Bi/CeO2–Decorated CuS Electrocatalysts for CO2-to-Formate Conversion
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PROVIDER: S-EPMC11243283 | biostudies-literature | 2024 Jun
REPOSITORIES: biostudies-literature
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Project description:Electrochemical CO2 reduction offers an effective means to store renewable electricity in value-added chemical feedstocks. Much effort has been made to develop catalysts that achieve high Faradaic efficiency toward Formate production, but the catalysts still need high operating potentials to drive the CO2–to–formate reduction. Here we report physical vapor deposition to fabricate homogeneously alloyed, compositionally controlled Cu1-xBix bimetallic catalysts over a large area with excellent electrical conductivity. Operating electrochemical studies in Ar-saturated and CO2-saturated electrolytes identified that Cu–Bi catalysts notably suppress the competing H2 evolution reaction and enhance CO2–to–formate selectivity. We reported a formate Faradaic efficiency of >95% at an improved cathodic potential of ∼−0.72 V vs. RHE and a high formate cathodic energy efficiency of ∼70%. The electrochemical reaction is stable over 24 h at a current density of 200 mA cm−2. The work shows the advantages of bimetallic catalysts over single metal catalysts for increased reaction activity and selectivity.
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Project description:CO2 utilization
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Project description:NAD-dependent formate dehydrogenase (FDH) from Candida boidinii (CbFDH) has been widely used in various CO2-reduction systems but its practical applications are often impeded due to low CO2-reducing activity. In this study, we demonstrated superior CO2-reducing properties of FDH from Thiobacillus sp. KNK65MA (TsFDH) for production of formate from CO2 gas. To discover more efficient CO2-reducing FDHs than a reference enzyme, i.e. CbFDH, five FDHs were selected with biochemical properties and then, their CO2-reducing activities were evaluated. All FDHs including CbFDH showed better CO2-reducing activities at acidic pHs than at neutral pHs and four FDHs were more active than CbFDH in the CO2 reduction reaction. In particular, the FDH from Thiobacillus sp. KNK65MA (TsFDH) exhibited the highest CO2-reducing activity and had a dramatic preference for the reduction reaction, i.e., a 84.2-fold higher ratio of CO2 reduction to formate oxidation in catalytic efficiency (kcat/KB) compared to CbFDH. Formate was produced from CO2 gas using TsFDH and CbFDH, and TsFDH showed a 5.8-fold higher formate production rate than CbFDH. A sequence and structural comparison showed that FDHs with relatively high CO2-reducing activities had elongated N- and C-terminal loops. The experimental results demonstrate that TsFDH can be an alternative to CbFDH as a biocatalyst in CO2 reduction systems.
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Project description:Due to the high affinity of ceria (CeO2) towards carbon dioxide (CO2) and the high thermal and mechanical properties of cellulose triacetate (CTA) polymer, mixed-matrix CTA-CeO2 membranes were fabricated. A facile solution-casting method was used for the fabrication process. CeO2 nanoparticles at concentrations of 0.32, 0.64 and 0.9 wt.% were incorporated into the CTA matrix. The physico-chemical properties of the membranes were evaluated by SEM-EDS, XRD, FTIR, TGA, DSC and strain-stress analysis. Gas sorption and permeation affinity were evaluated using different single gases. The CTA-CeO2 (0.64) membrane matrix showed a high affinity towards CO2 sorption. Almost complete saturation of CeO2 nanoparticles with CO2 was observed, even at low pressure. Embedding CeO2 nanoparticles led to increased gas permeability compared to pristine CTA. The highest gas permeabilities were achieved with 0.64 wt.%, with a threefold increase in CO2 permeability as compared to pristine CTA membranes. Unwanted aggregation of the filler nanoparticles was observed at a 0.9 wt.% concentration of CeO2 and was reflected in decreased gas permeability compared to lower filler loadings with homogenous filler distributions. The determined gas selectivity was in the order CO2/CH4 > CO2/N2 > O2/N2 > H2/CO2 and suggests the potential of CTA-CeO2 membranes for CO2 separation in flue/biogas applications.
| S-EPMC8400081 | biostudies-literature
Project description:Abstract It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO2R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non‐renewable metal resources, which hampers their large‐scale implementation. Here, we report the preparation of bimetallic copper‐lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X‐ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano‐shape relationship between eCO2R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste. Bimetallic Cu‐Pb electrocatalysts were prepared from industrial metallurgical residues and used to electrochemically convert CO2 into valuable chemicals. The metlas were extracted through chemical treatment with ammonium chloride, and Cu−Pb electrocatalysts with varying ratios were prepared through electrodeposition. Compared with pure Cu, the bimetallic catalyst displayed a promotional effect on the conversion of carbon dioxide to carbon monoxide. In situ and ex situ characterization revealed that the interplay between in situ reduced Cu and Pb sites results in boosted CO production through synergistic effects.
| S-EPMC9796115 | biostudies-literature
Project description:Hydrogen production by electrocatalytic water splitting is an efficient and economical technology, however, is severely impeded by the kinetic-sluggish and low value-added anodic oxygen evolution reaction. Here we report the nickel-molybdenum-nitride nanoplates loaded on carbon fiber cloth (Ni-Mo-N/CFC), for the concurrent electrolytic productions of high-purity hydrogen at the cathode and value-added formate at the anode in low-cost alkaline glycerol solutions. Especially, when equipped with Ni-Mo-N/CFC at both anode and cathode, the established electrolyzer requires as low as 1.36 V of cell voltage to achieve 10 mA cm-2, which is 260 mV lower than that in alkaline aqueous solution. Moreover, high Faraday efficiencies of 99.7% for H2 evolution and 95.0% for formate production have been obtained. Based on the excellent electrochemical performances of Ni-Mo-N/CFC, electrolytic H2 and formate productions from the alkaline glycerol solutions are an energy-efficient and promising technology for the renewable and clean energy supply in the future.
