ChemCatChem
·
2022
·Vol. 15
·期 4
·e202201399
·
IF 5.497
Changle Fu,Liangliang Feng,Hongyan Yin,Yuhang Li,Guodong Li,Yongqiang Feng,Liyun Cao,Jianfeng Huang,Yipu Liu
Graphical Hierarchized Microflowers for Hydrogen Evoluation Reaction : A novel tactic of synergetic electronic coupling is successfully developed for rationally engineering hierarchical heterostructured electrocatalyst towards hydrogen evolution reaction. The exploration of economical and highly efficient electrocatalysts for hydrogen evolution reaction (HER) is paramount for the development of sustainable hydrogen economy. Herein, a novel three-dimensional (3D) hierarchical microflower electrocatalyst comprised of N-doped carbon-armored Ni 3 P/Ni/VN heterogeneous nanoparticles (Ni 3 P/Ni/VN@NC) is developed by combining a hydrothermal method with in-situ carbonization-phosphating strategy. The unique robust hierarchical structure derived from 3D NiV layered double hydroxide (NiV-LDH) skeleton as precursor provides multidimensional mass and charge transport channels as well as numerous active sites for HER, leading to the improved HER activity. More importantly, the possible electron transfer route of Ni 3 P→Ni→VN is demonstrated due to the charge pumping capability of VN during interfacial electron intercoupling among the tri-component, which endows Ni 3 P/Ni/VN with the favorable absorption of hydrogen-intermediates and thus upgraded HER kinetics over such heterostructure. The resulting Ni 3 P/Ni/VN@NC catalyst exhibits extremely low overpotentials of 81 mV and 134 mV to deliver a current density of 10 mA cm −2 without iR -compensation in alkaline and acidic media, respectively, and maintains continuous operation for over 90 h. This work enlightens the rational design of hierarchical multi-component heterostructured catalysts for efficient hydrogen production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Lian Xue,Ying Shi,Cunping Huang,Qiang Wu,Bingbing Chen,Weifeng Yao
Effective and affordable photocatalysts play an important role in the cost reduction of solar hydrogen production through photocatalytic water splitting. In this research, a Zn 2+ and Ni 2+ modified carbon hydrogen evolution cocatalyst (ZnNi-C) were synthesized and immobilized onto the surface of CdS (CdS@ZnNi-C) for photocatalytic hydrogen evolution (PHE). The preparation used an ethylenediaminetetraacetic acid disodium (EDTA)-assisted method. The hydrogen evolution rate and apparent quantum efficiency (AQE) at 420 nm for an optimized CdS@ZnNi-C photocatalyst are15.7 mmol/h/g and 31.4 %, respectively. The rate is 2.4 times and 3.7 times greater than those of Zn 2+ and Ni 2+ modified carbon cocatalysts (Zn-C) and (Ni-C) on CdS (CdS@Zn-C) and (CdS@Ni-C), respectively. Density functional theory calculations indicate that the elevated catalytic performance of CdS@ZnNi-C is due to the co-anchored Zn 2+ and Ni 2+ in carbon layers that lead to a favorable Gibbs free energy (ΔG H *) for hydrogen evolution. This approach is valuable for the design of stable and efficient photocatalysts for renewable hydrogen production.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiankan Zhang,Fengqi Zhao,Hui Li,Zhifeng Yuan,Ming Zhang,Yanjing Yang,Qing Pei,Ying Wang,Xueli Chen,Zhao Qin
Micron-sized aluminum particles tend to melt into agglomerates, leading to incomplete combustion, two-phase flow losses, and energy decrease of propellants. The higher ignition performance of core–shell Al@Ni makes it a promising candidate fuel with high combustion efficiency. However, little work has been done to study the combustion of Al@Ni in propellants. Here, we report a first attempt to investigate the combustion mechanism of core–shell Al@Ni in the double-based propellant containing high energy explosive HMX , and evaluate its potential as a fuel. Nickel in Al@Ni is determined to play a critical role during its intrinsic combustion and the combustion in propellants. In the condensed phase, the presence of Ni enhances the oxidation process by forming a porous oxide layer on the aluminum surface that promotes oxygen diffusion. Subsequently the phase transition and expansion of Ni break down this oxide layer, leading to the earlier ignition on the burning surface. Upon Al melting, the alloying of Ni and Al accelerates the volume expansion and surface tension reduction of the fuel, giving rise to vigorous melt-dispersion combustion and enhanced energy release. Enhanced thermal feedback and thermal decomposition exotherm combined to increase the burning rate of propellant. The resulting higher flame temperature allows the evaporation of small aluminum droplets into vapor to form smoke oxide productions, further reducing the size distribution of the condensed combustion products (CCPs). This study demonstrates the potential of Al@Ni as an effective fuel for double-based propellants, and provides the insight into its combustion mechanism in HMX-CMDB propellants, which is believed to be important for the development of novel aluminum-based fuels for solid propellants.
