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1.
Inorg Chem ; 62(13): 5253-5261, 2023 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-36942791

RESUMEN

Iron-nitrogen coordinated catalysts are regarded as efficient catalysts for the oxygen (O2) reduction reaction (ORR), wherein the coordination environment of Fe sites is critical to the catalytic activity. Herein, we explored the effect of the nitrogen-coordination structure of dual-atomic Fe2 sites (i.e., Fe2-N6-C and Fe2-N4-C) on the performance of the ORR. The half-wave potential (E1/2) of Fe2-N6-C is 0.880 V vs RHE, outperforming that of the tetracoordinate Fe2-N4-C (0.851 V) and commercial Pt/C (0.850 V) in alkaline electrolytes. The Fe2-N6-C-based zinc-air battery delivers a maximum power density of (258.6 mW/cm2) and superior durability under 10 mA/cm2. Theoretical calculations unveil that the moieties of Fe2-N6 profits the d-electron rearrangement of the Fe2 sites. The electronic and geometrical structure of Fe2-N6 promotes the O2 molecules adsorbed on the Fe2 site and reduces the dissociation energy barrier of O2, benefiting fracture of O-O bonds and acceleration of the transformation of O2 to *OOH (the first step of the ORR process). Such exploration of modulating the local N-coordination environment of Fe2 dimers paves an in-depth insight to design and optimize dual-atomic catalysts.

2.
Angew Chem Int Ed Engl ; 62(26): e202300873, 2023 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-36883799

RESUMEN

The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H2 O is well known to affect the dissociation process, but H2 O orientation is hard to control because of its random distribution. Herein, an atomically asymmetric local electric field was designed by IrRu dizygotic single-atom sites (IrRu DSACs) to tune the H2 O adsorption configuration and orientation, thus optimizing its dissociation process. The electric field intensity of IrRu DSACs is over 4.00×1010  N/C. The ab initio molecular dynamics simulations combined with in situ Raman spectroscopy analysis on the adsorption behavior of H2 O show that the M-H bond length (M=active site) is shortened at the interface due to the strong local electric field gradient and the optimized water orientation promotes the dissociation process of interfacial water. This work provides a new way to explore the role of single atomic sites in alkaline hydrogen evolution reaction.


Asunto(s)
Electricidad , Hidrógeno , Adsorción , Cinética , Agua
3.
J Am Chem Soc ; 144(7): 3039-3049, 2022 Feb 23.
Artículo en Inglés | MEDLINE | ID: mdl-35112839

RESUMEN

Electrochemical CO2 reduction is a promising way to mitigate CO2 emissions and close the anthropogenic carbon cycle. Among products from CO2RR, multicarbon chemicals, such as ethylene and ethanol with high energy density, are more valuable. However, the selectivity and reaction rate of C2 production are unsatisfactory due to the sluggish thermodynamics and kinetics of C-C coupling. The electric field and thermal field have been studied and utilized to promote catalytic reactions, as they can regulate the thermodynamic and kinetic barriers of reactions. Either raising the potential or heating the electrolyte can enhance C-C coupling, but these come at the cost of increasing side reactions, such as the hydrogen evolution reaction. Here, we present a generic strategy to enhance the local electric field and temperature simultaneously and dramatically improve the electric-thermal synergy desired in electrocatalysis. A conformal coating of ∼5 nm of polytetrafluoroethylene significantly improves the catalytic ability of copper nanoneedles (∼7-fold electric field and ∼40 K temperature enhancement at the tips compared with bare copper nanoneedles experimentally), resulting in an improved C2 Faradaic efficiency of over 86% at a partial current density of more than 250 mA cm-2 and a record-high C2 turnover frequency of 11.5 ± 0.3 s-1 Cu site-1. Combined with its low cost and scalability, the electric-thermal strategy for a state-of-the-art catalyst not only offers new insight into improving activity and selectivity of value-added C2 products as we demonstrated but also inspires advances in efficiency and/or selectivity of other valuable electro-/photocatalysis such as hydrogen evolution, nitrogen reduction, and hydrogen peroxide electrosynthesis.

