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1.
ChemSusChem ; : e202401514, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39198215

RESUMEN

Silicon dioxide (SiO2) from rice husk can be extracted and be used as support for Ni-based catalysts. The impregnation method (IM) is usually used for preparing Ni/SiO2 catalysts, but its catalytic activity in CO2 hydrogenation to CH4 remains unsatisfactory. In this work, we explored alternative preparation methods, using ammonia evaporation method (AEM) and hydrothermal method (HM) to prepare the catalysts. The results showed that the catalysts prepared by AEM and HM were significantly superior to that prepared by IM. Notably, the catalyst synthesized by AEM from sustainable silica exhibited the best performance, achieving 81.69% CO2 conversion and over 99% methane selectivity at low reaction temperature of 300 °C. The characterization techniques indicate that the Ni/SiO2-AEM catalyst can form nickel phyllosilicate with lamellar structure, leading to better Ni dispersion and higher specific surface area. Furthermore, the results of in-situ DRIFTS have revealed the potential catalytic mechanism over Ni/SiO2 catalysts, indicating that it involves pathways with both the CO* and HCOO* as the key intermediates.

2.
ACS Appl Mater Interfaces ; 16(36): 47524-47534, 2024 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-39205406

RESUMEN

Efficiently converting atmospheric carbon dioxide (CO2) is crucial for sustainable human development. In this study, we conducted systematic in situ Fourier transform infrared tests to examine how hydrogen (H2) partial pressure affects the conversion of low-level CO2 (around 400 ppm) using nickel/titanium dioxide (Ni/TiO2). Results show that increasing H2 partial pressure significantly increases surface monodentate formate species, leading to enhanced methane (CH4) production at both 250 and 400 °C. Conversely, on Ni's surface, the key species are formyls and bidentate formate at 250 °C, but these decrease significantly at 400 °C. These findings indicate that low-level CO2 is more easily converted to CH4 over Ni/TiO2 than Ni, regardless of temperature. Additionally, the strong Ni-TiO2 interaction gives Ni/TiO2 an advantage in converting low CO2 concentrations, with excellent durability even at 400 °C. This study enhances our understanding of direct CO2 conversion and aids in the development of advanced CO2 emission reduction technologies.

3.
Bioresour Technol ; 408: 131223, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39111402

RESUMEN

This study investigated the effects of varying lipid ratios on the anaerobic co-digestion of high-lipid food waste (FW) in a mesophilic anaerobic membrane bioreactor (AnMBR). At a lipid concentration of 5 %, optimal biogas production (3.84 L/L/d) and lipid removal efficiency (78 %) were achieved; however, increasing lipid concentrations resulted in significant accumulations of long-chain fatty acids (LCFAs) and volatile fatty acids (VFAs). Batch tests further demonstrated the impact of various types of LCFAs, with stearic acid showing the slowest microbial growth rate (0.033d-1), confirming its role in the accumulation of acetate-dominated VFAs, potentially limiting the methanogenesis process at elevated lipid levels. Furthermore, at 8 % lipid content, the downregulation of key LCFA degradation enzymes and dominance of hydrogenotrophic methanogens indicated adverse conditions. The importance of the intricate interplay between LCFA degradation kinetics and microbial community for the system efficiency was evidenced, offering insights for optimizing and managing high-lipidic wastes.


Asunto(s)
Biodegradación Ambiental , Reactores Biológicos , Ácidos Grasos , Alimento Perdido y Desperdiciado , Membranas Artificiales , Anaerobiosis , Biocombustibles , Ácidos Grasos/metabolismo , Ácidos Grasos Volátiles/metabolismo , Cinética , Metabolismo de los Lípidos , Lípidos , Metano/metabolismo
4.
Chemistry ; : e202402516, 2024 Aug 21.
Artículo en Inglés | MEDLINE | ID: mdl-39168823

