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At least 379 records · Page 21

Separation characteristics of cations and natural organic matter in electrodialysis

Natural organic matter (NOM) in water can cause the formation of disinfection byproducts (DBPs) when NOM reacts with a disinfectant such as chlorine. Nanofiltration (NF) and reverse osmosis (RO) are effective treatment methods to remove NOM. However, the simultaneous presence of both NOM and divalent cations such as Ca 2+ can enhance fouling in NF and RO. Therefore, an appropriate pretreatment to remove such cations before NF or RO would delay fouling and perhaps improve water recovery and NOM removal efficiency. Electrodialysis (ED) is potentially an excellent pretreatment method because it separates inorganic ions well using ion exchange membranes (IEMs) but does not separate NOM well because of its size and consequent low diffusivity. This research focused on ion and NOM separation with ED using three different types of commercially available IEM pairs, two different commercially available NOM sources, and six different influents at 500 mg/L total dissolved solids in the presence or absence of both hardness (Ca 2+ and Mg 2+ ) and NOM. The target waters of interest in this research were drinking water supplies that require little or no desalination but substantial removal of NOM; after NOM separation in NF or RO, some or all of the ED concentrate can be added to the NF/RO permeate to create the finished water prior to disinfection. The results indicate that ED can effectively separate alkaline earth metal ions without separation of NOM. Cation exchange membranes with high exchange capacity, high selectivity for divalent cations are desirable, and both anion and cation exchange membranes should have low affinity for organic adsorption. As a result, the process would work particularly well for NOM with relatively low hydrophobicity, since NOM adsorption to most surfaces increases with hydrophobicity.

36 MATERIALS SCIENCE↗

Flow-Assisted Selective Mineral Extraction from Seawater

The sustainable production of critical materials from natural sources requires a paradigm shift away from currently used resource-intensive processes. In this paper, we report a single-step, laminar co-flow method (LCM) that leverages non-equilibrium conditions to selectively extract pure Mg(OH) 2 from natural seawater. Conventional seawater-based Mg extraction involves adding individual or a combination of precipitants to obtain Mg(OH) 2 , but the co-existence of Ca 2+ unavoidably results in CaCO 3 impurities requiring additional purification steps. Here we show that the non-equilibrium conditions in LCM achieved using a microfluidics device and by simply co-injecting a NaOH solution with seawater can result in improved selectivity for Mg(OH) 2 unlike in conventional bulk mixing method. The resulting precipitates are characterized for composition and the process yield and purity are optimized through systematic variations of the reaction time and the concentration of NaOH. This is the first demonstration of LCM for selective separation, and as a one-step process that does not rely on novel sorbents, membranes, or external stimuli, it is easy to scale-up. LCM has the potential to be broadly relevant to selective separations from complex feed streams and diverse chemistries—enabling more sustainable materials extraction and processing.

54 ENVIRONMENTAL SCIENCES↗

Effect of Viscosity of a Deep Eutectic Solvent on CO 2 Capture Performance in an Energy-Efficient Membrane Contactor-Based Process

Greenhouse gas contributions to climate change have driven intense interest in the separation of CO 2 from wet flue gas streams. Deep eutectic solvents (DESs) are an emerging class of highly selective CO 2 absorbents. A prototypical DES, reline, is a mixture of choline chloride and urea. Reline is a thermally stable, nontoxic, and biodegradable solvent with negligible volatility and is inexpensive. We demonstrate a scalable and energy-efficient hollow fiber membrane contactor (HFMC)-based process using a green solvent for CO 2 capture. This process uses reline in HFMC to provide close interfacial interactions and contact between DES and CO 2 . This approach overcomes the disadvantages associated with direct absorption in DES and could potentially be applied to a variety of solvent-based CO 2 capture methods. Commercial, low-cost polymer hollow fiber membranes were evaluated for the capture of CO 2 with reline. From a mixed gas containing N 2 and CO 2 , the DES-based HFMC separated CO 2 with a purity of 97 mol %. The effect of the viscosity of reline on the CO 2 capture performance was investigated by adding water to the reline. The addition of water to reline significantly reduced its viscosity, which led to a permeate flux of 170 mmol/(m 2 ·h) at 35 °C, 4 bar, and 60 wt % water in solvent, which was approximately 8 times higher than that of the pure reline in the membrane contactor system. In situ Fourier transform infrared spectroscopy and nuclear magnetic resonance (NMR) revealed that reline absorbs CO 2 by physical absorption without forming new chemical compounds and that CO 2 separation by reline occurs via the pressure swing mechanism. This research provides fundamental insights about green physical solvent-based separation processes and a pathway toward industrial deployment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hydrocarbon-based membranes cost-effectively manage species transport and increase performance in thermally regenerative batteries

