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1.
Proc Natl Acad Sci U S A ; 120(9): e2217081120, 2023 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-36812199

RESUMO

Carbon capture is one of the essential low-carbon technologies required to achieve societal climate goals at the lowest cost. Covalent organic frameworks (COFs) are promising adsorbents for CO2 capture because of their well-defined porosity, large surface area, and high stability. Current COF-based CO2 capture is mainly based on a physisorption mechanism, exhibiting smooth and reversible sorption isotherms. In the present study, we report unusual CO2 sorption isotherms featuring one or more tunable hysteresis steps with metal ion (Fe3+, Cr3+, or In3+)-doped Schiff-base two-dimensional (2D) COFs (Py-1P, Py-TT, and Py-Py) as adsorbents. Synchrotron X-ray diffraction, spectroscopic and computational studies indicate that the sharp adsorption steps in the isotherm originate from the insertion of CO2 between the metal ion and the N atom of the imine bond on the inner pore surface of the COFs as the CO2 pressure reaches threshold values. As a result, the CO2 adsorption capacity of the ion-doped Py-1P COF is increased by 89.5% compared with that of the undoped Py-1P COF. This CO2 sorption mechanism provides an efficient and straightforward approach to enhancing the CO2 capture capacity of COF-based adsorbents, yielding insights into developing chemistry for CO2 capture and conversion.

2.
Small ; : e2402529, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38767079

RESUMO

Unlocking CO2 capture potential remains a complex and challenging endeavor. Here, a blueprint is crafted for optimizing materials through CO2 capture and developing a synergistic hybridization strategy that involves synthesizing CO2-responsive hydrogels by integrating polymeric networks interpenetrated with polyethyleneimine (PEI) chains and inorganic CaCl2. Diverging from conventional CO2 absorbents, which typically serve a singular function in CO2 capture, these hybrid PEAC hydrogels additionally harness its presence to tune their optical and mechanical properties once interacting with CO2. Such synergistic functions entail two significant steps: (i) rapid CO2-fixing through PEI chains to generate abundant carbamic acid and carbamate species and (ii) mineralization via CaCl2 to induce the formation of CaCO3 micro-crystals within the hydrogel matrix. Due to the reversible bonding, the PEAC hydrogels enable the decoupling of CO2 through an acid fumigation treatment or a heating process, achieving dynamic CO2 capture-release cycles up to 8 times. Furthermore, the polyethyleneimine-acrylamide-calcium chloride (PEAC) hydrogel exhibits varying antibacterial attributes and high interfacial adhesive strength, which can be modulated by fine-tuning the compositions of PEI and CaCl2. This versatility underscores the promising potential of PEAC hydrogels, which not only unlocks CO2 capture capabilities but also offers opportunities in diverse biological and biomedical applications.

3.
Small ; 20(5): e2305533, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37786306

RESUMO

CO2 capture and conversion technology are highly promising technologies that definitely play a part in the journey towards carbon neutrality. Releasing CO2 by mild stimulation and the development of high efficiency catalytic processes are urgently needed. The magnetic field, as a thermodynamic parameter independent of temperature and pressure, is vital in the enhancement of CO2 capture and conversion process. In this review, the recent progress of magnetic field-enhanced CO2 capture and conversion is comprehensively summarized. The theoretical fundamentals of magnetic field on CO2 adsorption, release and catalytic reduction process are discussed, including the magnetothermal, magnetohydrodynamic, spin selection, Lorentz forces, magnetoresistance and spin relaxation effects. Additionally, a thorough review of the current progress of the enhancement strategies of magnetic field coupled with a variety of fields (including thermal, electricity, and light) is summarized in the aspect of CO2 related process. Finally, the challenges and prospects associated with the utilization of magnetic field-assisted techniques in the construction of CO2 capture and conversion systems are proposed. This review offers a reference value for the future design of catalysts, mechanistic investigations, and practical implementation for magnetic field enhanced CO2 capture and conversion.

4.
Small ; : e2401422, 2024 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-39118560

RESUMO

Silica-supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO2 uptake in amine-based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane-treated Santa Barbara Amorphous-15 (SBA-15) supports and the corresponding enhancement in CO2 uptake compared to various SBA-15-based control supports are presented. The relationship between CO2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO2 and H2O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1H T1-T2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA-15-supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface.

