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1.
Dalton Trans ; 53(10): 4823-4832, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38372568

RESUMO

Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e- ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e- pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e- ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e- ORR electrocatalysts based on the rational engineering of the metal-support interaction.

2.
Small ; : e2311336, 2024 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-38385851

RESUMO

The electrocatalytic conversion of nitrate (NO3 - ) to NH3 (NO3 RR) at ambient conditions offers a promising alternative to the Haber-Bosch process. The pivotal factors in optimizing the proficient conversion of NO3 - into NH3 include enhancing the adsorption capabilities of the intermediates on the catalyst surface and expediting the hydrogenation steps. Herein, the Cu/Cu2 O/Pi NWs catalyst is designed based on the directed-evolution strategy to achieve an efficient reduction of NO3 ‾. Benefiting from the synergistic effect of the OV -enriched Cu2 O phase developed during the directed-evolution process and the pristine Cu phase, the catalyst exhibits improved adsorption performance for diverse NO3 RR intermediates. Additionally, the phosphate group anchored on the catalyst's surface during the directed-evolution process facilitates water electrolysis, thereby generating Hads on the catalyst surface and promoting the hydrogenation step of NO3 RR. As a result, the Cu/Cu2 O/Pi NWs catalyst shows an excellent FE for NH3 (96.6%) and super-high NH3 yield rate of 1.2 mol h-1  gcat. -1 in 1 m KOH and 0.1 m KNO3 solution at -0.5 V versus RHE. Moreover, the catalyst's stability is enhanced by the stabilizing influence of the phosphate group on the Cu2 O phase. This work highlights the promise of a directed-evolution approach in designing catalysts for NO3 RR.

3.
Dalton Trans ; 53(7): 2903-2916, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38269643

RESUMO

Electrochemical water splitting has been regarded a promising method for the production of green hydrogen, addressing the need for efficient energy conversion and storage. However, it is severely hindered by the oxygen evolution reaction (OER) because of its multi-step four-electron transfer pathway with sluggish reaction kinetics. Microporous metal-organic-frameworks (MOFs), by virtue of large specific surface area, high porosity, tunable composition and morphology, find widespread use as precursors of metal-carbon nanostructures. The resulting carbon nanomaterials can well inherit the characteristics and advantages of the crystalline MOF precursors, and exhibit versatile application prospects in the fields of environment and energy, particularly in OER. Herein, a meticulous overview of the synthesis strategy for MOF-derived metal-carbon nanostructures and the origins of their enhanced OER properties has been demonstrated. We comprehensively illustrate these aspects across three dimensions: MOF selection, metal introduction, and carbon structures. Finally, the challenges and future prospects for this emerging field will be presented.

4.
J Chem Phys ; 160(2)2024 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-38189618

RESUMO

The sluggish oxygen evolution reaction (OER) in overall electrocatalytic water splitting poses a significant challenge in hydrogen production. A series of transition metal phosphides are emerging as promising electrocatalysts, effectively modulating the charge distribution of surrounding atoms for OER. In this study, a highly efficient OER electrocatalyst (CoP-CNR-CNT) was successfully synthesized through the pyrolysis and phosphatization of a Co-doped In-based coordination polymer, specifically InOF-25. This process resulted in evenly dispersed CoP nanoparticles encapsulated in coordination polymer-derived carbon nanoribbons. The synthesized CoP-CNR-CNT demonstrated a competitive OER activity with a smaller overpotential (η10) of 295.7 mV at 10 mA cm-2 and a satisfactory long-term stability compared to the state-of-the-art RuO2 (η10 = 353.7 mV). The high OER activity and stability can be attributed to the high conductivity of the carbon network, the abundance of CoP particles, and the intricate nanostructure of nanoribbons/nanotubes. This work provides valuable insights into the rational design and facile preparation of efficient non-precious metal-based OER electrocatalysts from inorganic-organic coordination polymers, with potential applications in various energy conversion and storage systems.

