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1.
《International Journal of Hydrogen Energy》2023,48(14):5506-5517
A series of manganese corroles bearing different substituents had been prepared and characterized by UV–vis, 1H NMR, 19F NMR, HRMS and XPS. These manganese corrole complexes were applied to electrocatalytic hydrogen evolution reaction (HER) for the first time. The results showed that manganese corroles are effective catalysts for HER in DMF solvent by using acetic acid (AcOH), trifluoroacetic Acid (TFA) and p-toluenesulfonic acid (TsOH) proton sources, and strong acid leads to higher electrocatalytic activity. When using TsOH as proton source, protonation of corroles ligand may be involved in HER. The electrocatalytic HER activity can be improved by increasing the electron-withdrawing substituent of the corrole macrocycle in both organic and aqueous media. 相似文献
2.
Pengfei Zhou Dong Liu Zhaorui Wen Mingpeng Chen Qingju Liu Ye Ke Shengwen Li Shi Chen Chi Tat Kwok Shuangpeng Wang Yuxin Tang Hui Pan 《International Journal of Hydrogen Energy》2021,46(36):18878-18886
Hydrogen evolution reaction (HER) is a critical process in electrocatalytic water splitting for hydrogen production. However, the development of low-cost electrocatalysts for highly efficient HER is still a huge challenge. Hence, we fabricate a multi-metal phosphide on Ni foam, FeCoNiNbxP, through a facile hydrothermal reaction followed by phosphorization. We find that Nb promotes the formation of metal phosphides, and the main phases of the catalysts with Nb are multiphase phosphides. Importantly, the Nb incorporation significantly improves the HER activity of FeCoNiP. We show that FeCoNiNb0.3P has the best HER activity, which only requires an overpotential of 78 mV to achieve a current density of 10 mA cm?2 in 1 M KOH, and demonstrates excellent stability under both constant potential and varied current densities. Our findings show that the multiple-metal compounds are beneficial to the improvement of catalytic activity and provide guidance on the design of novel catalysts for applications. 相似文献
3.
《International Journal of Hydrogen Energy》2023,48(29):10891-10902
Two cobalt complexes [Co(L1)2](ClO4)2⋅4CH3CN (1) and [Co(L2)2](ClO4)2⋅2CH3CN⋅0.5H2O (2) of the new click-derived bistriazolylpyridines 2,6-bis(1-(pyridin-2-yl)-1H-1,2,3-triazol-4-yl)isonicotinate methyl ester (L1) and 2,6-bis-(1-methoxycarbonylmethyl-1H-1,2,3-triazol-4-yl)isonicotinate methyl ester (L2) were synthesized and characterized. The electrocatalytic hydrogen evolution reaction (HER) mediated by complexes 1 and 2 was studied in CH3CN in the presence of acetic acid. Both complexes catalyzed HER with low overpotentials and high Faradaic efficiencies (370 mV and 93% for 1, 300 mV and 95% for 2). The distal substituents on the triazolyl moiety of the bistriazolylpyridines have apparent impacts on the redox and catalytic properties of 1 and 2. The catalytic behaviors were further studied using spectroelectrochemistry and the reductant cobaltocene. It was found that the reduction of the bistriazolylpyridines was necessary for the catalytic activity. Plausible pathways were proposed for the HER mediated by 1 and 2. This work provided some hints for the preparation of HER catalysts based on the redox-active triazolylpyridine ligands. 相似文献
4.
《International Journal of Hydrogen Energy》2022,47(64):27452-27459
Electrocatalytic hydrogen evolution reaction (HER) is a simple way to generate environment-friendly hydrogen energy. Due to the high price and low content, the wide application of noble metal-based electrocatalysts is limited. It is of great significance to study inexpensive, high-performance non-precious metal-based electrocatalysts. In this work, bimetallic nitride (Co/WN@NC) was successfully prepared through a one-step high-temperature calcination way using dicyandiamide (DCA), bimetallic polyoxometalates, and cobalt nitrate. Co/WN@NC exhibits outstanding catalytic performance with the same overpotentials of 143 mV in both alkaline and acidic media at 10 mA cm?2. The Tafel slopes are 90 mV dec?1 and 118 mV dec?1, respectively. Co/WN@NC exhibits good stability in acidic and alkaline solutions for up to 30 h. The splendid catalytic performance can be mainly ascribed to the synergistic effect between Co and WN. This work shows experimental guiding significance for preparing simple transition metal-based electrocatalysts. 相似文献
5.
