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At least 1,351 records · Page 75

Treasuring trash: Pt/SrTiO 3 catalysts process plastic waste into high-value materials

Single-use plastics are ubiquitous throughout modern society because they have properties that make them desirable in a wide variety of applications, including low cost of production, high thermal and chemical stability, and tunable mechanical properties. Several of the recycling methods currently used to process single-use plastic waste, such as mechanical recycling and pyrolysis, do not selectively process plastic materials into uniform products, as would be advantageous for repurposing these materials in pursuit of a circular economy. Catalytic hydrogenolysis, whereby C–C bonds in polymers are broken over a supported catalyst in the presence of H 2 , is a promising approach to converting plastics into value-added products that can be sold commercially without further purification. Here, in this account, we present some recent advances in polyolefin hydrogenolysis, with a focus on Pt nanoparticles on SrTiO 3 nanocuboid supports (Pt/STO). Current developments in this field, general challenges, and future directions are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Selectivity mechanisms of ion intercalation in Prussian blue analogs

Prussian blue analogs (PBAs) are a family of materials with facile, reversible, and selective ion transport capability for various ions via electrochemical intercalation, owing to their vacancy structure. The large tunable compositional space of PBAs allows for manipulation of intercalation behavior and selectivity by controlling structural vacancy level through choice of transition metal centers and modifications to the synthesis process. However, a lack of understanding of the mechanisms of ion selectivity hinders the material’s design process. Here, for this work, we investigated the origins of ion selectivity using a model PBA, copper hexacyanoferrate, and focused on eight technologically and biologically prominent ions, for which we determined a sequence of selectivity: Rb + > K + > Na + > Ba 2+ > Sr 2+ ≈ Ca 2+ > Mg 2+ > Li + . We provide electrochemical, structural, and redox evidence of strong correlation between the ion identity, the dominant charge-compensating redox, and preferred occupancy site. Specifically, using synchrotron anomalous X-ray diffraction (AXRD), we reveal that monovalent ions exhibit significant association with the corner sites of the unit cell and iron redox, whereas divalent ions display affinity toward the center site with higher ratios of copper redox. Informed by selectivity results, we applied CuHCFe to Li purification and achieved 99.9% purity. Our findings demonstrate an approach to elucidating ion intercalation behavior in order to distinguish and manipulate material properties to optimize separation performance.

Prussian blue analog↗

Zeolite-like MOF nanocrystals incorporated 6FDA-polyimide mixed-matrix membranes for CO 2 /CH 4 separation

MOF mixed-matrix membranes (MMMs) are regarded as potential candidates for energy-efficient natural gas purification. Our work reports the fabrication of high-performance 6FDA-polyimide MMMs, based on the incorporation of zeolite-like MOF (ZMOF) as fillers, and their associated permeation studies for CO 2 /CH 4 separation. To eliminate micron-sized crystals, a facile repeating sedimentation approach was used to harvest nanocrystals from the as-synthesized bulk ZMOF crystalline powder material. This enables the deployment of ZMOF nanocrystals with relatively uniform dimension and morphology in the polymer matrix. Typical 6FDA-polyimides encompassing distinct diamine moieties (6FDA-DAM, 6FDA-DETDA-DABA or PDMC) were explored as polymer matrices to disclose the transport property matching the hosted ZMOF filler. Mixed-gas permeation measurements revealed that the incorporation of the ZMOF filler affords a concurrent enhancement of the CO 2 permeability and the CO 2 /CH 4 selectivity for the three tested 6FDA-polyimides. Particularly, the highly permeable 6FDA-DAM showed a considerably enhanced performance for CO 2 /CH 4 that transcends the 2008 Robeson upper-bound. Detailed analysis of the sorption data and diffusion coefficients suggest that the enhanced transport property in the ZMOF-based MMM is plausibly attributed to the combination of the higher CO 2 sorption capacity and selectivity, and favorable gas diffusivity via the CO 2 -philic framework of ZMOF in moderately confined pores.

