Processes
·
2023
·Vol. 11
·期 11
·3181
·
IF 3.5
Chuangchuang Yang,Qiaoling Dai,Anpeng Hu,Hui Yuan,Qinghe Yang
In this present work, a new kind of sulfurized hydrodesulfurization catalyst was synthesized via the hydrothermal treatment of MoS2, NiCO3·2Ni(OH)2·4H2O, and Al2O3precursors, followed by annealing under a H2atmosphere, which does not require a sulfurization process compared to traditional preparation methods. The influence of the annealing temperature and the type of Al2O3precursor on the interactions between MoS2and Al2O3were studied using X-ray fluorescence spectroscopy, X-ray diffraction, N2adsorption–desorption, Raman spectroscopy, X-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. The results indicated an increase in the number of stacked layers of the MoS2catalyst, accompanied by a decrease in the degree of decoration of Ni atoms onto MoS2nanoslabs, as a result of the strengthened MoS2–Al2O3interaction. Subsequently, the efficiency of hydrodesulfurization (HDS) was evaluated using dibenzothiophene as a representative reactant, while establishing a correlation between the structure of the catalyst and its performance. The catalysts, using pseudo-boehmite as the precursor and calcined at 500 °C, synthesized by calcining pseudo-boehmite as the precursor for Al2O3at a temperature of 500 °C and possessing suitable metal–support interactions, exhibited a reduced number of MoS2stacking layers and lateral dimensions, along with an optimal decoration degree of Ni atoms, thereby resulting in the highest level of HDS activity.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Yuqing Hu,Puhui Deng,Wenying Wang,Linping Zhang,Yu Hou
Element doping and collaboration with other cocatalysts are two vital strategies to improve the photoelectrochemical properties and overcome the drawbacks of CdS for better photocatalytic performance. In this work, a series of manganese cadmium sulfides (MnxCd1–xS) were obtained by a solvothermal method. When x is equal to or greater than 0.3, MnxCd1–xS is composed of Mn–Cd–S sosoloid and MnS. Among all these MnxCd1–xS products, the Mn0.5Cd0.5S sample showed the best photocatalytic hydrogen production (5.99 mmol g–1 h–1). To further elevate the hydrogen production rate of Mn0.5Cd0.5S, four kinds of Ni-POMs were coupled with it as cocatalysts, and all these composite photocatalysts displayed enhanced performance. The highest efficiency was observed for 15-Ni4–Mn0.5Cd0.5S, which is up to 36.58 mmol g–1 h–1. Various characterizations indicated that Ni4P2W18, Mn–Cd–S sosoloid and MnS in the 15-Ni4–Mn0.5Cd0.5S composite form a double type-II heterojunction, which facilitates the separation and transfer of photogenerated carriers.
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Crystals
·
2023
·Vol. 13
·期 11
·1587
·
IF 2.7
Yiyi Xiao,Hui Huang,Jinkun Guo,Mi Yan,Liyuan Wei,Yu Liu,Shiliang Huang,Rufang Peng,Bo Jin
Energetic complexes represent a crucial research direction for the design and synthesis of novel energetic materials. In this work, 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105), a significant explosive compound with exceptional comprehensive properties, was selected as the ligand for coordinating with various metal ions. Four novel energetic complexes, Ni(C4H3N6O5)2·DMF (1), Co(C4H3N6O5)2·2DMF (2), Mn(C4H3N6O5)3·3/2DMF (3), and Cu3(C4H2N6O5)3·3DMF (4) were successfully synthesized, and their crystal structures were identified by a single-crystal X-ray diffraction technique. The structural analyses illustrated that LLM-105 can form either a mononuclear metal complex after the deprotonation of one amino group or a trinuclear metal complex after the deprotonation of two amino groups. Compound1exhibits a planar quadrilateral geometry, while both compounds2and3display distorted octahedral configurations. Compound4has three metal centers and exhibits two coordination configurations of distorted tetragonal pyramid geometry and planar quadrilateral geometry. The detonation performances of compounds1–4were also theoretically calculated, revealing their favorable explosive properties. These findings emphasize the diverse coordination modes of LLM-105 and the structural variability and adjustability of its complexes, offering valuable insights for regulating both the structure and performance of the LLM-105 complex as well as researching its deprotonation.Keywords:energetic complexes;LLM-105 ligand;single-crystal structure;coordination modes
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 43
·19974-19982
·
IF 3.3
Hao Fan,Qin Peng,Zhenxing Shen,Xuefeng He,Yiming Yang
Nitric oxide (NO), a major atmospheric pollutant and a precursor to haze, can be removed using the denitration catalyst. Mn and Ni are commonly used as denitration catalyst additives owing to their adsorption abilities for NO and ammonia (NH3). In this study, we synthesized Mn- and Ni-loaded Pt-modified sulfated cerium oxide (PtSCe) catalysts using an impregnation method and explored the effects of these elements. The results revealed that the two elements had contrasting effects on the denitration activity of the catalysts. Mn improved the water vapor and sulfur resistance of the PtSCe sample by increasing the concentration of weak acid sites, enhancing the redox ability, and increasing the content of surface-adsorbed oxygen. The elevation in oxygen vacancies, stimulated by the presence of Ce3+ and Mn3+, swiftly replenished the reactive oxygen species, thereby sustaining the high denitration efficiency of the MnPt/SCe sample. Active sites on the catalyst surface included NH3 adsorbed on Lewis acid sites, NH4+, and –NH2, along with bridging, monodentate, and bidentate nitrate groups. Regarding the catalyst reaction mechanism, we determined that the selective catalyst reduction of NH3-SCR over MnPt/SCe followed both the Eley–Rideal and Langmuir–Hinshelwood mechanisms. These findings offer crucial insights into the intricate relationship between metals, sulfates, and carrier molecules, thus providing implications for future catalyst design.