5.
Small ; 20(15): e2306353, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-37997226

RESUMO

Metal-organic frameworks (MOFs) represent a relatively new family of materials that attract lots of attention thanks to their unique features such as hierarchical porosity, active metal centers, versatility of linkers/metal nodes, and large surface area. Among the extended list of MOFs, Zr-based-MOFs demonstrate comparably superior chemical and thermal stabilities, making them ideal candidates for energy and environmental applications. As a Zr-MOF, NU-1000 is first synthesized at Northwestern University. A comprehensive review of various approaches to the synthesis of NU-1000 MOFs for obtaining unique surface properties (e.g., diverse surface morphologies, large surface area, and particular pore size distribution) and their applications in the catalysis (electro-, and photo-catalysis), CO2 reduction, batteries, hydrogen storage, gas storage/separation, and other environmental fields are presented. The review further outlines the current challenges in the development of NU-1000 MOFs and their derivatives in practical applications, revealing areas for future investigation.

6.
Inorg Chem ; 63(1): 642-652, 2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-38131603

RESUMO

The design of hierarchical electrocatalysts with plentiful active sites and high mass transfer efficiency is critical to efficiently and sustainably carrying out the oxygen evolution reaction (OER), which presents a challenging and pressing need. In this study, a hierarchical Ni(OH)2@NiFe-Prussian blue analogue nanoarray grown on nickel foam (NF) [labeled as Ni(OH)2@NiFe-PBA/NF] was synthesized by combining a mild electrodeposition method with an ion-exchange strategy. The resultant Ni(OH)2@NiFe-PBA/NF displays superhydrophilic/superaerophobic properties that optimize the contact with the electrolyte, improve mass transfer efficiency, and expedite detachment of O2 bubbles during the electrocatalytic OER. Specifically, Ni(OH)2@NiFe-PBA/NF exhibits exceptional capability in the OER with low overpotentials of 224 and 240 mV at the current densities of 50 and 100 mA cm-2, respectively, accompanied by a low Tafel slope of 37.1 mV dec-1 and outstanding stability over 100 h at a fixed potential of 1.78 V vs reversible hydrogen electrode (RHE). Furthermore, Ni(OH)2@NiFe-PBA/NF demonstrates remarkable OER performance even in alkaline simulated seawater. During the OER process, active metal-OOH intermediates were formed by the partial self-reconstruction of NiFe-PBA in the heterostructure, as revealed by in situ Raman spectroscopy.

7.
Small ; : e2308732, 2023 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-38072778

RESUMO

Metal-organic frameworks (MOFs), as a subclass of porous crystalline materials with unique structures and multifunctional properties, play a pivotal role in various research domains. In recent years, significant attention has been directed toward composite materials based on MOFs, particularly MOF-on-MOF heterostructures. Compared to individual MOF materials, MOF-on-MOF structures harness the distinctive attributes of two or more different MOFs, enabling synergistic effects and allowing for the tailored design of diverse multilayered architectures to expand their application scope. However, the rational design and facile synthesis of MOF-on-MOF composite materials are in principle challenging due to the structural diversity and the intricate interfaces. Hence, this review primarily focuses on elucidating the factors that influence their interfacial growth, with a specific emphasis on the interfacial engineering of heterogeneous reactions, in which MOF-on-MOF hybrids can be conveniently obtained by using pre-fabricated MOF precursors. These factors are categorized as internal and external elements, encompassing inorganic metals, organic ligands, lattice matching, nucleation kinetics, thermodynamics, etc. Meanwhile, these intriguing MOF-on-MOF materials offer a wide range of advantages in various application fields, such as adsorption, separation, catalysis, and energy-related applications. Finally, this review highlights current complexities and challenges while providing a forward-looking perspective on future research directions.