4.
Angew Chem Int Ed Engl ; 61(44): e202212640, 2022 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-36074055

RESUMEN

Carbon dioxide electroreduction (CO2 RR) is a sustainable way of producing carbon-neutral fuels. Product selectivity in CO2 RR is regulated by the adsorption energy of reaction-intermediates. Here, we employ differential phase contrast-scanning transmission electron microscopy (DPC-STEM) to demonstrate that Sn heteroatoms on a Ag catalyst generate very strong and atomically localized electric fields. In situ attenuated total reflection infrared spectroscopy (ATR-IR) results verified that the localized electric field enhances the adsorption of *COOH, thus favoring the production of CO during CO2 RR. The Ag/Sn catalyst exhibits an approximately 100 % CO selectivity at a very wide range of potentials (from -0.5 to -1.1 V, versus reversible hydrogen electrode), and with a remarkably high energy efficiency (EE) of 76.1 %.

5.
Microb Pathog ; 158: 104959, 2021 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-34022353

RESUMEN

BACKGROUND: Interleukin-4 (lL-4) is a critical negative cytokine in tuberculosis (TB) immune process, acting through modulating macrophages activation and Th1/Th2 balance. rs2243250 has been demonstrated to be associated with enhanced promoter strength in IL-4 expression. We performed a meta-analysis to assess the association between IL-4 rs2243250 polymorphism and TB risk. METHODS: We identified relevant studies by a comprehensive search of PubMed, Web of Science, and Embase databases, published up to February 10, 2021. The pooled odds ratios (ORs) and its 95% confidential intervals (95%CIs) were used to evaluate the associations under five genetic models. All statistical analyses were conducted with STATA 12.0 software. RESULTS: Totally 11 qualified studies involving 3097 TB cases and 3697 controls were enrolled in this meta-analysis. Overall, we didn't detect any significant association between IL-4 rs2243250 polymorphism and TB risk (T vs. C: OR = 1.05, 95% CI = 0.85-1.30, p = 0; 65; TT + TC vs. CC: OR = 1.05, 95% CI = 0.73-1.50, p = 0.81; TT vs. TC + CC: OR = 1.10, 95% CI = 0.81-1.50, p = 0.54; TT vs. CC: OR = 1.17, 95% CI = 0.71-1.94, p = 0.54; TC vs. CC: OR = 1.03, 95% CI = 0.73-1.45, p = 0.88). Significant heterogeneity was identified in analyses under all genetic models. However, in the subgroup of European population, the recessive model provided an OR of 2.54 (1.30-4.96), with no significant between-study heterogeneity. CONCLUSION: In conclusion, our meta-analysis indicated that IL-4 rs2243250 may increase TB risk in European population in recessive genetic model. Further research is needed to clarify the cause of ethnic difference in genetic association study.


Asunto(s)
Interleucina-4 , Tuberculosis , Estudios de Asociación Genética , Predisposición Genética a la Enfermedad , Humanos , Interleucina-4/genética , Polimorfismo Genético , Polimorfismo de Nucleótido Simple , Tuberculosis/genética
6.
Angew Chem Int Ed Engl ; 60(48): 25241-25245, 2021 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-34550636

RESUMEN

Atomically dispersed transition metal sites have been extensively studied for CO2 electroreduction reaction (CO2 RR) to CO due to their robust CO2 activation ability. However, the strong hybridization between directionally localized d orbits and CO vastly limits CO desorption and thus the activities of atomically dispersed transition metal sites. In contrast, s-block metal sites possess nondirectionally delocalized 3s orbits and hence weak CO adsorption ability, providing a promising way to solve the suffered CO desorption issue. Herein, we constructed atomically dispersed magnesium atoms embedded in graphitic carbon nitride (Mg-C3 N4 ) through a facile heat treatment for CO2 RR. Theoretical calculations show that the CO desorption on Mg sites is easier than that on Fe and Co sites. This theoretical prediction is demonstrated by experimental CO temperature program desorption and in situ attenuated total reflection infrared spectroscopy. As a result, Mg-C3 N4 exhibits a high turnover frequency of ≈18 000 per hour in H-cell and a large current density of -300 mA cm-2 in flow cell, under a high CO Faradaic efficiency ≥90 % in KHCO3 electrolyte. This work sheds a new light on s-block metal sites for efficient CO2 RR to CO.

