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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Journal of Energy Chemistry
·
2023
·
IF 13.1
Zhiyang Huang,Miao Liao,Shifan Zhang,Lixia Wang,Mingcheng Gao,Zuyang Luo,Tayirjan Taylor Isimjan,Bao Wang,Xiulin Yang
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks (MOFs) is crucial to improve their oxygen evolution reaction (OER) performance. Herein, we introduce a novel strategy of dysprosium (Dy) doping, using the unique 4 f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs. Our method involves constructing Dy-doped Ni-MOF (Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach. Experiments and density functional theory (DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy. The resulting benefits include a reduced work function and a closer proximity of the d -band center to the Fermi level, which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates. Furthermore, the Dy@Ni-MOF achieves superhydrophilicity, ensuring effective electrolyte contact and thus accelerating reaction kinetics. Ex-situ and in-situ analysis results manifest Dy 2 O 3 /NiOOH as the actual active species. Therefore, Dy@Ni-MOF shows impressive OER performance, significantly surpassing Ni-MOF. Besides, the overall water splitting device with Dy@Ni-MOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm −2 and demonstrates long-term stability for 100 h, positioning it as a promising substitute for precious metal catalysts.
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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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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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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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高影响因子
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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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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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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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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Chi Zhang,Zhuohong Xie,Yi Liang,Dingding Meng,Zheng Wang,Xin He,Weiye Qiu,Mei Chen,Ping Liang,Zhonghua Zhang
Ni(OH) 2 has been long studied as an effective oxygen evolution electrocatalyst . Nevertheless, its catalytic activity can still be further enhanced by microstructural modification and Fe-doping. In this study, with the assistance of adsorbent ferrihydrite (FH), we obtain Fe-doped β-Ni(OH) 2 nanoplates with Fe 2 O 3 nanoparticles decorated on the surface via a facile hydrothermal process. The Fe-doping, decorated Fe 2 O 3 nanoparticles , and special microstructure endow β-Ni(OH) 2 nanoplates with an improved oxygen evolution activity in alkaline solutions. For the sample with optimal FH amount, the overpotential to motivate a current density of 10 mA cm −2 is 280 mV, with a low Tafel slope of ~64.17 mV dec −1 . During the 10 h i-t test at 1.50 V vs. RHE , the current density has an attenuation of only 23.7%. The study opens a facile avenue to modify Ni(OH) 2 -based OER catalyst from perspectives of both microstructures and compositions .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Tao Zhang,Xiaoying Jin,Gary Owens,Zuliang Chen
Dye-contaminated wastewater resulting from rapid industrialization and urbanization is a global problem. In this study, a ZIF-8@Fe/Ni sample was synthesized for the removal of malachite green (MG), removing more than 99% of an initial MG concentration of 50 mg L −1 within 120 min with a 318 K adsorption capacity of 151.520 mg g −1 . To understand the dye removal mechanism based on adsorption and reduction, ZIF-8@Fe/Ni was characterized by various techniques. XRD showed that the ZIF-8@Fe/Ni composite had a characteristic peak attributable to Fe/Ni around 44.8°, where the presence of Fe/Ni did not affect the structure of ZIF-8. SEM confirmed that ZIF-8@Fe/Ni was successfully prepared, while XRD and FTIR revealed that the structure of ZIF-8@Fe/Ni remained stable following the introduction of Fe/Ni. XPS showed that while Fe/Ni nanoparticles existed in ZIF-8-Fe/Ni, partial oxidation also occurred. GC–MS demonstrated the creation of two major MG degradation products, (4-aminophenyl) (phenyl) methanone and 4-aminophenol. While the overall adsorption process of MG to ZIF-8@Fe/Ni conformed to pseudo-second-order kinetics, degradation followed pseudo-first-order reduction kinetics. When applied to the remediation of wastewater, ZIF-8@Fe/Ni removed 92% of MG. Overall, this study demonstrated that ZIF-8@Fe/Ni could be a promising material for the treatment of wastewater.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 127
·期 6
·1-10
·
IF 2.584
Liu Yurong,Niu Shaoyu,Hu Rong
In this work, the ferric cobalt sulfide/aminated graphene quantum dots (FeCo 2 S 4 /NH 2 -GQDs) nanoflowers grown on Ni foam substrate have been successfully fabricated via a facile two-step hydrothermal method. The as-prepared FeCo 2 S 4 /NH 2 -GQDs nanoflowers can expose plenty of electroactive sites, provide fast charge transfer paths and buffer the drastic volume change during long-term charge–discharge cycles. Therefore, the FeCo 2 S 4 /NH 2 -GQDs nanoflowers exhibit excellent supercapacitive performance, including high specific capacitance, excellent rate capability and cycling stability. The specific capacitance of FeCo 2 S 4 /NH 2 -GQDs composite electrode reaches 2314.8 and 1802.5 F g −1 at the current density of 1 and 10 A g −1 , respectively, while maintaining superior cycling stability with 95.1% capacitance retention after 5000 cycles. This study proves that NH 2 -GQDs are promising materials to enhance the electrochemical performance of bimetallic sulfides, providing a new insight for the design and fabrication of novel electrode materials for high-performance supercapacitors.
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危险品化学品经营许可证（带存储）