Low-temperature heat (T<130°C) can be utilized by thermally regenerative batteries (TRBs) for power production, allowing the thermal energy to be converted to storable chemical potential energy. However, TRBs suffer from high ohmic losses and ammonia crossover, which has slowed their development. In this study, we examined how the use of six different membranes influenced TRB performance, determined the most influential membrane parameters, and identified promising membrane candidates that cost-effectively increase TRB performance. Of the six membranes examined, an inexpensive, hydrocarbon CEM (Selemion CMVN) had low ammonia crossover without compromising resistance, resulting in good performance across all metrics studied. A thin anion exchange membrane (Sustainion, 50 microns) showed a high peak power density of 82 mW cm –2 due to low resistance, but the average power density and energy density were low due to high ammonia flux. Full discharge curves using Selemion CMVN provided an average power density of 26 ± 7 mW cm –2 with an energy density of 2.9 Wh L –1 , which were large improvements on previous TRBs. A techno-economic analysis showed that Selemion CMVN had the lowest levelized cost of storage ($410 per MWh) at an applied current density of 50 mA cm –2 .

25 ENERGY STORAGE↗

Mixed matrix membranes for post-combustion carbon capture: From materials design to membrane engineering

Mixed matrix materials (MMMs) containing nanofillers dispersed in continuous polymer matrices have emerged as an exciting and versatile platform to develop membranes with superior CO 2 /N 2 separation performance for post-combustion carbon capture. Both polymers and nanofillers can be vertically designed and engineered to combine the advantages of excellent processability (derived from polymers) and strong size-sieving ability or/and significant permanent porosity (originated from nanofillers). However, the MMMs face major challenges, such as interfacial incompatibility, particle agglomeration, and poor thin-film formability. This report provides a comprehensive yet critical review of various polymers and nanofillers (such as metal-organic frameworks, covalent organic frameworks, and two-dimensional materials) with promising CO 2 /N 2 separation properties. We exhaustively describe strategies to improve interfacial compatibility, such as in situ syntheses of polymers and nanofillers and functionalization of both components to improve adhesion. Moreover, we highlight various approaches to engineer the MMMs into thin-film composite (TFC) membranes. The review reveals the structure/property relationship in these MMMs and outlines the challenges and opportunities to realize their potential for practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hierarchically Porous Carbons with Highly Curved Surfaces for Hosting Single Metal FeN 4 Sites as Outstanding Oxygen Reduction Catalysts

Iron–nitrogen–carbon (Fe₋N₋C) materials have emerged as a promising alternative to platinum-group metals for catalyzing the oxygen reduction reaction (ORR) in proton-exchange-membrane fuel cells. However, their low intrinsic activity and stability are major impediments. Herein, an Fe₋N–C electrocatalyst with dense FeN 4 sites on hierarchically porous carbons with highly curved surfaces (denoted as FeN 4 - hc C) is reported. The FeN 4 - hc C catalyst displays exceptional ORR activity in acidic media, with a high half-wave potential of 0.85 V (versus reversible hydrogen electrode) in 0.5 m H 2 SO 4 . When integrated into a membrane electrode assembly, the corresponding cathode displays a high maximum peak power density of 0.592 W cm -2 and demonstrates operating durability over 30 000 cycles under harsh H 2 /air conditions, outperforming previously reported Fe–N₋C electrocatalysts. These experimental and theoretical studies suggest that the curved carbon support fine-tunes the local coordination environment, lowers the energies of the Fe d-band centers, and inhibits the adsorption of oxygenated species, which can enhance the ORR activity and stability. This work provides new insight into the carbon nanostructure–activity correlation for ORR catalysis. It also offers a new approach to designing advanced single-metal-site catalysts for energy-conversion applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Innovations in Sustainable Passive Wastewater Treatment - 20236