7.
Small ; 14(13): e1703739, 2018 03.
Artículo en Inglés | MEDLINE | ID: mdl-29430832

RESUMEN

Proper design and simple preparation of nonnoble bifunctional electrocatalysts with high cost performance and strong durability for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is highly demanded but still full of enormous challenges. In this work, a spontaneous gas-foaming strategy is presented to synthesize cobalt nanoparticles confined in 3D nitrogen-doped porous carbon foams (CoNCF) by simply carbonizing the mixture of citric acid, NH4 Cl, and Co(NO3 )2 ·6H2 O. Thanks to its particular 3D porous foam architecture, ultrahigh specific surface area (1641 m2 g-1 ), and homogeneous distribution of active sites (C-N, Co-Nx , and Co-O moieties), the optimized CoNCF-1000-80 (carbonized at 1000 °C, containing 80 mg Co(NO3 )2 ·6H2 O in precursors) catalyst exhibits a remarkable bifunctional activity and long-term durability toward both ORR and OER. Its bifunctional activity parameter (ΔE) is as low as 0.84 V, which is much smaller than that of noble metal catalyst and comparable to state-of-the-art bifunctional catalysts. When worked as an air electrode catalyst in rechargeable Zn-air batteries, a high energy density (797 Wh kg-1 ), a low charge/discharge voltage gap (0.75 V), and a long-term cycle stability (over 166 h) are achieved at 10 mA cm-2 .

8.
Guang Pu Xue Yu Guang Pu Fen Xi ; 36(11): 3608-14, 2016 Nov.
Artículo en Zh | MEDLINE | ID: mdl-30199153

RESUMEN

UV-Vis absorbance, fluorescence, and Gas Chromatography Mass Spectrometry (GC-MS) were applied to the comparative study on sediment dissolved organic nitrogen (DON) in five typical lakes (Erhai lake, Dianchilake, Poyang lake, Wuhan Dong lake, and Taihu lake) in different lake regions with different nutrition status, revealing the relationship between structural and compositional characteristics of sediment DON and trophic level of lakes. The obtained results showed that: ①Structure of lake sediment DON in Yungui Plateau region is more stable, compared with those in Eastern Plain region, indicating its lower bioavailability. ②In Yungui Plateau region, the source and compositional characteristics of sediment DON weremore complex in Dianchi lake (a seriously polluted lake), and its sediment DON bioavailabilitywas relatively higher. While, with respect to the less polluted Erhai lake, the source of sediment DON is more simple with a higher stability in DON structure and composition, which is beneficial for maintaining its good water quality. ③In Eastern Plain region, nutrition status of Taihu lake was similer to Donghu lake. The structure and composition of sediment DON was complex. But the lower aromaticityand fewer Aromatic ring substituents abundance made their relatively weak nutrient retention ability, posing risk to water quality. With regard to Poyang Lake, the structure and composition of sediment DON was relatively simple, but nutrient retention ability was relatively strong, which played a positive role in maintaining good water quality. ④P(Ⅲ+Ⅴ, n)/P(Ⅰ+Ⅱ, n) values(the content ratio of humic-like substanceto protein-like substances)were in sequence of Dianchi Lake (33.14)>Erhai Lake(21.49)>Taihu Lake(9.06)>Donghu Lake(7.04)>Poyang Lake(4.83), while E(4)/E(6) values (the ratio of UV-Vis absorbance at 465 and 665 nm) were in sequence of Dianchi Lake (27.00)>Donghu Lake(6.65)>Poyang Lake(5.47)>Taihu(3.50)>Erhai Lake(2.31). In addition, P(Ⅲ+Ⅴ, n)/P(Ⅰ+Ⅱ, n) and E(4)/E(6) valueswere positively correlated with thecontents of the different nitrogen (N) forms in the sediments. The above information suggested that P(Ⅲ+Ⅴ, n)/P(Ⅰ+Ⅱ, n) and E(4)/E(6) values exhibited good discrimination degree among different trophic status lakes, and they were considered to indirectly indicate the nutrition levels of lakes to a certain extent.

