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1.
Artigo em Inglês | MEDLINE | ID: mdl-38761179

RESUMO

Although thin-film composite membranes have achieved great success in CO2 separation, further improvements in the CO2 permeance are required to reduce the size and cost of the CO2 separation process. Herein, we report the fabrication of composite membranes with high CO2 permeability using a laser-patterned porous membrane as the support membrane. High-aspect-ratio micropatterns with well-defined micropores on their surface were carved on microporous polymer supports by a direct laser writing process using a short-pulsed laser. By using a Galvano scanner and optimizing the laser conditions and target materials, in-plane micropatterns, such as microhole arrays, microline grating, microlattices, and out-of-plane hierarchical micropatterns, were created on porous membranes. An aqueous suspension of hydrogel microparticles doped with an amine-based mobile carrier was sprayed onto the patterned surface to form a defect-free thin separation layer. The surface area of the separation layer on the patterned support is up to 80% larger than that of flat pristine membranes, resulting in a 52% higher CO2 permeance (1106 GPU) with a CO2/N2 selectivity of 172. The laser-patterned porous membranes allow the development of inexpensive and high-performance functional membranes not only for CO2 separation but also for other applications, such as water treatment, cell culture, micro-TAS, and membrane reactors.

2.
J Colloid Interface Sci ; 670: 348-356, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38763030

RESUMO

The depressed directional separation of photogenerated carriers and weak CO2 adsorption/activation activity are the main factors hampering the development of artificial photosynthesis. Herein, Na ions are embedded in graphitic carbon nitride (g-C3N4) to achieve directional migration of the photogenerated electrons to Na sites, while the electron-rich Na sites enhance CO2 adsorption and activation. Na/g-C3N4 (NaCN) shows improved photocatalytic reduction activity of CO2 to CO and CH4, and under simulated sunlight irradiation, the CO yield of NaCN synthesized by embedding Na at 550°C (NaCN-550) is 371.2 µmol g-1 h-1, which is 58.9 times more than that of the monomer g-C3N4. By means of theoretical calculations and experiments including in situ fourier transform infrared spectroscopy, the mechanism is investigated. This strategy which improves carrier separation and reduces the energy barrier at the same time is important to the development of artificial photosynthesis.

3.
Int J Biol Macromol ; : 132480, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38763242

RESUMO

Polylactic acid (PLA) is an eco-friendly material that can help address the problems of petroleum depletion and pollution. Blending renewable biomass materials with PLA to create composite foams with a tunable pore structure, superior performance, and low cost is a green technique for improving the pore structure and mechanical characteristics of single PLA foams. PLA/TP composites were created using melted tomato peel pomace powder (TP), which has a lamellar structure, as a reinforcing agent. Then, the relationship between the vesicle structure, morphology, and properties of the PLA/TP composite foams produced through supercritical CO2 intermittent foaming were investigated. The findings revealed that TP considerably enhanced the rheological characteristics and crystalline behavior of PLA. The PLA/TP composite foam had a better cell structure, compression characteristics, and wettability than pure PLA. The expansion ratio of the PLA/TP composite could reach 18.8, and its thermal conductivity decreased from 174.2 mW/m·K at 100 °C to 57.8 mW/m·K at 120 °C. Furthermore, annealing before foaming decreased the average composite foam blister size from 110.09 to 66.53 µm, and the annealing process also improved compression performance. This study contributes to solving environmental difficulties and creating PLA foams with controlled bubble structures, uniform bubble sizes, and outstanding overall performance.