RESUMEN

On the way to carbon neutrality, directly catalyzing atmospheric CO2 into high-value chemicals might be an effective approach to mitigate the negative impacts of rising airborne CO2 concentrations. Here, we pioneer the investigation of the influence of the H2/CO2 partial pressure ratio (PPR) on air-level CO2 methanation. Using Ni/CeO2 as a case catalyst, increasing H2/CO2 PPR significantly improves low-temperature CO2 conversion and high-temperature CH4 selectivity, i.e., from 10 of H2/CO2 PPR on, CO2 is completely methanized at 250 °C, and nearly 100% CH4 selectivity is achieved at 400 °C. 100-hour stability tests demonstrate the practical application potential of Ni/CeO2 at 250 °C and 400 °C. In-situ DRIFTS reveal that reinforced formate pathway by increasing H2/CO2 PPR is responsible for the high CH4 yield. In contrast, even though the CO pathway dominated CO2 conversion on Ni is enhanced by rising H2/CO2 PPR, but at a high reaction temperature, the promoted CO desorption still leads to lower CH4 selectivity. This work offers deep insights into the direct air-level CO2 resourceization, contributing to the achievement of airborne CO2 reductions.

5.
Chemistry ; : e202402102, 2024 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-39087665

RESUMEN

In photocatalysis, the resulted heat by the relaxation of most of incident light no longer acts as the industrially favorite driving force back to the target photo-reaction due to more or less the negative relation between photocatalytic efficiency and temperature. Here, we reported a visible light-sensitized protocol that completely reversed the negatively temperature-dependent efficiency in photo-driven CO2 methanation with saturated water vapor. Uniform Pt/N-TiO2/PDI self-assembly material decisively injects the excited electron of PDI sensitizer into N-TiO2 forming Ti-H hydride which is crucially temperature-dependent nucleophilic species to dominate CO2 methanation, rather than conventionally separated and trapped electrons on the conductor band. Meanwhile, the ternary composite lifts itself temperature from room temperature to 305.2 °C within 400s only by the failure excitation upon simulated sunlight of 2.5 W/cm2, and smoothly achieves CO2 methanation with a record number of 4.98 mmol g-1 h-1 rate, compared to less than 0.02 mmol g-1 h-1 at classic Pt/N-TiO2/UV photocatalysis without PDI sensitization. This approach can reuse ~53.9% of the relaxed heat energy from the incident light thereby allow high-intensity incident light as strong as possible within a flowing photo-reactor, opening the most likely gateways to industrialization.

6.
ChemSusChem ; : e202400779, 2024 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-38958605

RESUMEN

Biogas offers significant benefits as a renewable energy source, contributing to decarbonization, waste management, and economic development. This comprehensive review examines the historical, technological, economic, and global aspects of biomethane production, focusing on the key players such as China, the European Union, and North America, and associated opportunities and challenges as well as future prospects from an Australia perspective. The review begins with an introduction to biogas, detailing its composition, feedstock sources, historical development, and anaerobic digestion (AD) process. Subsequently, it delves into major biomethane production technologies, including physicochemical absorption, high-pressure water scrubbing (HPWS), amine scrubbing (AS), pressure swing adsorption (PSA), membrane permeation/separation (MP), and other technologies including organic solvent scrubbing and cryogenic separation. The study also discusses general guidelines of techno-economic assessments (TEAs) regarding biomethane production, outlining the methodologies, inventory analysis, environmental life cycle assessment (LCA), and estimated production costs. Challenges and opportunities of biogas utilization in Australia are explored, highlighting and referencing global projections, polarization in production approaches, circularity in waste management, and specific considerations for Australia. The review concludes discussing future perspectives for biomethane, emphasizing the importance of technological advancements, policy support, and investment in realizing its full potential for sustainable energy and waste management solutions.

7.
Adv Sci (Weinh) ; : e2406828, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38984724

RESUMEN

Photothermal CO2 methanation reaction represents a promising strategy for addressing CO2-related environmental issues. The presence of efficient tandem catalytic sites with a localized high-temperature is an effective pathway to enhance the performance of CO2 methanation. Here the bimetallic RuCo nanoparticles anchored on ZrO2 fiber cotton (RuCo/ZrO2) as a photothermal catalyst for CO2 methanation are prepared. A significant photothermal CO2 methanation performance with optimal CH4 selectivity (99%) and rate (169.93 mmol gcat -1 h-1) is achieved. The photothermal energy of the RuCo bimetallic nanoparticles, confined by the infrared insulation and low thermal conductivity of the ZrO2 fiber cotton (ZrO2 FC), provides a localized high-temperature. In situ spectroscopic experiments on RuCo/ZrO2, Ru/ZrO2, and Co/ZrO2 indicate that the construction of tandem catalytic sites, where the Co site favors CO2 conversion to CO while incorporating Ru enhances CO* adsorption for subsequent hydrogenation, results in a higher selectivity toward CH4. This work opens a new insight into designing tandem catalysts with a photothermal confinement effect in CO2 methanation reaction.