《International Journal of Hydrogen Energy》2020,45(11):6110-6119
Hydrogen evolution reaction (HER) is regarded as a feasible strategy for producing high-purity hydrogen from abundant water. It is significant yet challenging for synthesis of Pt-based pH-universal HER electrocatalysts by substantially reducing the Pt loading without any decay in the activity. Herein, bimetallic PtRh alloyed dendritic nanoassemblies (DNAs) were efficiently prepared by a facile one-pot solvothermal strategy in oleylamine (OAm), coupling with the aid of glycine and cetyltrimethylammonium chloride (CTAC). By virtue of the unique branch-like structures and compositions advantages, the PtRh DNAs catalyst showed steeply enhanced HER activity with small overpotentials (i.e. 28 mV in 1.0 M KOH, 23 mV in 1.0 M phosphate buffer solution and 27 mV in 0.5 M H2SO4) at the current density of 10 mA cm−2, surpassing those of commercial Pt/C under such conditions. This work provides a facile and rational strategy to construct advanced Pt-based bimetallic electrocatalyst for energy-correlated applications. 相似文献
6.
《International Journal of Hydrogen Energy》2020,45(53):28682-28695
The excessive exhaustion of conventional fossil fuels and increasingly severe environmental issues prompt us to grope for high-performance and cost-effective catalysts for hydrogen evolution reaction (HER) by electrocatalytic water splitting. In this work, nanocoral-like NiSe2 catalysts modified with CeO2 have been successfully prepared through one-pot hydrothermal route and utilized to electrocatalytic HER in alkaline solution. It turns out that nanocoral-like NiSe2 (labeled as CNS-2) catalyst delivers current densities of 10 and 50 mA cm−2 at overpotentials of only 130 and 242 mV, respectively. Additionally, CNS-2 takes on a small Tafel slope of 115 mV dec−1 and low charge transfer resistance, revealing a quicker Faradaic process and more favorable HER kinetics. Furthermore, it displays considerable long-term stability during the constant hydrogen producing. The strategy of fabricating NiSe2 modified with CeO2 unfolds a novel angle of view for exploiting highly efficient and durable catalysts for electrocatalytic HER. 相似文献
7.
《International Journal of Hydrogen Energy》2022,47(7):4631-4640
In this study, polyaniline (PANI) with abundant protonated regions was used for the first time as a palladium (Pd) support for enhanced performance in hydrogen evolution reaction (HER). For this purpose, the hierarchical Pd@PANI nanofiber electrode was easily synthesized by electrochemical polymerization of aniline on Au followed by potential-controlled electrochemical deposition of Pd nanoclusters on the PANI. The reported catalyst was characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and field-emission scanning electron microscopy. Linear sweep voltammetry analysis was performed to evaluate the HER performance. Ion transfer behavior was investigated using electrochemical impedance spectroscopy analysis. The electrochemical tests show that the Pd@PANI/Au electrode has a low overpotential of ~60 mV at 10 mA cm?2 and a small Tafel slope of 35 mV dec?1 for HER in acidic media, with high catalytic activity and stability. These features will make the Pd@PANI/Au a promising candidate as a high-performance electrocatalyst for HER applications. 相似文献
8.
《International Journal of Hydrogen Energy》2020,45(16):9535-9545
Reasonable design of efficient and stable catalysts with low cost and abundant natural reserves is vital for electrocatalytic water splitting. Herein, novel nanotremella-like Bi2S3/MoS2 composites with different mass ratios between Bi2S3 and MoS2 have been successfully prepared through a hydrothermal approach and further applied to hydrogen evolution reaction (HER) in 1.0 M KOH electrolyte for the first time. When the mass ratio of Bi2S3 and MoS2 is 5:5, as-prepared nanotremella-like Bi2S3/MoS2 (marked as BMS-5) manifests favorable HER catalytic activity with overpotential of 124 mV at current density of 10 mA cm−2 and relatively low Tafel slope of 123 mV dec−1. Moreover, it exhibits an extraordinary durability for uninterrupted hydrogen generation. The enhanced HER performances are ascribed to the synergistic effects between Bi2S3 and MoS2, giving rise to large electrocatalytic active area and fast HER kinetics. The results pave a new path to design and construct excellent Bi2S3/MoS2 nanomaterials for electrocatalytic hydrogen generation. 相似文献
9.
