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31.
《International Journal of Hydrogen Energy》2022,47(59):24796-24806
Developing inexpensive and efficient electrocatalysts for hydrogen evolution reaction (HER) in both acidic and alkaline mediums is of great significance to the hydrogen energy industry. Hereby, we prepared a mixture of precursors with homogeneous composition by using the chelating ability of soybean protein isolate (C and N source) and phytic acid (dopant and phosphating agent) with cobalt ions, and achieved one-step synthesis and construction of Co2P/N–P co-doped porous carbon composite by carbonization at 800 °C. The as-synthesized Co2P/NPPC-800 electrocatalyst exhibits low HER overpotentials of 121 and 125 mV at 10 mA cm?2 in 0.5 M H2SO4 and 1.0 M KOH, which are close to those of the commercial Pt/C catalyst. Additionally, the NPPC substrate surrounding the Co2P could diminish the corrosion during the HER, and Co2P/NPPC-800 displays good stability and durability. Furthermore, this work offers a convenient synthesis strategy for phosphide/doped porous carbon composites in other electrochemical energy technologies. 相似文献
32.
《International Journal of Hydrogen Energy》2022,47(71):30494-30502
Metal-organic frameworks (MOFs) have emerged as efficient electrocatalysts due to the features of high specific surface area, rich pore structure and diversified composition. It is still challenging to synthesize self-supporting MOF-based catalysts using simple and low-cost fabrication methods. Herein, we successfully fabricated Ni-doped MIL-53(Fe) supported on nickel-iron foam (Ni-MIL-53(Fe)/NFF) as efficient electrocatalyst. A facile two-step solvothermal method without adding any metal salts was used, which can simplify the fabrication process and reduce the experimental cost. In the fabrication process, the bimetallic Ni-MIL-53(Fe)/NFF was in situ converted from an intermediate NiFe2O4/NFF. The obtained material exhibits outstanding electrocatalytic oxygen evolution performance with a low overpotential of 248 mV at 50 mA cm?2, and a small Tafel slope of 46.4 mV dec?1. This work sheds light on the simple and efficient preparation of bimetallic MOF-based material, which is promising in electrocatalysts. 相似文献
33.
《International Journal of Hydrogen Energy》2022,47(77):32940-32954
The combination of inorganic (e.g., ferrite nanoparticles) and organic (e.g., conducting polymers) materials in the fabrication of heterojunctions or composites is an attractive scheme in the field of photocatalysis. We took the advantage of this phenomenon by fabricating MFerrite (M = Co, Ni, and Zn) @polypyrrole (MFerrite@Ppy) nanocomposites with a varying weight percentage of Ppy for the hydrogen production through photocatalytic water splitting under visible light irradiation. The structural, spectral, morphological, compositional, and optical features of the as-prepared nanocomposites were analyzed in full depth. The average crystallite sizes were estimated to be 30–40 nm from the XRD patterns which were further validated by TEM images from which a core-shell structure of the composites can be inferred. Likewise, the SEM images revealed spherical Ppy particles with a diameter in the range of 100–300 nm. From a photocatalytic viewpoint, CoFerrite@30Ppy is endowed with some peculiar characteristics including but not limited to strong light-harvesting ability (ranging between 300 and 650 nm), narrow optical band gap (as low as 1.6 eV), and higher photoluminescence (PL) lifetime (6.41 ns) which justify why it stands out among all composites in terms of photocatalysis. Under 8 h illumination of simulated visible light and using triethanolamine (TEOA) as a hole scavenger and Eosin-Y (EY) as a dye sensitizer, the photocatalytic hydrogen evolution (HER) amount for CoFerrite@30Ppy was found to be 10.44 mmol g?1, far greater than any other composite catalysts in this study. From the PL spectra, it can be pointed out that sensitization of CoFerrite with 30 wt % Ppy conduces to simultaneous deceleration of the electron-hole recombination process and acceleration of the transference of excitons within the system. 相似文献
34.