8.
Molecules ; 29(14)2024 Jul 13.
Artículo en Inglés | MEDLINE | ID: mdl-39064888

RESUMEN

CO-selective methanation (CO-SMET) is an efficient hydrogen-rich (H2-rich) gas purification technology for proton exchange membrane fuel cells. It is vital to develop suitable catalysts with good low-temperature activity for CO-SMET reactions. In this study, RuNi/TiZrx-mixed metal oxide (RuNi/TiZrx-MMO) catalysts with different molar ratios of Zr/Ti, derived from a Zr-promoted NiTi-layered double hydroxide (NiTi-LDH) precursor were successfully prepared using the co-precipitation and wet impregnation methods. The RuNi/TiZr0.2-MMO catalyst possesses higher catalytic performance in a lower temperature window of 180-280 °C, which can reduce the CO concentration to be below 10 ppm. The characterization results obtained from XRD, BET, SEM, TEM, XPS, TPR, and TPD suggest that the addition of ZrO2 increases the surface area of the catalyst, improves the dispersion of metallic nanoparticles, increases the reducibility of Ni species on the RuNi/TiZr0.2-MMO catalyst's surface, and enhances the adsorption and activation ability of CO, resulting in remarkable catalytic performance at lower reaction temperatures. Moreover, the RuNi/TiZr0.2-MMO catalyst demonstrated long-term catalytic stability and carbon resistance.

9.
ChemSusChem ; : e202400478, 2024 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-38923202

RESUMEN

Catalytic conversion of carbon dioxide (CO2) into value-added chemicals is of pivotal importance, well the cost of capturing CO2 from dilute atmosphere is super challenge. One promising strategy is combining the adsorption and transformation at one step, such as applying alkali solution that could selectively reduce carbonate (CO3 2-) as consequences of CO2 adsorption. Due to complexity of this system, the mechanistic details on controlling the hydrogenation have not been investigated in depth. Herein, Ru/TiO2 catalyst was applied as a probe to elucidate the mechanism of CO3 2- activation, in which with thermodynamic and kinetic investigations, a compact Langmuir-Hinshelwood reaction model was established which suggests that the overall rate of CO3 2- hydrogenation was controlled by a specific C-O bond rupture elementary step within HCOO- and the Ru surface was mainly covered by CO3 2- or HCOO- at independent conditions. This assumption was further supported by negligible kinetic isotope effects (kH/kD≈1), similarity on reaction barriers of CO3 2- and HCOO- hydrogenation (ΔH≠ hydr,Na2CO3 and ΔH≠ hydr,HCOONa) and a non-variation of entropy (ΔS≠ hydr≈0). More interestingly, the alkalinity of the solution is certainly like a two sides in a sword and could facilitate the adsorption of CO2 while hold back catalysis during CO3 2- hydrogenation.

10.
ACS Appl Mater Interfaces ; 16(27): 34936-34946, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38922846

RESUMEN

Ni-based oxides are promising catalysts for CO2 methanation. However, Ni-based catalysts also have some unresolved issues and drawbacks in practical applications. The activity and selectivity of Ni-based catalysts in CO2 methanation at low temperatures still need to be improved. Here, Ni/ZrO2 nanofibers with high surface areas (up to 101.2 m2/g) were prepared by electrospinning methods. The Ni/ZrO2-ES (also named as 66Ni/ZrO2) catalyst showed excellent catalytic performance in CO2 methanation (the CO2 conversion = 81% and CH4 selectivity = 99% at 350 °C) and excellent stability for 100 h, which was better than most reported Ni/ZrO2 catalysts. However, the comparison sample Ni/ZrO2-CP prepared by the coprecipitation method had poor catalytic performance (the CO2 conversion = 54% and CH4 selectivity = 90% at 350 °C). Within 100 h, the CO2 conversion decreased to 30% and the CH4 selectivity decreased to 52%. Both EPR and O1S XPS confirmed that Ni/ZrO2 nanofibers can form more reactive oxygen species vacancies, and CO2-TPD confirmed that nanofibers had more CO2 adsorption sites compared with the control sample Ni/ZrO2-CP. In situ DRIFTS analysis showed that bidentate carbonate and monodentate carbonate were key intermediates in CO2 methanation. The catalytic performance of Ni/ZrO2 nanofiber catalysts would be attributed to higher dispersion of Ni species on the surface of nanofibers, high specific surface area (101.2 m2/g), more oxygen vacancies, more CO2 adsorption sites, and the synergistic effect between Ni nanoparticles and ZrO2 nanofibers. This work may inspire the rational design of Ni/ZrO2 nanofiber catalysts with rich oxygen vacancies for low-temperature CO2 methanation.