5.
Small ; : e2406165, 2024 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-39126365

RESUMO

The calcium looping technology employing CaO-based sorbents is pivotal for capturing CO2 from flue gas. However, the intrinsic low thermodynamic stability of CaO-based sorbents and the requisite molding step induce severe sintering issues, diminishing their cyclic stability. Herein, a high-entropy fluorite oxide (HEFO) inert stabilizer premised on entropy stabilization and synergistic effect strategies is introduced. HEFO-modified, CaO-based sorbent pellets are synthesized via a rapid cigarette butt-assisted combustion process (15 min) combined with the graphite molding method. Post-multiple cycles, their CO2 capture capacity reaches 0.373 g g-1, which is 2.6-fold superior to that of pure CaO, demonstrating markedly enhanced anti-sintering properties. First, the subtle morphological and crystallographic modifications suggest that the inherent entropy stability of HEFO imparts robust thermal resistance. Concurrently, the disordered structure of single-phase HEFO exhibits a high affinity for CaO, resulting in an interface binding energy of -1.83 eV, in sharp contrast to the -0.112 eV of pure CaO, thereby restricting CaO migration. Additionally, the multi-element synergistic effect of HEFO reduces the energy barrier by 0.15 eV, leading to a 40% and 140% increase in carbonation and calcination rates, respectively. This work presents highly efficient and rapidly synthesized CaO-based sorbent pellets, showcasing promising potential for industrial application.

6.
Small ; : e2401156, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38686695

RESUMO

In this work, a new type of multifunctional materials (MFMs) called self-regenerative Ni-doped CaTiO3/CaO is introduced for the integrated CO2 capture and dry reforming of methane (ICCDRM). These materials consist of a catalytically active Ni-doped CaTiO3 and a CO2 sorbent, CaO. The article proposes a concept where the Ni catalyst can be regenerated in situ, which is crucial for ICCDRM. Exsolved Ni nanoparticles are evenly distributed on the surface of CaTiO3 under H2 or CH4, and are re-dispersed back into the CaTiO3 lattice under CO2. The Ni-doped CaTiO3/CaO MFMs show stable CO2 capture capacity and syngas productivity for 30 cycles of ICCDRM. The presence of CaTiO3 between CaO grains prevents CaO/CaCO3 thermal sintering during carbonation and decarbonation. Moreover, the strong interaction of CaTiO3 with exsolved Ni mitigates severe accumulation of coke deposition. This concept can be useful for developing MFMs with improved properties that can advance integrated carbon capture and conversion.

7.
Appl Environ Microbiol ; 90(5): e0026824, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38619268

RESUMO

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.


Assuntos
Dióxido de Carbono , Methanobacteriaceae , Methanobacteriaceae/genética , Methanobacteriaceae/metabolismo , Methanobacteriaceae/crescimento & desenvolvimento , Dióxido de Carbono/metabolismo , RNA Ribossômico 16S/genética , Genoma Arqueal , Filogenia , Fenótipo , Águas Residuárias/microbiologia , Metano/metabolismo , Nutrientes/metabolismo
8.
Chemistry ; : e202400874, 2024 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-38853144

RESUMO

MXenes, a class of two-dimensional transition metal carbides, nitrides, and carbonitrides, have garnered significant attention due to their remarkable potential for energy storage, electrocatalysis, and gas separation applications. The fabrication processes of MXene involve building up the MXene structure from constituent elements and the selective elimination of M-A bonds from the precursor MAX. However, considerable efforts are still required to design and develop efficient MXene-based technologies. This review article aims to briefly analyse the synthesis methods employed for MXene production, ranging from direct synthesis and conventional chemical wet etching approach to the more recent molten salt etching technique. The review highlights the advancements made in achieving precise control over the terminal groups, which is paramount for tailoring the properties of MXenes for specific applications. Furthermore, the potential of MXene-based materials for carbon capture applications, particularly in developing advanced adsorbents, is emphasized. The in-depth examination of MXene synthesis techniques and their implications for carbon capture applications provides a solid foundation for developing and optimizing these promising materials.