Sustainable water treatment systems, engineered to mimic natural processes and utilize natural materials, yield economic and environmental benefits through reductions in long term operational inputs, including: power, chemicals, and labor. Golder is an industry leader in the development and implementation of sustainable technologies at operating and closed mines. We continue to innovate these technologies and customize solutions to meet client needs by applying past experience and focused research. Sustainable (or passive) water treatment systems include ponds, wetlands, flow-through natural media beds, and limestone drains. These systems can blend in with a natural environment, are highly cost-effective for long-term water treatment, and can outcompete traditional active treatment technologies. Application of sustainable technologies relative to active technologies can be influenced by the influent water matrix, effluent limitations, flow rate of water requiring treatment, and available land area. In this presentation, four Golder-developed systems are reviewed as case studies, demonstrating our continued progressive approach to advancing sustainable water treatment technologies to meet industry needs. These case studies focus on design innovations and operational performance from data collected from the operational systems. Resources (power, chemicals, labor) required for the operation of each case study are compared with those that would be required for operation of their active treatment technology alternatives. - Case Study 1 presents an anaerobic biochemical reactor (BCR), a technology typically implemented for metals treatment and acid neutralization, for the treatment of sulfate to low concentrations (<250 mg/L). Active treatment via reverse osmosis (RO) membrane filtration is typically required for treatment of sulfate to similar concentrations, this innovation provides potential for sustainable treatment to replace the need for energy, chemical, labor, and waste (brine) intensive RO treatment for specific applications. Magnetite waste rock materials from the site were upcycled for use in this system to provide sequestration of the sulfide generated in the BCR. - Case Study 2 examines another novel application of the conventional BCR, modified for the removal of radionuclides and metals (uranium, radium, and selenium) at a closed uranium mine. - Case Study 3 presents implementation of sustainable treatment for mine drain water from a historic mine site, now a state park with around 100,000 visitors per year. The system includes a pond, wetland, and manganese removal bed surrounded by public trails designed to maintain the character of the park. The system treats for arsenic, iron, and manganese at relatively high flows (up to 1,200 gpm), with large seasonal fluctuations in flow and quality. - Case Study 4 is a unique project for which Golder is currently designing a sustainable treatment system, with no energy input, to treat nitrate in mine water post-closure at a site near the arctic circle. In this unprecedented application, climate, management of freshet, and space availability presented substantial technical challenges. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Tuning gas separation performance of polyimide membranes with macrocyclic crown ether units

Membrane-based gas separation is an energy-efficient alternative to conventional thermally-driven separation processes. However, polymer membranes face the permeability-selectivity trade-off challenge, which stems from the broad size distribution of free volume voids. Here, this study reports a molecular design strategy to address this challenge through incorporating macrocyclic crown ether (CE) moieties into the backbone of Matrimid® polyimide, a commercial gas separation membrane. A series of CE-containing Matrimid®-like copolyimides were synthesized with systematically varied CE molar contents ranging from 3 to 20%. These copolyimides formed ductile, defect-free thin films suitable for membrane fabrication. Gas permeation tests revealed a non-monotonic relationship between permeability/selectivity and CE content. Notably, the copolyimide with only 5% CE demonstrated a 61% increase in CO 2 /CH 4 selectivity and a 13% increase in CO 2 permeability relative to pristine Matrimid®. Higher CE contents did not yield further performance improvements, which is likely due to the competing effects of chain packing disruption and π–π interactions among CE moieties at high content. This hypothesis was supported by wide-angle X-ray scattering (WAXS) analysis, density measurements, and fractional free volume calculations. These findings highlight the potential of macrocyclic crown ether incorporation strategies in fine tuning the microstructure of commercial polyimide gas separation membranes to surpass the traditional permeability-selectivity trade-off.

CO2 separation↗

(Invited) Understanding Multi-Component Transport and Reaction Phenomena in Bipolar Membranes Used for Electrosynthesis