11.
Bioresour Technol ; 406: 130981, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38879053

RESUMEN

Biological H2-assisted biogas upgrading has gained significant attention as an environmentally friendly substitute to common physico-chemical upgrading techniques, but is largely limited by the low solubility of H2. This study evaluated the design of a ceramic membrane contactor module for H2 injection. H2 dissolution was maintained at high efficiency by controlling gas supply and sludge recirculation rate, achieving a biogas quality of average 98.8% CH4 during the stable operation phase with a 108% increase in the CH4 production rate. This also outperforms conventional H2 injection using diffuser sparging which could only achieve a biogas quality of 84% CH4 content. Microbial community analysis found high Methanobacterium spp. abundance within the archaea at 95.2% at the end of the operation, allowing the dominance of the hydrogenotrophic methanogenesis pathway for high upgrading efficiencies. The system is a high-performance external membrane connector module coupled to common anaerobic digestion systems for biogas upgrading.


Asunto(s)
Biocombustibles , Cerámica , Hidrógeno , Membranas Artificiales , Metano , Cerámica/química , Metano/metabolismo , Hidrógeno/metabolismo , Reactores Biológicos , Aguas del Alcantarillado/microbiología , Anaerobiosis
12.
Front Microbiol ; 15: 1392410, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38725680

RESUMEN

H2 produced from renewable energies will play a central role in both greenhouse gas reduction and decarbonization by 2050. Nonetheless, to improve H2 diffusion and utilization as a fuel, large storage capacity systems are needed. Underground storage of natural gas in depleted reservoirs, aquifers and salt caverns is a well-established technology. However, new challenges arise when it comes to storing hydrogen due to the occurrence and activity of indigenous microbial populations in deep geological formations. In a previous study, four Italian natural gas reservoirs were characterized both from a hydro-chemical and microbiological point of view, and predictive functional analyses were carried out with the perspective of underground hydrogen storage (UHS). In the present work, formation waters from the same reservoirs were used as inoculant during batch cultivation tests to characterize microbial activity and its effects on different gas mixtures. Results evidence a predominant acidogenic/acetogenic activity, whilst methanogenic and sulfate reducing activity were only marginal for all tested inoculants. Furthermore, the microbial activation of tested samples is strongly influenced by nutrient availability. Obtained results were fitted and screened in a computational model which would allow deep insights in the study of microbial activity in the context of UHS.

13.
Biotechnol Biofuels Bioprod ; 17(1): 66, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38750538

RESUMEN

BACKGROUND: Power-to-gas is the pivotal link between electricity and gas infrastructure, enabling the broader integration of renewable energy. Yet, enhancements are necessary for its full potential. In the biomethanation process, transferring H2 into the liquid phase is a rate-limiting step. To address this, we developed a novel tubular foam-bed reactor (TFBR) and investigated its performance at laboratory scale. RESULTS: A non-ionic polymeric surfactant (Pluronic® F-68) at 1.5% w/v was added to the TFBR's culture medium to generate a stabilized liquid foam structure. This increased both the gas-liquid surface area and the bubble retention time. Within the tubing, cells predominantly traveled evenly suspended in the liquid phase or were entrapped in the thin liquid film of bubbles flowing inside the tube. Phase (I) of the experiment focused primarily on mesophilic (40 °C) operation of the tubular reactor, followed by phase (II), when Pluronic® F-68 was added. In phase (II), the TFBR exhibited 6.5-fold increase in biomethane production rate (MPR) to 15.1 ( L CH 4 /L R /d) , with a CH4 concentration exceeding 90% (grid quality), suggesting improved H2 transfer. Transitioning to phase (III) with continuous operation at 55 °C, the MPR reached 29.7 L CH 4 /L R /d while maintaining the grid quality CH4. Despite, reduced gas-liquid solubility and gas-liquid mass transfer at higher temperatures, the twofold increase in MPR compared to phase (II) might be attributed to other factors, i.e., higher metabolic activity of the methanogenic archaea. To assess process robustness for phase (II) conditions, a partial H2 feeding regime (12 h 100% and 12 h 10% of the nominal feeding rate) was implemented. Results demonstrated a resilient MPR of approximately 14.8 L CH 4 /L R /d even with intermittent, low H2 concentration. CONCLUSIONS: Overall, the TFBR's performance plant sets the course for an accelerated introduction of biomethanation technology for the storage of volatile renewable energy. Robust process performance, even under H2 starvation, underscores its reliability. Further steps towards an optimum operation regime and scale-up should be initiated. Additionally, the use of TFBR systems should be considered for biotechnological processes in which gas-liquid mass transfer is a limiting factor for achieving higher reaction rates.