8.
Adv Sci (Weinh) ; 10(33): e2303789, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37822155

RESUMO

The electrocatalytic conversion of nitrate (NO3 ‾) to NH3  (NO3 RR) offers a promising alternative to the Haber-Bosch process. However, the overall kinetic rate of NO3 RR is plagued by the complex proton-assisted multiple-electron transfer process. Herein, Ag/Co3 O4 /CoOOH nanowires (i-Ag/Co3 O4  NWs) tandem catalyst is designed to optimize the kinetic rate of intermediate reaction for NO3 RR simultaneously. The authors proved that NO3 ‾ ions are reduced to NO2 ‾ preferentially on Ag phases and then NO2 ‾ to NO on Co3 O4  phases. The CoOOH phases catalyze NO reduction to NH3  via NH2 OH intermediate. This unique catalyst efficiently converts NO3 ‾ to NH3  through a triple reaction with a high Faradaic efficiency (FE) of 94.3% and a high NH3  yield rate of 253.7 µmol h-1  cm-2  in 1 M KOH and 0.1 M KNO3  solution at -0.25 V versus RHE. The kinetic studies demonstrate that converting NH2 OH into NH3  is the rate-determining step (RDS) with an energy barrier of 0.151 eV over i-Ag/Co3 O4  NWs. Further applying i-Ag/Co3 O4  NWs as the cathode material, a novel Zn-nitrate battery exhibits a power density of 2.56 mW cm-2  and an FE of 91.4% for NH3  production.

9.
Inorg Chem ; 62(45): 18680-18688, 2023 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-37907390

RESUMO

Photocatalytic H2 evolution has recently attracted much attention due to the reduction of nonrenewable energy sources and the increasing demand for renewable sustainable energies. Meanwhile, metal-organic frameworks (MOFs) are emerging potential photocatalysts due to their structural adaptability, porous configuration, several active sites, and a wide range of performance. Nevertheless, there are still limitations in the photocatalytic H2 evolution reaction of MOFs with higher charge recombination rates. Herein, a copper-organic framework with dual-functionalized linkers {[Cu2(L)(H2O)2]·(5DMF)(4H2O)}n (fluorinated MOF(Cu)-NH2; H4L = 3,5-bis(2,4-dicarboxylic acid)-4-(trifluoromethyl)aniline) and with a rare 2-nodal 4,12-connected shp topology has been synthesized by a ligand-functionalization strategy and evaluated for the photocatalytic production of H2 to overcome this issue. According to the photocatalytic H2 evolution results, fluorinated MOF(Cu)-NH2 showed a hydrogen evolution rate of 63.64 mmol·g-1·h-1 exposed to light irradiation, indicating values 12 times that of the pure ligand when cocatalyst Pt and photosensitizer Rhodamine B were present. In addition, this MOF showed a maximum water absorption of 205 cm3·g-1. When dual-functionalized linkers are introduced to the structure of this MOF, its visible-light absorption increases considerably, which can be associated with nearly narrower energy band gaps (2.18 eV). More importantly, this MOF contributes to water absorption and electron collection and transport, acting as a bridge that helps to separate and transfer photogenerated charges while shortening the electron migration path because of the functional group in its configuration. The current paper seeks to shed light on the design of advanced visible-light photocatalysts with no MOF calcination for H2 photocatalytic production.

10.
Chem Commun (Camb) ; 59(86): 12875-12878, 2023 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-37818592

RESUMO

Nickel-based electrocatalysts for the oxygen evolution reaction (OER) show the disadvantages of low activity and poor stability. In this paper, an FeNi alloy is wrapped by an amino-modified MOF-5-derived N-doped carbon layer to address these problems. Additionally, the improvement resulting from Fe doping of NiOOH catalysts is theoretically supported.

