Inorganic Chemistry Frontiers
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2022
·Vol. 9
·期 15
·3679-3691
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IF 7.779
Lei Fan,Lianming Zhao,Yuchao Lv,Tinghu Wang,Yupeng Tian,Jianye Fu,Xinmei Liu
The synthesis of highly-dispersed non-noble metal based catalysts and their application in hydrogenation/dehydrogenation still remain challenging. Therefore, it is of great importance to protect metals from aggregation in both calcination and reduction processes. In this research, density functional theory (DFT) calculations were used to elucidate the stabilization effect of ionic liquid [Bmim][BF4] on Ni in the reduction process, showing that [Bmim][BF4] could efficiently inhibit Ni aggregation on the support. By further analysis combined with theoretical calculations, we found that the degree of metal dispersion before reduction directly determines the effect of [Bmim][BF4]. Guided by the DFT results, the method of co-assisted preparation of Ni/SAPO-11 using [Bmim][BF4] and lysine was adopted. Lysine forms a coordination compound with nickel oxides. The steric hindrance generated by the Ni–lysine complex can effectively inhibit the aggregation of nickel oxides during the calcination process. The DFT calculations revealed that during the reduction process, [BF4−] plays a dominant role in stabilization and electronic modulation by directly interacting with Ni on the support. The combination effects of [Bmim][BF4] and lysine effectively inhibit metal aggregation, leading to ultra-small nickel particles with a mean size of 4.4 nm over the obtained catalyst. Furthermore, the presence of [Bmim][BF4] also tunes the electronic state of Ni species. Using hexane isomerization as a probe reaction, the result indicates the excellent catalytic activity of the obtained catalyst (≈93.7% isomer selectivity at 63.5% conversion), much superior to that of Ni/SAPO-11 obtained from the traditional impregnation route (≈75.8% isomer selectivity at 64.6% conversion). This work provides a new method for the preparation of highly effective non-noble metal supported catalysts.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2022
·
IF 7.129
Mai Luo,Ling Chen,Jinchao Wei,Xiping Cui,Zehua Cheng,Ting Wang,Incheng Chao,Yunyang Zhao,Hao Gao,Peng Li
Exogenous pollution of Chinese medicinal materials by pesticide residues and heavy metal ions has attracted great attention. Relying on the rapid development of nanotechnology and multidisciplinary fields, fluorescent techniques have been widely applied in contaminant detection and pollution monitoring due to their advantages of simple preparation, low cost, high throughput and others. Most importantly, synchronous detection of multi-targets has always been pursued as one of the major goals in the design of fluorescent probes. Herein, we firstly develop a simultaneous sensing method for methyl-paraoxon (MP) and Nickel ion (Ni, Ⅱ) by using carbon based fluorescent nanocomposite with ratiometric signal readout and nanozyme. Notably, the designed system showed excellent effectiveness even when the two pollutants co-exist. Under the optimum conditions, this method provides low limits of detection of 1.25 µM for methyl-paraoxon and 0.01 µM for Ni (Ⅱ). To further verify the reliability, recovery studies of these two analytes were performed on ginseng radix et rhizoma, nelumbinis semen, and water samples. In addition, smartphone-based visual analysis has been introduced to expand its applicability in point of care detection. This work not only expands the application of the dual-mode approach to pollutant detection, but also provides insights into the analysis of multiple pollutants in a single assay.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Lina Lv,Baozhong Zhang,Panpan Tian,Lingling Xie,Wenhao Wei,Jintao He,Min Lin,Huina Zhu,Hanyu Chen,Baoshan He
In this project, we developed an electrochemical aptamer sensor based on the coordinated catalysis toward thionine (Thi) of nickel metal-organic framework (Ni-MOF) and gold nanoparticles (AuNPs) to sensitively detect the enrofloxacin (ENR), which belonged to a third-generation quinolone antibiotic for treat diseases caused by bacteria. In order to improve the analytical performance of the sensor, Ni-MOF and gold AuNPs, as the substrate material, could increase the load of the aptamer (Apt) and synergistically catalyze thionine (Thi). Therefore, ultrathin sheets of gold triangular nanosheets (AuTNSs) were prepared as signal labeling materials, which were loaded with a large amount of Thi and complementary deoxyribonucleic acid (cDNA). With the help with Ni-MOF and AuNPs catalysis toward Thi, under optimal conditions, the aptasensor exhibited a massive detection range of 1×10 −2 pg·mL −1 to 1×10 3 pg·mL −1 (S/N = 3) and a detection limit of 5.6×10 −3 pg·mL −1 for ENR. Meanwhile, the proposed sensor has a high sensitivity, satisfactory repeatability and long-time stability, and could be well applied to the detection of food samples.
