CO Conversion Rate Research Articles

Ni-Co Bimetallic Catalysts Supported on Mixed Oxides (Sc-Ce-Zr) for Enhanced Methane Dry Reforming.

Dry methane reforming (DRM) presents a viable pathway for converting greenhouse gases into useful syngas. Nevertheless, the procedure requires robust and reasonably priced catalysts. This study explored using cost-effective cobalt and nickel combined into a single catalyst with different metal ratios. The reaction was conducted in a fixed reactor at 700 °C. The findings indicate that the incorporation of cobalt significantly enhances catalyst performance by preventing metal sintering, improving metal dispersion, and promoting beneficial metal-support interactions. The best-performing catalyst (3.75Ni+1.25Co-ScCeZr) achieved a good conversion rate of CH4 and CO2 at 46.8 %, and 60 % respectively after 330 minutes while maintaining good stability. The TGA and CO2-TPD analysis results show that the addition of Co to Ni reduces carbon formation, and increases the amount of strong basic sites and isolated O2- species, and the total amount of CO2 desorbed. These results collectively highlight the potential of cobalt-nickel catalysts for practical DRM applications and contribute to developing sustainable energy technologies.

Model-based optimization strategies for direct hydrogenation of carbon dioxide to dimethyl ether

This study discusses model-based optimization strategies for CO2 hydrogenation to dimethyl ether (DME) over a CuZnZr (CZZ) and ferrite (FER) mixed catalyst system in a packed-bed reactor configuration. A two-dimensional axisymmetric, nonisothermal packed-bed reactor model was developed using COMSOL Multiphysics 6.2 software. The model solves two-dimensional (radial and axial) heat and mass transport equations in the packed-bed and integrates intraparticle diffusion and heat transfer in a 1D approach. This powerful feature differs from a traditional porous media approach and takes into account any heat and mass transfer limitations that may exist. Analysis shows that the heat transfer limitations are negligible, but strong internal mass transfer limitations were observed at 10 ≤ WHSV ≤ 90 h−1 on the FER catalyst and at 240 °C. The optimum catalyst composition (i.e., mixing ratio) varies depending on the operating regime. The FER catalyst weight in the mixture can be as low as 5 wt.%, but the ideal composition depends on the internal mass transfer limitation and its relationship with the operating regime (i.e., weight hourly space velocity, temperature). A catalyst composition of 80 wt.% CZZ and 20 wt.% FER was suggested; this composition can provide high CO2 conversion and DME production rates at a wide range of temperatures and flow rates.

Investigation of highly efficient CO2 hydrogenation at ambient conditions using dielectric barrier discharge plasma

The increasing utilization of CO2 for synthesizing high-value fuels or essential chemicals is a potentially effective approach to mitigating global warming and climate change. Compared to thermal catalytic CO2 conversion under hash operating conditions (400∼500°C, 10 MPa), non-thermal plasma can overcome kinetic barriers and trigger reactions beyond thermal equilibrium at ambient temperature and pressure. In this study, the effects of operating conditions (discharge frequency, input power, and gas flow rate) and geometrical parameters (discharge length, discharge gap, and dielectric materials) have been extensively analyzed using typical cylindrical dielectric barrier discharge (DBD) plasma. The discharge characteristics changed by operating conditions (including waveforms of applied voltage and current) are compared, indicating higher applied voltage and lower gas flow rate can strengthen the filamentary discharges. The results demonstrate CO2 conversion rate increases with the increase of applied voltage and the decrease of CO2/H2 ratio, achieving its maximum value of 43.0% at 20 mL/min. The highest energy efficiency of 3771.9 μg/kJ for CO generation is obtained at the applied voltage of 5.5 kV and gas flow rate of 40 mL/min, respectively. Besides, the constructure of plasma reactor also impacts the performance of CO2 conversion. On the one hand, the discharge gap has a significant role in the variation of CO2 conversion and product selectivity, which is attributed to the electric field density and corresponding electron-induced reaction. On the other hand, the circulating water-cooling jacket was used to find out the influence of reaction temperature, which switched the product from CO to CH4. This work will pave the way for a sustainable alternative towards future CO2 conversion and utilization.