36 MATERIALS SCIENCE↗

2-Aminoimidazole reduces fouling and improves membrane performance

Biofouling is difficult to control and hinders the performance of membranes in all applications but is of particular concern when natural waters are purified. Fouling, via multiple mechanisms (organic-only, biofouling-only, cell-deposition-only, and organic + biofouling), of a commercially available membrane (control) and a corresponding membrane coated with an anti-biofouling 2-aminoimidazole (2-AI membrane) was monitored and characterized during the purification of a natural water. Results show that the amount of bacterial cell deposition and organic fouling was not significantly different between control and 2-AI membranes; however, biofilm formation, concurrent or not with other fouling mechanisms, was significantly inhibited (95–98%, p < 0.001) by the 2-AI membrane. The limited biofilm that formed on the 2-AI membrane was weaker (as indicated by the polysaccharide to protein ratio) and thus presumably easier to remove. The conductivity rejection by the 2-AI and control membranes was not significantly different throughout the 75-h experiments, but the rejection of dissolved organic carbon by biofouled (biofouling-only, cell-deposition-only, and organic + biofouling) 2-AI membranes was statistically higher (10–12%, p = 0.003–0.07). When biofouled, the water permeance of the 2-AI membranes decreased significantly less (p < 0.05) over 75 hours than that of the control membranes, whether or not other additional types of fouling occurred concurrently. Despite the initially lower water permeances of 2-AI membranes (11% lower on average than controls), the 2-AI membranes outperformed the controls (10–11% higher average water permeance) after biofilm formation occurred. Overall, 2-AI membranes fouled less than controls without detriment to water productivity and solute rejection.

59 BASIC BIOLOGICAL SCIENCES↗

Boric acid removal with polyol-functionalized polyether membranes

Poor selectivity of conventional desalination membranes for boron often necessitates multi-stage treatment trains to achieve desired boron removal for end uses such as irrigation. One approach to membrane design for improved single-pass boric acid removal is via incorporation of chelating ligands that selectively sorb boron. In this study, membranes based on epoxy-amine cross-linked poly(glycidyl glycidyl ether) (PGGE) were synthesized and functionalized with N-methyl-d-glucamine (NMDG), a polyol known to interact selectively with boron. PGGE and PGGE-NMDG membranes exhibited boron sorption isotherms that were well-described by dual mode isotherms. PGGE-NMDG sorbed 2.5 mmol B/g dry polymer from a neutral aqueous solution containing 100 mmol B/L, which was almost three times the adsorption density of a commercial boron selective resin, Amberlite IRA743. Further, the membranes were regenerated in acid without a significant loss of boron sorption capacity over four cycles. Interactions between boron and NMDG and PGGE sites (e.g., epoxides) impacted boron diffusion in both membranes. The use of ligand functionalized membranes to capture target solutes such as boron requires high loading of interacting sites to maximize uptake capacity. Establishing fundamental structure/property rules for boron selectivity could lead to new material designs with improved boron separation properties for water purification.

36 MATERIALS SCIENCE↗

Compact ammonia reforming at low temperature using catalytic membrane reactors

Ammonia is a leading carrier for the storage and transport of renewable hydrogen, but its deployment requires scalable technologies for efficient decomposition and purification. In this work, we report on the efficient delivery of high purity hydrogen from ammonia decomposition using a catalytic membrane reactor (CMR). Improvements to the electroless plating process reduced the Pd membrane thickness by >35%, resulting in commensurate increases in hydrogen permeance without sacrificing selectivity. To increase throughput a commercial Ru/Al 2 O 3 catalyst was added to the lumen, and the CMR could process ammonia flowrates 10–50 times higher than an equivalent packed bed reactor while maintaining the same level of conversion. It is shown that the earth-abundant zeolite clinoptilolite could reduce ammonia impurities in the permeated H 2 to the levels required by PEM fuel cells (<25 ppb). Performance increased significantly across a >500-h durability test due to improvements in membrane permeability. Finally, the results show that CMRs are a viable technology for distributed production of hydrogen from ammonia.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Salt and ion transport in a series of crosslinked AMPS/PEGDA hydrogel membranes