9.
Chemistry ; : e202402437, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39110634

RESUMO

Two water-stable indium metal-organic frameworks, (NH2Me2)3[In3(BTB)4]·12DMA·4.5H2O (In-MOF-1) and (NH2Me2)9[In9O6(BTB)8(H2O)4(DMSO)4]·27DMSO·21H2O (In-MOF-2) (BTB = 4,4¢,4¢¢-benzene-1,3,5-tribenzoate) with 3D interpenetrate structure has been constructed by regulating solvents. Structure analysis revealed that In-MOF-1 has a three-dimensional (3D) structure with a single metal core, while In-MOF-2 features an octahedron cage constructed by three kinds of metal clusters to further form a 3D structure. The fluorescence investigations show that In-MOF-1 and In-MOF-2 are potential MOF-based fluorescent sensors to detect acetone and Fe3+ ions in EtOH or water with high sensitivity, excellent selectivity, recyclability and a low detection limit. Moreover, the fluorescence mechanisms of In-MOF-1 and In-MOF-2 toward acetone and Fe3+ ions were further explained. In addition, In-MOF-2 has higher thermal and framework stability than In-MOF-1. The activated In-MOF-2 presents a high BET surface area of 998.82 m2g-1 and a pore size distribution of 8 to 16 Å. At the same time, In-MOF-2 exhibits high selective CO2 adsorption for CO2/CH4 and CO2/N2, respectively. Furthermore, the adsorption sites and adsorption isotherms were predicted using Grand Canonical Monte Carlo (GCMC) simulations, and the adsorption energy of the lowest-energy adsorption configuration was calculated using molecular dynamics (MD) simulations.

10.
Chemphyschem ; 25(16): e202400324, 2024 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-38728169

RESUMO

In this study, we elucidate the reaction mechanism for capturing CO2 with the ZnL1(MeOH) complex (L1=diacetyl-2-(4-methyl-3-thiosemicarbazone)-3-(2-hydrazinatopyridine)) in a methanol solution, using density functional theory calculations. One pathway involves the protonation of ZnL1(MeOH) by methylcarbonic acid, followed by ligand exchange of MeOH with MeOCO2 -. An alternative mechanism suggests a tautomerization between ZnL1(MeOH) and Zn(HL1)(OMe), followed by CO2 insertion. The latter pathway is energetically more favorable than the former and more complex than initially proposed. In fact, we unveiled that the solvent catalyzes tautomerization, as one explicit methanol molecule acts as a proton transfer agent. Then, Zn(HL1)(OMe) captures CO2, yielding a methylcarbonate bound to the metal center. The final step involves a rearrangement that leads to the cleavage of the Zn-O(Me)(COO) bond and the formation of a new Zn-O(COOMe) bond, along with the rotation of the methylcarbonate group. We consider an additional mechanism that combines tautomerization and ligand exchange but is endergonic and requires a high activation barrier for the ligand exchange. Furthermore, we evaluate the ligand basicity through the pKa calculated values of the Zn(II) complexes, the effects of varying the ligand from 4-methyl-thiosemicarbazone to 4-ethyl (L2), 4-phenethyl (L3), and 4-benzyl (L4) derivatives, and reversibility of the reaction in an argon environment.

11.
Environ Sci Technol ; 58(23): 10052-10059, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38818669

RESUMO

The excessive energy consumed restricts the application of traditional postcombustion CO2 capture technology and limits the achievement of carbon-neutrality goals. Catalytic-rich CO2 amine regeneration has the potential to accelerate proton transfer and increase the energy efficiency in the CO2 separation process. Herein, we reported a Ce-metal-organic framework (MOF)-derived composite catalyst named HZ-Ni@UiO-66 with a hierarchical structure, which can increase the CO2 desorbed amount by 57.7% and decrease the relative heat duty by 36.5% in comparison with the noncatalytic monoethanolamine (MEA) regeneration process. The composite catalyst of the CeO2 coating from the UiO-66 precursor on the HZ-Ni carrier shows excellent stability with a long lifespan. The HZ-Ni@UiO-66 catalyst also shows a universal catalytic effect in typical blended amine systems with a large cyclic capacity. The HZ-Ni@UiO-66 catalyst effectively decreases the energy barrier of the CO2 desorption reaction to reduce the time required to reach thermodynamics, consequently saving the energy consumption generated by water evaporation. This research provides a new avenue for advancing amine regeneration with less heat duty at low temperatures.