14.
Sci Rep ; 14(1): 12282, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38811763

RESUMEN

To improve the utilization of byproduct gases in the steel plant, the coke oven gas (COG) methanation combined with blast furnace gas (BFG) and basic oxygen furnace gas (BOFG) was proposed in viewpoint of economy and environment. The optimization mathematics model based on Gibbs free energy minimization was established to predict the thermodynamic feasibility of the proposed methanation. To solve the proposed model, the convenient method was implemented by using the Gibbs module in Aspen Plus software. Effects of operation parameters on the methanation performance were revealed to identify the optimized conditions. To reduce the solid carbon concentration, it was found that the optimized conditions of temperature, pressure and stoichiometric number were 650 °C, 30 bar and 3.0, respectively. Moreover, it was discovered that 10 mol% of BFG or BOFG could be mixed into COG to obtain the maximum methane yield. In addition, it was testified that there were the good agreements between calculated results and industrial and published data, which indicated that the proposed methanation was thermodynamically feasible. Therefore, the simple and easy method was developed to evaluate the methanation operating conditions from the aspect of thermodynamic equilibrium, which provided the basic process conditions of byproduct gases methanation to enhance the steel plant efficiency and reduce carbon emissions.

15.
Environ Res ; 256: 119230, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-38810832

RESUMEN

The conversion of carbon dioxide (CO2) to methane (CH4) is a strategy for sequestering CO2. Zero-valent iron (ZVI) has been proposed as an alternative electron donor for the CO2 reduction to CH4. In this study, the effects of ZVI concentrations on the abiotic production of H2 (without the action of microorganisms) in the first part and on the biological conversion of CO2 to CH4 using ZVI as a direct electron donor in the second part were examined. In the abiotic H2 production, the increase in the ZVI concentration from 16 to 32, 64, and 96 g/L was found to have positive effects on both the amounts of H2 generated and the rates of H2 production because the extent of ZVI oxidation positively correlates with increasing surface area. Nevertheless, the increase in ZVI concentration from 96 to 224 g/L did not benefit the H2 production because the ZVI dissolution was suppressed by the increasing aqueous pH above 10. In the bioconversion of CO2 to CH4 using ZVI as an electron donor, the main methanogenesis pathway occurred via hydrogenotrophic methanogenesis at pH 8.7-9.5 driven by the genus Methanobacterium of the class Methanobacteria. At ZVI concentrations of 64 g/L and above, the production of volatile fatty acid (VFA) became clear. Acetate was the main VFA, indicating the induction of homoacetogenesis at ZVI concentrations of 64 g/L and above. In addition, the presence of propionate as the second major VFA suggests the production of propionate from CO2 and acetate under conditions with high H2 partial pressure. The results indicated that the pathway for ZVI/CO2 conversion to CH4 was competitive between hydrogenotrophic methanogenesis and homoacetogenesis.