《International Journal of Hydrogen Energy》2021,46(74):36763-36770
The hydrogen evolution reaction (HER) is a key step for producing hydrogen by water electrolysis, and an economical, facile and environment friendly method of fabricating catalysts for HER is urgent and essential. In this work, we design a high efficient and stable HER catalyst though a simple adsorption and pyrolysis method. The fabricated catalyst presents ruthenium (Ru) quantum dots (QDs) uniformly distributes on the carbon nanofibers (CNF) with a three dimensional (3D) networks structure (Ru@CNF). By means of quantum size effect of Ru QDs and the 3D networks structure of the carbon nanofibers, the former is beneficial to provide more catalytic active sites and the latter is in favour of electron transport. The sample Ru@CNF exhibits a low overpotential of 20 mV at a current density of 10 mA cm−2 and Tafel slope of 31 mV dec−1 in 1 M KOH, which is better than that of Pt/C (28 mV and 36 mV dec−1), and most of reported Ru-based and transition metal catalysts. Furthermore, it exhibits robust stability when testing at an overpotential of 75 mV for 24 h. Therefore, this work provides a low-cost, simple and feasible method for fabricating HER catalyst, which possesses commercial application prospect in the field of producing hydrogen by water electrolysis. 相似文献
10.
《International Journal of Hydrogen Energy》2022,47(2):902-916
Tungsten carbides (W2C and WC) materials, as promising non-precious electrocatalysts, possess highly efficient activity for HER. Herein, N-doped graphene supported tungsten carbide (N–W2C/WC) nanocomposite is synthesized by spray drying process followed with a two-step pyrolysis treatment, which exhibits a remarkable hydrogen evolution reaction (HER) activity and excellent stability in acidic solution and alkaline solution. N–W2C/WC displays low overpotentials of 166 mV and 125 mV to achieve a current density of 10 mA cm?2 and small Tafel slopes of 60.97 and 62.66 mV dec?1 in 0.5 M H2SO4 and 1.0 M KOH, respectively. After 1000 cycles, the electrocatalytic activity of N–W2C/WC is almost no change in acidic media but slightly decreases in alkaline media. This work might provide a new way to explore high comprehensive performance tungsten-based electrocatalyst for HER. 相似文献
11.
Xiaobing Xu Wei Zhong Mengmeng Chen Lei Zhang Guangxiang Liu Youwei Du 《International Journal of Hydrogen Energy》2021,46(12):8567-8577
There are many tremendous challenges to enhance the hydrogen evolution reaction (HER) activity of MoS2. In this study, nanoflower-like Co–MoS2/NiCoS structure supported on reduced Graphene Oxide (rGO) was rationally developed via a simple hydrothermal route, where the synergistic regulations of both interface structural and electronic conductivity were successfully presented by using controllable interface engineering and Co metal ions doped into MoS2 nanosheets. Ascribed to the 3D flower-like nanostructure with massive active sites, the interface coupling effect between MoS2 and Ni–Co–S phase, and Co-doped MoS2 can modulate its surface electronic density. The optimal Co–MoS2/NiCoS/rGO hybrid exhibits excellent HER activity in 1.0 M KOH, with a small overpotential (η10, 84 mV) at 10 mA cm?2 and a low Tafel slope (46 mV dec?1), accompanied by good stability. This work provides an effective route to produce other electrocatalysts based on interface structure and electronic conductivity engineering for HER in the future. 相似文献
12.