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MOLECULES
·
2023
·Vol. 28
·期 19
·6843
·
IF 4.6
Fumei Shi,Yilan Chen,Chuanheng Dong,Jiajia Wang,Chunman Song,Yalin Zhang,Zhen Li,Xianqiang Huang
Polyoxometalates (POMs) exhibit unique structural characteristics and excellent physical and chemical properties, which have attracted significant attention from scholars in the fields of anticancer research and chemotherapy. Herein, we successfully synthesized and structurally characterized two novel polyoxovanadates (POVs), denoted as POVs-1and POVs-2, where [M(1-vIM)4]2[VV4O12]·H2O (M: NiIIand MnII, 1-vinylimidazole abbreviated as 1-vIM) serve as ligands. The two POVs are isomeric and consist of fundamental structural units, each comprising one [V4O12]4−cluster, two [M(1-vIM)4]2+cations, and one water molecule. Subsequently, we evaluated the cell viability of human hepatocellular carcinoma (HepG-2) cells treated with the synthesized POVs using the MTT (3-[4,5-dimethylthiazol-2-yl]-2,5-diphenyl tetrazoliumbromide) assay. And the changes in cell nucleus morphology, mitochondrial membrane potential (Δψm), and reactive oxygen species levels in HepG-2 exposed to POVs were monitored using specific fluorescent staining techniques. Both hybrid POVs showed potent inhibitory activities, induing apoptosis in HepG-2 cells along with significant mitochondria dysfunction and a burst of reactive oxygen species. Notably, the inhibitory effects of POVs-2were more pronounced than those of POVs-1, which is primarily attributed to the different transition metal ions present. These findings underscore the intricate relationship between the metal components, structural characteristics, and the observed antitumor activities in HepG-2 cells.Keywords:polyoxovanadates;imidazole ligands;human hepatocellular carcinomas;anticancer;apoptosis
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Analytical Methods
·
2017
·Vol. 9
·期 19
·2812-2820
·
IF 1.9
Yanyi Fu,Qinglin Sheng,Jianbin Zheng
Au nanoparticles supported on nickel hydroxide nanowires with multiple cavities (Au/m-Ni(OH)2) were synthesized and used for the enhanced electrochemical sensing of dopamine (DA). m-Ni(OH)2 nanowires were first fabricated based on an anion exchange strategy and then chosen as supports for Au nanoparticles without an additional stabilizer and surfactant. The morphology and composition of the nanocomposites were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopy (EDS). TEM observations revealed that Au nanoparticles were uniformly embedded in the cavities of m-Ni(OH)2 nanowires, with a high dispersion and a narrow size of 2 nm. Electrochemical investigations indicated that the as-prepared sensor exhibited fascinating performance towards the oxidation of DA. The linear range for DA detection was 0.45 μM to 1.78 mM with a low detection limit of 0.09 μM (S/N = 3). Additionally, the DA sensor possessed an excellent selectivity in the presence of potentially interfering substances such as ascorbic acid (AA), uric acid (UA) and glucose (Glu). Therefore, it is expected that Au/m-Ni(OH)2 nanocomposites could be used as electroactive materials for developing DA sensors.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Rui Yu,Zhaokuan Li,Qing Wang,Yongzhi Lan
Porous structures grown in situ increase the electrode contact area with the electrolyte, reduce ion diffusion distance, and enhance electrode material electrochemical properties. In this paper, we have adopted a dual-channel electrodeposition strategy with simultaneous electrodeposition and phosphorylation to construct metal-semiconductor contact heterostructures by depositing Ni@NiCo phosphate microspherical nanostructures directly on a copper foam (CF) (Ni@NiCoP/CF) framework at room temperature . The results show that Ni@NiCoP/CF has excellent electrochemical performance with a high specific capacity of 200 mAh g –1 at 1 A g –1 , 147.2 mAh g –1 at 20 A g –1 and 93.6 % after 5000 cycles, showing excellent ration performances and cycling stability. In addition, the hybrid supercapacitor composed of Ni@NiCoP/CF as the positive electrode and activated carbon as the negative electrode achieves a high energy density of 48.7 Wh kg −1 at 874 W kg −1 and has excellent cycling stability with 113.23 % capacity retention after 30,000 charge/discharge cycles at a high current density of 10 A g –1 . This study serves as a guide for the development of high-performance capacitor cathode materials with high electrochemical activity and capacity.