A robust floating oxygen-doped graphitic carbon nitride sheet for efficient photocatalytic CO2 conversion

Photocatalytic CO2 reduction offers a promising approach for converting CO2 into valuable chemicals. However, typical conversion systems suffer from inefficient CO2 mass transfer and complex recycling processes. In this study, we developed a floating sheet as a robust photocatalytic CO2 conversion system by integrating graphitic carbon nitride (CN) nanosheets onto polytetrafluoroethylene (PTFE) fiber membrane, followed by oxygen (O) doping into the CN (CN-O) via oxygen-plasma treatment. The floatable CN-O/PTFE sheet exhibits slight wettability in water under 0.25 MPa of CO2 pressure in our reactor system, facilitating the delivery of dissolved CO2 to the CN-O photocatalyst surface. O-doping enhances the visible light absorption and improves the separation and transport efficiency of photogenerated electrons and holes due to O-doping-induced states in CN. Consequently, the floating CN-O/PTFE system achieves an exceptional photocatalytic CO2 conversion rate of 102.3 μmol g-1h−1, approximately 4.8 times higher than a conventional CN-powder dispersion system in water. Moreover, the sheet demonstrates excellent cycling durability, with no significant exfoliation of the catalytic layer or reduction in CO2 photoreduction activity after 20 consecutive cycles. This study presents a novel approach to designing photocatalytic systems for efficient CO2 conversion.

Preparation activated tailings by pH swing process: Towards yielding cemented tailings backfill and in-situ CO2 mineralization

In-situ CO2 mineralization of tailings has shown great potential for large-scale CO2 sequestration, but its development is seriously limited by the low CO2 conversion rate. This study proposed an innovative pH swing process to produce activated tailings through magnesium extraction from raw tailings and subsequent leachate precipitation. By the combination of activated tailings and high-belite calcium sulfoaluminate cement, a new type of cemented activated tailings backfill (CATB) was developed. The results demonstrate that 82.33% of magnesium is extracted from raw tailings and precipitates in the form of Mg(OH)2 serving as the dominating carbonation active phase during the pH swing process. Besides the aragonite forms in the carbonated cemented raw tailings backfill (CRTB), carbonated CATB also contains calcite, nesquehonite, and hydromagnesite. Substituting activated tailings for raw tailings led to the higher CO2 absorption capability (ranging from 8.88% to 14.17% with various binder-to-tailings ratios). These indicate that the activated tailings have a promising application scenario in large scale in-situ CO2 mineralization.

Selective CO2 hydrogenation to methanol over a novel ternary In-Co-Zr catalyst

To address the challenges of global warming and energy shortages, the technology to convert CO2 into methanol is of great significance Indium-cobalt catalysts have attracted widespread attention due to their significant activity and excellent stability. Herein, In-Co and In-Co-Zr catalyst rich in In2O3 were prepared through a citric acid-assisted co-precipitation method. The results show that the In-Co-Zr catalyst can significantly enhance the activity for hydrogenating CO2 to methanol, achieving a CO2 conversion rate of 17.4 % and a methanol selectivity of 77.7 % under the conditions (5.0 MPa, 310 °C, GHSV = 10.28 l·gcat-1·h-1, H2/CO2 ratio of 4). At a GHSV of 48 l·gcat-1·h-1, the space–time yield of methanol was 0.79 gMeOH·gcat-1·h-1, and the catalyst exhibited stable catalytic activity over a continuous reaction period of 120 h. It was revealed that the incorporation of ZrO2 could significantly improve methanol selectivity of In-Co catalyst. Moreover, an increased oxygen vacancy and strong interaction of the In-Co-Zr catalysts are conducive to improving the CO2 adsorption strength and capacity. It is expected that this novel ternary In-Co-Zr catalyst could inspire new opportunities for designing and developing multi-component hybrid catalysts for highly active, stable and selective CO2 hydrogenation to methanol

Enhancement of H2-water mass transfer using methyl-modified hollow mesoporous silica nanoparticles for efficient microbial CO2 reduction