9.
Cell Physiol Biochem ; 34(2): 288-98, 2014.
Artículo en Inglés | MEDLINE | ID: mdl-25034045

RESUMEN

BACKGROUND/AIMS: Obesity contributes to the development of cardiometabolic disorders such as type 2 diabetes, fatty liver disease and cardiovascular disease. Salvianolic acid B (Sal B) is a molecule derived from the root of Salvia miltiorrhiza (Danshen), which is a traditional Chinese medicine that is widely used to treat cardiovascular diseases. However, the role of Sal B in obesity and obesity-related metabolic disorders is unknown. In this study, we aimed to investigate the effects of Sal B on high-fat diet-induced obesity and determine the possible mechanisms involved. METHODS: Male C57BL/6J mice fed a high-fat diet for 12 weeks received a supplement of Sal B (100 mg/kg/day) by gavage for a further 8 weeks. These mice were compared to control mice fed an un-supplemented high-fat diet. 3T3-L1 preadipocytes were used in vitro studies. RESULTS: Sal B administration significantly decreased body weight, white adipose tissue weight, adipocyte size and lipid (triglyceride and total cholesterol) levels in obese mice. Eight weeks of Sal B administration also improved the intraperitoneal glucose tolerance test (IPGTT) and intraperitoneal insulin tolerance test (IPITT) scores in high-fat diet-induced obese mice. In 3T3-L1 preadipocytes that were cultured in vitro and induced to differentiate, Sal B reduced the accumulation of lipid droplets and lipid content in a dose-dependent manner. Immunoblotting indicated that Sal B decreased peroxisome proliferator-activated receptor gamma (PPARγ) and CCAAT/enhancer binding protein α (C/EBPα) expression but increased the expression of GATA binding protein 2 and 3 (GATA 2, GATA 3) both in vivo and in vitro. CONCLUSION: Our data suggest that Sal B may reduce obesity and obesity-related metabolic disorders by suppressing adipogenesis. The effects of Sal B in adipose tissue may be related to its action on PPARγ, C/EBPα, GATA-2 and GATA-3.


Asunto(s)
Benzofuranos/farmacología , Dieta Alta en Grasa , Obesidad/fisiopatología , PPAR gamma/metabolismo , Aumento de Peso/efectos de los fármacos , Células 3T3-L1 , Animales , Hiperlipidemias/prevención & control , Masculino , Ratones , Ratones Endogámicos C57BL , Obesidad/etiología
10.
Chem Commun (Camb) ; 60(47): 6039-6042, 2024 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-38775147

RESUMEN

It is a challenge to design a photocathode with well-defined active sites for efficient photoelectrocatalytic CO2 reduction. Herein, single-atom Ni sites are integrated into Si nanowires to develop a novel photocathode, denoted as Ni-NC/Si. The photocathode demonstrates a stable faradaic efficiency for CO production, approaching nearly 100% at -0.6 V vs. RHE. The introduction of single-atom Ni sites provides sufficient active sites for CO2 reduction, thereby improving the selectivity towards CO formation.

11.
Nat Commun ; 15(1): 1264, 2024 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-38341446

RESUMEN

Nitrate (NO3‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm-2 and enables an over 99% NO3--to-NH3 conversion efficiency. We also convert NO3‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3‒-to-NH3 conversion.

12.
ACS Appl Mater Interfaces ; 15(19): 23115-23123, 2023 May 17.
Artículo en Inglés | MEDLINE | ID: mdl-37129923

RESUMEN

In rechargeable Li-O2 batteries, the electrolyte and the electrode are prone to be attacked by aggressive intermediates (O2- and LiO2) and products (Li2O2), resulting in low energy efficiency. It has been reported that in the presence of water, the formation of low-activity LiOH is more stable for electrolyte and electrode, effectively reducing the production of parasitic products. However, the reversible formation and decomposition of LiOH catalyzed by solid catalysts is still a challenge. Here, a freestanding metal-organic framework (MOF)-derived honeycomb-shape porous MnOC@CC cathode was prepared for Li-O2 batteries by in situ growth of urchin-like Mn-MOFs on carbon cloth (CC) and carbonization. The battery with the MnOC@CC cathode exhibits an ultrahigh practical discharge specific capacity of 22,838 mAh g-1 at 200 mA g-1, high-rate capability, and more stable cycling, which is superior to the MnOC powder cathode. X-ray diffraction and Fourier transform infrared results identify that the discharge product of the batteries is LiOH rather than highly active Li2O2, and no parasitic products were found during operation. The MnOC@CC cathode can induce the formation of flower-like LiOH in the presence of water due to its unique porous structure and directional alignment of Mn-O centers. This work achieves the reversible formation and decomposition of LiOH in the presence of water, offering some insights into the practical application of semiopen Li-O2 batteries.