《International Journal of Hydrogen Energy》2019,44(31):16537-16547
Hydrogen evolution reaction has been recognized as a green technology in the field of electrochemical energy conversion and storage devices. Nevertheless, it is necessary task to finding an economical and effective electrocatalysts for HER. Among the different HER catalysts, the cobalt disulfide (CoS2) showed an excellent HER activity owing to its low cost, easy to synthesize and good stability. Hence, in this work, we prepared a series of CoS2/CNT composites with different contents CNT from 4 to 12 wt% by a simple one-step hydrothermal method to investigate the influence of CNT on HER activity of CoS2. The structural and morphological properties of the obtained samples were analyzed through XRD, SEM, HR-TEM, and XPS. The SEM images of CoS2/CNT composite showed the spherical-shaped CoS2 covered by the CNT nanostructure. In addition, the electrochemical tests were carried out using 0.5 M H2SO4 solution in order to assess their HER activity. The attained electrochemical results showed that the CoS2/CNT composite with 8% CNT offers an outstanding HER activity with the smallest overpotential of 155 mV at 10 mA cm−2 and lowest Tafel slope of 59 mV dec−1 when compared with other composites. Also, the optimized CoS2/CNT composite provided excellent stability in the acidic medium after 1000 cycles. Therefore, the as-synthesized CoS2/CNT composite will be an efficient, low-cost and Pt-free electrocatalyst for HER application. 相似文献
13.
《International Journal of Hydrogen Energy》2022,47(12):7713-7723
Molybdenum disulfide (MoS2) is a 2D layered structured material with a Mo:S of 1:2 and is a great attention seeker for hydrogen production through water-splitting. In the present work, we prepared nanostructured MoSx with different sulfur molar concentrations (x = 2, 1, 0.5) through a one-step hydrothermal method. The decrease in sulfur concentration resulted in a new phase that is MoO3 with a Mo:S of 1:0.5. The structural, morphological, and optical properties of all the samples were studied through X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform Infrared spectroscopy (FTIR), and Ultraviolet–Visible (UV–Vis) spectroscopy, respectively. Moreover, the electrochemical behavior was studied using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), linear sweep voltammetry (LSV), and Tafel slope. Optimum properties were observed for Mo:S (1:1) with an onset potential of 96 mV, an overpotential of 130 mV for hydrogen evolution reaction (HER) coupled with a specific capacitance of 889 F/g and low charge transfer resistance of 43 Ω. Further, it was noted that the electrocatalytic activity of MoS1 was better than that of the composite and bare MoO3. It is proposed that the excellent electrochemical activity arises from sulfur vacancies which provide active sites for HER and a free path for ions to flow through the material. 相似文献
14.
《International Journal of Hydrogen Energy》2023,48(79):30741-30750
The development of multifunctional electrocatalysts is crucial for enhancing the efficiency of electrochemical conversion in energy devices. Here we have synthesized TiO2-x nanosheets (NSs) supported metallic Pd nanoparticles (Pd/TiO2-x NSs) as an electrocatalyst using a simple impregnation process. High electrochemical surface areas (ECSAs) and strong metal support interactions (SMSI) of the electrocatalyst showed improved ORR performance throughout a wide pH range under ambient conditions. The outstanding durability of the catalyst was proven by the square-wave potential cycling experiment at 60 °C. Additionally, it was shown that Pd/TiO2-x NSs showed improved HER activity and stability in 0.5 M H2SO4. The catalyst had an overpotential of 19.5 mV for the 10 mA cm−2 and a low Tafel slope of 41 mV dec−1. The catalyst also showed higher stability for about 30 h in HER performance. This work will help in rationally building nanostructured electrocatalysts loaded on carbon-free support for efficient electrochemical energy storage devices. 相似文献
15.