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CERAMICS INTERNATIONAL
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2022
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IF 5.532
Jiali Song,Yu Gao,Guoguo Tan,Qikui Man,Zhi Wang
Spinel ferrites are widely used for electromagnetic wave (EMW) absorption applications. In this study, spinel Ni–Zn ferrites with excellent microwave absorption properties were synthesized. Their EMW absorption characteristics and interaction mechanisms were studied to lay the foundation for the study of the role of Ni–Zn ferrite as a magnetic substrate for composites. Herein, Ni 0 · 5 Zn 0 · 5 Fe 2 O 4 was prepared by the hydrothermal method (H-NZFO) and the sol–gel auto-combustion method (S-NZFO); both samples exhibited distinct microwave absorption properties. The S-NZFO absorber (thickness = 3.72 mm) demonstrated the best dual-zone microwave absorption with two strong reflection loss peaks at 5.1 and 10.5 GHz. The corresponding effective absorption bandwidth (EAB) reached 9.0 GHz, which covered part of the S-band and all of the C- and X-bands. These results were attributed to the high saturation magnetization, outstanding complex permeability, and multiple magnetic loss channels of S-NZFO. The H-NZFO sample exhibited excellent absorption capability and matching thickness. At a thickness as low as 1.71 mm, the minimum reflection loss ( RL min ) of the H-NZFO absorber reached -60.2 dB at 13.1 GHz. The maximum bandwidth corresponding to RL below -10 dB was 4.6 GHz. These results can be attributed to small particle size, high complex permittivity, and multiple dielectric loss channels of H-NZFO. The observed wide effective absorption bandwidth of S-NZFO and strong microwave absorption capability of H-NZFO suggest the potential of both materials as substrates for efficient microwave absorbers in military as well as civilian absorption applications.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2022
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IF 6.364
Qiuyu Cheng,Xin Chen,Peng Jiang,Qiuying Wang,Zhiwei Wang,M.A. Subramanian
Novel blue pigments based on Ba 0.956 Mg 0.912 Al 10.088- x Ni x O 17 (0 ≤ x ≤ 0.3) and Ba 0.956 Mg 0.912 Al 10.088- x Co x O 17 (0 ≤ x ≤ 0.3) solid solutions were successfully synthesized by solid state method. The XRD results confirmed the structure of the as-synthesized sample belongs to hexagonal β -alumina structure with the space group of P 6 3 / mmc. The d-d electron transitions in Ni 2+ /Co 2+ tetrahedral sites in the visible light range are the reason for the blue colors. Then, the as-prepared blue oxides were sintered with ZrO 2 powders at 1400 °C to prepare blue zirconia ceramic materials. Based on XRD and SEM analysis, the pigment phase is stable after high-temperature sintering with ZrO 2 , and a clear grain boundary is observed. The XCT results indicate the prepared blue ceramics are dense and very small pores are rarely distributed inside the blue zirconia ceramic body. Additionally, the mechanical properties of the fabricated blue ceramics were maintained compared to pure ZrO 2 ceramic.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuwei Ma,Guangtong Hai,Juming Liu,Jinxiao Bao,Yan Li,Ge Wang
Ni-doped cadmium sulfide (CdS) nanospheres with nickel phosphide (Ni 2 P) loading (Ni 2 P@CdS-Ni) were successfully prepared via the two-step thermal treatment growth and chemical reduction method in this work. Firstly, the thermal treatment method was applied to introduce the Ni 2+ into the lattice of CdS and induce the Ni-precursor loaded on surface of the CdS intimately. Then, the Ni-precursor was reduced into Ni(OH) 2 by using the chemical reduction process. Furthermore, the Ni 2 P were loaded on the CdS via the second thermal phosphorization reaction. The loaded Ni 2 P would evidently accelerate the transfer of photo-generated electrons between CdS-Ni and Ni 2 P and meanwhile effectively decrease the charges recombination. Moreover, the results of UV–vis DR spectra and density functional theory (DFT) calculations confirmed that Ni cations doped in the lattice of CdS lead to a doping level at the bottom of the conduct band, which narrowed the bandgap. The work function indicated that doped Ni 2+ helps to enhance the migration and separation of the photo-induced charge. Based on the synergistic effects, 3.7% Ni 2 P@CdS-Ni-3 presented a relatively high hydrogen evolution rate of 176.6 mmol h −1 g −1 under visible light irradiation (λ ≥ 420 nm), which is 63 times of the common CdS.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lei Zuo,Junfeng Wang,Deqing Mei,Derick Adu-Mensah,Yaping Gao