13.
J Phys Chem Lett ; 14(27): 6301-6308, 2023 Jul 13.
Artículo en Inglés | MEDLINE | ID: mdl-37399566

RESUMEN

The low solubility of CO2 molecules and the competition of the hydrogen evolution reaction (HER) in aqueous electrolytes pose significant challenges to the current photoelectrochemical (PEC) CO2 reduction reaction. In this study, inspired by the bilayer phospholipid molecular structure of cell membranes, we developed a Cu2O/Sn photocathode that was modified with the bilayer surfactant DHAB for achieving high CO2 permeability and suppressed HER. The Cu2O/Sn/DHAB photocathode stabilizes the *OCHO intermediate and facilitates the production of HCOOH. Our findings show that the Faradaic efficiency (FE) of HCOOH by the Cu2O/Sn/DHAB photoelectrode is 83.3%, significantly higher than that achieved with the Cu2O photoelectrode (FEHCOOH = 30.1%). Furthermore, the FEH2 produced by the Cu2O/Sn/DHAB photoelectrode is only 2.95% at -0.6 V vs RHE. The generation rate of HCOOH by the Cu2O/Sn/DHAB photoelectrode reaches 1.52 mmol·cm-2·h-1·L-1 at -0.7 V vs RHE. Our study provides a novel approach for the design of efficient photocathodes for CO2 reduction.

14.
Chem Commun (Camb) ; 59(39): 5914-5917, 2023 May 11.
Artículo en Inglés | MEDLINE | ID: mdl-37170969

RESUMEN

The limited mass transfer of CO2 and the competitive hydrogen evolution reaction (HER) during photoelectrochemical (PEC) CO2 reduction usually result in low CO2 reduction activity. Here, we constructed a Cu2O/Sn/PTFE photocathode with a hydrophobic surface based on Cu2O by physical vapor deposition and a dipping method. The CO faradaic efficiency (FE) increased from 34.5% (Cu2O) to 95.1% (Cu2O/Sn/PTFE) at -0.7 V vs. RHE, and the FEH2 decreased from 27.9% (Cu2O) to 3.8% (Cu2O/Sn/PTFE). The introduction of the hydrophobic layer enhances the local CO2 concentration on the electrode surface and effectively isolates H+ from the aqueous electrolyte, thereby enhancing the CO2 reduction activity.

15.
Waste Manag ; 143: 186-194, 2022 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-35272201

RESUMEN

With the growing number of lithium-ion batteries (LIBs) that are consumed by worldwide people, recycling is necessary for addressing environmental problems and alleviating energy crisis. Especially, it is meaningful to regenerate LIBs from spent batteries. In this paper, the microwave hydrothermal method is used to replenish lithium, assemble particles and optimize the crystal structure of the spent lithium cobalt oxide. The microwave hydrothermal process can shorten the reaction time, improve the internal structure, and uniformize the particle size distribution of lithium cobalt oxide. It helps to construct a regenerated lithium cobalt oxide (LiCoO2) battery with high-capacity and high-rate properties (141.7 mAh g-1 at 5C). The cycle retention rate is 94.5% after 100 cycles, which is far exceeding the original lithium cobalt oxide (89.7%) and LiCoO2 regenerated by normal hydrothermal method (88.3%). This work demonstrates the feasibility to get lithium cobalt oxide batteries with good structural stability from spent lithium cobalt oxide batteries.


Asunto(s)
Litio , Microondas , Cobalto , Suministros de Energía Eléctrica , Humanos , Óxidos , Reciclaje
16.
ACS Appl Mater Interfaces ; 14(42): 47737-47746, 2022 Oct 26.
Artículo en Inglés | MEDLINE | ID: mdl-36228181

RESUMEN

Hydrogen generation through photoelectrochemical (PEC) technology is one of the most appropriate ways for delivering sustainable fuel. Simultaneously, anisotropic properties will be exhibited by the materials with low crystal symmetry, allowing the tuning of the PEC properties by controlling the crystallographic orientation and exposed facets. Therefore, we synthesized copper tungstate films (CuWO4) with highly exposed (100) crystal facets by regulating anions in the precursor solution. According to experimental characterization and density functional theory calculations, the CuWO4 film with a high exposure ratio of the (100) crystal facet has promoted charge transport with trap-free mode and reduced recombination of electrons and holes. Meanwhile, the oxygen evolution reaction is promoted on the (100) facet because of the relatively low energy barrier. Compared to the CuWO4 with other mixed exposure facets, CuWO4 with a highly exposed (100) facet presents a twofold current density (0.38 mA/cm2) and one-fifteenth electron transit time (0.698 ms) and also has great stability (more than 6 h). These results provide an easy way to enhance the PEC performance by modulating the exposure facets of the film electrode.