R. Solmaz A. Döner İ. Şahin A.O. Yüce G. Kardaş B. Yazıcı M. Erbil 《International Journal of Hydrogen Energy》2009
The long-term stability of NiCoZn coating for hydrogen evolution reaction (HER) was investigated in 1 M KOH solution under 100 mA cm−2 current density at room temperature. The effect of electrolysis on the corrosion behavior of NiCoZn coating was also studied. The alloy prepared on a copper electrode (Cu/NiCoZn) was etched in a concentrated alkaline solution (30% NaOH) to produce a porous and electrocatalytic surface suitable for use in the HER. The bulk and surface compositions of coating before and after alkaline leaching were determined by atomic absorption spectroscopy (AAS) and energy dispersive X-ray (EDX) analysis. The surface morphologies of freshly prepared and aged electrodes were investigated by scanning electron microscopy (SEM). Their catalytic activity towards the HER was assessed by recording cathodic current–potential curves and electrochemical impedance spectroscopy (EIS) techniques. It was found that the NiCoZn coating has a compact and porous structure. The long-term operation at 100 mA cm−2 current density showed that the electrochemical activity of Cu/NiCoZn electrode increased slightly with increasing electrolysis time. The activation of electrode related to the removal of any existing corrosion products and accumulations from the pores and formation of cracks during hydrogen gas evolution. The corrosion tests showed that the corrosion resistance of Cu/NiCoZn electrode changed after electrolysis. 相似文献
16.
Yingying Xing Di Li Longhua Li Huamei Tong Deli Jiang Weidong Shi 《International Journal of Hydrogen Energy》2021,46(11):7989-8001
Electrocatalytic hydrogen evolution under alkaline media holds great promising in hydrogen energy production. Transition-metal sulfides (TMSs) are attractive for electrocatalytic alkaline hydrogen evolution, yet their catalytic performance is unsatisfactory owing to the sluggish water dissociation kinetics. Herein, a Mn/N co-doping strategy is proposed to regulate the water dissociation kinetics of Co9S8 nanowires array grown on nickel foam thus improve the activity of hydrogen evolution reaction (HER). The optimal Mn/N co-doping Co9S8 (Mn–N–Co9S8) catalyst achieves low overpotentials of 102 and 238 mV at 10 and 100 mA cm?2 in the 1 M KOH solution, respectively, remarkably higher than the single-doping Mn–Co9S8 and N–Co9S8 as well as superior to many reported Co9S8-based HER electrocatalysts. Density functional theory (DFT) calculation results confirm that the water dissociation barrier of the Mn–N–Co9S8 is reduced significantly owing to the synergistic co-doping of Mn and N, which accounts for the enhanced alkaline HER performance. This study offers an effective strategy to enhance the alkaline HER activity of TMSs by accelerating water dissociation kinetic via the cation and anion co-doping strategy. 相似文献
17.
Wanmeng Dong Hui Liu Xiaoxu Liu Haoyu Wang Xinru Li Lejie Tian 《International Journal of Hydrogen Energy》2021,46(14):9360-9370
As a two-dimensional material, molybdenum disulfide (MoS2) exhibits great potential to replace metal platinum-based catalysts for hydrogen evolution reaction (HER). However, poor electrical conductivity and low intrinsic activity of MoS2 limit its application in electrocatalysis. Herein, we prepare a defective-MoS2/rGO heterostructures material containing 1T phase MoS2 and evaluate its HER performance. The experimental results shown that defective-MoS2/rGO heterostructures exhibits outstanding HER performance with a low overpotential at 154.77 mV affording the current density of 10 mA cm?2 and small Tafel slope of 56.17 mV dec?1. The unique HER performance of as-prepared catalyst can be attributed to the presence of 1T phase MoS2, which has more active sites and higher intrinsic conductivity. While the defects of as-prepared catalyst fully expose the active sites and further improve catalytic activity. Furthermore, the interaction between MoS2 and rGO heterostructures can accelerate electron transfer kinetics, and effectively ensure that the obtained catalyst displays excellent conductivity and structural stability, so the as-prepared catalyst also exhibits outstanding electrochemical cycling stability. This work provides a feasible and effective method for preparation of defective-MoS2/rGO heterostructures, which also supplies a new strategy for designing of highly active and conductive catalysts for HER. 相似文献
18.
