JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Junzheng Jiang,Yunfan Qiu,Hao Dong,Lei Yang,Yaping Miao,Liwei Xiong,Biao Gao,Xuming Zhang,Paul K. Chu,Xiang Peng
Molybdenum nitrides have garnered significant attention for their potential in the hydrogen evolution reaction (HER) due to their metallic behavior, abundant reserves, and pH-universal stability. However, their unsatisfactory hydrogen adsorption limits industrial applications. Heterostructures can be designed to introduce defects and modulate the electronic structure of catalysts to optimize hydrogen adsorption to enhance HER. Nevertheless, the exact active sites at the heterointerface and the fundamental mechanisms underlying the HER process remain inadequately understood. Herein, a composite electrocatalyst in which metallic Ni and MoN phases (Ni/MoN) form the heterointerface between them is fabricated. The heterointerface produces strong electronic interactions between Ni and MoN to facilitate electron transfer from MoN to Ni, and the built-in electric field facilitates charge transfer during electrocatalysis. This optimized electronic configuration with abundant active sites delivers excellent performance in alkaline HER. Density-functional theory calculations demonstrate that H 2 O dissociates at the Ni site, whereas H 2 desorption occurs at the Mo site. As a result, Ni/MoN/CC requires an overpotential of only 95 mV to achieve a current density of 10 mA cm −2 and a Tafel slope of 104 mV dec −1 . Moreover, it maintains a high current density of 100 mA cm −2 for 100 h with negligible morphological or compositional changes. The strategy of modulating the electronic structure of low-cost, transition metal-based heterostructured electrocatalysts is an effective and commercially viable means to design and develop high-performance electrocatalysts for water splitting.
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PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 5
·053507
·
IF 3.1
Wenzheng Wu,Xiaojie Tang,Jing Wang,Chenghan Zhao
With the rapid development of electronics, additive manufacturing of complex three-dimensional microscale metal and alloy structures has emerged as one of the future directions for advanced technologies. In this study, a localized electrochemical deposition technique was developed which enables the fabrication of microscale three-dimensional metal structures in an ambient environment. Notably, we investigated the effects of voltage, initial electrode gap, and electrolyte composition on the deposition of Cu-Ni alloy. Furthermore, we successfully fabricated Cu-Ni equiatomic micro-columns, providing possibilities for the micro/nanoscale fabrication of commercial K-Monel copper. Finally, based on these foundations, we successfully shaped overhanging structures with various angles as well as an "H" structure using a rotating cathode substrate, demonstrating their potential in the fabrication of Cu-Ni alloy micro components.
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ACS Nano
·
2024
·
IF 15.8
Miao Chang,Fangyuan Cheng,Wen Zhang,Mengyi Liao,Qing Li,Chun Fang,Jiantao Han
Surface engineering is sought to stabilize nickel-rich layered oxide cathodes in high-energy-density lithium-ion batteries, which suffer from severe surface oxygen loss and rapid structure degradation, especially during deep delithiation at high voltages or high temperatures. Here, we propose a well-designed oxygen-constraining strategy to address the crisis of oxygen evolution. By integrating a La, Fe gradient diffusion layer and a LaFeO3 coating into the Ni-rich layered particles, along with incorporating an antioxidant binder into the electrodes, three progressive lines of defense are constructed: immobilizing the lattice oxygen at the subsurface, blocking the released oxygen at the interface, and capturing the residual singlet oxygen on the external surface. As a result, effective surface passivation, mitigated bulk and surface degradation, suppressed side reactions, and enhanced electrochemical performance are achieved, far beyond conventional single surface modification. The Ni-rich layered oxide cathodes with integrated oxygen-constraining modifications demonstrate impressive cycling stability in both half-cells and full cells, achieving stable long-term cycling even at a high cutoff voltage of 4.7 V and a high temperature of 45 °C. This work provides a multilevel oxygen-constraining strategy, which can be extended to various layered oxide cathodes involving oxygen release challenges, providing an effective path for the development of high-energy-density lithium-ion batteries.