Inorganic-microbial hybrid catalysis is an emerging technology that uses electrical energy to drive microorganisms to reduce CO2 into high value-added compounds, and it has broad application prospects in CO2 reduction. However, the low current density (production yield) limits its practical application. Hydrogen-mediated inorganic-microbial hybrid catalysis system can achieve higher current density, but it is limited by low H2 mass transfer. Here, silica nanoparticles were used to enhance the hydrogen mass transfer for highly efficient CO2 reduction. Solid silica (SN), mesoporous silica (MSN), hollow mesoporous silica (HMSN), and methyl-modified hollow mesoporous silica (MHMSN) were firstly prepared and tested for the enhancement of hydrogen mass transfer. Of these, MHMSN nanoparticles at a concentration of 0.3 wt% were the best at enhancing gas-liquid mass transfer, the volumetric mass transfer coefficient (KLa) and saturated dissolved hydrogen concentration of H2 are 0.53 min-1 and 1.81 mg l-1, respectively. Compared with the control group without added nanoparticles, MHMSN significantly increased the solubility and KLa of H2. This can be attributed that the addition of MHMSN promoted the detached process of hydrogen bubbles from the electrode surface, which made the diameter of hydrogen bubbles smaller, increased the gas-liquid mass transfer area, and strengthened the mass transfer process of H2. Furthermore, it was added to the inorganic-microbial hybrid catalysis system to effectively promote the microbial carbon reduction process, achieving a polyhydroxybutyrate (PHB) yield of up to 700 mg l-1, and the electron utilization rate and CO2 conversion rate were 51 % and 58 % higher than the control group, respectively. These results demonstrated that the addition of MHMSN is an effective approach to enhancing the performance of H2-mediated inorganic-microbial hybrid catalysis system.

Preparation of nano Cu-Mo2C interface supported on ordered mesoporous biochar of ultrahigh surface area for reverse water gas shift reaction

High conversion rate and selectivity are challenges for CO2 utilization through catalytic reverse water gas shift (RWGS) reaction. Herein, a novel mesoporous biochar (MB) supported Cu-Mo2C nano-interface was prepared by consecutive physical activation of coconut shells followed by carbothermal hydrogen reduction of bimetal. As compared with traditional carbon materials, this MB exhibited ultra-high specific surface area (2693 m2 g–1) and mesopore volume of mesopore (0.81 cm3 g–1) with a narrow distribution (2–5 nm), responsible for the high dispersion of binary Cu-Mo2C sites, CO2 adsorption and mass transfer in the reaction system. Moderate carbothermal reduction led to the sufficient reduction of Mo ion with carbon matrix of MB and dispersive growth of nano Cu-Mo2C binary sites (~ 6.1 nm) on the surface of MB. Cu+ species were formed from Cu0 via electron transfer and showed high dispersion with simultaneous boosted bimetal loading due to the strong interaction between nano Mo2C and Cu. These were advantageous to the intrinsic activity and stability of the Cu-Mo2C binary sites and their accessibility to the reactant molecules. Under the RWGS reaction conditions of 500 °C, atmospheric pressure, and 300,000 ml/g/h gas hour space velocity, the CO2 conversion rate over Cu-Mo2C/MB reached 27.74 × 10–5 molCO2/gcat/s at very low H2 partial pressure, which was more than twice that over traditional carbon supported Cu-Mo2C catalysts. In addition, this catalyst exhibited 99.08% CO selectivity and high stability for more than 50 h without a decrease in activity and selectivity. This study offers a new development strategy and a promising candidate for industrial RWGS.Graphical

Precisely Tuning Band Gaps of Hexabenzocoronene-Based MOFs Toward Enhanced Photocatalysis.

Precise adjusting the band gaps in metal-organic frameworks (MOFs) is crucial for improving their visible-light absorption capacity during photocatalysis, presenting both a formidable challenge and a charming opportunity. This present study employed a symmetry-reduction strategy to pre-design six novel 4-connected ligands with systematic substituents (-NO2, -H, -tBu, -OCH3, -OH and -NH2) and synthesized the corresponding pillared-layer Zr-MOFs (NKM-668) retaining the hexaphenylbenzene fragment. Subsequently, the NKM-668 MOFs were transformed into large-π-conjugated hexabenzocoronene-based MOFs (pNKM-668) via the Scholl reaction. These twelve MOFs exhibited broad and tunable band gaps over 1.41 eV (ranging from 3.25 eV to 1.84 eV), and the photocatalytic CO2 conversion rate raised by 33.2-fold. This study not only enriches the type of hexaphenylbenzene-based MOFs, but also paves the way for nanographene-containing MOFs in the further application of photocatalysis.