Salt permeability and ionic conductivity are critical properties for membranes in water purification and energy applications. Both properties depend on individual ion sorption and diffusion coefficients, which are significantly influenced by polymer chemical and physical parameters such as fixed charge concentration and membrane water content. However, systematic studies connecting polymer structure to ion transport properties are still lacking. In this study, a series of uncharged and charged membranes were synthesized using poly(ethylene glycol) diacrylate (PEGDA) as a cross-linker and 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPS) as a charged monomer. Membrane fixed charge concentration and water uptake were systematically varied by adjusting AMPS content in the pre-polymerization mixture. Salt sorption and permeability coefficients and ionic conductivity of these membranes were measured as a function of NaCl solution concentration (0.01–1 M). Combining the solution-diffusion model and Nernst-Planck equation, individual ion diffusion coefficients were calculated. Experimental Na + diffusion coefficients for all materials were well described by the Mackie and Meares tortuosity model, highlighting the strong influence of water content on ion diffusivity in both uncharged and charged polymers. Model predictions for Cl – diffusion coefficients agree reasonably well with experimental values, with some deviations occurring in more highly charged membranes. Finally, this discrepancy might result from interactions not captured by the Mackie and Meares model (e.g., fixed charge-ion interactions).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Oxidative coupling of methane (OCM) conversion into C 2 products through a CO 2 /O 2 co-transport membrane reactor

Oxidative coupling of methane (OCM), which transforms CH 4 into C 2 products (C 2 H 6 and C 2 H 4 ) with molecular O 2 as the oxidant, is one of the most studied direct methane conversions (DMCs). However, a major technical hurdle to the OCM process is to achieve high CH 4 conversion at high C 2 (C 2 H 6 and C 2 H 4 ) selectivity. One rudimentary cause for this “tradeoff” behavior is the high chemical reactivity of the products (C 2 H 6 or C 2 H 4 ), which can be re-oxidized by O 2 . To overcome this thermodynamic challenge, minimizing the oxidizing power of the oxidant and lowering the local oxygen partial pressure are keys. Here, In this work, we demonstrate a new membrane reactor that capture CO 2 /O 2 from a flue gas and uses it for OCM conversion. The results show that the co-captured CO 2 /O 2 mixture converts CH 4 into C 2 H 6 in the presence of a 2%Mn–5%Na 2 WO 4 /SiO 2 catalyst, followed by thermal cracking of C 2 H 6 into C 2 H 4 and H 2 . The presence of CO 2 decreases the local partial pressure of O 2 , thus reducing the propensity of C 2 -products re-oxidation and leading to a higher C 2 selectivity. We show that a small button-type membrane reactor can achieve 12% C 2 yield with ~57% C 2 -selectivity using a diluted CH 4 -Ar mixture as the feedstock. We expect higher C 2 yield with tubular plug-flow membrane reactors in the future. We also highlight the unique advantage of the membrane reactor in intensifying CO 2 capture from both flue gas and OCM purification process into one single step.

42 ENGINEERING↗

Finely tuning the microporosity in phosphoric acid doped triptycene-containing polybenzimidazole membranes for highly permselective helium and hydrogen recovery

High-performance polymer membranes with well-defined microporosity and size-sieving ability are especially attractive for helium and hydrogen recovery. Here, in this study, we report novel macromolecular engineering of polybenzimidazole (PBI) membranes that integrate hierarchical triptycene units for high permeability and polyprotic acid doping for size sieving via controllable manipulation of microporous architecture. The triptycene moieties disrupt chain packing and introduce additional configurational free volume, leading to significantly boosted He and H 2 permeabilities compared to previously reported PBI membranes. The acid doping resulted in crosslinked PBI membranes via hydrogen bonding and proton transfer with dramatically enhanced gas selectivities. Via adjusting the H 3 PO 4 -doping level, triptycene-based polybenzimidazole (TPBI) composite membranes (TPBI-(H 3 PO 4 ) x ) exhibit the highest gas selectivities for He enrichment (i.e., α(He/CH 4 ) = 7052 ± 156) and H 2 purification (i.e., α(H 2 /CH 4 ) = 5128 ± 110) among existing polymeric gas separation membranes. Additionally, under mixed-gas conditions at 150 °C, the TPBI-(H 3 PO 4 ) 0.98 membrane displays a H 2 permeability of 46.7 Barrer and a H 2 /CO 2 selectivity of 16, far beyond the Robeson's 2008 upper bound for H 2 /CO 2 separation. The facile and diverse tunability and excellent gas separation performance make TPBI-(H 3 PO 4 ) x membranes highly attractive for helium and hydrogen separation.