The amounts of methyl stearate (C18:0) and trans-methyl oleate (trans-C18:1) increase during the catalytic transfer hydrogenation (CTH) process of biodiesel. Although it could improve the oxidation stability of biodiesel, its low temperature performance would be worsened. As for it, ultrasonic was introduced in the CTH to control the generation of C18:0 and trans-C18:1. In this study, the ultrasonic-assisted CTH was performed using Raney-Ni as catalyst, isopropanol as hydrogen donor and water as solvent. The effect of operating parameters such as reaction temperature, stirring rate, catalyst dosage, isopropanol amount and water amount on hydrogenation process was investigated. It was revealed that the optimum reaction conditions were determined as reaction temperature 80 °C, stirring rate 600 rpm, catalyst dosage 10 wt%, isopropanol amount 32 g and water amount 100 g in the aspect of the iodine value of bioidesel and the yield of C18:0 and trans-C18:1. The process of the ultrasonic-assisted CTH for biodiesel could be well described by pseudo-first order kinetic model. The conversion rate constants from C18:2 to C18:1 ( k 1 ) and from C18:1 to C18:0 ( k 2 ) were 0.02649 min −1 and 0.00438 min −1 , respectively. Ultrasonic field effectively repressed the selectivity of trans-C18:1 and further decreased the iodine value of biodiesel. On the basis of the same iodine value, the yield of C18:0 and hydrogenation time reduced with ultrasonic. Overall, ultrasonic is an effective intensification method for the CTH of biodiesel in the aspect of product selectivity and reaction rate.
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ANALYTICA CHIMICA ACTA
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2022
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IF 6.911
Tianrun Zhang,Xiuwei Xuan,Mingji Li,Cuiping Li,Penghai Li,Hongji Li
Molecularly imprinted polymer (MIP) membranes prepared in situ present several advantages: they maintain the original morphology, adhere strongly to the collector, and exhibit a controllable structure. In this study, a Ni-polyacrylamide (PAM)-MIP matrix was fabricated in situ on glassy carbon via the one-step electro-polymerization of AM monomers in the presence of Ni and template molecules. Ni 2+ ions were introduced as oxidants to promote AM polymerization and bulking agents to fabricate a three-dimensional porous PAM-MIP matrix. The Ni-PAM-based MIP sensor exhibited a quantitative dual response toward dopamine (DA) and adenine (Ade) in the pH range of 5.0–9.0. The linear concentration range changed depending on the pH environment, and the concentrations of DA and Ade ranged from 0.6 to 200 μM and from 0.4 to 300 μM, respectively. The ranges of detection limits (S/N = 3) were 0.12–0.37 μM for DA and 0.15–0.36 μM for Ade. In addition, the dual-MIP sensor exhibited high reliability in the detection of DA and Ade in human serum owing to its excellent anti-interference ability and long-term stability. The technique developed in this study is expected to facilitate the construction of multi-target response electrochemical biosensors and the reliable determination of small molecules with high selectivity and stability.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 13
·7263-7270
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IF 14.511
Xin Kang,Dongxu Wang,Jiancong Liu,Chungui Tian,He Xu,Jialu Xu,Honggang Fu
Improving the intrinsic catalytic activity of the active phases and mass transfer of the reactants and products are key issues in heterogeneous catalysis. Herein, we construct hollow zeolites with a thin shell of about 10 nm and mesopore structure as supports to load NiMoSX catalysts. On one hand, the nanocages with hollow structures can effectively confine the growth of NiMoSX catalysts, leading to a shorter slab length, higher sulfidation degree, more Ni–Mo–S active sites, and enhanced intrinsic activity. The deep hydrodesulfurization (HDS) activity for dibenzothiophene (DBT) of the NiMoSX/Hol-ZSM-5 catalyst is superior to that of NiMoSX on nanosized ZSM-5 with a reaction rate constant kHDS value of 18.74 × 10−7 mol g−1 s−1. On the other hand, the accessible nanocages and mesopore structure greatly facilitate the mass transfer process and inhibit the formation of carbon deposits, which enhances the HDS stability of NiMoSX/Hol-ZSM-5 to over 80 h. This hollow structure-confined strategy sheds light on the design of novel highly efficient supported catalysts, which we believe could be extended to other heterogeneous catalysis systems.