4.
ACS Nano ; 2024 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-38764286

RESUMO

The electrochemical CO2 reduction reaction (CO2RR) has emerged as a promising approach for sustainable carbon cycling and valuable chemical production. Various methods and strategies have been explored to boost CO2RR performance. One of the most promising strategies includes the construction of stable ionic interfaces on metallic or molecular catalysts using organic or inorganic cations, which has demonstrated a significant improvement in catalytic performance. The stable ionic interface is instrumental in adjusting adsorption behavior, influencing reactive intermediates, facilitating mass transportation, and suppressing the hydrogen evolution reaction, particularly under acidic conditions. In this Perspective, we provide an overview of the recent advancements in building ionic interfaces in the electrocatalytic process and discuss the application of this strategy to improve the CO2RR performance of metallic and molecular catalysts. We aim to convey the future trends and opportunities in creating ionic interfaces to further enhance carbon utilization efficiency and the productivity of CO2RR products. The emphasis of this Perspective lies in the pivotal role of ionic interfaces in catalysis, providing a valuable reference for future research in this critical field.

5.
Angew Chem Int Ed Engl ; : e202406564, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38766872

RESUMO

How to achieve CO2 electroreduction in high efficiency is a current challenge with the mechanism not well understood yet. The metal-organic cages with multiple metal sites, tunable active centers, and well-defined microenvironments may provide a promising catalyst model. Here, we report self-assembly of Ag4L4 type cuboctahedral cages from coordination dynamic Ag+ ion and triangular imidazolyl ligand 1,3,5-tris(1-benzylbenzimidazol-2-yl) benzene (Ag-MOC-X, X= NO3, ClO4, BF4) via anion template effect. Notably, Ag-MOC-NO3 achieves the highest CO faradaic efficiency in pH-universal electrolytes of 86.1%(acidic), 94.1%(neutral) and 95.3% (alkaline), much higher than those of Ag-MOC-ClO4 and Ag-MOC-BF4 with just different counter anions. In situ attenuated total reflection Fourier transform infrared spectroscopy observes formation of vital intermediate *COOH for CO2-to-CO conversion. The density functional theory calculations suggest that the adsorption of CO2 on unsaturated Ag-site is stabilized by C-H⋅⋅⋅O hydrogen-bonding of CO2 in a microenvironment surrounded by three benzimidazole rings, and the activation of CO2 is dependent on the coordination dynamics of Ag-centers modulated by the hosted anions through Ag⋅⋅⋅X interactions. This work offers a supramolecular electrocatalytic strategy based on Ag-coordination geometry and host-guest interaction regulation of MOCs as high-efficient electrocatalysts for CO2 reduction to CO which is a key intermediate in chemical industry process.

6.
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.

7.
Adv Sci (Weinh) ; : e2404423, 2024 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-38767186

RESUMO

Establishing an advanced ecosystem incorporating freshwater harvesting, plastic utilization, and clean fuel acquisition is profoundly significant. However, low-efficiency evaporation, single energy utilization, and catalyst leakage severely hinder sustainable development. Herein, a nanofiber-based mortise-and-tenon structural Janus aerogel (MTSJA) is strategically designed in the first attempt and supports Z-scheme catalysts. By harnessing of the upper hydrophilic layer with hydrophilic channels embedding into the hydrophobic bottom layer to achieve tailoring bottom wettability states. MTSJA is capable of a fully-floating function for lower heat loss, water supply, and high-efficiency solar-to-vapor conversion. Benefiting from the ultrasonic cavitation effect and high sensitivity of materials to mechanical forces, this is also the first demonstration of synergistic solar and ultrasound fields to power simultaneous evaporation desalination and waste plastics as reusable substrates generating fuel energy. The system enables persistent desalination with an exceptional evaporation rate of 3.1 kg m-2 h-1 and 82.3% efficiency (21 wt.% NaCl solution and 1 sun), and realizes H2, CO, and CH4 yields with 16.1, 9.5, and 3 µmol h-1 g-1, respectively. This strategy holds great potential for desalination and plastics value-added transformation toward clean energy and carbon neutrality.