42 ENGINEERING↗

The need for ion-exchange membranes with high charge densities

Ion-exchange membranes (IEMs) are essential for controlling ion transport in electrochemical membrane-based technologies for water purification, energy generation, and energy storage. In general, IEMs must exhibit high ionic conductivity and selectivity, both of which are significantly influenced by the charge and water content of the hydrated membrane. In this perspective, we compiled the charge and water contents of approximately 1,000 IEMs reported over the past several decades to assess their range and variability, as well as to reveal gaps and set clear targets for future membrane design. We compared the charge and water content of negatively and positively charged membranes, as well as membranes developed for desalination and energy applications. The majority of IEMs, regardless of structure or intended application, have volumetric charge densities below 3 mol/L[membrane]. This narrow range of charge densities limits the performance of IEMs and contributes to the observed tradeoff between ion throughput and selectivity. It is critical to develop IEMs with higher charge densities to overcome this performance limitation. Further, we highlighted several design strategies that yielded IEMs with fixed charge densities higher than 3 mol/L[membrane]. These strategies provide valuable insights and can guide the design of next-generation IEMs with high charge densities.

36 MATERIALS SCIENCE↗

Surface engineering of polymeric membranes with metal oxides for improved fouling resistance and superior oil-water separation

Rapid industrial growth has increased the need for efficient membranes to separate oil-water emulsions. Polyvinylidene fluoride (PVDF) membranes, although widely used due to their chemical inertness and favorable mechanical properties, suffer from fouling due to their intrinsic hydrophobicity. Modifying these membranes after fabrication offers a practical solution as it easily fits into existing large-scale manufacturing processes. Atomic layer deposition (ALD), an atomically-precise vapor phase surface modification technique, can create ultrathin metal oxide layers that greatly improve membrane hydrophilicity without significantly affecting the original pore size. However, PVDF's lack of reactive chemical moieties makes ALD challenging. Here, in this study, we present a simple alkali treatment that greatly enhances ALD nucleation and growth on PVDF membranes. This treatment imparts exceptional oil-water emulsion separation capabilities and antifouling behavior in PVDF membranes after just a few ALD cycles, surpassing the performance of PVDF membranes coated with hundreds of ALD cycles. This dramatic reduction in the number of ALD cycles required could enable cost-effective modification of commercial PVDF membranes at scale using spatial, roll-to-roll ALD. These modified membranes outperform reported modified PVDF membranes, with >99 % permeance recovery and <1 % irreversible loss of permeance and >98 % oil rejection from oil-water emulsions over 100 h continuous operation, making them promising for advanced water purification technologies.

Atomic layer deposition↗

Exfoliation of surfactant swollen layered MWW zeolites into two-dimensional zeolite nanosheets using telechelic liquid polybutadiene

We report two-dimensional (2D) zeolites have the potential to enhance mass transport by reducing diffusion lengths and thus find applications in catalysis and separation. High aspect ratio 2D zeolite nanosheets are required for fabrication of thin, high-flux zeolite membranes. Preparation of 2D zeolite nanosheets can be achieved by exfoliation of layered zeolite precursors, which usually requires multiple steps including swelling with cationic surfactants, exfoliation by applying a mechanical force such as shearing or sonication, purification and removal of the surfactants. The exfoliation of surfactant swollen layered zeolite precursors has been studied using molten polystyrene and telechelic liquid polybutadiene, but still requires extensive shearing force. Recently, a novel one-step exfoliation method has been developed for nonswollen MWW zeolite precursors using tetrabutylammonium hydroxide (TBAOH) solution. In this work, we study the exfoliation of surfactant swollen MWW layered precursors (with and without aluminum) in commercially available liquid hydroxyl-terminated polybutadiene (HTPB) with the aim to provide fundamental understanding of the interaction between the liquid polybutadiene and the surfactant swollen layered zeolite precursors. It was found that surfactant swollen ITQ-1, (ITQ-1(S)), a pure silica layered precursor with MWW framework after being swollen with a cationic surfactant, can be exfoliated in liquid HTPB at room temperature without applying any additional shearing force. The aluminum containing surfactant swollen MWW precursors can be also exfoliated in HTPB at room temperature, but require additional shearing forces. The exfoliation process was monitored using rheology experiments and studied by tuning the composition of the zeolite precursors. The interaction between the layered zeolite precursor and the hydroxyl group of the liquid polybutadiene allows the polymer to intercalate the precursor and exfoliate it into nanosheets. The presence of framework aluminum and the nature of the organic structure directing agents (OSDAs) are key parameters affecting the exfoliation process. Framework Al is unfavorable for the exfoliation possibly due to the surface charges introduced by the aluminum. Bulky OSDA, trimethyladamantammonium (TMAda + ), in the interlayer spacing may facilitate the exfoliation.

