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Steam reforming (SR) is a process for converting transportation fuels into hydrogen-rich gas, which can be fed to SOFCs for on-board power supplies. Herein, we prepare Mg x Ni 1-x O (0.5
Ni(OH) 2 has been acknowledged as a promising oxygen evolution reaction (OER) electrocatalyst owing to its good electrochemical activity and low cost. However, application of the pristine Ni(OH) 2 is limited by the poor conductivity and low exposure of the active sites. Herein, a [email protected] (OH) 2 composite is prepared through a hydrothermal reaction. Heat treatment temperature proves to have a great influence on the electrocatalytic activity. In 0.1 M KOH electrolyte, the composite treated at 175 °C shows an overpotential of only 287 mV to reach the current density of 10 mA·cm −2 . Besides, the low Tafel slope (42 mV·dec −1 ) and superior stability (15 h at 10 mA·cm −2 ) also confirm the composite as an excellent OER electrocatalyst. The brilliant activity and stability toward OER can be attributed to the promoted coupling between Ni and Fe centers and the improved conductivity due to the 2D 18 p-electrons ring conjugate structure of hemin. Besides, effective hydrogen bonds between Ni(OH) 2 and hemin hinder the aggregation of Ni(OH) 2 , which ensures the catalyst enormous accessible active sites. This work offers a new method for the modification of Ni(OH) 2 as OER electrocatalysts. And the application of hemin also serves as a successful case for the use of biomass materials in OER electrocatalysis .
In this study, a nickel (Ni)-based catalyst was loaded onto steel slag that was rich in metal oxides using impregnation method. The effects of the catalyst on hydrogen-rich gas produced using sludge steam gasification were discussed. Under the conditions of 900 ℃, steam flowrate of 1.5 g min −1 and 20% Ni-based loading rate, the gas and H 2 yield reached 0.78 Nm 3 kg −1 and 15.72 mol kg −1 . At this time, the volume fraction of H 2 was as high as 45.096%. Compared with the raw sludge gasification without Ni-based catalyst, the gas and H 2 yield were increased by 39.22% and 60.15% respectively. However, excessive flowrate of steam (≥1.5 g min −1 ) and excessive rate of loading of Ni-based (≥25%) catalyst would lead to a decrease in the production of gas. In addition, the impregnation method could effectively disperse NiO particles on the surface of the support, increasing the ratio of active sites on the surface of catalyst and improving the catalytic activity. These characteristics indicated that the Ni-based steel slag catalysts prepared by the impregnation method had high application potential in the process of sludge steam gasification, and provided a novel idea for solid wastes recycling.
The efficient utilization of renewable biogas has attracted ever-increasing interest in the past few decades. Ni–Ce1−xZrxO2 supported on monolithic SiC-F (named Ni–Ce1−xZrxO2/SiC-F) is developed and applied in biogas reforming. Monolithic Ni–Ce1−xZrxO2/SiC-F catalysts were comprehensively characterized by ICP-AES, XRD, SEM, HR-TEM, CO2-TPD, etc. The promotional roles of Ce1−xZrxO2 in coke elimination as well as CO2 activation were deeply analyzed via in situ CH4-TPSR/CO2-TPO and in situ H2-TPR/CO2-TPSR. Ni–Ce1−xZrxO2/SiC-F exhibits satisfactory catalytic activity and ability to inhibit sintering and coke-deposition due to (a) the homogeneous dispersion of Ni nanoparticles (NPs) and (b) the strong interaction between Ce1−xZrxO2 solid solutions and Ni NPs. At 900 °C and a weight hourly space velocity (WHSV) of 24 000 mL gcat−1 h−1, an excellent CH4/CO2 conversion of 90/92% was initially achieved over the Ni–Ce1−xZrxO2/SiC-F catalyst, followed by a slight decrease after 150 h, but remained basically stable for the next 250 h.