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Results in Chemistry
·
2022
·
IF 0
Han Sun,Haiping Huang,Chao Hu,Yu Yan,Yongmei Hu,Shengda Guo,Jing-Lin Chen
Cu-Ni oxide nanocomposite was synthesized via solvothermal method with nickel (II) nitrate and copper nitrate as Ni and Cu resource respectively. AuNPs/oxide nanocomposite was obtained by dispersing the oxide into the pre-synthesized Au colloid. Transmission electron microscope (TEM) shows that the synthesized oxides are nanoplate morphology. Interplanar distance from the high resolution TEM (HRTEM) image shows that the Ni and Cu in the oxide are multivalent state. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) characterization further proves that the Ni and Cu are multivalent state, and the Au is Au 0 form in the nanocomposte. EDS-mapping images confirm large numbers of AuNPs are uniformly absorbed onto the ultra-thin multivalent Cu-Ni oxide nanoplate. The electrochemical properties of multivalent oxide (m-v oxide) with or without AuNPs decoration are investigated in 0.1 M potassium chloride electrolyte with 2.0 mM Ferri/Ferro-Cyanide. When employed for the electrochemical catalysis in methanol oxidation reaction (MOR), the AuNPs/m-v oxide exhibits better electrochemistry performance than m-v oxide. The current density of AuNPs/m-v oxide (21.1 mA/cm 2 ) is 3.4 times bigger than that of m-v oxide/GCE (6.2 mA/cm 2 ). What’s more, it shows good electrochemical stability and lower slope of the Tafel plot (41.87 mV/dec).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Hua Yang,Zhang Zhang,Yongsheng He,Peng Wang,Zhuangzhuang Ren,Lizhi Wu,Yu Tang,Li Tan
Ni-based catalysts have been widely investigated in the partial oxidation of methane (POM). However, sintering and carbon deposition are severe problems for Ni-based catalysts in the POM reaction. Here, Ni/Al2O3 catalysts with Al2O3 supports prepared by different synthesis methods are used to investigate the effect of strong metal–support interaction (SMSI) and their relationships to the catalytic performance. As a result, the different strengths of SMSI between Ni species and various Al2O3 supports contribute to generating different contents of the reduced metallic Ni0 sites in the catalysts, which affects the catalytic activity in the POM reaction obviously. The surface unsaturated pentahedral coordination Al3+ centers supply SMSI in the Ni/Al2O3-H catalyst to prevent the catalyst from sintering and coking in the POM reaction, which results in better catalytic activity and catalyst stability. A new view is provided to solve the design of stable metal oxide catalysts by utilizing their SMSI effect.
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APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Dongjie Jia,Xianyu Li,Rongyan Cai,Bochao Ma,Qixian Zhao,Tonglin Chigan,Peipei Yang
Two-dimensional MXene and its composites are among the most attractive electromagnetic wave absorption (EMA) materials due to their unique structure. While previous studies have investigated 2D/2D MoS 2 /Ti 3 C 2 T x heterojunctions for EMA, there is still a need for further adjustments to interface structure to enhance polarized electron density and electron transfer capacity. In this study, Cl-Ti 3 C 2 T x was prepared by Lewis acid molten salt etching of Ti 3 AlC 2 , and S-Ti 3 C 2 T x was prepared by replacing Cl with S. MoS 2 nanosheets were grown on the surface of S-Ti 3 C 2 T x by a simple hydrothermal method, forming a Ti-S-Mo covalent interface. The EMA properties of the composites were further optimized by adjusting the interface oriented polarization and electronic structure through Ni doping. Compared to MoS 2 /TiO 2 /Ti 3 C 2 T x , the electromagnetic wave absorption performance of Ni-MoS 2 /TiO 2 /Ti 3 C 2 T x had been significantly improved. When the Ni doping amount was 0.086 mmol, the minimum reflection loss of Ni-MoS 2 /TiO 2 /Ti 3 C 2 T x could reach −48.04 dB at 8.64 GHz, with an effective absorption bandwidth of 3.28 GHz. This study provides theoretical basis and experimental evidence for the follow-up research of MXene-based composite EMA materials.
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