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PubMed
高影响因子
Advanced Energy Materials
·
2024
·
IF 24.4
Hongyan Zhang,Hao Zhou,Hua Wang,Yikai Wang,Xuehan Yang,Dan Wu,Pan Yuan,Maoshuai He,Wenxian Wei,Tao Yang
Water electrolysis holds the promise of transforming electric-power into hydrogen energy through a carbon free process and its widespread application highly depends on anodic oxygen evolution reaction (OER) efficiency. Transition metal-based OER catalysts meet the requirements of long-term development for cost effectiveness, and their performance can be improved by a variety of band electronic structure modulating methods. Herein, a multihybridization strategy is proposed, i.e., p-d, s-sp , and d-d hybridization are emphasized together, which guides the design of an effective vanadium (V), boron (B)-FeNiP catalyst. Density functional theory analysis reveals the existence of multihybridization and the difference between Fe and Ni in terms of hybridization strength, band configuration, and interfacial charge transfer. Specially, Fe and Ni sites are simultaneously optimized to their highest performance upon the dual B, V incorporation. As a result, the VB-FeNiP catalyst displays outstanding OER performance, regarding a Tafel slope of 57.64 mV dec −1 , an overpotential of 175 mV at 100 mA cm −2 , and exceptional stability. Here the synergistic effect of multihybridization in the design of transition metal-based catalysts is highlighted and the work in pursuit of effective way based on regulating band configuration to developing high performance OER catalysts would be evoked.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 9
·6807-6818
·
IF 2.993
Gao Shuwen,Sui Yanwei,Wei Fuxiang,Qi Jiqiu,Meng Qingkun,He Yezeng
Metal–organic frameworks (MOF) used directly in supercapacitors have attracted much attention for their special porous structure and potential high performance. Here, the Ni-MOF is fabricated by one-step facile hydrothermal method with a modification of mixed solution with DMF and water instead of pure DMF. After characterization, the Ni-MOF exhibits loosely stacked layer-cuboid structure with abundant mesoporous, which is beneficial for the charge transfer and ion transport for supercapacitors. In the three-electrode system, this Ni-MOF serving as working electrode shows remarkable specific capacitance of 804 Fg −1 at 1 Ag −1 , excellent rate capacitance of 534 Fg −1 at 10 Ag −1 , and with 302 Fg −1 retention after 5000 cycles, when measured in 2 M KOH electrolyte solution. To make a further research into the practical utility of the Ni-MOF, the Ni-MOF//AC asymmetrical supercapacitor device is assembled with the Ni-MOF and active carbon acted as positive and negative electrode materials, respectively. This device exhibits high specific energy of 31.5 Wh kg −1 , at specific power of 800 W kg −1 . All these results demonstrate that this Ni-MOF is a kind of promising electrode material for high-performance supercapacitors.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Qian Zhang,Xunzhu Jiang,Yang Su,Yang Zhao,Botao Qiao
With the increasing production of propane from shale gas and the growing demand for propylene, propane dehydrogenation (PDH) has gained significant attention as a promising route for the on-purpose production of propylene. As a cheap yet efficient catalyst, Ni-based catalysts have attracted interest because of its ability to activate alkane. Single-atom catalysts (SACs) can maximize the metal atom utilization. Here, we demonstrate that anatase TiO 2 supported Ni SAC (Ni 1 /A-TiO 2 ) exhibits not only superior intrinsic activity and propylene selectivity but also much better stability than the corresponding Ni nanoparticle (NP) catalyst (Ni NP /A-TiO 2 ) in PDH reaction at 580 °C. The rate of propylene production on Ni 1 /A-TiO 2 is about 1.96 mol C3H6 g Ni −1 h −1 , about 65 times higher than that of Ni NP /A-TiO 2 sample (0.03 mol C3H6 g Ni −1 h −1 ). In combination of high-angle annular dark-field scanning transmission electron microscopy, in-situ diffuse reflectance infrared Fourier transform spectra, in-situ X-ray photoelectron spectroscopy and X-ray absorption spectroscopy characterizations, we confirm that the Ni SAC mainly contains individual Ni atom singly dispersed on the support in positive Ni (II) valence state. In addition, as a result of strong metal-support interaction (SMSI) between Ni NP and TiO 2 carrier under reduced conditions, the Ni NPs sites are encapsulated by TiO x overlayer (~2 nm thick) thus display poor reaction performance.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yilin Zhang,Yanhui Long,Kaiyi Wang,Xiaosong An,Liboting Gao,Zijiang Zhao,Jianhua Yan,Hao Zhang
Developing alternatives to the energy-intensive Haber–Bosch (H–B) process for ammonia synthesis is imperative yet challenging. Herein, Ni-modified zeolitic imidazolate framework (ZIF) Ni@ZIF-67 nanocrystals were synthesized and applied in a dielectric barrier discharge reactor for plasma-assisted ammonia synthesis under ambient pressure. Introducing ZIF-67 into the plasma enhanced the ammonia synthesis rate by an order of magnitude, evidencing strong plasma–catalyst synergism. The superior performance was attributed to the unique microstructure featuring a high specific surface area and abundant porosity, which improved gas adsorption and intensified microdischarge within the plasma. Further incorporation of Ni into ZIF-67 (Ni@ZIF-67) resulted in a maximum ammonia synthesis rate of 289.45 μmol g–1 min–1 and an energy yield of 1.83 g kWh–1─a 32.0% improvement over ZIF-67─while maintaining structural stability over repeated cycles. Moreover, the confinement of NH3 within sub-Debye-length micropores suppressed plasma-induced decomposition. The addition of Ni further significantly boosted both the hydrogen/ammonia adsorption capability and discharge efficiency, which promoted ammonia formation, especially in a H2-rich atmosphere. These findings underscored the potential of Ni@ZIF-67 as a promising catalyst for plasma-assisted ammonia synthesis, providing a viable alternative to the conventional H–B process.