Assuntos
Aminas , Dióxido de Carbono , Cério , Dióxido de Carbono/química , Cério/química , Catálise , Aminas/química , Estruturas Metalorgânicas/química
12.
Environ Sci Technol ; 58(16): 6978-6987, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38598712

RESUMO

Decarbonization of the cement sector is essentially required to achieve carbon neutrality to combat climate change. Amine-based CO2 capture is a leading and practical technology to deeply remove CO2 from the cement industry, owing to its high retrofittability to existing cement plants and extensive engineering experience in industrial flue gas decarbonization. While research efforts have been made to achieve low-carbon cement with 90% CO2 removal, a net-zero-emission cement plant that will be required for a carbon neutrality society has not yet been investigated. The present study proposed an advanced amine-based CO2 capture system integrated with a cement plant to achieve net-zero CO2 emission by pushing the CO2 capture efficiency to 99.7%. Monoethanomaine (MEA) and piperazine/2-amino-2-methyl-1-propanol (PZ-AMP) amine systems, which are considered to be the first- and second-generation capture agents, respectively, were detailed investigated to deeply decarbonize the cement plant. Compared to MEA, the advanced PZ-AMP system exhibited excellent energy performance with a regeneration duty of ∼2.6 GJ/tonne CO2 at 99.7% capture, 39% lower than the MEA process. This enabled a low CO2 avoided cost of $72.0/tonne CO2, which was 18% lower than that of the MEA-based zero-emission process and even 16.2% lower than the standard 90% MEA process. Sensitivity analysis revealed that the zero-emission capture cost of the PZ-AMP system would be further reduced to below $56/tonne CO2 at a $4/GJ steam production cost, indicating its economic competitiveness among various CO2 capture technologies to achieve a zero-emission cement plant.


Assuntos
Aminas , Dióxido de Carbono , Dióxido de Carbono/química , Aminas/química , Materiais de Construção
13.
Environ Sci Technol ; 58(33): 14608-14617, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39105763

RESUMO

We present methods and insights for the design of CO2 capture, transport, and storage systems for industrial facilities with a case study focus on Louisiana. Our analytical framework includes (1) evaluating the scale and concentration of capturable CO2 emissions at individual facilities for the purpose of estimating the cost of CO2 capture retrofits that utilize various energy supply sources to meet parasitic demands; (2) screening to identify potential CO2 storage sites and estimate their capacities, injectivities, and costs; and (3) designing cost-minimized trucking or pipeline infrastructure connecting CO2 capture plants with storage sites, considering existing land uses, demographics, and a variety of social and environmental justice factors. Estimated levelized costs of capture at Louisiana's 190 industrial facilities range from below $50/tCO2 to above $500/tCO2, depending on facility-specific features. We identified 98 potential storage sites with storage costs ranging from $8 to $17/tCO2. We find that in most situations, pipelines are the least-costly mode of CO2 transport. When industrial facilities in a region share pipelines, aggregate pipeline mileage and average transport costs are dramatically lower than without sharing. Shared pipeline networks designed to avoid disadvantaged communities require right-of-way areas compared to those for networks that transect such communities, but result in 25% higher average per-tonne transport cost.


Assuntos
Dióxido de Carbono , Louisiana , Meios de Transporte , Indústrias , Poluentes Atmosféricos
14.
Environ Sci Technol ; 58(25): 10881-10896, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38861036

RESUMO

One of the most promising approaches to address the global challenge of climate change is electrochemical carbon capture and utilization. Solid electrolytes can play a crucial role in establishing a chemical-free pathway for the electrochemical capture of CO2. Furthermore, they can be applied in electrocatalytic CO2 reduction reactions (CO2RR) to increase carbon utilization, produce high-purity liquid chemicals, and advance hybrid electro-biosystems. This review article begins by covering the fundamentals and processes of electrochemical CO2 capture, emphasizing the advantages of utilizing solid electrolytes. Additionally, it highlights recent advancements in the use of the solid polymer electrolyte or solid electrolyte layer for the CO2RR with multiple functions. The review also explores avenues for future research to fully harness the potential of solid electrolytes, including the integration of CO2 capture and the CO2RR and performance assessment under realistic conditions. Finally, this review discusses future opportunities and challenges, aiming to contribute to the establishment of a green and sustainable society through electrochemical CO2 valorization.


Assuntos
Dióxido de Carbono , Eletrólitos , Dióxido de Carbono/química , Eletrólitos/química , Mudança Climática , Técnicas Eletroquímicas
15.
Environ Sci Technol ; 58(10): 4606-4616, 2024 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-38427797

RESUMO

Transforming hazardous species into active sites by ingenious material design was a promising and positive strategy to improve catalytic reactions in industrial applications. To synergistically address the issue of sluggish CO2 desorption kinetics and SO2-poisoning solvent of amine scrubbing, we propose a novel method for preparing a high-performance core-shell C@Mn3O4 catalyst for heterogeneous sulfur migration and in situ reconstruction to active -SO3H groups, and thus inducing an enhanced proton-coupled electron transfer (PCET) effect for CO2 desorption. As anticipated, the rate of CO2 desorption increases significantly, by 255%, when SO2 is introduced. On a bench scale, dynamic CO2 capture experiments reveal that the catalytic regeneration heat duty of SO2-poisoned solvent experiences a 32% reduction compared to the blank case, while the durability of the catalyst is confirmed. Thus, the enhanced PCET of C@Mn3O4, facilitated by sulfur migration and simultaneous transformation, effectively improves the SO2 resistance and regeneration efficiency of amine solvents, providing a novel route for pursuing cost-effective CO2 capture with an amine solvent.