2D nanosheets↗

The Plasmodium falciparum MESA erythrocyte cytoskeleton-binding (MEC) motif binds to erythrocyte ankyrin

The MESA erythrocyte cytoskeleton binding (MEC) motif is a 13-amino acid sequence found in 14 exported Plasmodium falciparum proteins. First identified in the P. falciparum Mature-parasite-infected Erythrocyte Surface Antigen (MESA), the MEC motif is sufficient to target proteins to the infected red blood cell cytoskeleton. To identify host cell targets, purified MESA MEC motif was incubated with a soluble extract from uninfected erythrocytes, precipitated and subjected to mass spectrometry. The most abundant co-purifying protein was erythrocyte ankyrin (ANK1). A direct interaction between the MEC motif and ANK1 was independently verified using co-purification experiments, the split-luciferase assay, and the yeast two-hybrid assay. A systematic mutational analysis of the MEC motif demonstrated the critical role of the conserved aspartic acid residue at the C-terminus of the MEC motif for binding to both erythrocyte inside-out vesicles and to ANK1. Using a panel of ANK1 constructs, the MEC motif binding site was localized to the ZU5C domain, which has no known function. The MEC motif had no impact on erythrocyte deformability when introduced into uninfected erythrocyte ghosts, suggesting the MEC motif’s primary function is to target exported proteins to the cytoskeleton. Finally, we show that PF3D7_0402100 (PFD0095c) binds to ANK1 and band 4.1, likely through its MEC and PHIST motifs, respectively. In conclusion, we have provided multiple lines of evidence that the MEC motif binds to erythrocyte ANK1.

Kilili, Geoffrey K.↗

Comparative structural and thermal stability studies of Cuc m 2.0101, Art v 4.0101 and other allergenic profilins

Worldwide, more than one-third of the population suffers from allergies. A significant fraction of officially registered allergens originate from the profilin family of proteins. Profilins are small ubiquitous proteins which are found in plants, viruses and various eukaryotes including mammals. Additionally, although they are primarily regarded as minor allergens, profilins are important players in immunoglobulin E (IgE) cross-reactivity. However, in some populations profilins are recognized by IgE from at least 50% of patients allergic to a given allergen source. Cuc m 2.0101 is recognized by IgE in more than 80% of muskmelon-allergic patients. The recombinant isoallergen Cuc m 2.0101 was produced in significant quantities and its X-ray crystal structure was determined. In addition, a new Art v 4.0101 (mugwort profilin) structure was determined. The profilins Cuc m 2.0101 and Art v 4.0101 were compared in terms of their structure and thermal stability. Furthermore, structural similarities and IgE cross-reactivity between profilins from different sources are discussed to explain the molecular basis of various clinical syndromes involving this group of allergens. Special emphasis is placed on discussion of profilins’ quaternary structures and their relation to biological function, as well as to protein allergenicity. Moreover, a potential impact of protein purification protocols on the structure of profilins is highlighted.

60 APPLIED LIFE SCIENCES↗

Probing lead acetate in solution using X-ray diffraction

Here, for the purpose of water purification involving toxic metal sensing and removal, high energy X-ray diffraction experiments have been performed on lead acetate Pb(Ac) 2 solutions, liquid and amorphous glutathione disulfide (GSSG), and their mixtures. The data have been interpreted using Empirical Potential Structure Refinement and pair distribution function analysis. At the highest concentration of 1 M Pb(Ac) 2 in water, the lead molecules are found to cluster and the second shell in the water structure becomes slightly more ordered as the water molecules become compressed. Liquid and amorphous GSSG are found to hydrogen bond primarily via OH-O interactions, while NH-O bonds are much more distorted. Aqueous solutions of Pb(Ac) 2 + GSSG show the closest Pb-O (carboxyl) and Pb-N (amine) bonds both at a distance of 2.5 ± 0.1 Å at a concentration of 1 M Pb(Ac) 2 in water. At 0.75 M Pb(Ac) 2 in water, strong Pb-S bonds are found at a distance of 2.8 ± 0.1 Å. The implications for lead removal using capacitive deionization are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unlocking the magic in mycelium: Using synthetic biology to optimize filamentous fungi for biomanufacturing and sustainability