11.
J Colloid Interface Sci ; 652(Pt B): 1338-1346, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37714748

RESUMO

The sluggish kinetics of the electrocatalytic oxygen evolution reaction (OER) pose a significant challenge in the field of overall water splitting. Transition metal phosphides have emerged as promising catalysts for OER by modulating the charge distribution of surrounding atoms. In this study, we employed self-sacrificing templates to fabricate hollow N-doped carbon spheres containing small-sized Co2P embedded within carbon nanotubes through high-temperature calcination and phosphorization, referred to as HNCS-CNT-CoP. The obtained HNCS-CNT-CoP electrocatalyst exhibited excellent OER performance in an alkaline electrolyte due to the optimization of OH* adsorption energy and the large specific surface area created by the hollow structure. It demonstrated a low overpotential of 302 mV at a current density of 10 mA cm-2 and a low Tafel slope of 68.5 mV dec-1, attributed to the electron transport facilitated by the in situ formed carbon nanotubes. Furthermore, theoretical calculations revealed a suitable reaction energy (1.17 eV) in the critical formation of Co2P-*OOH for HNCS-CNT-CoP, significantly lower than the the rate-determining step of HNCS-CNT-Co (10.08 eV). These findings highlight the significance of hollow structures and Co2P-doping in the design of highly active non-noble metal OER electrocatalysts, enabling the reduction of energetic reaction barriers for future applications.

12.
Inorg Chem ; 62(36): 14757-14763, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37639239

RESUMO

The complex process of the anodic oxygen evolution reaction (OER) severely hinders overall water splitting, which further limits the large-scale production and application of hydrogen energy. In this work, one type of bimetallic coordination polymer of ZnCoBTC using the MOF-on-MOF strategy has been synthesized where both Co(II) and Zn(II) cations exhibit the same coordination environment. By applying an electric potential, the predesigned bimetallic MOF precursor can be conveniently degraded into CoOxHy as an active species for efficient OER. Owing to the dissolution of ZnOxHy species, in situ formed disordered defects on the external surface of the catalyst increase the specific surface area as well as expose abundant active materials. Therefore, the ZnCoOxHy nanosheet shows excellent OER performance and reaches an overpotential of only 334 mV at 10 mA cm-2 with a Tafel slope of 66.4 mV dec-1, indicating fast reaction kinetics. The results demonstrate that metals with the same coordination environment can undergo in situ replacement or secondary growth on the pristine MOF, and they can be electrochemically degraded into highly efficient catalysts for future energy applications.

13.
J Colloid Interface Sci ; 650(Pt B): 2056-2064, 2023 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-37330332

RESUMO

Functional carbon nanomaterials play a crucial role in the cathodic oxygen reduction reaction (ORR) for sustainable fuel cells and metal-air batteries. In this study, we propose an effective approach to immobilize iron phthalocyanines (FePc) by employing a porous N-doped carbon material, denoted as NC-1000, derived from a sheet-shaped coordination polymer. The resulting NC-1000 possesses substantial porosity and abundant pore defects. The nitrogen sites within NC-1000 not only facilitate FePc adsorption but also optimize the electron distribution at the Fe-N site. The FePc@NC-1000 composite material exhibits a significant number of active centers in the form of Fe-N4 moieties, showcasing satisfactory ORR activity. Specifically, it demonstrates an onset potential of 0.99 V, a positive half-wave potential of 0.86 V, a large limiting current of 5.96 mA cm-2, and a small Tafel slope of 44.41 mV dec-1. Additionally, theoretical calculations and experimental results confirm the favorable performance and durability of zinc-air batteries assembled using FePc@NC-1000, thereby highlighting their considerable potential for practical applications. Overall, this study provides a comprehensive exploration of the enhanced catalytic performance and increased stability of metal-organic framework-derived functional carbon nanomaterials as cost-effective, efficient, and stable catalysts for the ORR.

14.
ACS Appl Mater Interfaces ; 15(15): 18928-18939, 2023 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-37014152

RESUMO

In alkaline solutions, the electrocatalytic conversion of nitrates to ammonia (NH3) (NO3RR) is hindered by the sluggish hydrogenation step due to the lack of protons on the electrode surface, making it a grand challenge to synthesize NH3 at a high rate and selectivity. Herein, single-stranded deoxyribonucleic acid (ssDNA)-templated copper nanoclusters (CuNCs) were synthesized for the electrocatalytic production of NH3. Because ssDNA was involved in the optimization of the interfacial water distribution and H-bond network connectivity, the water-electrolysis-induced proton generation was enhanced on the electrode surface, which facilitated the NO3RR kinetics. The activation energy (Ea) and in situ spectroscopy studies adequately demonstrated that the NO3RR was exothermic until NH3 desorption, indicating that, in alkaline media, the NO3RR catalyzed by ssDNA-templated CuNCs followed the same reaction path as the NO3RR in acidic media. Electrocatalytic tests further verified the efficiency of ssDNA-templated CuNCs, which achieved a high NH3 yield rate of 2.62 mg h-1 cm-2 and a Faraday efficiency of 96.8% at -0.6 V vs reversible hydrogen electrode. The results of this study lay the foundation for engineering catalyst surface ligands for the electrocatalytic NO3RR.