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ADVANCED MATERIALS
·
2022
·Vol. 35
·期 5
·2205262
·
IF 32.086
Runyao Zhao,Yiding Wang,Guipeng Ji,Jiajun Zhong,Fengtao Zhang,Meifang Chen,Shengrui Tong,Peng Wang,Zhonghua Wu,Buxing Han,Zhimin Liu
Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers a promising strategy to lower CO 2 emission while producing value-added chemicals. A great challenge facing CO 2 RR is how to improve energy efficiency by reducing overpotentials. Herein, partially nitrided Ni nanoclusters (NiN x ) immobilized on N-doped carbon nanotubes (NCNT) for CO 2 RR are reported, which achieves the lowest onset overpotential of 16 mV for CO 2 -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN x /NCNT affords a CO generation rate of 43.0 mol g −1 h −1 at a low potential of −0.572 V (vs RHE). DFT calculations reveal that the NiN x nanoclusters favor *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO 2 RR overpotential. As NiN x /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm −2 , with total energy efficiency of 62.2%.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Yan Zhang,Chuang Chen,Qiu-Hui Zheng,Zhan-Kuo Guo,Bao-Xia Dong,Yun-Lei Teng
Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped NiII-triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni–S–CT (T = 800, 900, 1000 °C) materials with Ni3S2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i–t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni–S–CT catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni–S–C1000 exhibited the best catalytic activity (FECO of 66.6% and jCO of 1.28 mA/cm2). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni3S2 to illustrate the ECR activity origination. It is the first report on Ni3S2-based catalysts in the application of ECR.
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Small
·
2022
·Vol. 19
·期 2
·2205719
·
IF 15.153
Wenjun He,Rui Zhang,Da Cao,Ying Li,Jun Zhang,Qiuyan Hao,Hui Liu,Jianling Zhao,Huolin L. Xin
Exploiting active and stable non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER) at large current density plays a key role in realizing large-scale industrial hydrogen generation. Herein, a self-supported microporous Ni(OH) x /Ni 3 S 2 heterostructure electrocatalyst on nickel foam (Ni(OH) x /Ni 3 S 2 /NF) that possesses super-hydrophilic property through an electrochemical process is rationally designed and fabricated. Benefiting from the super-hydrophilic property, microporous feature, and self-supported structure, the electrocatalyst exhibits an exceptional HER performance at large current density in 1.0 M KOH, only requiring low overpotential of 126, 193, and 238 mV to reach a current density of 100, 500, and 1000 mA cm −2 , respectively, and displaying a long-term durability up to 1000 h, which is among the state-of-the-art non-precious metal electrocatalysts. Combining hard X-rays absorption spectroscopy and first-principles calculation, it also reveals that the strong electronic coupling at the interface of the heterostructure facilitates the dissociation of H 2 O molecular, accelerating the HER kinetics in alkaline electrolyte. This work sheds a light on developing advanced non-precious metal electrocatalysts for industrial hydrogen production by means of constructing a super-hydrophilic microporous heterostructure.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 47
·22778-22785
·
IF 3.925
Xiaozhi Li,Jutao Qiao,Dan Luo,Siyi Xu,Yuefeng Liu,Hao Liu
In this study, Ni nanoparticles were grown on a silver-coated nylon yarn (SCNY) surface by electrochemical deposition to prepare SCNY@Ni. The hierarchical Ni–Ag nanostructure promoted their synergistic effect, which enhanced the electrocatalytic behavior of glucose oxidation. The test result of SCNY@Ni showed its high sensitivity (115.26 μA mM−1 cm−2 and 67.37 μA mM−1 cm−2) with a wide linear response (from 2 μM to 1 mM and from 1 mM to 22 mM) of glucose con-centration range, a low detection limit (LOD) of 2 μM, fast response time (3 s), and good selectivity for glucose determination in the presence of sucrose (SU), aceta-mino phenol (AP), D-fructose (D-Fru), ascorbic acid (AA), dopamine (DA), hydro-quinone (HQ) and uric acid (UA) as potential interference species. Also, SCNY@Ni exhibited excellent stability, repeatability, reproducibility and flexibility. It has good prospects for large-scale production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Run Yu,Qianqiao Chen,Wenhua Li,Xinyuan Yu,Qin Zhong
Severe photocorrosion and fast photoexcited charges recombination hinder the application of Cu 2 O in photoelectrochemical (PEC) water splitting. In this work, Ni-doped metal-organic frameworks is firstly applied to improve the performance of electrodeposited Cu 2 O. A decorative layer of Ni-doped Cu 3 (BTC) 2 (Ni-CuBTC) was in-suit constructed on Cu 2 O through solvothermal followed by ion-exchange. Cu 2 O/Ni-CuBTC photocathodes increase absorption edge to ∼800 nm, positive shift flat band position to 0.4 V, and decrease Tafel value to 74 mV/dec. These results confirm the decorative layer can extend light absorption, facilitate photoexcited charge separation and transfer, and enhance HER activity. A photocurrent density of −1.51 mA/cm 2 at 0 V RHE is obtained with the decoration of Ni-CuBTC, which is 3.4 times of pristine Cu 2 O photocathode. Here, the PEC water splitting performance of electrodeposited Cu 2 O has been significantly improved with noble-metal-free decorations, which provides a new idea for solving the defects of Cu 2 O based photocathode.
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CERAMICS INTERNATIONAL
·
2022
·
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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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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CHEMICAL ENGINEERING JOURNAL
·
2022
·
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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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 13
·7263-7270
·
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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