8.
Artigo em Inglês | MEDLINE | ID: mdl-38767933

RESUMO

Highly efficient electrochemical CO2-to-CO conversion is a promising approach for achieving carbon neutrality. While nonmetallic carbon electrocatalysts have shown potential for CO2-to-CO utilization in H-type cells, achieving efficient conversion in flow cells at an industrial scale remains challenging. In this study, we present a cost-effective synthesis strategy for preparing ultrathin 2D carbon nanosheet catalysts through simple amine functionalization. The optimized catalyst, NCNs-2.5, demonstrates exceptional CO selectivity with a maximum Faradaic efficiency of 98% and achieves a high current density of 55 mA cm-2 in a flow cell. Furthermore, the catalyst exhibits excellent long-term stability, operating continuously for 50 h while maintaining a CO selectivity above 90%. The superior catalytic activity of NCNs-2.5 is attributed to the presence of amine-N active sites within the carbon lattice structure. This work establishes a foundation for the rational design of cost-effective nonmetallic carbon catalysts as sustainable alternatives to metals in energy conversion systems.

9.
Data Brief ; 54: 110491, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38774245

RESUMO

Understanding and predicting CO2 emissions from individual power plants is crucial for developing effective mitigation strategies. This study analyzes and forecasts CO2 emissions from an engine-based natural gas-fired power plant in Dhaka Export Processing Zone (DEPZ), Bangladesh. This study also presents a rich dataset and ELM-based prediction model for a natural gas-fired plant in Bangladesh. Utilizing a rich dataset of Electricity generation and Gas Consumption, CO2 emissions in tons are estimated based on the measured energy use, and the ELM models were trained on CO2 emissions data from January 2015 to December 2022 and used to forecast CO2 emissions until December 2026. This study aims to improve the understanding and prediction of CO2 emissions from natural gas-fired power plants. While the specific operational strategy of the studied plant is not available, the provided data can serve as a valuable baseline or benchmark for comparison with similar facilities and the development of future research on optimizing operations and CO2 mitigation strategies. The Extreme Learning Machine (ELM) modeling method was employed due to its efficiency and accuracy in prediction. The ELM models achieved performance metrics Root Mean Square Error (RMSE), Mean Absolute Error (MAE), and Mean Absolute Scaled Error (MASE), values respectively 3494.46 (<5000), 2013.42 (<2500), and 0.93 close to 1, which falls within the acceptable range. Although natural gas is a cleaner alternative, emission reduction remains essential. This data-driven approach using a Bangladeshi case study provides a replicable framework for optimizing plant operations and measuring and forecasting CO2 emissions from similar facilities, contributing to global climate change.

11.
J Exp Bot ; 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38776254

RESUMO

The ATP-driven bicarbonate transporter 1 (BCT1), a four-component complex in the cyanobacterial CO2-concentrating mechanism, could enhance photosynthetic CO2 assimilation in plant chloroplasts. However, directing its subunits (CmpA, CmpB, CmpC and CmpD) to three chloroplast sub-compartments is highly complex. Investigating BCT1 integration into Nicotiana benthamiana chloroplasts revealed promising targeting strategies using transit peptides from the intermembrane space protein Tic22 for correct CmpA targeting, while the transit peptide of the chloroplastic ABCD2 transporter effectively targeted CmpB to the inner envelope membrane. CmpC and CmpD were targeted to the stroma by RecA and recruited to the inner envelope membrane by CmpB. Despite successful targeting, expression of this complex in CO2-dependent Escherichia coli failed to demonstrate bicarbonate uptake. We then used rational design and directed evolution to generate new BCT1 forms that were constitutively active. Several mutants were recovered, including a CmpCD fusion. Selected mutants were further characterized and stably expressed in Arabidopsis thaliana, but the transformed plants did not have higher carbon assimilation rates or decreased CO2 compensation points in mature leaves. While further analysis is required, this directed evolution and heterologous testing approach presents potential for iterative modification and assessment of CO2-concentrating mechanism components to improve plant photosynthesis.