Modulating stacking mode and molecular polarization in CTF/molecule heterojunction for meliorating photocatalytic CO2 conversion with nearly 100% CO selectivity

Herein, two conjugated molecules, i.e., D-π-A TAPT and non-D-A TAPB, are finely designed to incorporate with covalent triazine framework (CTF) in A-A and A-B stacking mode via π-π interaction, respectively. The transient photocurrent response of the generated AA-CTF/TAPT Z-Scheme heterostructure is 1.14 × 10-7 A, significantly higher than that of the other two metal-free heterostructures (AA-CTF/TAPB and AB-CTF/TAPT). The promoted photocarrier transportation is attributed to strong polarization (dipole moment = 2.634 D) imposed by the D-π-A effect in TAPT that motivates the interfacial charge separation, and the coexisting charge transfer channel built by the ordered A-A stacking mode in AA-CTF that expedites the charge delivery. The photocatalytic CO2 conversion conducted by AA-CTF/TAPT gives the optimal CO conversion rate as 7.47 μmol·g−1·h−1, and with nearly 100 % product selectivity obtained, which is attributable to the lower energy barrier of CO desorption barrier (−1.07 eV) rather than that of CHO* formation (1.52 eV) for generating CH4.

Unraveling the role of reducing atmospheres on Fe-Zn-Al catalysts for highly selective carbon dioxide hydrogenation to light olefins

This study investigates the carbon dioxide (CO2) hydrogenation performance of Fe-Zn-Al catalysts pretreated under four distinct reducing atmospheres (H2, H2/N2, H2/CO, and CO/N2), elucidating their impact on CO2 conversion, CO selectivity, and light olefins selectivity. Combined with the characterization results, it was found that various catalyst components were obtained after activation in different atmospheres, but Fe5C2 was observed in all the catalysts after the CO2 hydrogenation reaction. The catalytic performance is intricately linked to the type of surface species produced after reduction and the Fe5C2 content. In a comparative perspective, the catalytic activity of the same catalyst in the four atmospheres followed the sequence H2>H2/N2>CO/N2>H2/CO. Notably, catalyst pretreatment with H2 yielded the highest CO2 conversion rate at 31.6 % and light olefins selectivity at 40.2 %. These results can be attributed to the highest electron density detected by XPS for the iron species on the spent catalyst and to the largest concentration of Fe5C2 formed during the reaction in the hydrogen reduced sample.

CO2 hydrogenation over Fe-Mn-Zn spinel oxide nanohybrids precatalysts

Catalytic CO2 hydrogenation using green hydrogen is a promising approach for mitigating CO2 emissions and utilizing CO2 as a feedstock. While Fe-based catalysts produce long-chain hydrocarbons under high-pressure CO2 hydrogenation reactions, the C2+ hydrocarbon yield tends to be insufficient at low-pressure conditions over the catalyst. This study reports the enhancement of light olefin selectivity of CO2 hydrogenation over Fe-based catalysts at low pressure via nanoscale hybridization with manganese (Mn) and zinc (Zn) oxides. The resulting hybridized catalyst exhibited distinctive performance in terms of CO2 hydrogenation to light olefins at relatively low pressure (0.7 MPa) in terms of CO2 conversion rate and C2–C4 yield with high olefin rates. Mn and Zn incorporation in Fe oxide decreased the reduction temperature, forming more Fe carbide phase. CO2 adsorption capability at relevant temperatures seems to be improved when Mn and Zn are present. This mixed oxide precatalyst approach can be extended to other elements.