Assuntos
Dióxido de Carbono , Prótons , Elétrons , Solventes , Aminas , Enxofre
16.
Environ Sci Technol ; 58(4): 1882-1893, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38214663

RESUMO

The expansion of renewable energy and the large-scale deployment of carbon dioxide (CO2) capture and storage (CCS) can decarbonize the power sector. The use of CO2 to extract geothermal heat from naturally porous and permeable sedimentary basins to generate electricity (CO2-plume geothermal (CPG) system) presents an opportunity to simultaneously generate renewable energy and geologically store CO2. In this study, we estimate the life cycle greenhouse gas (GHG) impacts of CPG systems through 12 scenarios in which CPG systems are combined with one of six CO2 sources (e.g., bioenergy with carbon capture and storage (BECCS) and iron and steel facilities) and operate in two geological settings. We find the life cycle GHG emissions of CPG systems ranging from -0.25 to -6.18 kg CO2eq/kWh. CPG systems can achieve the highest emissions reductions when utilizing the CO2 captured from BECCS. We evaluate uncertainty through a Monte Carlo simulation, demonstrating consistent net reductions in life cycle emissions and a local, one-parameter-at-a-time sensitivity analysis that identifies the CO2 capture capacity as the high-impact parameter of the results. Through the production of electricity, CPG systems can provide additional environmental benefits to the deployment of large-scale CCS.


Assuntos
Gases de Efeito Estufa , Gases de Efeito Estufa/análise , Dióxido de Carbono/análise , Energia Renovável , Efeito Estufa
17.
Macromol Rapid Commun ; 45(7): e2300647, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38243849

RESUMO

The rise in universal population and accompanying demands have directed toward an exponential surge in the generation of polymeric waste. The estimate predicts that world-wide plastic production will rise to ≈590 million metric tons by 2050, whereas 5000 million more tires will be routinely abandoned by 2030. Handling this waste and its detrimental consequences on the Earth's ecosystem and human health presents a significant challenge. Converting the wastes into carbon-based functional materials viz. activated carbon, graphene, and nanotubes is considered the most scientific and adaptable method. Herein, this world provides an overview of the various sources of polymeric wastes, modes of build-up, impact on the environment, and management approaches. Update on advances and novel modifications made in methodologies for converting diverse types of polymeric wastes into carbon nanomaterials over the last 5 years are given. A remarkable focus is made to comprehend the applications of polymeric waste-derived carbon nanomaterials (PWDCNMs) in the CO2 capture, removal of heavy metal ions, supercapacitor-based energy storage and water splitting with an emphasis on the correlation between PWDCNMs' properties and their performances. This review offers insights into emerging developments in the upcycling of polymeric wastes and their applications in environment and energy.


Assuntos
Metais Pesados , Nanoestruturas , Nanotubos , Humanos , Polímeros , Ecossistema
18.
Environ Res ; 249: 118426, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38342202

RESUMO

The advancement and engineering of novel crystalline materials is facilitated through the utilization of innovative porous crystalline structures, established via KOH-treated monolithic graphene oxide frameworks. These materials exhibit remarkable and versatile characteristics for both functional exploration and applications within the realm of CO2 capture. In this comprehensive study, we have synthesized monolithic reduced graphene oxide-based adsorbents through a meticulous self-assembly process involving different mass ratios of GO/malic acid (MaA) (1:0.250, 1:0.500, and 1:1 by weight). Building upon this foundation, we further modified MGO 0.250 through KOH-treatment by chloroacetic acid method, leading to the creation of MGO 0.250_KOH, which was subjected to CO2 capture assessments. The comprehensive investigation encompassed an array of parameters including morphology, specific surface area, crystal defects, functional group identification, and CO2 capture efficiency. Employing a combination of FT-IR, XRD, Raman, BET, SEM, HR-TEM, and XPS techniques, the study revealed profound insights. Particularly notable was the observation that the MGO 0.250_KOH adsorbent exhibited an exceptional CO2 capture performance, leading to a significant enhancement of the CO2 capture capacity from 1.69 mmol g-1 to 2.35 mmol g-1 at standard conditions of 25 °C and 1 bar pressure. This performance enhancement was concomitant with an augmentation in surface area, elevating from 287.93 to 419.75 m2 g-1 (a nearly 1.5-fold increase compared to MGO 1.000 with a surface area of 287.93 m2 g-1). The monolithic adsorbent demonstrated a commendable production yield of 82.92%, along with an impressive regenerability of 98.80% at 100 °C. Additionally, adsorbent's proficiency in CO2 adsorption, rendering it a promising candidate for post-combustion CO2 capture applications. These findings collectively underscore the capacity adsorbents to significantly amplify CO2 capture capabilities. The viability of employing this strategy as an uncomplicated pre-treatment technique in various industrial sectors is a plausible prospect, given the study's outcomes.