17.
Chem Commun (Camb) ; 58(67): 9421-9424, 2022 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-35916216

RESUMEN

The generation of multi-carbon products on the Cu2O photocathode remains a great challenge. Herein, effective charge separation and surface catalytic reaction are achieved for photoelectrochemical CO2 reduction through plasmon metal (Ag) decoration on Cu2O nanowires. The Cu2O/Ag composite photocathode achieves a 47.7% faradaic efficiency for CH3COOH and the generation rate is 212.7 µmol cm-2 h-1 under illumination, which is about five times that in dark (44.4 µmol cm-2 h-1) at -0.7 V vs. RHE.

18.
J Colloid Interface Sci ; 628(Pt A): 1067-1076, 2022 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-36163054

RESUMEN

As one of the most promising candidates for power sources, the rechargeable Zn-air batteries have attracted much attention due to their high energy density. However, Zn-air batteries suffer from sluggish kinetics of oxygen reduction (ORR) and oxygen evolution reaction (OER) during the discharge and charge process. Herein, a FeN2-doped carbon with a unique three-dimensional (3D) porous structure (CeO2-FeNC-5) was synthesized as an electrocatalyst for Zn-air batteries by one-step pyrolysis and introducing CeO2 to tune the coordination environment of Fe atoms. Extended X-ray absorption fine structure (EXAFS) results indicate that the introduction of CeO2 can convert FeN3 moieties into FeN2 moieties. The CeO2-FeNC-5 exhibits a more positive half-wave potential of 0.902 V for ORR, and a low overpotential of 0.327 V at 10 mA cm-2 for OER. Furthermore, the Zn-air battery with CeO2-FeNC-5 achieve a maximum power density (169 mW cm-2), a high open voltage platform (1.47 V) and superior cycling stability (200 h). The unique 3D porous structure provides channels for mass transport and exposes sufficient active sites to facilitate the ORR and OER processes. Calculations prove that FeN2 moieties are beneficial to O2 adsorption on Fe/N-doped carbon surface. This work provides an effective strategy for designing and synthesizing FeNx-doped carbon matrix electrocatalysts for sustainable metal-air batteries.

19.
ACS Appl Mater Interfaces ; 13(24): 28140-28149, 2021 Jun 23.
Artículo en Inglés | MEDLINE | ID: mdl-34111922

RESUMEN

It is still a challenge to achieve efficiently controlled preparation of functional oxygen reduction reaction (ORR) carbon electrocatalysts with multi-preferred structures (hierarchically porous networks and specific carbon-nitrogen bonds) from carbohydrate-containing small molecules via simple one-step pyrolysis. Based on the step-by-step spontaneous gas-foaming strategy, we successfully prepare 3D hierarchically porous networks with tunable N sites (NP/NG ≈ 1:1) by pyrolyzing diverse carbohydrates (glucose, maltose, and cyclodextrin) using nonmetal-metal dual inorganic sacrificial templates. In situ evaporation templates can simplify the procedure of the experiments and avoid the active site loss compared with traditional hard templates. Crucially, dual inorganic sacrificial templates can induce abundant defects and microscopic pore structures (the specific surface area increased from 922.403 to 1898.792 m2·g-1) and tunable N sites compared with single nonmetal sacrificial templates. The regulatory mechanism of dual inorganic templates on N sites (NP/NG ≈ 1:1) is independent of the polymeric state of carbohydrate precursors or even the carbonization condition of the pyrolysis process. A series of carbon materials prepared by this strategy all have ORR-preferred structures and exhibit low ORR overpotentials compared with Pt/C. For instance, the Zn-air battery with ßCD-DSC-950-1 exhibits an open-circuit potential of 1.51 V and a peak power density of 180.89 mW·cm-2, higher than those of Pt/C (1.47 V, 174.94 mW·cm-2). In general, the conversion of carbohydrate-containing small molecules to functional carbon materials provides a new strategy for the development of carbonaceous electrocatalysts.

20.
Chem Commun (Camb) ; 57(49): 6011-6014, 2021 Jun 17.
Artículo en Inglés | MEDLINE | ID: mdl-34028484

RESUMEN

Bi-C catalysts with the three-phase interfaces of CO2 (gas), electrolyte (liquid) and catalyst (solid) exhibit a remarkable electrocatalytic CO2 reduction (ECR) to formate selectivity (above 95% faradaic efficiency) with a high current (100 mA cm-2) in a broad potential range.

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