Filamentous fungi drive carbon and nutrient cycling across our global ecosystems, through its interactions with growing and decaying flora and their constituent microbiomes. The remarkable metabolic diversity, secretion ability, and fiber-like mycelial structure that have evolved in filamentous fungi have been increasingly exploited in commercial operations. The industrial potential of mycelial fermentation ranges from the discovery and bioproduction of enzymes and bioactive compounds, the decarbonization of food and material production, to environmental remediation and enhanced agricultural production. Despite its fundamental impact in ecology and biotechnology, molds and mushrooms have not, to-date, significantly intersected with synthetic biology in ways comparable to other industrial cell factories (e.g. Escherichia coli,Saccharomyces cerevisiae, and Komagataella phaffii). In this review, we summarize a suite of synthetic biology and computational tools for the mining, engineering and optimization of filamentous fungi as a bioproduction chassis. A combination of methods across genetic engineering, mutagenesis, experimental evolution, and computational modeling can be used to address strain development bottlenecks in established and emerging industries. These include slow mycelium growth rate, low production yields, non-optimal growth in alternative feedstocks, and difficulties in downstream purification. In the scope of biomanufacturing, we then detail previous efforts in improving key bottlenecks by targeting protein processing and secretion pathways, hyphae morphogenesis, and transcriptional control. Bringing synthetic biology practices into the hidden world of molds and mushrooms will serve to expand the limited panel of host organisms that allow for commercially-feasible and environmentally-sustainable bioproduction of enzymes, chemicals, therapeutics, foods, and materials of the future.

59 BASIC BIOLOGICAL SCIENCES↗

Theory of the photomolecular effect

It is well-known that water in liquid and vapor phases exhibits weak visible-light absorption. Recent experiments, however, show that at the liquid-air interface, absorption drastically increases, accelerating evaporation beyond thermal limits by 2–5 times. Strikingly, evaporation peaks at green wavelengths, despite no corresponding absorptance peak. The underlying mechanism of this observation, termed the photomolecular effect, remains puzzling, particularly as water molecules do not exhibit resonance peaks in the visible spectrum. Here, we present a theoretical model explaining the effect. We show that surface-bound water clusters undergo non-resonant photon-driven evaporation, with green light being particularly effective. Crucially, we do not expect green light to couple more strongly than other wavelengths to the molecules at the surface, rather the energy of green light is more effectively used to vaporize water. Our model accounts for why the evaporation peak does not align with absorptance and provides a quantum mechanical explanation of how a single photon can vaporize an entire molecular cluster. This model challenges conventional views on water-light interactions, revealing a fundamentally non-thermal evaporation mechanism. Furthermore, our findings have implications for water purification, energy-efficient drying, and climate modeling, opening new pathways for optimizing evaporation-based technologies.

Interfacial evaporation↗

Probing local electrochemistry via mechanical cyclic voltammetry curves

Understanding the mechanical response of an electrode during electrochemical cycling and its correlation to the device electrochemical performance is crucial to improving the performance of insertion-type energy storage devices, electrochemical actuators, water purification, ion separation and neuromorphic computing applications. Here, we visualized the electro-chemo-mechanical coupling behaviors during charge storage of anhydrous and hydrated WO 3 electrodes via in situ atomic force microscopy (AFM) and developed the concept of mechanical cyclic voltammetry (mCV) curves. The relationship between electrochemical current and strain was investigated with simplified models and the results revealed that the proton insertion/deinsertion process could be described through potential-dependent electro-chemo-mechanical coupling coefficients which might indicate changes in insertion processes during electrode cycling. The mCV mapping results highlight the local heterogeneity and show that the charging processes varied across the electrode. These local variations could be further correlated to local morphology, crystal orientations or chemical compositions with proper electrode designs.

36 MATERIALS SCIENCE↗