Assuntos
Dióxido de Carbono , Grafite , Grafite/química , Dióxido de Carbono/química , Adsorção , Porosidade
19.
Environ Res ; 246: 118119, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38191038

RESUMO

In this study, a precipitation-based synthesis method has been employed to prepare magnesium calcites with the general formula Ca1-xMgxCO3, with the objective of use them in the calcium looping (CaL) process for CO2 capture (CaL-CCS) and thermochemical energy storage (CaL-CSP). The structure and microstructure of the samples have been characterized. It has been found by X-ray diffraction that the samples with a Ca:Mg molar ratio of 0.5:0.5 and 0.55:0.45 are phase pure, while the samples with molar ratios of 0.7:0.3 and 0.8:0.2 are composed by two phases with different stoichiometry. In addition, the sample prepared with calcium alone shows the aragonite phase. The microstructure of the magnesium-containing samples is composed of nanocrystals, which are aggregated in spherical particles whereas the aragonite sample presents a typical rod-like morphology. The multicycle tests carried out under CaL-CCS conditions show that an increase on the MgO content in the calcined samples results in a reduced value of effective conversion when compared to aragonite. On the other hand, under CaL-CSP conditions, the samples with the higher MgO content exhibit nearly stable effective conversion values around 0.5 after 20 cycles, which improve the results obtained for aragonite and those reported for natural dolomite tested under the same conditions.


Assuntos
Cálcio , Magnésio , Cálcio/química , Magnésio/química , Dióxido de Carbono/química , Óxido de Magnésio , Carbonato de Cálcio/química
20.
Int J Phytoremediation ; 26(3): 427-447, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37583119

RESUMO

The chemically activated biochar was produced through the pyrolysis of rice husk. Thermal gravimetric and elemental analysis were conducted to characterize the raw rice husk. The activated biochar product underwent evaluation through SEM, BET and, FT-IR analysis. This cost-effective activated carbon was utilized as an adsorbent for the elimination of environmental pollutants. At a temperature of 25 °C, the activated biochar product exhibited an impressive maximum CO2 adsorption capacity of 152 mg/g. This exceptional performance can be attributed to its notable surface area and porosity, measuring at 2,298 m2/g and 0.812 cm3/g, respectively. This product was also utilized to remove methyl red (MR) dye from an aqueous solution. The optimal parameters for the removal of MR were determined as follows: a pH of 6.0, a temperature of 25 °C, an initial MR concentration of 50 mg/L, and an adsorbent dosage of 0.4 g/L. At a duration of 140 min, the system attained its maximum equilibrium adsorption capacity, reaching a value of 62.06 mg/g. Furthermore, the calculated maximum MR removal efficiency stood at an impressive 99.31%. The thermodynamic studies demonstrated that the MR removal process was spontaneous, exothermic, and increased randomness. Kinetic studies suggested that the pseudo-second-order model can fit well.


Rice is the staple food for a significant portion of the world's population. Rice husk, which is released during the production and processing of rice, is one of the most important agricultural wastes worldwide. In this study, low cost activated carbon was produced by converting renewable resource such as rice husk biomass into a product with high added value. The resulting product, with its high surface area, can offer a more sustainable, cost-effective, and versatile alternative for a range of industrial, environmental, and medical applications.


Assuntos
Poluentes Ambientais , Oryza , Poluentes Químicos da Água , Purificação da Água , Carvão Vegetal/química , Cinética , Espectroscopia de Infravermelho com Transformada de Fourier , Poluentes Químicos da Água/química , Biodegradação Ambiental , Adsorção , Concentração de Íons de Hidrogênio
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