Ni and carbon materials exhibit remarkable catalysis for the hydriding reaction of Mg. But the underlying mechanism of Ni/C hybrid catalysis is still unclear. In this work, density functional theory (DFT) calculation is applied to investigate the effect of Ni/C co-incorporation on the hydriding reaction of Mg crystal. The morphology and crystal structure of the Ni/C co-incorporated Mg sample show that the co-incorporated structure is credible. The transition state searching calculation suggests that both the incorporations of Ni and C are beneficial for the H 2 dissociation. But Ni atom has a dramatic improvement for H 2 dissociation and makes the H diffusion become limiting step of the hyriding reaction. The Ni d z 2 orbit and H s orbit accept the electrons and combine together compactly, while the Ni d xy orbit is half-occupied. The catalytic effect of Ni on H 2 dissociation can be ascribed to the bridging effect of Ni d xy orbit. The incorporation of C can weaken the over-strong interaction between Ni and H which hindered the H diffusion on Mg(0001). The Ni/C co-incorporated Mg(0001) shows the best performance during hyriding reaction compared with the clean and single incorporated Mg(0001).
Iron phosphide (FeP) with high theoretical capacity (926 mAh g −1 ) and low voltage window for lithium-ion batteries (LIBs) arouses extensive concern. However, inferior electron conductivity and FeP aggregation limit its applications. To settle these drawbacks, with the Ni doping, Ni-FeP@carbon (Ni-FeP@C) core–shell structure prepared by solvothermal method and phosphating process has been designed as the anode material for LIBs. Ni doping not only affected the morphology of FeP, but also improved electrical conductivity and excellent structural stability, accelerating the migration of lithium ions. Carbon shell coating promoted electron transfer and suppressed the volume fluctuation of FeP during discharge and charge process. As a consequence, the Ni-FeP@C composite delivered outstanding specific capacity (855.7 mAh g −1 at 0.1 A g −1 ) and long-cyclic performance (488 mAh g −1 after 1000 cycles at 2.0 A g −1 ). For the assembled full cell, the battery exhibited the promising cycling performance (50.4 mAh g −1 after 70 cycles at 0.1 A g −1 ). As expected, cation doping strategy in this work is of great significance for the further application of FeP materials in advanced lithium ion batteries.
The construction and modulation of hierarchical pore structure in metal-organic frameworks (MOFs) has become a hot topic owing to the advantages of hierarchical pore MOFs (HP-MOFs) in matter storage and mass transfer related applications. Herein, we report the engineering of crystalline defect in a bimetallic MOF for the construction and tuning of HP-MOF. A microporous MOF system showing metal-center-dependent water stability, namely, {[M3F(bdc)3 tpt] (solvents)}n (M = Zn2+ and Ni2+, H2bdc = 1,4-benzenedicarboxylic acid, tpt = 2,4,6-tris(4-pyridyl)triazine), was utilized as a platform for the construction of HP-MOF. By tuning the Zn2+/Ni2+ ratio in the reactant, a bimetallic MOF with a highly tunable Zn2+/Ni2+ ratio could be obtained. The relatively labile Zn2+-based coordination bonding in the bimetallic MOF could be readily and targeted broken through water treatment for the engineering of crystalline defects-based hierarchical pore structure. The resultant HP-MOF reveals a dramatically increased pore volume with the presence of mesopore and macropore. In addition, the anionic framework of HP-MOF could be utilized for the selective adsorption of a cationic dye methylene blue, and a relatively high capacity (250 mg·g–1, five times compared with the pristine microporous MOF) could be achieved.
Layered double hydroxide (LDH) films have been used to protect metal substrates because of their superior barrier performance and capability of capturing corrosive anions (such as Cl − ) by exchange with interlayer anions. In this preliminary work, we determined that some photoactive LDHs (such as NiAl-LDH) can also provide cathodic protection to metals under light illumination, stemming from the light-generated electrons of semiconducting LDHs, if the energy level of the conduction band of LDHs is higher than the Fermi level of the metal. The current experimental results prove that the corrosion resistance of stainless steel is enhanced by the attached NiAl-LDH films in the dark and is further increased under light illumination due to photogenerated cathodic protection.
Facilitating charge separation and increasing surface active sites have always been the goals of photocatalysis. Herein, we synthesized a Ni-doped Zn0.8Cd0.2S hollow sphere photocatalyst with a facile one-step hydrothermal method. Energy-dispersive spectroscopy mapping showed the high dispersion of Ni ions in the Zn0.8Cd0.2S hollow spheres. The experimental results confirmed that Ni doping reduced the band structure of the substrate, suppressed the recombination of photo-induced electrons and holes, and provided more reactive sites. Therefore, the photocatalytic activity had been greatly improved. As a consequence, the detected photocatalytic H2 evolution rate increased up to 33.81 mmol·h–1·g–1 over an optimal Ni doping (5 wt %) of Zn0.8Cd0.2S hollow spheres, which was 20.87-fold higher than that of pure CdS. Elemental mapping showed that the Zn element was mainly distributed in the outermost layer of the hollow spheres; this might be the critical factor that enabled Ni-doped ZnxCd1–xS to maintain excellent stability.