12.
Small ; : e2402459, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38751061

RESUMO

The electrocatalytic conversion of inert CO2 to value-added chemical fuels powered by renewable energy is one of the benchmark approaches to address excessive carbon emissions and achieve carbon-neutral energy restructuring. However, the adsorption/activation of supersymmetric CO2 is facing insurmountable challenges that constrain its industrial-scale applications. Here, this theory-guided study confronts these challenges by leveraging the synergies of bimetallic sites and defect engineering, where pyrochlore-type semiconductor A2B2O7 is employed as research platform and the conversion of CO2-to-HCOOH as the model reaction. Specifically, defect engineering intensified greatly the chemisorption-induced CO2 polarization via the bimetallic coordination, thermodynamically beneficial to the HCOOH production via the *HCO2 intermediate. The optimal V-BSO-430 electrocatalyst with abundant surface oxygen vacancies achieved a superior HCOOH yield of 116.7 mmol h-1 cm-2 at -1.2 VRHE, rivalling the incumbent similar reaction systems. Furthermore, the unique catalytic unit featured with a Bi1-Sn-Bi2 triangular structure, which is reconstructed by defect engineering, and altered the pathway of CO2 adsorption and activation to allow the preferential affinity of the suspended O atom in *HCO2 to H. As a result, V-BSO-430 gave an impressive FEHCOOH of 93% at -1.0 VRHE. This study held promises for inspiring the exploration of bimetallic materials from the massive semiconductor database.

13.
Small ; : e2400769, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38751231

RESUMO

In the field of photocatalytic CO2 reduction, quantum dot (QD) assemblies have emerged as promising candidate photocatalysts due to their superior light absorption and better substrate adsorption. However, the poor contacts within QD assemblies lead to low interfacial charge transfer efficiency, making QD assemblies suffer from unsatisfactory photocatalytic performance. Herein, a novel approach is presented involving the construction of strongly interfacial fused CdS QD assemblies (CdS QD gel) for CO2 reduction. The novel CdS QD gel demonstrates outstanding photocatalytic performance for CO2 methanation, achieving a CH4 generation rate of ≈296 µmol g-1 h-1, with a selectivity surpassing 76% and an apparent quantum yield (AQY) of 1.4%. Further investigations reveal that the robust interfacial fusion in these CdS QDs not only boosts their ability to absorb visible light but also significantly promotes charge separation. The present work paves the way for utilizing QD gel photocatalysts in realizing efficient CO2 reduction and highlights the critical role of interfacial engineering in photocatalysts.

14.
Angew Chem Int Ed Engl ; : e202404884, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38760322

RESUMO

In this paper, we report a high-performance carbon nitride supported Cu single-atom catalyst featuring defected low-coordination Cu-N2 motif (Cu-N2-V). Lead many recently reported photocatalysts and its Cu-N3 and Cu-N4 counterparts, Cu-N2-V exhibits superior photocatalytic activity for CO2 reduction to ethanol, delivering 69.8 µmol g-1 h-1 ethanol production rate, 97.8% electron-based ethanol selectivity, and a yield of ~10 times higher than Cu-N3 and Cu-N4. Revealed by the extensive experimental investigation combined with the DFT calculation, the superior photoactivity of Cu-N2-V stems from its unique defected Cu-N2 configuration. Firstly, Cu in Cu-N2-V exist in Cu+/Cu2+ dual valence states, although predominantly in Cu+. The Cu+ sites support CO2 activation and the Cu+/Cu2+ sites are conducive for strong *CO adsorption and subsequent *CO-*CO dimerization enabling C-C coupling. Secondly, the Cu sites in Cu-N2-V are rich in electrons and thus highly active. Together they dictate the rate-determining step on CO2 photoreduction to ethanol and lower the Gibbs free energy change. Furthermore, the defected configuration also promotes light adsorption and charge separation efficiency. Collectively, these make Cu-N2-V an effective and high-performance catalyst for solar-driven CO2 conversion to ethanol. This study also reveals the valence state change of Cu in Cu-N2-V during the CO2 photoreduction reaction.