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Project description:CO2 sequestration in deep-subsurface formations including oil reservoirs is a potential measure to reduce the CO2 concentration in the atmosphere. However, the fate of the CO2 and the ecological influences in carbon dioxide capture and storage (CDCS) facilities is not understood clearly. In the current study, the fate of CO2 (in bicarbonate form; 0∼90 mM) with 10 mM of formate as electron donor and carbon source was investigated with high-temperature production water from oilfield in China. The isotope data showed that bicarbonate could be reduced to methane by methanogens and major pathway of methanogenesis could be syntrophic formate oxidation coupled with CO2 reduction and formate methanogenesis under the anaerobic conditions. The bicarbonate addition induced the shift of microbial community. Addition of bicarbonate and formate was associated with a decrease of Methanosarcinales, but promotion of Methanobacteriales in all treatments. Thermodesulfovibrio was the major group in all the samples and Thermacetogenium dominated in the high bicarbonate treatments. The results indicated that CO2 from CDCS could be transformed to methane and the possibility of microbial CO2 conversion for enhanced microbial energy recovery in oil reservoirs.
| S-EPMC4801891 | biostudies-literature
Project description: Not available
| S-EPMC11575495 | biostudies-literature
Project description:The unavoidable self-reduction of Bismuth (Bi)-based catalysts to zero-valence Bi often results in detrimental adsorption of OCHO*, leading to unsatisfactory selectivity of HCOOH in the electroreduction of carbon dioxide (CO2). A novel Bi-tannin (Bi-TA) complex is developed, which undergoes in situ reconstruction into a Bi/Bi₂O₂CO₃ phase during CO2 reduction. This reconstructed catalyst exhibits high activity and selectivity, achieving a Faradaic Efficiency (FE) for formate production exceeding 90%, peaking at 96%. Operando spectroscopic and theoretical analyses reveal that the Biδ+ active site in Bi/Bi₂O₂CO₃ significantly enhances the formation of the OCHO* intermediate, crucial for formate production. The study offers a promising approach to overcoming the limitations of Bi-based catalysts in CO2 reduction to formate.
| S-EPMC11905003 | biostudies-literature
Project description:Crystalline platinum nanoparticles supported on carbon nanofibers were synthesized for use as an electrocatalyst for polymer electrolyte membrane fuel cells. The nanofibers were prepared by a method of electrospinning from polymer solution with subsequent pyrolysis. Pt nanoneedles supported on polyacrylonitrile pyrolyzed electrospun nanofibers were synthesized by chemical reduction of H2[PtCl6] in aqueous solution. The synthesized electrocatalysts were investigated using scanning, high resolution transmission and scanning transmission electron microscopies, EDX analysis and electron diffraction. The shape and the size of the electrocatalyst crystal Pt nanoparticles were controled and found to depend on the method of H2[PtCl6] reduction type and on conditions of subsequent thermal treatment. Soft Pt reduction by formic acid followed by 100 °C thermal treatment produced needle-shape Pt nanoparticles with a needle length up to 25 nm and diameter up to 5 nm. Thermal treatment of these nanoparticles at 500 °C resulted in partial sintering of the Pt needles. When formic acid was added after 24 h from the beginning of platinization, Pt reduction resulted in small-size spherical Pt nanoparticle of less than 10 nm in diameter. Reduction of H2[PtCl6], preadsorbed on electrospun nanofibers in formic acid with further treatment in H2 flow at 500 °C, resulted in intensive sintering of platinum particles, with formation of conglomerates of 50 nm in size, however, individual particles still retain a size of less than 10 nm. Electrochemically active surface area (ECSA) of Pt/C catalyst was measured by electrochemical hydrogen adsorption/desorption measurements in 0.5 M H2SO4. ECSA of needle-shape Pt nanoparticles was 25 m2 g-1. It increased up to 31 m2 g-1 after thermal treatment at 500 °C, likely, due to amorphous structures removal from carbon nanofibers and retaining of Pt nanoneedle morphology. ECSA of small-size spherical Pt nanoparticles was 26 m2 g-1. Further thermal treatment at 500 °C in vacuum decreased ECSA down to 20 m2 g-1 due to Pt sintering and Pt active sites deactivation. The thermal treatment of small-size spherical Pt nanoparticles in H2 flow at 500 °C produced agglomerates of Pt nanoparticles with ECSA of 14 m2 g-1.
| S-EPMC9070620 | biostudies-literature