《International Journal of Hydrogen Energy》2022,47(78):33352-33360
Developing highly efficient and stable noble metal-free electrocatalysts with excellent catalytic surface for oxygen evolution reactions (OER) is an essential link for stimulating hydrogen generation from water electrolysis. Herein, the scalloped nickel/iron vanadium oxide coated vanadium dioxide (named as VO2@NFVO) has been successfully decorated via a urea-induced chemical etching-reconstruction process in the alkaline solution containing Fe2+ and Ni2+. Corresponding experimental measurements clearly show that favorable chemical etching occurs with the formation of new phases (eg, Ni3V2O8, FeVO4), which make it expose a large number of active sites and regulate the electron density of the active center, thus thereby dramatically enhancing the electrocatalytic performance by promoting electron transfer and optimizing the adsorption energy of reaction intermediates. Under optimized condition, the obtained VO2@NFVO delivers excellent activity merely with smaller overpotential of 290 mV at 10 mA cm?2, outperforming benchmark RuO2 catalyst in an alkaline solution. Moreover, its superior durability is verified by chronoamperometry testing. This simple etching-reconstruction strategy opens a new avenue for the preparation of vanadium-based electrocatalysts. 相似文献
35.
《International Journal of Hydrogen Energy》2022,47(81):34376-34386
Searching high-active, stable and abundant bifunctional catalysts to replace noble metals for hydrogen and oxygen evolution reactions (HER and OER) is desired. Herein, petal-like NiCoP sheets were synthesized on carbon paper covered with a 3D nitrogen-doped carbon nanofiber network (NiCoP/CNNCP) by a simple hydrothermal process followed by phosphorization. The HER overpotential in 0.5 M H2SO4 and OER overpotential in 1 M KOH of the NiCoP/CNNCP electrode only required 55 mV and 260 mV to drive a current density of 10 mA cm?2, respectively, which was comparable or even better than most nickel-and cobalt-based phosphide catalysts. The overall water-splitting electrolyzer with an asymmetric electrolyte system assembled using NiCoP/CNNCP as bifunctional electrodes required an extremely low cell voltage of 1.04 V to achieve a current density of 10 mA cm?2, which was much lower than almost all alkaline electrolysis systems. 相似文献
36.
《International Journal of Hydrogen Energy》2022,47(93):39486-39498
Adjusting the band gap of organic-inorganic composites by chemical bonding can effectively construct Step-scheme (S-scheme) heterojunctions, featuring properties of fast photogenerated charge migration and excellent photocatalytic performance. In this work, a novel perylene-3, 4, 9, 10-tetracarboxylicdiimide (PDI)-titanium dioxide (TiO2) heterojunction is elaborately synthesized through simple solvent compounding method. The monodispersed spherical TiO2 nanoparticles was prepared with the capping agents of oleylamine and oleic acid, and suffered by a ligand exchange process with nitrosonium tetrafluoroborate (NOBF4) to remove oleylamine and oleic acid. The NOBF4 ligands were further replaced by PDI super molecular nanosheets to obtain two dimensional (2D)-zero dimensional (0D) PDI-TiO2 composites. TiO2 nanoparticles are evenly anchored on the surface of PDI nanosheets with intimate contact. The PDI-TiO2 composites has emerged considerably superior activity in hydrogen evolution. The highest hydrogen evolution rate for PDI-TiO2composites with the PDI weight percentage of 2.4% was 9766 μmol h?1 g?1 under solar light irradiation, which is 2.56 times of TiO2-NOBF4 catalyst. Moreover, PDI-TiO2 composites possess stoichiometric overall water splitting performance with H2 and O2 release rates of 238.20 and 114.18 μmol h?1 g?1. The superior photocatalytic performance of PDI-TiO2 composites can be attributed to the dramatic increase in visible and NIR light absorption caused by π-π stacking structure of PDI, the prevented charge recombination by the S-scheme heterojunction, and the enhanced oxygen evolution by the stronger oxidation capability of PDI. PDI supramolecular nanosheets may work as a novel functional support for many types of semiconductor nanomaterials as graphene, which will display a wide range of application prospects in the energy and environmental fields. 相似文献
37.