15.
Angew Chem Int Ed Engl ; : e202404387, 2024 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-38757232

RESUMO

The electrochemical CO2 reduction reaction (CO2RR) has been widely studied as a promising means to convert anthropogenic CO2 into valuable chemicals and fuels. In this process, the alkali metal ions present in the electrolyte are known to significantly influence the CO2RR activity and selectivity. In this study, we report a strategy for preparing efficient electrocatalysts by introducing a cation-relaying ligand, namely 6-mercaptohexanoic acid (MHA), into atom-precise Au25 nanoclusters (NCs). The CO2RR activity of the synthesized Au25(MHA)18 NCs was compared with that of Au25(HT)18 NCs (HT = 1-hexanethiolate). While both NCs selectively produced CO over H2, the CO2-to-CO conversion activity of the Au25(MHA)18 NCs was significantly higher than that of the Au25(HT)18 NCs when the catholyte pH was higher than the pKa of MHA, demonstrating the cation-relaying effect of the anionic terminal group. Mechanistic investigations into the CO2RR occurring on the Au25 NCs in the presence of different catholyte cations and concentrations revealed that the CO2-to-CO conversion activities of these Au25 NCs increased in the order Li+ < Na+ < K+ < Cs+, and are gated by the cation-coupled electron transfer step. These results were confirmed by the Nernstian shifts of the polarization curves at different cation concentrations.

16.
Adv Sci (Weinh) ; : e2402892, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38757555

RESUMO

Rechargeable Li-CO2 batteries are considered as a promising carbon-neutral energy storage technology owing to their ultra-high energy density and efficient CO2 capture capability. However, the sluggish CO2 reduction/evolution kinetics impedes their practical application, which leads to huge overpotentials and poor cyclability. Multi-element transit metal oxides (TMOs) are demonstrated as effective cathodic catalysts for Li-CO2 batteries. But there are no reports on the integration of defect engineering on multi-element TMOs. Herein, the oxygen vacancy-bearing Li-Ni-Co-Mn multi-oxide (Re-NCM-H3) catalyst with the α-NaFeO2-type structure is first fabricated by annealing the NiCoMn precursor that derived from spent ternary LiNi0.8Co0.1Mn0.1O2 cathode, in H2 at 300 °C. As demonstrated by experimental results and theory calculations, the introduction of moderate oxygen vacancy has optimized electronic state near the Fermi level (Ef), eventually improving CO2 adsorption and charge transfer. Therefore, the Li-CO2 batteries with Re-NCM-H3 catalyst deliver a high capacity (11808.9 mAh g-1), a lower overpotential (1.54 V), as well as excellent stability over 216 cycles at 100 mA g-1 and 165 cycles at 400 mA g-1. This study not only opens up a sustainable application of spent ternary cathode, but also validates the potential of multi-element TMO catalysts with oxygen defects for high-efficiency Li-CO2 batteries.

17.
Artigo em Inglês | MEDLINE | ID: mdl-38757947

RESUMO

The in-plane heterojunctions with atomic-level thickness and chemical-bond-connected tight interfaces possess high carrier separation efficiency and fully exposed surface active sites, thus exhibiting exceptional photocatalytic performance. However, the construction of in-plane heterojunctions remains a significant challenge. Herein, we prepared an in-plane ZnIn2S4/In(OH)3 heterojunction (ZISOH) by partial conversion of ZnIn2S4 to In(OH)3 through the addition of H2O2. This in situ oxidation etching-hydrolysis approach enables the ZISOH heterojunction to not only preserve the original nanosheet morphology of ZnIn2S4 but also form an intimate interface. Moreover, generated In(OH)3 serves as an electron-accepting platform and also promotes the adsorption of CO2. As a result, the heterojunction exhibits a remarkably enhanced performance for photocatalytic CO2 reduction. The production rate and selectivity of CO reach 1760 µmol g-1 h-1 and 78%, respectively, significantly higher than those of ZnIn2S4 (842 µmol g-1 h-1 and 65%). This work puts forward a feasible and facile approach to construct in-plane heterojunctions to enhance the photocatalytic performance of two-dimensional metal sulfides.