Efficient photocatalytic CO2 and Cr(VI) reduction on carbon spheres/g-C3N4 composites with enriched nitrogen vacancies

In this study, carbon spheres (CS)/g-C3N4 composite materials were fabricated by a hydrothermal method, and the characterizations have confirmed the successful anchoring of CS onto the surface of g-C3N4, constructing enriched nitrogen vacancies during the synthesis process. The photocatalytic CO2 reduction activity of g-C3N4 is enhanced by all of these advantageous factors. The significant enhancement can be attributed to the tight interfacial interaction between CS and g-C3N4, which endows with the photocatalyst a larger specific surface area, higher light utilization efficiency and stronger capability for photoinduced charges separation. Furthermore, the presence of nitrogen vacancies further accelerates the separation and migration efficiency of photogenerated charges, provides additional active sites to promote the adsorption and activation of CO2 molecules, thereby effectively boosting the photocatalytic activity for CO2 reduction. The CO2 conversion rate on CS/g-C3N4 composite materials is higher than that on the reference g-C3N4. The apparent quantum yield (AQY) is also superior to that of the reference g-C3N4 under three different monochromatic light irradiations. The stability of the catalyst was verified through cycling experiments, indicating promising potential practical industrial application. The CO2 reduction mechanism and transformation pathways were elucidated using in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The photocatalytic reduction rate constant of Cr(VI) by 50CS/CN is 2.9 times higher than that by CN. This study introduces a facile approach for synthesizing g-C3N4-based photocatalytic materials, providing an interesting strategy to boost photocatalytic activity of g-C3N4 for photocatalytic CO2 and Cr(VI) reduction.

Effective CO2 Thermocatalytic Hydrogenation with High Coke Resistance on Ni-CZ/Attapulgite Composite

Converting CO2 into methane is considered a promising and economically viable technology for global transportation and utilization of this greenhouse gas. This study involves the preparation of a Ni-CZ (CeO2-ZrO2)/ATP (attapulgite) catalyst through the co-precipitation and impregnation methods. XRD, SEM, TEM, N2 absorption-desorption isotherms, XPS, H2-TPR, CO2-TPD, TG/DSC, and Raman were adapted to characterize the obtained samples. Real-time GC was used to measure the catalytic performances and to intensively study the impact of Ni loading content and ATP to CZ ratio on the catalytic performance of the products. DRIFTs was used to monitor the interstitial radicals in the catalytic reactions and to deduce the catalytic mechanisms. The results indicate that the composite catalytic matrix composed of CZ assembled on ATP demonstrated higher CO2 methanation stability and better carbon deposition resistance ability than the single CZ or ATP as the carrier, which should be attributed to the improved specific surface area and pore volume of the ATP assembled matrix and the enhanced dispersibility of the CZ and Ni species. The adoption of CZ solid solutions improves the oxygen storage capability of the catalyst, thereby providing continued mobile O2− in the matrix and accelerating the molecular exchange rate in the catalytic reactions. The ideal loading quantity of nickel contents on the CZA matrix is 15%, as the CO2 conversion decreases at elevated temperatures when the Ni loading content reaches 20%. Among the tested samples, the 15Ni-0.8CZA sample showed the best catalytic performance of 75% CO2 conversion and 100% CH4 selectivity at 400 °C. After 50 h of stability tests, the CO2 conversion rate still remained 70.84%, and the CH4 selectivity obtained 97.46%. No obvious coke was detected according to the Raman spectra of the used catalyst. The in situ DRIFTS experiment showed that formate is the main intermediate of the CO2 hydrogenation reaction on the 15Ni-0.8CZA catalyst.

Reverse water-gas shift in a novel spark-coupled dielectric barrier discharge plasma: Effects of electrode structure and gas parameters

