of water-dispersible nanocatalysts enables low-cost and green CO2 capture
Catalytic solvent regeneration is of interest to reduce energy consumption in CO2 separation, however, the development of engineered nanocatalysts remains a challenge. Here, a new avenue is presented for the next generation of advanced metal-organic frameworks (MOFs) in energy-efficient CO2 capture.
- Masood S. Alivand
- , Omid Mazaheri
- & Kathryn A. Mumford
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Article
| Open AccessVacancy-defect modulated pathway of photoreduction of CO2 on single atomically thin AgInP2S6 sheets into olefiant gas
CO2 conversion driven by light is a promising strategy to synchronously overcome global warming and energy-supply issues. Here the authors show that the sulfur defect engineering on a quaternary AgInP2S6 atomic layer can excitingly change the CO2 photoreduction reaction pathway to the generation of ethene.
- Wa Gao
- , Shi Li
- & Zhigang Zou
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Article
| Open AccessLow coordination number copper catalysts for electrochemical CO2 methanation in a membrane electrode assembly
Electrochemical conversion of carbon dioxide to methane can store intermittent renewable electricity in a staple of global energy. Here, the authors develop a moderator strategy to maintain the catalyst in a low coordination state, thereby enabling stable and selective electrochemical methanation.
- Yi Xu
- , Fengwang Li
- & David Sinton
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Article
| Open AccessDirect electrosynthesis of 52% concentrated CO on silver’s twin boundary
Isolating purified electrosynthesis product is a major challenge in electrochemical carbon dioxide reduction. Here, the authors report a nanotwinned silver electrocatalyst and a pneumatic-trough cell system to produce a 52% concentrated CO, which is further utilized as a carbon feedstock for graphene production.
- Can Tang
- , Peng Gong
- & Zhengzong Sun
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Article
| Open AccessCarbon dioxide utilization in concrete curing or mixing might not produce a net climate benefit
Carbon curing or mixing in concrete is promising for carbon dioxide sequestration. Here, the authors show that the increased use of binder material to compensate the loss in compressive strength and electricity for carbon dioxide curing is more likely to increase carbon dioxide emissions on a life cycle basis for carbon cured or mixed concrete.
- Dwarakanath Ravikumar
- , Duo Zhang
- & Victor Li
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Article
| Open AccessMorphology and mechanism of highly selective Cu(II) oxide nanosheet catalysts for carbon dioxide electroreduction
Copper oxides (CuO) can selectively catalyze the electrochemical reduction of CO2 to hydrocarbons and oxygenates. Here, the authors study the activity and morphological evolution of 2D CuO nanosheets under applied electrode potentials to conclude the primacy of dendritic shapes and involvement of a new coupling pathway.
- Xingli Wang
- , Katharina Klingan
- & Peter Strasser
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Article
| Open AccessFast operando spectroscopy tracking in situ generation of rich defects in silver nanocrystals for highly selective electrochemical CO2 reduction
Efficient electrocatalysts are crucial to the electrochemical carbon dioxide reduction. Here, the authors use the fast operando technique to explore a silver-based catalyst with improved catalytic performance benefiting from the suitable defect structures.
- Xinhao Wu
- , Yanan Guo
- & Zongping Shao
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Article
| Open AccessPyroelectric nanoplates for reduction of CO2 to methanol driven by temperature-variation
CO2 is a problematic greenhouse gas, although its conversion to alternative fuels represents a promising approach to limit its long-term effects. Here, the authors demonstrate that CO2 can be reduced to methanol through pyroelectric catalysis under temperature variation near room temperature.
- Lingbo Xiao
- , Xiaoli Xu
- & Guifu Zou
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Article
| Open AccessCarbon hollow fiber membranes for a molecular sieve with precise-cutoff ultramicropores for superior hydrogen separation
Energy-efficient hydrogen purification technologies are needed for the hydrogen economy. Here the authors report facile and scalable fabrication of asymmetric carbon molecular sieve membranes for the separation of hydrogen and carbon dioxide.
- Linfeng Lei
- , Fengjiao Pan
- & Michael D. Guiver
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Article
| Open AccessA direct coupled electrochemical system for capture and conversion of CO2 from oceanwater
Isolating CO2 to use in electrochemical CO2 reduction systems is an ongoing issue. Here, the authors present a proof-of-concept integrated system combining a bipolar membrane electrodialysis cell with a vapor-fed CO2 reduction cell for capture and conversion of CO2 from oceanwater.
- Ibadillah A. Digdaya
- , Ian Sullivan
- & Chengxiang Xiang
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Article
| Open AccessAlkaline thermal treatment of seaweed for high-purity hydrogen production with carbon capture and storage potential
While biomass may serve as a renewable source of carbon-neutral hydrogen, it is challenging both to utilize as-found bio-resources and to suppress CO2 formation. Here, authors convert wet, salty seaweed using alkaline thermal treatment to produce high-purity hydrogen and suppress carbon emission.
