Solid Electrolyte Reactor Research Articles

Electrochemical regeneration of high-purity CO2 from (bi)carbonates in a porous solid electrolyte reactor for efficient carbon capture

Electrochemical regeneration of high-purity CO2 from (bi)carbonates in a porous solid electrolyte reactor for efficient carbon capture

Solid electrolyte reactor for nitrate-to-ammonia

Solid electrolyte reactor for nitrate-to-ammonia

Electrochemical nitrate reduction to ammonia with cation shuttling in a solid electrolyte reactor

Electrochemical nitrate reduction to ammonia with cation shuttling in a solid electrolyte reactor

Continuous Direct Air Capture and Electrochemical Conversion of CO2 and H2O into Ethylene and Oxygen in Solid Electrolyte Reactor

Chemelectronics LLC has developed economical approach to use solar energy to convert CO2 directly captured from air using carbon dioxide capture conductive sorbent materials coated on carbon foam electrodes into chemical products (ethylene) and oxygen from nick foam electrodes separated with solid polyelectrolytes. We take advantage of commercial off-the-shelf solar panels as electricity to supply the electrochemical reduction of CO2 directly captured from air into chemical products with zero carbon emission.Based on the life cycle analysis, there is no CO2 emission from CO2 capture and conversion. The energy will be produced from solar panels.

Cobalt-Doped Bismuth Nanosheet Catalyst for Enhanced Electrochemical CO2 Reduction to Electrolyte-Free Formic Acid.

Electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) to valuable liquid fuels, such as formic acid/formate (HCOOH/HCOO-) is a promising strategy for carbon neutrality. Enhancing CO2RR activity while retaining high selectivity is critical for commercialization. To address this, we developed metal-doped bismuth (Bi) nanosheets via a facile hydrolysis method. These doped nanosheets efficiently generated high-purity HCOOH using a porous solid electrolyte (PSE) layer. Among the evaluated metal-doped Bi catalysts, Co-doped Bi demonstrated improved CO2RR performance compared to pristine Bi, achieving ~90 % HCOO- selectivity and boosted activity with a low overpotential of ~1.0 V at a current density of 200 mA cm-2. In a solid electrolyte reactor, Co-doped Bi maintained HCOOH Faradaic efficiency of ~72 % after a 100-hour operation under a current density of 100 mA cm-2, generating 0.1 M HCOOH at 3.2 V. Density functional theory (DFT) results revealed that Co-doped Bi required a lower applied potential for HCOOH generation from CO2, due to stronger binding energy to the key intermediates OCHO* compared to pure Bi. This study shows that metal doping in Bi nanosheets modifies the chemical composition, element distribution, and morphology, improving CO2RR catalytic activity performance by tuning surface adsorption affinity and reactivity.

Efficient industrial-current-density H2O2 production in neutral medium via external-shell boron regulation on single-atom VN4 sites

The unamiable electrolyte environment and insufficient kinetics of electrochemical two-electron oxygen reduction reaction (2e− ORR) hinders its application in producing H2O2. To address this issue, nitrogen-coordinated single atom vanadium with external shell boron regulation is designed for efficient H2O2 production in neutral medium. The optimal catalyst VN4B/NC showcase a 2e− ORR pathway selectivity of 96.6 % in 0.1 M Na2SO4. And the high current density (1.1 A cm−2) and excellent production rate (16.23 mmol cm−1 h−1) in flow cell further confirm its superior activity. Moreover, VN4B/NC exhibits potential application in solid electrolyte reactor, which is demonstrated by the production rate of 10.18 mmol cm−1 h−1 and long-term stability up to 100 h. Mechanism study suggest the external shell B regulation optimize the adsorption of OOH* intermediates on V sites, boosting the 2e− ORR pathway. This work provides novel insights to rational design of electrocatalysts for commodity chemicals production.

Continuous Direct Air Capture and Electrochemical Conversion of CO2 and H2O into Ethylene and Oxygen in a Solid Electrolyte Reactor

Continuous Direct Air Capture and Electrochemical Conversion of CO₂ and H₂O into Ethylene and Oxygen in a Solid Electrolyte Reactor

Strongly Coupled Ag/Sn–SnO2 Nanosheets Toward CO2 Electroreduction to Pure HCOOH Solutions at Ampere-Level Current

HighlightsThe strongly coupled Ag/Sn–SnO2 nanosheets (NSs) were prepared via a versatile electrochemical template strategy, and the generated electron-enriched Sn sites promote the formation of *OCHO and alleviate the energy barriers of *OCHO to *HCOOH.Ag/Sn–SnO2 NSs afford a superior activity toward CO2 electroreduction with current densities up to 2000 mA cm‒2 and near-unity selectivity for formate production.Ag/Sn–SnO2 NSs as the cathode in a membrane electrode assembly with porous solid electrolyte reactor enable the direct production of ~ 0.12 M pure HCOOH solution for 200 h.