Bipolar membranes (BPMs), which have long seen usage in electrodialysis reactors for the generation of acid and base, have recently demonstrated potential to become critical components in electrochemical synthesis devices. Because they can operate under large pH gradients, BPMs enable favorable environments for electrocatalysis at the individual electrodes. Critical to the implementation of BPMs in these devices is understanding the kinetics of water dissociation that occurs within the BPM junction as well as the co- and counter-ion crossover through the BPM, which both present significant obstacles to developing efficient and stable BPM-devices for electrosynthesis applications. Prior work has modeled ion transport in bipolar membranes in neutral salt solutions for electrodialysis. However, no model exists for the BPM under the harsh applied pH gradients that would be present in electrosynthesis, and there is significant need to explore the effects of the internal hydration on the lifetime and performance of BPMs in such environments. Additionally, a mechanistic understanding of water dissociation catalysis will be required to develop interfacial catalysts that enable the high current density operation required for scalable electrosynthesis of fuels. In this talk, we discuss modeling methodologies and physics inherent in BPMs and present our recent model of ion transport and water dissociation catalysis in BPMs across the pH scale. Specifically, we simulate multi-ion transport for a BPM with various electrolyte combinations on each side of the membrane, demonstrating the significance of co- and counter-ion crossover in BPMs operating under harsh pH gradients. We then investigate effects caused by hydration gradients that occur due to internal ion-exchange and examine potential methods for improving performance and mitigating crossover. Finally, we examine the impact of the interfacial water dissociation catalyst and perform sensitivity analysis on the key properties (catalyst point of zero charge and pKa) that dictate catalyst performance. These results provide information that is critical to developing a comprehensive understanding of multi-component phenomena in BPMs and to informing the design and implementation of BPMs in next-generation devices for the numerous electrosynthesis chemistries that benefit from operation under an applied pH gradient.

Bui, Justin C↗

Dissolved gas recovery from water using a sidestream hollow-fiber membrane module: First principles model synthesis and steady-state validation

This paper presents a first-principles model for the recovery of dissolved gases from liquids using a sidestream hollow-fiber membrane module. The model avoids the use of new empirical coefficients, thus providing a parametric understanding of the process behavior for future design and optimization of membrane modules. This type of first-principles model could be particularly useful when gas recovery is beneficial to biological or chemical reactions of interest, such as the acetogenesis reactions in two-stage anaerobic digesters. The steady-state behavior of the model was validated against both new experimental data for the recovery of H 2 , CH 4 and H 2 –CH 4 mixtures from pure water, as well as existing published data. The modeled gas recovery predictions agreed with experimental data to an absolute average error of 13%, and an average R value of 0.98. Parametric analysis of mixed-gas recovery suggests possible key transition points in the composition of the recovered gases. For example, at 40 °C, increasing trans-membrane pressure while keeping hydraulic residence time (HRT) under 0.5 s will result in an increase in the ratio of H 2 to CH 4 recovered. Otherwise, increasing trans-membrane pressure will instead decrease the ratio of H 2 to CH 4 recovered. The model has potential to be extended to transient analysis, but has yet to be validated with transient experimental data. Furthermore, this model was successfully implemented in both Python and MATLAB, and provides valuable insights for future net-energy optimization for anaerobic digestion systems with in-situ gas recovery.

Anaerobic Digestion↗

A Membrane Contactor Enabling Energy-Efficient CO 2 Capture from Point Sources with Deep Eutectic Solvents

We demonstrate a scalable and energy-efficient hollow fiber membrane contactor (HFMC)-based process using a green solvent for CO 2 capture. This process uses a deep eutectic solvent (DES) in an HFMC to provide close interfacial interactions and contact between the DES and CO 2 . This approach overcomes disadvantages associated with direct absorption in DES and could potentially be applied to a variety of solvent-based CO 2 capture methods. Commercial low-cost polymer hollow fiber membranes (e.g., microporous polypropylene) were evaluated for CO 2 capture with reline, a prototypical DES. Single-gas measurements showed that the DES-based polypropylene HFMC can capture and separate CO 2 while rejecting N2. From a mixed gas containing 50 mol % N 2 and 50 mol % CO ν , the DES-based HFMC separated CO 2 with a purity of 96.9 mol %. The effect of several process parameters including solvent flow rate, pressure, and temperature on the CO 2 separation performance was studied. The flux of the recovered CO 2 was 67.43 mmole/m 2 /h at a feed pressure of 4 bar. In situ Fourier transform infrared (FTIR) measurements combined with density functional theory (DFT)-based molecular dynamics simulations revealed that reline absorbs CO 2 by physical absorption without forming a new chemical compound, and CO 2 separation by reline occurs via the pressure swing mechanism. This research provides fundamental insights about physical solvent-based separation processes and a pathway toward practical deployment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Removal of As(III) by Electrically Conducting Ultrafiltration Membranes