Fengjun Yin Xiaohui Yang Lei Zheng Ling Fang Sha Wang Hong Liu 《American Institute of Chemical Engineers》2022,68(6):e17669
Acid–base transport is integral to many important interfacial reactions in various fields of chemistry, but its theoretical foundation is lacked. Herein, a common acid–base transport model is established owing to the success in deriving buffer transport equations. This model is applicable to most buffer systems by flexibly integrating the transport equations in terms of buffer components, and is verified through the model relationships of buffer transport limiting current by using hydrogen evolution reaction experiments. Based on model calculations, two diagram approaches are proposed to depict the dynamic pH response and aid buffer operation optimizations. The model and methods allow us to quantify the rate-limiting effect of acid–base transport on interfacial reactions and to precisely control the effect through medium regulations. Furthermore, the model has laid the foundation of dynamic pH effect on species transformation and process mechanism, which can be of wide interest in the chemistry encompassing interfacial reactions. 相似文献
38.
《International Journal of Hydrogen Energy》2022,47(4):2279-2292
A new catalyst for both water reduction and oxidation, based on an infinite chain, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n, is formed by the reaction of NiCl2, 1,3-propanediamine (tn) and K3 [Fe(CN)6]. {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can electro-catalyze hydrogen evolution from a neutral aqueous buffer (pH 7.0) with a turnover frequency (TOF) of 1561 mol of hydrogen per mole of catalyst per hour (H2/mol catalyst/h) at an overpotential (OP) of 837 mV {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n also can electro-catalyze O2 production from water with a TOF of ~45 mol O2 (mol cat)?1s?1 at an OP of 591 mV. Under blue light (λ = 469 nm), together with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H2A) as a sacrificial electron donor, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can photo-catalyze hydrogen generation from an aqueous buffer (pH 4.0) with a turnover number (TON) of 11,450 mol H2 per mole of catalyst (mol of H2 (mol of cat)?1) during 10 h irradiation. The average of apparent quantum yield (AQY) is as high as 40.96% during 10 h irradiation. Studies indicate that {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n exists in two forms: a cyano-bridged chain ({[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n) in solid, and a salt ([Ni(tn)2]3 [Fe(CN)6]2) in aqueous media; Catalytic reaction occurs on the nickel center of [Ni(tn)2]2+, and the introduction of [Fe(CN)6]3- can improve the catalytic efficiency of [Ni(tn)2]2+ for H2 or O2 generation. We hope these findings can afford a new method for the design of catalysts for both water reduction and oxidation. 相似文献
39.
《International Journal of Hydrogen Energy》2022,47(5):2992-3000
Energy depletion and environmental pollution are still serious challenges for human beings. The application of hydrogen energy should be a promising strategy to address this issue. However, the hydrogen production should be one shortcoming for hydrogen energy. The hydrogen evolution reaction (HER) based on electrocatalysis is an effective way to enhance the hydrogen generation with small energy consumption under ambient conditions. Many works have been devoted to develop high performance catalysts to satisfy the HER processes. Nevertheless, the mechanism about facet-dependence and composition-dependence influence is still need to deeply study. Hereon, based on density functional theory calculations, the [100], [110], and [111] facets of NixPy (Ni3P, Ni2P, NiP, NiP2, NiP3) systems were created and their HER catalytic activity were used to reveal the underline mechanism. By analyzing the variation of Gibbs free energy, it was found that the structural composition has a greater effect on HER than the facet. Significantly, the Ni2P(111) surface with Ni/P-termination has the best HER performance for all samples in present work. Through exploring the electron transfer of H with surrounding atoms during the HER process, the H adsorption mechanism as well as its reaction mechanism has been revealed. The deep insights in this work provide an important fundamental that the contents of non-metal for compounds catalysts can heavily influence the performance of HER, which should give more guidance for designing new catalysts. 相似文献
40.
《Ceramics International》2022,48(12):17086-17094
The composition of polymer derived ceramics could be readily tuned through controlling the structure and element content of the polymer precursors, and investigation on the effect of the element on microstructure evolution is important to the design of advanced ceramics. In this article, the effect of carbon content in SiBCO polymer precursors was systematically investigated. The polymer network and thermal stability of polymer precursors and the carbon content of pyrolyzed SiBCO ceramic could be readily tuned by controlling the DVB amount used. Carbon contributed to the formation of graphitic carbon in SiBCxO ceramics and inhibited the growth of β–SiC and SiO2 crystals at 1600 °C, but lead to an increase in the graphitic carbon phase at 1800 °C. 相似文献