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Progress in Natural Science-Materials International
·
2023
·
IF 4.7
Huiling Zhu,Kai Wang,Yao Qi,Ruixin Li,Jianxu Ding,Rui Liu
In this study, we synthesized a bayberry-like Ni–Co–Mn ternary hydroxide with a secondary nanoneedle structure using a modified and cost-effective hydrothermal process assisted by the surfactant cetyltrimethylammonium bromide (CTAB). The incorporation of CTAB and graphene in the preparation process significantly enhances the electrochemical performance of NiCoMn–OH. The achieved results are truly impressive, with a high specific capacity of 1450 F g −1 and an outstanding capacity retention of 52.57% over 5000 cycles. The superior performance could be attributed to the specific bayberry-like microstructure with high effective specific surface area, which allowed for facile and rapid transport of ions and electrons. Moreover, the synergistic effect of CTAB and graphene proved to be crucial in stabilizing the Co 2+ and Mn 2+ ions within the ternary hydroxide structure. We developed a hybrid capacitor using a NiCoMn–OH-CTAB/Graphene composite electrode and an active electrode, which delivered a superior energy density of 50.79 Wh kg −1 at a power density of 400 W kg −1 and a cycling stability of 60.37% after 10000 cycles. These results indicate that the NiCoMn–OH-CTAB/Graphene composite electrode has great potential as an electrode material for energy storage devices.
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Catalysts
·
2023
·Vol. 13
·期 10
·1366
·
IF 3.9
Ronghua Yuan,Weina Xu,Liquan Pan,Ruibin Li,Chuanying Xiao,Xiaochang Qiao
The Co-based perovskite La0.6Sr0.4CoO3has received significant attention as a potential electrocatalyst for its oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) due to its abundance, facile synthesis, and high oxygen kinetics. However, research on the catalytic performance of Ni-doped La0.6Sr0.4Co1−xNixO3as a bifunctional cathode catalyst for Zn-air batteries (ZABs) is still scarce. In this work, lanthanum strontium cobalt-based perovskite catalysts with various Ni contents (La0.6Sr0.4Co1−xNixO3, x = 0, 0.2, 0.5, and 0.8) were synthesized using a simple combustion method. The effects of Ni doping on the morphology, structure, surface oxygen-related species, and valence states of the transition metals of the perovskite were characterized. The electrochemical behaviors of the perovskite catalysts in both ORR and OER were also assessed. The characterization results revealed that proper Ni doping can decrease particle size, increase surface oxygen vacancies, and create mixed valence states of the transition metal and, thus, lead to improvement of the electrocatalytic activity of perovskite catalysts. Among the different perovskite compositions, La0.6Sr0.4Co0.8Ni0.2O3exhibited the best ORR/OER activity, with a higher limiting current density, smaller Tafel slope, higher half-wave potential, lower overpotential, and lower potential difference than the other compositions. When La0.6Sr0.4Co0.8Ni0.2O3was applied as the cathodic catalyst in a primary ZAB, it delivered a peak power density of 81 mW cm−2. Additionally, in rechargeable ZABs, the La0.6Sr0.4Co0.8Ni0.2O3catalyst exhibited a lower voltage gap (0.94 V) and higher stability during charge–discharge cycling than the commonly used catalyst Pt/C. These results indicate that Ni-doped La0.6Sr0.4Co0.8Ni0.2O3is a promising bifunctional electrocatalyst for ZAB.Keywords:Ni doping;perovskite;bifunctional electrocatalyst;oxygen reduction and evolution reaction;Zn-air battery
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Liming Chen,Lianmei Kang,Dandan Cai,Shipeng Geng,Yangyang Liu,Jian Chen,Shuqin Song,Yi Wang
Although Pt is a widely adopted commercial catalyst for the hydrogen evolution reaction (HER), its practical application is greatly limited by its prohibitive cost and high energy barrier for H 2 O dissociation in alkaline media. Herein, an ultrafine Pt-based catalyst decorated with oxygenophilic Ni-sites is rationally designed and successfully synthesized with Pt 5 (GS) 10 (HGS = l -reduced glutathione) nanocluster precursor. The optimized Ni-decorated Pt catalyst (Ni-Pt-C-500) with ultrafine nanoparticles (about 1.6 nm) exhibits a low overpotential (14.0 mV) at 10 mA cm −2 and a mild Tafel slope of 20.8 mV dec −1 in the HER, which is superior to its undecorated counterpart (Pt-C-500), the commercial 20 wt% Pt/C catalyst and most of the previously reported Pt-based electrocatalysts. Experimental observations and theoretical calculations indicate that H 2 O could be spontaneously adsorbed to Ni-sites of the Ni-Pt-C-500 catalyst. Mechanistic studies reveal that Ni-sites promote HER by accelerating the kinetic of H 2 O cleavage and optimizing the electronic structure of Pt. This work paves a new avenue for designing other ultrafine hybrid electrocatalysts based on metal nanoclusters to enhance catalytic reaction kinetics.