Asunto(s)
Dióxido de Carbono , Hidrógeno , Hierro , Metano , Metano/metabolismo , Dióxido de Carbono/metabolismo , Anaerobiosis , Hierro/metabolismo , Hidrógeno/metabolismo
16.
Environ Res ; 255: 119203, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38782347

RESUMEN

The hydrogenation of CO2 to CH4 has gained considerable interest in terms of sustainable energy and environmental mitigation. In this regard, the present work aims to investigate the adsorptive concentration and CO2 methanation performance over CoFe and NiFe bimetallic catalysts supported on fumed alumina-silica SA96 support at 170-450 °C and under atmospheric pressure. The catalysts were prepared by wet impregnation method, subjected to calcination and further reduced with hydrogen, and their performance in CO2 methanation was investigated in a hydrogen-rich 2%CO2-55%H2-43%He gas mixture. In this study, we describe the crystal and mesoporous structures of the prepared catalysts by in-situ XRD and ex-situ nitrogen adsorption, evaluate the NiFe and CoFe metal surface states before and after catalysis by XPS, visualize the surface morphology by SEM, estimate the catalytic activity by gas chromatography, and investigate the adsorbed surface species, showing the presence of *HCOO/*HCO and *CO intermediates, determine two possible pathways of CH4 formation on the studied catalysts by temperature-programmed desorption mass spectrometry, and correlate the structural and surface properties with high CO2 conversions up to 100% and methanation selectivities up to 72%. The latter is related to changes in the elemental chemical states and surface composition of CoFe and NiFe nanocatalysts induced by treatment under reaction conditions, and the surface reconstruction during catalysis transfers the part of active 3d transition metals into the pores of the SA96 support. Our thorough characterization study with complementary techniques allowed us to conclude that this high activity is related to the formation of catalytically active Ni/Ni3Fe and Co/CoFeOx nanoscale crystallites under H2 reduction and their maintenance under CO2 methanation conditions. The successfully applied combination of CO2 chemisorption and thermodesorption techniques demonstrates the ability to adsorb the CO2 molecules by supported NiFe and CoFe nanocatalysts and the pure alumina-silica SA96 support.


Asunto(s)
Óxido de Aluminio , Dióxido de Carbono , Cobalto , Metano , Níquel , Dióxido de Silicio , Propiedades de Superficie , Óxido de Aluminio/química , Catálisis , Dióxido de Carbono/química , Metano/química , Níquel/química , Cobalto/química , Dióxido de Silicio/química , Hierro/química , Adsorción
17.
Appl Environ Microbiol ; 90(5): e0026824, 2024 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-38619268

RESUMEN

A new variant of Methanothermobacter wolfeii was isolated from an anaerobic digester using enrichment cultivation in anaerobic conditions. The new isolate was taxonomically identified via 16S rRNA gene sequencing and tagged as M. wolfeii BSEL. The whole genome of the new variant was sequenced and de novo assembled. Genomic variations between the BSEL strain and the type strain were discovered, suggesting evolutionary adaptations of the BSEL strain that conferred advantages while growing under a low concentration of nutrients. M. wolfeii BSEL displayed the highest specific growth rate ever reported for the wolfeii species (0.27 ± 0.03 h-1) using carbon dioxide (CO2) as unique carbon source and hydrogen (H2) as electron donor. M. wolfeii BSEL grew at this rate in an environment with ammonium (NH4+) as sole nitrogen source. The minerals content required to cultivate the BSEL strain was relatively low and resembled the ionic background of tap water without mineral supplements. Optimum growth rate for the new isolate was observed at 64°C and pH 8.3. In this work, it was shown that wastewater from a wastewater treatment facility can be used as a low-cost alternative medium to cultivate M. wolfeii BSEL. Continuous gas fermentation fed with a synthetic biogas mimic along with H2 in a bubble column bioreactor using M. wolfeii BSEL as biocatalyst resulted in a CO2 conversion efficiency of 97% and a final methane (CH4) titer of 98.5%v, demonstrating the ability of the new strain for upgrading biogas to renewable natural gas.IMPORTANCEAs a methanogenic archaeon, Methanothermobacter wolfeii uses CO2 as electron acceptor, producing CH4 as final product. The metabolism of M. wolfeii can be harnessed to capture CO2 from industrial emissions, besides producing a drop-in renewable biofuel to substitute fossil natural gas. If used as biocatalyst in new-generation CO2 sequestration processes, M. wolfeii has the potential to accelerate the decarbonization of the energy generation sector, which is the biggest contributor of CO2 emissions worldwide. Nonetheless, the development of CO2 sequestration archaeal-based biotechnology is still limited by an uncertainty in the requirements to cultivate methanogenic archaea and the unknown longevity of archaeal cultures. In this study, we report the adaptation, isolation, and phenotypic characterization of a novel variant of M. wolfeii, which is capable of maximum growth with minimal nutrients input. Our findings demonstrate the potential of this variant for the production of renewable natural gas, paving the way for the development of more efficient and sustainable CO2 sequestration processes.