Electrocatalytic hydrogen evolution of a cobalt A2B triaryl corrole complex containing –N=PPh3 group
《International Journal of Hydrogen Energy》2022,47(44):19062-19072
A new cobalt 5,15-bis(perfluorophenyl)-10-(4-N-(triphenylphosphoranylidene)-2,3,5,6-tetrafluorophenyl) corrole complex (Co-BPNC-PPh3) containing –N=PPh3 group has been prepared by Staudinger reaction and characterized by the single-crystal X-ray structure determination. The electrocatalytic hydrogen evolution reaction (HER) of Co-BPNC-PPh3 by using acetic acid (AcOH), trifluoroacetic acid (TFA) and p-toluenesulfonic acid (TsOH) as proton sources in N, N-dimethylformamide (DMF) solvent had been investigated. The turn-over frequency (TOF) value of Co-BPNC-PPh3 was observed 450 h?1 at an overpotential of 838 mV in neutral aqueous solution, showing excellent electrocatalytic HER activity. This Co-BPNC-PPh3 exhibited excellent durability and stability in the 5-hours electrolysis. Its activity is also better than cobalt 5, 10, 15-(tris-pentatfulorophenyl) corrole (Co-TPFC-PPh3), which may be ascribed to the –N=PPh3 proton relay effect in the electrocatalytic HER. 相似文献
19.
《International Journal of Hydrogen Energy》2019,44(36):19771-19781
Porous Ni-Co-(WC)x ternary composite electrodes were fabricated by means of electrodeposition on a foam Ni substrate. The surface morphology and microstructure of the electrodes were characterized by scanning electron microscopy (SEM) and X-ray diffraction (XRD). The electrocatalytic properties of porous Ni-Co-(WC)x electrodes for hydrogen evolution reaction (HER) in 0.5 M H2SO4 solution at temperatures from 25 to 50 °C were conducted by means of cathodic polarization, electrochemical impedance spectroscopy (EIS), cyclic voltammetry and chronoamperometry (CA). These Ni-Co-WC electrodes are efficient electrocatalysts for HER. Compared with the porous Ni-Co electrode, the porous Ni-Co-(WC)x electrode exhibited a lower HER overpotential, a lower electrochemical impedance, a lower apparent activation energy and a higher exchange current density. The apparent exchange current density of porous Ni-Co-(WC)x (x = 10, 20, 30 and 40 g/l) is 2.01, 3.01, 7.8 and 19.91 times of porous Ni-Co electrode, respectively. With the increase of WC concentration and temperature, the apparent exchange current density of HER was enhanced. With the increase of WC concentration and potential, the HER resistance and the activation energy decreased. The Ni-Co-(WC)x electrode exhibited superior corrosion resistance and stability for HER. 相似文献
20.
J. Theerthagiri R. Sudha K. Premnath Prabhakarn Arunachalam J. Madhavan Abdullah M. Al-Mayouf 《International Journal of Hydrogen Energy》2017,42(18):13020-13030
Advanced electrocatalysts for the fabrication of sustainable hydrogen from water splitting are innermost to energy research. Herein, we report the growth of iron diselenide (FeSe2) nanorods on graphene oxide (GO) sheets using two-step process viz., simple hydrothermal reduction and followed by wet chemical process. The orthorhombic phase of FeSe2 incorporated GO nanosheet was developed as a low-cost and efficient electrocatalyst for hydrogen evolution reaction (HER) by water splitting. The phase purity, crystalline structure, surface morphology and elemental composition of the synthesized samples have been investigated by UV–visible absorption spectroscopy (UV–vis), fourier transform-infrared spectroscopy (FT-IR), X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM) and energy dispersive X-ray analysis (EDS). Voltammetry and Tafel polarization methods have been utilized to assess the performance of various weight ratio of GO nanosheet in FeSe2 nanorods towards H2 evolution. Detailed electrochemical investigations revealed that the 30% FeSe2/GO composite showed a tremendous electrocatalytic HER activity in acidic medium with high cathodic current density of 9.68 mA/cm2 at η = 250 mV overpotential and with a Tafel slope of 64 mV/dec. The 30% FeSe2/GO composite offers a high synergistic effect towards HER activity, which is mainly due to high electrochemical active catalytic sites, low charge-transfer resistance and enhanced electrocatalytic performances of H2 production. The present analysis revealed the possible application of FeSe2/GO composite as a promising low-cost alternative to platinum based electrocatalysts for H2 production. 相似文献