- Kang Zhang
- , Woo-Jae Kim
- & Ah-Hyung Alissa Park
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Article
| Open AccessAmbient weathering of magnesium oxide for CO2 removal from air
To remove CO2 from the atmosphere every year by mid-century will need new technologies. Here the authors proposed the use of magnesia (MgO) in ambient looping processes to remove CO2 from the air and they found that the proposed approach will cost $46–195 tCO2−1 net removed from the atmosphere considering both grid and solar electricity resources without including post-processing costs.
- Noah McQueen
- , Peter Kelemen
- & Jennifer Wilcox
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Article
| Open AccessElectrochemically mediated carbon dioxide separation with quinone chemistry in salt-concentrated aqueous media
Redox-active organic compounds that reversibly bind and release CO2 are promising candidates for carbon capture but are limited by the use of flammable, toxic aprotic electrolytes. Here the authors use salt-concentrated aqueous electrolytes in continuous CO2 separation with good performance metrics.
- Yayuan Liu
- , Hong-Zhou Ye
- & T. Alan Hatton
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Article
| Open AccessTailoring the separation properties of flexible metal-organic frameworks using mechanical pressure
Separation of gasses with similar physical and chemical properties can be energy demanding, and adsorption-based technologies may provide alternatives with lower energy consumption. Here, the authors show mechanical control of pore size aperture in flexible metal-organic frameworks for separation of gasses.
- Nicolas Chanut
- , Aziz Ghoufi
- & Philip L. Llewellyn
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Article
| Open AccessSynergistic effect of quinary molten salts and ruthenium catalyst for high-power-density lithium-carbon dioxide cell
Lithium-carbon dioxide cells are challenging due to the sluggish electron transfer in the Lithium carbonate in aprotic electrolyte. Here, the authors report synergistic effect of molten salt electrolyte and Ruthenium catalyst to enhance the electrochemical performance of Lithium-carbon dioxide batteries
- Kyungeun Baek
- , Woo Cheol Jeon
- & Seok Ju Kang
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Article
| Open AccessDouble layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold
Electrochemical CO2 reduction is a potential route to the sustainable production of valuable fuels and chemicals. In this joint experimental-theoretical work, the authors address the issue of the rate-limiting step on Gold and present insights from multi-scale simulations into the importance of the electric double layer on reaction kinetics and mass transport.
- Stefan Ringe
- , Carlos G. Morales-Guio
- & Karen Chan
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Article
| Open AccessRETRACTED ARTICLE: Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas
Conversion of CO2 into value-added chemicals by use of renewable energy is promising to achieve a carbon-neutral energy cycle. Here, the authors show that AgP2 is a stable, selective and efficient syngas catalyst for solar-to-fuel conversion with a 3-fold lower overpotential compared to the benchmark Ag catalyst.
- Hui Li
- , Peng Wen
- & Scott M. Geyer
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Article
| Open AccessEfficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites
Catalysts for CO electroreduction have focused on Cu, and their main products have been C2 chemicals. Here authors use the concept of asymmetric active sites to develop a class of doped Cu catalysts for C-C coupling, delivering record selectivity to n-propanol.
- Xue Wang
- , Ziyun Wang
- & Edward H. Sargent
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Article
| Open AccessDopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products
The electro-oxidative synthesis of valued chemicals offers to enhance the overall efficiency and economic viability of renewable electrosynthesis systems. Here, the authors use dopant-tuned catalysts to promote the electrosynthesis of dimethyl carbonate from CO and methanol via oxidative carbonylation.
- Tao-Tao Zhuang
- , Dae-Hyun Nam
- & Edward H. Sargent
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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
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Article
| Open AccessMolecular cobalt corrole complex for the heterogeneous electrocatalytic reduction of carbon dioxide
Electrochemical conversion of carbon dioxide to ethanol is one of the most challenging energy conversion reactions. Here the authors show selective electroreduction of carbon dioxide to ethanol by using a functionalized cobalt A3-corrole catalyst immobilized on a carbon paper electrode.
- Sabrina Gonglach
- , Shounik Paul
- & Soumyajit Roy
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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
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Perspective
| Open AccessCrowd oil not crude oil
Climate change represents an existential, global threat to humanity, yet its delocalized nature complicates climate action. Here, the authors propose retrofitting air conditioning units as integrated, scalable, and renewable-powered devices capable of decentralized CO2 conversion and energy democratization.
- Roland Dittmeyer
- , Michael Klumpp
- & Geoffrey Ozin
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Article
| Open AccessLiquid marble-derived solid-liquid hybrid superparticles for CO2 capture
Carbon capture is increasingly important to address current environmental challenges but developing effective carbon capture materials is challenging. Here, the authors report liquid marble-derived superparticles which overcome current limitations associated with both liquid and solid carbon capture materials.
- Xia Rong
- , Rammile Ettelaie
- & Hengquan Yang
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Article
| Open AccessFluorinated MOF platform for selective removal and sensing of SO2 from flue gas and air
Removal of SO2 from flue gas is of prime importance to avoid its poisoning of CO2-seperating agents. Here, the authors demonstrate that two fluorinated metal–organic frameworks selectively remove SO2 from synthetic flue gas and can sense SO2 with p.p.m.-level detection using quartz crystal microbalance transducers.
- M. R. Tchalala
- , P. M. Bhatt
- & M. Eddaoudi