The reverse water–gas shift (RWGS) reaction holds promise for producing raw materials used in the synthesis of high-value chemicals. However, the reaction is often hindered by low CO2 conversion rates at atmospheric pressure and low temperatures. To overcome this limitation, this study developed a novel reactor based on strengthened spark-coupled dielectric barrier discharge (SSCDBD) without a catalyst, leveraging local high temperatures to enhance performance. The effects of reactor structure and gas parameters on conversion rate and energy efficiency were systematically investigated. The results indicated that the SSCDBD device notably improved CO2 conversion compared to conventional plasma techniques, such as dielectric barrier discharge (DBD), spark discharge, and spark-coupled dielectric barrier discharge (SCDBD), with respective increases of 1000 %, 12.65 %, and 2.79 %. Notably, varying the length of the auxiliary electrode affects the capacitance of the equivalent capacitor and, consequently, the discharge intensity. Furthermore, Increasing the electrode length from 4 cm to 20 cm improved the CO2 conversion rate from 43.7 % to 59.8 %. Moreover, CO2 conversion was positively correlated with the discharge distance, which also affected the volume of the electric arc. However, distances exceeding 1.2 cm interfered with arc formation. At a CO2:H2 molar ratio of 1:1, with an auxiliary electrode length of 12 cm and a discharge distance of 0.8 cm, the maximum CO2 conversion rate of 66 % was achieved at a total feed flow rate of 100 mL min−1, while maintaining a CO selectivity higher than 99 %. Additionally, with a total feed flow rate of 400 mL min−1, CO2 conversion reached 29 % and energy efficiency peaked at 6.34 %.

Thermodynamic investigation of biomass-steam gasification in converter vaporisation flue for synthesis gas production

Biomass gasification for hydrogen production is a highly promising technology for energy conversion and utilisation. This paper proposed a novel technology for the injection of biomass and steam into the flue of a converter vaporisation to produce hydrogen-rich syngas. The feasibility of hydrogen generation through gasification between biomass, steam, and carbon dioxide in the high-temperature flue gas was investigated based on the thermodynamic principle of Gibbs free energy minimisation. The influence of gasification parameters on the composition of syngas was also explored. The results indicate that in the gasification process, biomass and steam injected into the converter vaporisation flue can effectively inhibit the generation of by-products such as tar. As the steam volume increases, the volume fraction of hydrogen in the product also increases, while the concentration of carbon monoxide decreases. By adjusting the steam-to-biomass ratio, syngas with a hydrogen content exceeding 20% can be produced. At a reaction temperature of 1200 °C, with a steam addition of 5%, a biomass addition of 8 g/L, and a [Formula: see text] ratio of 3, the gas products are composed of 25% hydrogen and 67% carbon dioxide. The process has the potential to achieve a hydrogen yield of up to 90%, a syngas yield of 94%, and a CO2 conversion rate of 70%. Additionally, the lower heating value of the syngas is measured at 11.24 MJ/Nm3. The research results have confirmed the viability of the new technology, thus establishing a theoretical foundation for the industrial implementation of injecting biomass and steam into the converter vaporisation flue to produce hydrogen-rich syngas.

Exploring carbon dioxide sequestration in desalination reject brine via NaOH reaction: A kinetics study

Seawater desalination is one of the most sustainable means of water supply in arid and semi-arid regions. Despite its undeniable potential to meet the global water demands, there are several environmental impacts associated with its operation, including the generation of reject brine and the emission of considerable amounts of CO2. Recently, the mineralization of carbon dioxide using desalination reject brine has emerged as a potential solution for simultaneous brine management and CO2 sequestration. In this study, the reaction kinetics of desalination reject brine with CO2 in the presence of NaOH are evaluated. The effect of various operating parameters, such as the temperature, CO2 concentration, NaOH dosage, brine salinity, CO2 flowrates and inert particles volume percent were investigated by varying them within the range of 15–55 °C, 3–20 %, 6–16 g/L, 5–72 g/L, 1–5 L/min and 0–20 %, respectively. The experimental data showed that the overall rate of CO2 conversion is equal to the sum of the rates observed for Ca2+ and Mg2+ carbonation reactions and increases proportionally with the increase in CO2 concentration. The addition of NaOH improved the Ca2+ carbonation reaction rate but had no effect on Mg2+ carbonation reactions within the investigated reaction conditions. Interestingly, increasing brine salinity had a negative effect on the reaction rate, while the change in temperature and inert particles had minimal effect on the overall reaction rate. Analysis of the solid products showed that Hydromagnesite and Calcite were the two major products obtained. Finally, experimental data were used to develop a rate model representing the CO2-Brine-NaOH system. The developed model will assist in successfully predicting the performance of the process and pave the way for efficient brine management and CO2 sequestration.