Hydrogen energy is regarded as one of the most important clean energy in the twenty-first century, and improving the catalytic efficiency of hydrogen evolution reaction (HER) is the basis for realizing the large-scale hydrogen production. Transition metal phosphides (TMPs) were proved to be efficient electrocatalysts for HER. In this work, we first synthesized the nickel-molybdenum bimetallic precursors, followed by high-temperature calcination in air. Finally, NiMoP/MoP nanorods (Ni–Mo–P NRs) was obtained by chemical vapor deposition (CVD) of phosphating. The target catalyst of Ni–Mo–P NRs was characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). For Ni–Mo–P NRs, the electrochemical test in 0.5 M H 2 SO 4 solution for HER showed that the optimal feeding ratio was Ni:Mo = 1:1. And the Ni 1 –Mo 1 –P NRs presented an onset potential of 63.2 mV, and an overpotential of 117.9 mV was required to drive the current density of 10 mA cm −2 . Meanwhile, The Tafel slope, exchange current density ( j 0 ), electrochemical double-layer capacitance ( C dl ) were 58.6 mV dec −1 , 0.10 mA cm −2 , 12.6 mF cm −2 , respectively. Moreover, there was no obvious activity diminish of Ni 1 –Mo 1 –P NRs after a long-term stability and durability test.
Electrochemical CO2reduction reaction (CO2RR) is eliciting considerable attention in relation to the carbon cycle and carbon neutrality. As for the practical application of CO2RR, the electrocatalyst is a crucial factor, but, even so, designing and synthesizing an excellent catalyst remains a significant challenge. In this paper, the coordination compound of Ni ions and dimethylglyoxime (DMG) was employed as a precursor to modify reduced graphene oxide (rGO) for CO2RR. The textural properties and chemical bonds of as-obtained rGO, N–C–rGO, Ni–rGO, Ni–N–C, and Ni–N–C–rGO materials were investigated in detail, and the role of Ni, N–C, and rGO in the CO2RR were researched and confirmed. Among all the catalysts, the Ni–N–C–rGO showed the optimal catalytic activity and selectivity with a high current density of 10 mA cm−2and FE(CO)% of 85% at −0.87 V vs. RHE. In addition, there was no obvious decrease in activity for 10 h. Therefore, the Ni–N–C–rGO is a promising catalyst for CO2RR to CO.Keywords:metallic Ni;N-doped carbon;reduced graphene oxide;electrocatalyst;electrochemical CO2reduction
Metal organic frameworks (MOFs) have potential applications in the field of energy storage due to high specific surface area and rich porosity, and captured widely attention in recent years. In this work, nickel/manganese-based MOFs (Ni/Mn-MOFs) were successfully fabricated by solvothermal reaction using 1,4-phthalic acid as the organic ligand, nickel nitrate hexahydrate, and manganese nitrate tetrahydrate providing center metal ions. The Ni/Mn-MOFs were analyzed by scanning electron microscope, powder X-ray diffraction, and nitrogen absorption/desorption isotherm. The results indicate that the obtained Ni/Mn-MOFs have coral-like microstructures and hierarchical pores with a specific surface area of 380.8 m 2 /g and an average pore diameter of 13.6 nm. Subsequently, the Ni/Mn-MOFs were used as the electrode materials for supercapacitors, and the electrochemical properties were investigated in the three-electrode system using 6.0 M KOH aqueous solution as the electrolyte. The results show that the specific capacitances of the coral-like Ni/Mn-MOFs are 531.5 and 317.9 F/g at the current density of 0.5 and 5 A/g, respectively. And the capacitance retention is 67.7% after 2300 cycles at 5 A/g, which implies that the coral-like Ni/Mn-MOFs have higher specific capacitance and favorable cycle stability. The above results indicate that the coral-like Ni/Mn-MOFs facilitate the electrolyte infiltration and ions transportation.
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