Redox-couple-assisted CO2 capture on solid-electrolyte reactor

Redox-couple-assisted CO2 capture on solid-electrolyte reactor

Continuous carbon capture in an electrochemical solid-electrolyte reactor.

Electrochemical carbon-capture technologies, with renewable electricity as the energy input, are promising for carbon management but still suffer from low capture rates, oxygen sensitivity or system complexity1-6. Here we demonstrate a continuous electrochemical carbon-capture design by coupling oxygen/water (O2/H2O) redox couple with a modular solid-electrolyte reactor7. By performing oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) redox electrolysis, our device can efficiently absorb dilute carbon dioxide (CO2) molecules at the high-alkaline cathode-membrane interface to form carbonate ions, followed by a neutralization process through the proton flux from the anode to continuously output a high-purity (>99%) CO2 stream from the middle solid-electrolyte layer. No chemical inputs were needed nor side products generated during the whole carbon absorption/release process. High carbon-capture rates (440 mA cm-2, 0.137 mmolCO2 min-1 cm-2 or 86.7 kgCO2 day-1 m-2), high Faradaic efficiencies (>90% based on carbonate), high carbon-removal efficiency (>98%) in simulated flue gas and low energy consumption (starting from about 150 kJ per molCO2) were demonstrated in our carbon-capture solid-electrolyte reactor, suggesting promising practical applications.

Hydrophobic, Ultrastable Cuδ+ for Robust CO2 Electroreduction to C2 Products at Ampere-Current Levels.

Copper (Cu) is the only known material that can efficiently electrocatalyze CO2 to value-added multicarbon products. Owing to the instability of the Cuδ+ state and microscopic structure in reactions, Cu catalysts are still facing big challenges with low selectivity and poor durability, particularly at high current densities. Herein, we report a rational one-step surface coordination approach for the synthesis of Cu dendrites with an ultrastable Cuδ+ state and hydrophobicity (Cu CF), even after exposure to air for over 6 months. As a result, Cu CF exhibited a C2 FE of 90.6% at a partial current density of 453.3 mA cm-2 in a flow cell. A 400 h stable electrolysis at 800 mA and even a ground-breaking stable operation at a large industrial current of 10 A were achieved in the membrane electrode assembly (MEA) form. We further demonstrated a continuous production of C2H5OH solution with 90% relative purity at 600 mA over 50 h in a solid-electrolyte reactor. Spectroscopy and computation results suggested that Cu(II) carboxylate coordination species formed on the surface of Cu CF, which ensured the stability of the Cuδ+ state and hydrophobicity. As a result, rich active sites and a stable three-phase interface on the catalyst surface were achieved, along with the optimized *CO adsorption strength and adsorption configuration. The mixed *CO adsorption configurations on Cu CF made the *CO dimerization process easier, which promoted the conversion of CO2 to C2 products. This work provides a promising paradigm for the design and development of Cu-based catalysts with ultrahigh stability under industrial current densities.

Synergy of Cu/C3N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid

AbstractElectrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g‐C3N4) supported Cu nanoparticles (Cu−CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm−2 in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C3N4 interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate −*CHO is advantage around the Cu/C3N4 interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu−CN catalyst in the industrial application.

Synergy of Cu/C3 N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid.

Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g-C3 N4 ) supported Cu nanoparticles (Cu-CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm-2 in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C3 N4 interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate -*CHO is advantage around the Cu/C3 N4 interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu-CN catalyst in the industrial application.

(Invited) Electrifying CO2 into Fuels and Chemicals in a Solid Electrolyte Reactor

Electrochemical CO2 reduction, with the energy input from renewable electricity, provides a green and alternative route for the generation of chemicals and fuels. However, its practice is currently challenged at two systematical levels: the lack of selective electrocatalysts to combat the strong completion from water reduction, and the lack of novel reactors for large-scale reaction rates and efficient product separation. In this talk, I will introduce the rational design of both catalytic materials and reactors towards practical CO2 reduction performances. By dispersing transition metals into isolated single atoms with electronic structures significantly different from their bulk counterparts, we can dramatically suppress the competing hydrogen evolution and deliver an ultra-high CO2 reduction selectivity of more than 95% under ambient conditions in water. Scaled-up synthesis and efficient reactors demonstrated the potential for practical applications. Furthermore, by designing a solid electrolyte reactor, we successfully demonstrated a continuous generation of pure liquid fuel solutions via CO2 reduction. This technology eliminates the product separation process required in traditional CO2 reduction electrolyzers, opening up its practical applications in the future.

Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media

Electrochemical oxygen reduction to hydrogen peroxide (H2O2) in acidic media, especially in proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach to promote the H2O2 selectivity (over 80%) under industrial-relevant generation rates (over 400 mA cm−2) in strong acidic media using just carbon black catalyst and a small number of alkali metal cations, representing a 25-fold improvement compared to that without cation additives. Our density functional theory simulation suggests a “shielding effect” of alkali metal cations which squeeze away the catalyst/electrolyte interfacial protons and thus prevent further reduction of generated H2O2 to water. A double-PEM solid electrolyte reactor was further developed to realize a continuous, selective (∼90%) and stable (over 500 hours) generation of H2O2 via implementing this cation effect for practical applications.

Recovering carbon losses in CO2 electrolysis using a solid electrolyte reactor

Recovering carbon losses in CO2 electrolysis using a solid electrolyte reactor

Electricity + Air + Water = Hydrogen Peroxide

Hydrogen peroxide (H2O2) is one of the most important chemicals in the world, and is currently produced exclusively by the energy- and waste-intensive anthraquinone cycling process. Electrochemical synthesis of H2O2, including both oxygen reduction reaction (ORR) and water oxidation reaction (WOR) to H2O2, provides a promising alternative route to realize green and delocalized H2O2 production. In this talk I will introduce both catalytic materials design and solid electrolyte reactor engineering for highly active and selective generation of pure H2O2 solutions.

Copper-catalysed exclusive CO2 to pure formic acid conversion via single-atom alloying.

Converting CO2 emissions, powered by renewable electricity, to produce fuels and chemicals provides an elegant route towards a carbon-neutral energy cycle. Progress in the understanding and synthesis of Cu catalysts has spurred the explosive development of electrochemical CO2 reduction (CO2RR) technology to produce hydrocarbons and oxygenates; however, Cu, as the predominant catalyst, often exhibits limited selectivity and activity towards a specific product, leading to low productivity and substantial post-reaction purification. Here, we present a single-atom Pb-alloyed Cu catalyst (Pb1Cu) that can exclusively (~96% Faradaic efficiency) convert CO2 into formate with high activity in excess of 1 A cm-2. The Pb1Cu electrocatalyst converts CO2 into formate on the modulated Cu sites rather than on the isolated Pb. In situ spectroscopic evidence and theoretical calculations revealed that the activated Cu sites of the Pb1Cu catalyst regulate the first protonation step of the CO2RR and divert the CO2RR towards a HCOO* path rather than a COOH* path, thus thwarting the possibility of other products. We further showcase the continuous production of a pure formic acid solution at 100 mA cm-2 over 180 h using a solid electrolyte reactor and Pb1Cu.

Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates

Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm−2) while maintaining high H2O2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H2O2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H2O2 solutions with high selectivity (up to 95%) and high H2O2 partial currents (up to ~400 mA cm−2), illustrating the catalyst’s great potential for practical applications in the future.

Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction

Electrochemical CO2 or CO reduction to high-value C2+ liquid fuels is desirable, but its practical application is challenged by impurities from cogenerated liquid products and solutes in liquid electrolytes, which necessitates cost- and energy-intensive downstream separation processes. By coupling rational designs in a Cu catalyst and porous solid electrolyte (PSE) reactor, here we demonstrate a direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction. With optimized edge-to-surface ratio, the Cu nanocube catalyst presents an unprecedented acetate performance in neutral pH with other liquid products greatly suppressed, delivering a maximal acetate Faradaic efficiency of 43%, partial current of 200 mA⋅cm-2, ultrahigh relative purity of up to 98 wt%, and excellent stability of over 150 h continuous operation. Density functional theory simulations reveal the role of stepped sites along the cube edge in promoting the acetate pathway. Additionally, a PSE layer, other than a conventional liquid electrolyte, was designed to separate cathode and anode for efficient ion conductions, while not introducing any impurity ions into generated liquid fuels. Pure acetic acid solutions, with concentrations up to 2 wt% (0.33 M), can be continuously produced by employing the acetate-selective Cu catalyst in our PSE reactor.