Development of membrane bioreactor for conversion of flue Gas-CO2 to C1 and C2 biomolecules

The capture and utilization of CO2 (CCU) from flue gases constitute a novel carbon feedstock for producing renewable chemicals and fuels. To lower the energy demand of CCU, Bio-Integrated Carbon Capture and Utilization (BICCU) was recently presented, where CO2-consuming microorganisms simultaneously desorb and convert CO2 captured from flue gas by methyl diethanolamine (MDEA) with H2 from water-electrolysis as the electron donor. The limiting factor is the microbial toxicity of MDEA, which restricts the capacity of the process. Furthermore, producing soluble molecules like the C2 platform molecule acetate is not possible without contaminating the product with capture agent. To resolve both challenges, we here propose a three-phase membrane system, where the MDEA and microorganisms are separated by a CO2-permeable membrane. Biological batch experiments with a mixed mesophilic culture confirmed the increased capacity of the BICCU-process for producing both methane and acetate when introducing a CO2-permeable membrane to the system to alleviate microbial inhibition by the capture agent and avoid contamination of soluble bioproducts. When using O2-rich flue gas from a biogas combustion engine, the CO2 conversion rate decreased by 18.0 % compared to a clean 20:80 CO2:N2 gas mixture, yet anaerobic metabolisms were still active in the mixed inoculum. Abiotic experiments furthermore showed that the microbial CO2 consumption maintained the gradient across the membrane and enhanced the CO2-flux by a factor of 3.1 ± 0.3. The membrane-based BICCU concept is expected to hold great promise particularly for producing acetate from flue gas-CO2, as the in situ separation eliminates the need for costly downstream separation.

Enhancing CO2 conversion in a temperature-controlled DBD plasma reactor with HKUST-1 catalyst: Water removal and CuO/Cu2O-derived approach

Due to a synergy effect, using dielectric barrier discharge (DBD) plasma technology combined with catalysts for CO2 decomposition, a major contributor to global warming, is recognized as an effective approach to transforming CO2 into valuable products such as CO, which is a crucial feedstock for chemical synthesis. Herein, HKUST-1 was synthesized using the hydrothermal method for CO2 conversion in the DBD reactor. To enhance catalyst performance in the plasma region, HKUST-1 was treated with O2 plasma to increase its specific surface area. Additionally, HKUST-1 was calcined at 300 °C to produce the CuO/Cu2O catalyst. Since the recombination reaction in the CO2 conversion is increased at higher temperatures, the reactor heat is removed using fan cooling and a water circulation system. In the presence of the HKUST-1 catalyst, the CO2 conversion rate significantly increased by 132 %, 82 %, and 12 % in reactors operating without cooling, with fan cooling, and with water cooling circulation, respectively compared to the reactors without catalyst, at a flow rate of 50 ml/min and maximum input power. The catalysts have been characterized using a comprehensive suite of analytical techniques, including FTIR, XRD,TEM, SEM, EDS, and BET analysis. The BET analysis indicates that the specific surface area of HKUST-1 after O2 plasma treatment is increased by 52 %, which causes an increasing conversion rate of up to 18 %. The CuO/Cu2O catalyst demonstrated maximum CO2 conversion of 21 % at an input power of 140 W and achieved energy efficiency of 8.6 % at 40 W. The presence of oxygen vacancies within this catalyst enhances the process of CO2 decomposition.

Cobalt‐Potassium Synergistic Modification Effects on Fe‐Based Catalysts for CO2 Hydrogenation to Low‐Carbon Olefins

ABSTRACTTo enhance the CO2 hydrogenation activity and low‐carbon olefin selectivity of Fe‐based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al2O3 catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H2‐TPR, XPS, CO2‐TPD, NH3‐TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO2 hydrogenation activity and low‐carbon olefin selectivity of Fe/Al2O3 catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron‐rich active metal centers in the catalyst, facilitating the adsorption and activation of CO2, while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low‐carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C2+ hydrocarbon products. Under the synergistic effect of K and Co, the CO2 conversion activity of the Fe‐based catalyst significantly increased, achieving a CO2 conversion rate of 37%, while the selectivity towards C2‐C4= increased to 31.9%.