Asunto(s)
Dióxido de Carbono , Methanobacteriaceae , Methanobacteriaceae/genética , Methanobacteriaceae/metabolismo , Methanobacteriaceae/crecimiento & desarrollo , Dióxido de Carbono/metabolismo , ARN Ribosómico 16S/genética , Genoma Arqueal , Filogenia , Fenotipo , Aguas Residuales/microbiología , Metano/metabolismo , Nutrientes/metabolismo
18.
ACS Nano ; 18(17): 11449-11461, 2024 Apr 30.
Artículo en Inglés | MEDLINE | ID: mdl-38644575

RESUMEN

Bimetallic alloy nanoparticles have garnered substantial attention for diverse catalytic applications owing to their abundant active sites and tunable electronic structures, whereas the synthesis of ultrafine alloy nanoparticles with atomic-level homogeneity for bulk-state immiscible couples remains a formidable challenge. Herein, we present the synthesis of RuxCo1-x solid-solution alloy nanoparticles (ca. 2 nm) across the entire composition range, for highly efficient, durable, and selective CO2 hydrogenation to CH4 under mild conditions. Notably, Ru0.88Co0.12/TiO2 and Ru0.74Co0.26/TiO2 catalysts, with 12 and 26 atom % of Ru being substituted by Co, exhibit enhanced catalytic activity compared with the monometallic Ru/TiO2 counterparts both in dark and under light irradiation. The comprehensive experimental investigations and density functional theory calculations unveil that the electronic state of Ru is subtly modulated owing to the intimate interaction between Ru and Co in the alloy nanoparticles, and this effect results in the decline in the CO2 conversion energy barrier, thus ultimately culminating in an elevated catalytic performance relative to monometallic Ru and Co catalysts. In the photopromoted thermocatalytic process, the photoinduced charge carriers and localized photothermal effect play a pivotal role in facilitating the chemical reaction process, which accounts for the further boosted CO2 methanation performance.

19.
Small ; 20(32): e2400700, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38488718

RESUMEN

Solar-driven carbon dioxide (CO2) methanation holds significant research value in the context of carbon emission reduction and energy crisis. However, this eight-electron catalytic reaction presents substantial challenges in catalytic activity and selectivity. In this regard, researchers have conducted extensive exploration and achieved significant developments. This review provides an overview of the recent advances and challenges in efficient selective photocatalytic CO2 methanation. It begins by discussing the fundamental principles and challenges in detail, analyzing strategies for improving the efficiency of photocatalytic CO2 conversion to CH4 comprehensively. Subsequently, it outlines the recent applications and advanced characterization methods for photocatalytic CO2 methanation. Finally, this review highlights the prospects and opportunities in this area, aiming to inspire CO2 conversion into high-value CH4 and shed light on the research of catalytic mechanisms.

20.
Chemphyschem ; 25(10): e202301002, 2024 May 17.
Artículo en Inglés | MEDLINE | ID: mdl-38443312

RESUMEN

By combining the advantages of dielectric barrier discharge (DBD) low temperature plasma and fluidized bed, the effect of plasma on the performance of supported Mo-based catalyst was studied in this paper. The performance of the catalyst obtained by plasma treatment, calcined, plasma+calcined was compared, and the appropriate catalyst preparation scheme was explored. Comparing with the three catalysts, it was concluded that the catalyst average conversion after 30 W plasma treatment is 33.40 %, which was 8.94 % and 12.75 % higher than the other two, respectively. The structure and properties of the catalyst were characterized by N2-Physisorption, H2-chemisorption, XRD, TEM, XPS, Raman and NO-pulse adsorption. Then, by analyzing the characterization results, it can be seen that plasma can make the catalyst have a higher specific surface area and a more dispersed active metal with smaller grain size. Through the surface species identification characterization, it was found that plasma can produce more defective structures and expose more active sites, which is the main reason for the difference in conversion.

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