15.
Adv Sci (Weinh) ; 10(19): e2300797, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37083242

RESUMO

The photocatalytic transformation of carbon dioxide (CO2 ) into carbon-based fuels or chemicals using sustainable solar energy is considered an ideal strategy for simultaneously alleviating the energy shortage and environmental crises. However, owing to the low energy utilization of sunlight and inferior catalytic activity, the conversion efficiency of CO2 photoreduction is far from satisfactory. In this study, a MOF-derived hollow bimetallic oxide nanomaterial is prepared for the efficient photoreduction of CO2 . First, a unique ZIF-67-on-InOF-1 heterostructure is successfully obtained by growing a secondary Co-based ZIF-67 onto the initial InOF-1 nanorods. The corresponding hollow counterpart has a larger specific surface area after acid etching, and the oxidized bimetallic H-Co3 O4 /In2 O3 material exhibits abundant heterogeneous interfaces that expose more active sites. The energy band structure of H-Co3 O4 /In2 O3 corresponds well with the photosensitizer of [Ru(bpy)3 ]Cl2 , which results in a high CO yield of 4828 ± 570 µmol h-1  g-1 and stable activity over a consecutive of six runs, demonstrating adequate photocatalytic performance. This study demonstrates that the rational design of MOF-on-MOF heterostructures can completely exploit the synergistic effects between different components, which may be extended to other MOF-derived nanomaterials as promising catalysts for practical energy conversion and storage.

16.
Front Chem ; 11: 1148073, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36926381

RESUMO

Robust DUT-67 was synthesized by the hydrothermal method and characterized by powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). To systematically study the removal of Cr(VI) ion by DUT-67, single-factor, competition ion, material regeneration, kinetic, and thermodynamic experiments were designed. The experimental results show that DUT-67 had a maximum removal rate of 96.1% and a maximum adsorption capacity of 105.42 mg g-1 with material regeneration and outstanding selective adsorption. In addition, the process of removal of the Cr(VI) ion from an aqueous solution by DUT-67, which accorded with the pseudo-second-order kinetics model and Langmuir model, was studied, and its adsorption mechanism was reasonably explained by the theoretical calculation.

17.
Small ; 19(19): e2207847, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36772894

RESUMO

IrO2 as benchmark electrocatalyst for acidic oxygen evolution reaction (OER) suffers from its low activity and poor stability. Modulating the coordination environment of IrO2 by chemical doping is a methodology to suppress Ir dissolution and tailor adsorption behavior of active oxygen intermediates on interfacial Ir sites. Herein, the Re-doped IrO2 with low crystallinity is rationally designed as highly active and robust electrocatalysts for acidic OER. Theoretical calculations suggest that the similar ionic sizes of Ir and Re impart large spontaneous substitution energy and successfully incorporate Re into the IrO2 lattice. Re-doped IrO2 exhibits a much larger migration energy from IrO2 surface (0.96 eV) than other dopants (Ni, Cu, and Zn), indicating strong confinement of Re within the IrO2 lattice for suppressing Ir dissolution. The optimal catalysts (Re: 10 at%) exhibit a low overpotential of 255 mV at 10 mA cm-2 and a high stability of 170 h for acidic OER. The comprehensive mechanism investigations demonstrate that the unique structural arrangement of the Ir active sites with Re-dopant imparts high performance of catalysts by minimizing Ir dissolution, facilitating *OH adsorption and *OOH deprotonation, and lowering kinetic barrier during OER. This study provides a methodology for designing highly-performed catalysts for energy conversion.