18.
ACS Nano ; 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38758185

RESUMO

Defect engineering and nitrogen doping being effective strategies for modulating the surface chemical state of the carbon matrix have been widely explored to promote the catalytic activity in the territory of electrochemical energy storage and conversion devices. However, the controllable synthesis of carbon material with high-density specific defects and high nitrogen doping is still full of challenges. Here, we first synthesize one-dimensional necklace-like nitrogen-doped carbon nanochains (N-CNCs) with abundant defects on carbon fiber paper (CFP) by chemical vapor deposition (CVD) method. The resultant nanostructures are a bunch of interconnected carbon spheres with a hollow structure at the internode and present the complete one-dimensional nanochain configuration. Specifically, the N-CNCs with a corrugated surface possesses high content of sp3 defects (31.2%) and nitrogen (23.6 at %). Combining finite element analysis and experimental results, it reveals that the robust shear field generated by etching gas releasing from thermal decomposition of melamine in situ modulates the CVD process via changing the size and force environment of the metal catalyst droplets for formation of N-CNCs. Benefiting from the high ratio of sp3/sp2 and nitrogen doped on the surface, the N-CNCs@CFP displays a superior electrocatalytic performance for CO2RR, delivering CO Faradaic efficiency of 95.9% and a current density of 23.2 mA cm-2 at -0.86 V vs RHE. This work provides promising synthesis strategy and some inspirations for construction of ultradense and specific defects coupling with nitrogen doping sites into carbon materials to achieve high-efficiency electrocatalysis applications.

19.
Chemphyschem ; : e202400425, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38758533

RESUMO

Using the state of the art theoretical methods, we have provided a comprehensive mechanistic understanding of the CO2 hydrogenation into HCOOH, H2CO, and CH3OH by 2,6-bis(diisopropylphosphinomethyl)pyridine (PNP)-ligated Fe pincer complex, featuring one CO and two H as co-ligands. For the computational investigation, a verified structural model containing methyl groups in place of the experimental isopropyl groups was used. Three catalytic conversions involving hydrogenation of CO2 into formic acid (HCOOH), HCOOH into formaldehyde and methanol were studied in different solvent medium. Our modelled complex appears to be a viable base-free catalyst for the conversion of CO2 into HCOOH and HCOOH into H2CO, based on the free energy profiles, which show apparent activation energy barriers of 16.28 kcal/mol and 23.63 kcal/mol for the CO2 to HCOOH and HCOOH to H2CO conversion, respectively. However, the computed results show that, due to the huge energy span of H2CO to CH3OH conversion, complete hydrogenation of CO2 into methanol could not occur under moderate conditions. Morpholine co-catalyst, which can lower the hydrogenation barrier by taking part in a simultaneous H-atom donation-acceptance process, could have assisted in completing this step.

20.
Adv Mater ; : e2312894, 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38722084

RESUMO

Electrochemical CO2 reduction reaction (CO2RR) powered by renewable energy provides a promising route to CO2 conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes a large amount of CO2 to produce (bi)carbonate byproducts, leading to significant challenges at the device level, thereby impeding the further deployment of this reaction. Conducting CO2RR in acidic electrolytes offers a promising solution to address the "carbonate issue"; however, it presents inherent difficulties due to the competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst and electrode designs to achieve high selectivity and activity. This review encompasses recent developments of acidic CO2RR, from mechanism elucidation to catalyst design and device engineering. This review begins by discussing the mechanistic understanding of the reaction pathway, laying the foundation for catalyst design in acidic CO2RR. Subsequently, an in-depth analysis of recent advancements in acidic CO2RR catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular catalysts, and catalyst surface enhancement. Furthermore, the progress made in device-level applications is summarized, aiming to develop high-performance acidic CO2RR systems. Finally, the existing challenges and future directions in the design of acidic CO2RR catalysts are outlined, emphasizing the need for improved selectivity, activity, stability, and scalability.

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