As(III) species are the predominant form of arsenic found in groundwater. However, nanofiltration (NF) and reverse osmosis (RO) membranes are often unable to effectively reject As(III). In this study, we fabricate highly conducting ultrafiltration (UF) membranes for effective As(III) rejection. Here, these membranes consist of a hydrophilic nickel-carbon nanotubes layer deposited on a UF support, and used as cathodes. Applying cathodic potentials significantly increased As(III) rejection in synthetic/real tap water, a result of locally elevated pH that is brought upon through water electrolysis at the membrane/water interface. The elevated pH conditions convert H 3 ASO 3 to H 2 AsO 3 – /HAsO 3 2– that are rejected by the negatively charged membranes. In addition, it was found that Mg(OH) 2 that precipitates on the membrane can further trap arsenic. Importantly, almost all As(III) passing through the membranes is oxidized to As(V) by hydrogen peroxide produced on the cathode, which significantly decreased its overall toxicity and mobility. Although the high pH along the membrane surface led to mineral scaling, this scale could be partially removed by backwashing the membrane. To the best of our knowledge, this is the first report of effective As(III) removal using low-pressure membranes, with As(III) rejection higher than that achieved by NF and RO, and high water permeance.

42 ENGINEERING↗

Selective Electrocatalysis Imparted by Metal-Insulator Transition for Durability Enhancement of Automotive Fuel Cells.

Repetitive start-up and shut-down events in polymer electrolyte membrane fuel cells for automotive applications lead to serious corrosion of the cathode due to an instantaneous potential jump that results from unintended air leakage into the anodic flow field followed by a parasitic oxygen reduction reaction (ORR) on the anode. Here we report a solution to the cathode corrosion issue during the start-up/shut-down events whereby intelligent catalyst design is used to selectively promote the hydrogen oxidation reaction (HOR) while concomitantly suppressing the ORR on the anode. Platinum thin layers supported on hydrogen tungsten bronze (Pt/HxWO3) suppressed the ORR by converting themselves into an insulator following exposure to oxygen, while selectively promoting the HOR by regaining metallic conductivity following subsequent exposure to hydrogen. The HOR-selective electrocatalysis imparted by a metal-insulator transition in Pt/HxWO3 demonstrated a remarkably enhanced durability of membrane electrode assemblies compared to those with commercial Pt/C catalysts.

Jung, Sang-Mun↗

Performance of Polymer Electrolyte Membrane Water Electrolysis Systems: Configuration, Stack Materials, Turndown and Efficiency

A cell model is developed and validated to analyze the performance of polymer electrolyte membrane water electrolysis (PEMWE) stacks and systems. It is used to characterize the oxygen evolution reaction (OER) activity on a TiO2-supported IrO2 catalyst and an unsupported IrO2 powder catalyst. Electrochemical, stack, and system thermoneutral potentials are defined and determined for isothermal and non-isothermal stack operation. Conditions are determined under which the system thermoneutral potential or flammability of H2 in the O2 anode stream limits the stack turndown and operating temperature. Performance is analyzed of a complete PEMWE system with an electrolyzer stack containing an IrO2/TiO2 anode catalyst (2 mg/cm2 Ir loading) and N117-like membrane mitigated for H2 crossover, anode balance-of-plant (BOP) components, cathode BOP system with temperature swing adsorption for H2 purification, and electrical BOP system with transformer and rectifier. At the rated power condition, defined as 2 A/cm2 at 1.9 V, 80 °C, and 30 bar H2 pressure, the stack/system efficiency is 65.3%/60.3% at beginning of life (BOL), decreasing to 59.3%/53.9% at end of life (EOL). The peak stack/system efficiency is 76.3%/70.2% at BOL, decreasing to 71.2%/65.6% at EOL. Improvements in catalyst activity and membrane are identified for a 50% increase in current to 3 A/cm2 at 1.8 V.

36 MATERIALS SCIENCE↗

Large fluxes of fatty acids from membranes to triacylglycerol and back during N-deprivation and recovery in Chlamydomonas