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Journal of Water Process Engineering
·
2023
·
IF 7
Xinrui Liu,Rui Guo,Xia Qin,Cuicui Xu
In this work, a Ni foam/CNTs/Cu composite electrode was prepared via the impregnation and electrodeposition methods. The electrode enhanced the total nitrogen removal and N 2 selectivity , when served as a cathode for NO 3 − -N reduction. SEM, EDS, XRD, and XPS characterization revealed that both CNTs and metallic copper were introduced onto the surface of the Ni foam substrate successfully. Besides, the LSV, CV, EIS and C dl results indicated more electrochemical active sites were in the Ni foam/CNTs/Cu electrodes than in Ni foam/Cu electrodes. Under optimal preparation conditions, the Ni foam/CNTs/Cu electrode showed N 2 selectivity of 68.89 % and nitrate removal rate of 96.75 % in 100 mg/L nitrate solution with Na 2 SO 4 as electrolyte. The selectivity of N 2 could be significantly enhanced by adding Cl − as electrolyte, and the nitrogen selectivity increased with the increase of Cl − concentration. At 1.25 g/L NaCl, the Ni foam/CNTs/Cu electrode could achieve >95 % nitrate and total nitrogen removal and close to 100 % N 2 selectivity. The N 2 selectivity of the Ni foam/CNTs/Cu electrode was 2.534 and 1.8 times of the Ni foam/Cu electrode when 0.5 g/L Na 2 SO 4 and 0.5 g/L NaCl were used as electrolytes, respectively. Consequently, to achieve the same nitrate reduction effect, the Ni foam/CNTs/Cu electrode could reduce the amount of NaCl compared with Ni foam/Cu electrode. The electrodes were tested in 6 cycles and proved to be stable. At last, a potential mechanism of nitrate‑nitrogen removal by the electrocatalytic process was suggested.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Samuel Guemou,Liuting Zhang,Shuai Li,Yiqun Jiang,Tao Zhong,Zichuan Lu,Ren Zhou,Fuying Wu,Qian Li
The design of an excellent active catalyst to improve the sluggish kinetic and thermodynamic properties of magnesium hydride (MgH 2 ) remains a great challenge to achieve its practical application. In this study, a novel Ni-Nb/rGO nanocomposite catalyst was successfully prepared by one-spot hydrothermal and subsequent calcination methods. The novel Ni-Nb/rGO nanocomposite exhibits an exceptional catalytic effect on improving MgH 2 sorption properties. Specifically, the onset desorption temperature of MgH 2 + 10 wt% Ni-Nb/rGO composite is reduced to 198 °C, much lower than that of undoped MgH 2 (330 °C). Interestingly, the composite can release 5.0, 5.9, and 6.0 wt% H 2 within 10 min at 245, 260, and 275 °C, respectively. Furthermore, the dehydrogenated MgH 2 + 10 wt% Ni-Nb/rGO composite starts to absorb hydrogen even at room temperature with approximate 2.75 wt% H 2 uptake at 75 °C under 3 MPa H 2 pressure within 30 min and exhibits excellent stability by maintaining 6.0 wt% hydrogen content after 20 cycles at 300 °C. Chou's model suggests that the de/hydrogenation kinetics of Ni-Nb/rGO-modified MgH 2 switches from surface penetration model to diffusion model at lower temperatures. Additionally, the activation energies ( E a ) for the de/hydrogenation of MgH 2 + 10 wt% Ni-Nb/rGO are reduced to 57.8 kJ/mol and 33.9 kJ/mol, which are significantly lower than those of undoped MgH 2 . The work demonstrates that the addition of a novel ternary Ni-Nb/rGO catalyst is an effective strategy to not only boost the sorption kinetics of MgH 2 but also maintain its cycling property.
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