18.
Inorg Chem ; 62(7): 3288-3296, 2023 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-36735285

RESUMO

Conventional enzyme-based glucose biosensors have limited extensive applications in daily life because glucose oxidase is easily inactivated and is expensive. In this paper, we propose a strategy to prepare a new type of cost-effective, efficient, and robust nonenzymatic Ni-CNT-O for electrochemical glucose sensing. It is first followed by the pyrolysis of Ni-ABDC nanostrips using melamine to grow carbon nanotubes (CNTs) to give an intermediate product of Ni-CNT, which is further accompanied by partial oxidation to enable the facile formation of hierarchical carbon nanomaterials with improved hydrophilicity. A series of physicochemical characterizations have fully proved that Ni-CNT-O is a carbon-coated heterostructure of Ni and NiO nanoparticles embedded into coordination polymer-derived porous carbons. The obtained Ni-CNT-O exhibits a better electrocatalytic activity for glucose oxidation stemming from the synergistic effect of a metal element and a metal oxide than unoxidized Ni-CNT, which also shows high performance with a wide linear range from 1 to 3000 µM. It also offers a high sensitivity of 79.4 µA mM-1 cm-2, a low detection limit of 500 nM (S/N = 3), and a satisfactory long-term durability. Finally, this glucose sensor exhibits good reproducibility, high selectivity, as well as satisfactory results by comparing the current response of simulated serum within egg albumen.


Assuntos
Nanopartículas , Nanoestruturas , Nanotubos de Carbono , Nanotubos de Carbono/química , Reprodutibilidade dos Testes , Glucose/química , Nanoestruturas/química , Técnicas Eletroquímicas
19.
ChemSusChem ; 16(1): e202201947, 2023 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-36302718

RESUMO

The exploration of non-noble metal electrocatalysts with high catalytic activity and stability for oxygen evolution reaction (OER) has become particularly urgent. Here, FeNi-based Prussian blue analogues (PBAs) were obtained by adding different solvents, where PBA particles preferentially grew on the surface plane/edge of coordination polymer precursor (Ni-ABDC) with various polarities. This resulted in the formation of FeNi-PBA-plane/edge morphologies, respectively. Notably, on account of more exposed PBAs, FeNi nanoparticles were uniformly supported on the porous N-doped carbon nanomaterials. Among them, the calcined FeNi-NC-800 underwent an interesting pre-activation process and exhibited a low overpotential of 281 mV at 10 mA cm-2 and a small Tafel slope of 82 mV dec-1 in 1.0 m KOH. This bimetallic sample showed superior OER activity and stability in comparison with control materials, which could be attributed to its abundant FeNi nanoparticles, high nitrogen content, large specific surface area, and synergistic effects between Fe and Ni atoms. In addition, relevant theoretical calculation on the optimal catalyst, FeNi-NC-800, further demonstrated its efficient OER performance with effective Fe-doping in the Ni-based oxyhydroxides.

20.
Small ; 19(10): e2201550, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36563116

RESUMO

Using petrol to supply energy for a car or burning coal to heat a building generates plenty of greenhouse gas (GHG) emissions, including carbon dioxide (CO2 ), water vapor (H2 O), methane (CH4 ), nitrous oxide (N2 O), ozone (O3 ), fluorinated gases. These up-and-coming metal-organic frameworks (MOFs) are structurally endowed with rigid inorganic nodes and versatile organic linkers, which have been extensively used in the GHG-related applications to improve the lives and protect the environment. Porous MOF materials and their derivatives have been demonstrated to be competitive and promising candidates for GHG separation, storage and conversions as they shows facile preparation, large porosity, adjustable nanostructure, abundant topology, and tunable physicochemical property. Enormous progress has been made in GHG storage and separation intrinsically stemmed from the different interaction between guest molecule and host framework from MOF itself in the recent five years. Meanwhile, the use of porous MOF materials to transform GHG and the influence of external conditions on the adsorption performance of MOFs for GHG are also enclosed. In this review, it is also highlighted that the existing challenges and future directions are discussed and envisioned in the rational design, facile synthesis and comprehensive utilization of MOFs and their derivatives for practical applications.

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