Abstract Microalgae accumulate triacylglycerol (TAG) during nutrient deprivation and break it down after nutrient resupply, and these processes involve dramatic shifts in cellular carbon allocation. Due to the importance of algae in the global carbon cycle, and the potential of algal lipids as feedstock for chemical and fuel production, these processes are of both ecophysiological and biotechnological importance. However, the metabolism of TAG is not well understood, particularly the contributions of fatty acids (FAs) from different membrane lipids to TAG accumulation and the fate of TAG FAs during degradation. Here, we used isotopic labeling time course experiments on Chlamydomonas reinhardtii to track FA synthesis and transfer between lipid pools during nitrogen (N)-deprivation and resupply. When cells were labeled before N-deprivation, total levels of label in cellular FAs were unchanged during subsequent N-deprivation and later resupply, despite large fluxes into and out of TAG and membrane lipid pools. Detailed analyses of FA levels and labeling revealed that about one-third of acyl chains accumulating in TAG during N-deprivation derive from preexisting membrane lipids, and in total, at least 45% of TAG FAs passed through membrane lipids at one point. Notably, most acyl chains in membrane lipids during recovery after N-resupply come from TAG. Fluxes of polyunsaturated FAs from plastidic membranes into TAG during N-deprivation were particularly noteworthy. These findings demonstrate a high degree of integration of TAG and membrane lipid metabolism and highlight a role for TAG in storage and supply of membrane lipid components.

Plant Sciences↗

Capillary-driven Condensation for Heat Transfer Enhancement in Steam Power Plants

A novel condensation method was developed to enhance the efficiency of steam power plants. The method consists of a hierarchical structure on the surface of condenser tubes consisting of a wicking structure overlaid with a porous hydrophobic membrane. The project is divided into two main efforts. First, a structure with highly defined geometry was made utilizing microfabrication on silicon. This structure helped us elucidate the physics of steam condensation at the surface, more easily model the heat transfer coefficient, and demonstrate the first proof-of-concept for our proposed condensation approach. The structures on silicon achieved a heat transfer coefficient ~ 240% higher than the theoretical filmwise value at the same operating condition. Second, the method is explored for scalability by fabricating surfaces with industrial class materials followed by heat transfer measurements on flat surfaces. An HTC enhancement of 50% over the experimental filmwise value was achieved on hierarchical copper surfaces made of commercially available copper foams and meshes, showing the potential of achieving heat transfer enhancement using low cost and scalable materials. Scalable fabrication of the hydrophobic membrane and the porous copper wick were also investigated. Our heat and mass transfer model predicts a > 5x heat transfer enhancement on a scalable version of capillary driven condenser made of membrane covered porous copper. The results demonstrate the promise of capillary-driven condensation surfaces for heat transfer applications.

20 FOSSIL-FUELED POWER PLANTS↗

Elastic Single-Ion Conducting Polymer Electrolytes: Toward a Versatile Approach for Intrinsically Stretchable Functional Polymers

Fabrication of stretchable functional polymeric materials usually relies on the physical adhesion between functional components and elastic polymers, while the interfacial resistance is a potential problem. Herein, a versatile approach on the molecular-level intrinsically stretchable polymer materials with defined functionality is reported. The single-ion conducting polymer electrolytes (SICPEs) were employed to demonstrate the proposed concept along with its potential application in stretchable batteries/electronics with improved energy efficiency and prolonged cell lifetime. The obtained membranes exhibit 88–252% elongation before breaking, and the mechanical properties are well adjustable. The galvanostatic test of the assembled cells using the obtained SICPE membrane exhibited a good cycling performance with a capacity retention of 81.5% after 100 cycles. The applicability of a proposed molecular-level design for intrinsically stretchable polymer materials is further demonstrated in other types of stretchable functional materials, including poly(vinylcarbazole)-based semiconducting polymers and poly(ethylene glycol)-based gas separation membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Achieving Higher Activity of Acidic Oxygen Evolution Reaction Using an Atomically Thin Layer of IrO x over Co 3 O 4

The development of electrocatalysts with reduced iridium (Ir) loading for the oxygen evolution reaction (OER) is essential to produce low-cost green hydrogen from water electrolysis under acidic conditions. Herein, an atomically thin layer of iridium oxide (IrO x ) has been uniformly dispersed onto cobalt oxide (Co 3 O 4 ) nanocrystals to improve the efficient use of Ir for acidic OER. In situ characterization and theoretical calculations reveal that compared to the conventional IrOx cluster, the atomically thin layer of IrO x shows stronger interaction with the Co 3 O 4 and consequently higher OER activity due to the Ir-O-Co bond formation at the interface. Equally important, the facile synthetic method and the promising activity in the proton exchange membrane water electrolyzer, reaching 1 A cm -2 at 1.7 V with remarkable durability, enable potential scale-up applications. In conclusion, these findings provide a mechanistic understanding for designing active, stable and lower-cost electrocatalysts with well-defined structures for acidic OER.

58 GEOSCIENCES↗