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Materials Today Energy
·
2025
·
IF 8.6
Hongliang Fu,Qiaowei Wang,Yue Lian,Yongfeng Hu,Jing Zhao,Huaihao Zhang
It is crucial to rationally design catalysts with high activity and strong stability for electrolytic water oxygen evolution reaction (OER). Here, Ni-FeNbO 4 @NC microspheres were successfully synthesized as OER catalysts by interface optimization and Ni-doping. To address FeNbO 4 problems such as easy agglomeration, low catalytic activity and poor electrical conductivity, the catalyst was incorporated in N p-orbital of imidazole and metals (Ni and Fe) empty d-orbitals to form coordination compound, thus avoiding oxides direct contact and effectively improving dispersion. Moreover, Ni-doping provides additional catalytic active sites, good current impact resistance and large intrinsic conductivity for Ni-FeNbO 4 @NC. Besides, under high-temperature carbonization, the Ni-FeNbO 4 surface imidazole evolves into N-containing carbon layer, which enhances overall electrical conductivity to reduces ohmic overpotential. According to density functional theory calculations (DFT), Ni-doping lowers Gibbs free energy of OER decisive rate step, and enlarges reaction kinetics. From in-situ Fourier Transform infrared spectroscopy (FTIR) and in-situ differential electrochemical mass spectrometry (DEMS), Ni-FeNbO 4 @NC displays multiple types of catalytic active sites (Ni∗, and C-N∗) and efficient oxygen production efficiency. Under the synergistic effect of interface optimization and Ni-doping, Ni-FeNbO 4 @NC exhibits good catalytic activity in OER (low overpotential: 286 mV@10 mA cm −2 , small Tafel slope: 56.7 mV dec −1 , 50 h long stability).
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xinling Zhang,Yongxiao Tuo,Qing Lu,Yuanyuan Liu,Jiabing Luo,Hui Zhang,Jingyuan Shang,Yan Zhou,Jun Zhang
The impact of carbon material curvature is often underestimated in studies of carbon-based electrocatalysts for the CO 2 reduction reaction (CO 2 RR). To clarify its role, we tuned the diameter of nitrogen-doped carbon nanotube (NCNT) by controlling the size of embedded Ni nanoparticles (50 to 120 nm), in which the Ni-modified C-N species has been identified as an efficient site for CO 2 RR to CO. We found that the FE CO and TOF increase with the curvature of NCNT, particularly in the high potential window that is the diffusion-limited region. This enhancement is attributed to accelerated CO desorption since the electrophobic nature of high-curvature C-N defects reduces hybridization between *CO and active sites. These insights highlight curvature engineering as a promising strategy to enhance CO current density in carbon-based electrocatalysts.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Tong Zhang,Haiyong Wang,Chenguang Wang,Qiying Liu
Acetol is the important platform molecule, which showed diversified applications in organic synthesis, pharmaceutic, food and polymer industrials. The production of acetol from selective fructose hydrogenolysis is of scientific and practical interests. However, by catalysis, precisely controlling the target C-C and C-O bonds splitting is an open challenge, resulting in the low target product yields. Herein, by regulating the metal-support-interactions, which enhanced electron transfer capacity and improved acetol production from fructose hydrogenolysis through controlling the important intermediate species, obtaining the highest 53.6 % yield and an average conversion rate of 1.24 × 10 −5 mol/(g cat .s) within short time of 10 min. The interfacial charge transfer in the surface structure of the catalyst along with the Ni metal content was revealed by various characterizations. This research provides a preliminary method for electron transfer regulation of Ni/CeO 2 catalysts in acetol production from fructose hydrogenolysis, showing practical application potentials due to the simple preparation of the catalyst that possibly contribute to the reactions on a large scale.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2015
·
IF 2.729
Yijing Xia,Qizhou Dai,Jianmeng Chen
The novel nickel modified PbO 2 electrodes were successfully prepared via electrodeposition in nitrate solution. The influence of nickel content on the physico-chemical properties and electrocatalytic performance of PbO 2 electrodes was investigated. The electrodes were characterized by SEM, EDX and XRD techniques. A limited amount of doping nickel could produce a more compact PbO 2 film and diminish the size of the crystal grains. The steady-state polarization curves and the cyclic voltammetry analysis showed that the 1% Ni–PbO 2 electrode had the highest oxygen evolution potential and the optimal electrochemical oxidation ability. The cyclic voltammograms with various scan rates showed that the oxidation of aspirin on these PbO 2 electrodes was a typical diffusion-controlled electrochemical process. Stability tests of different PbO 2 electrodes showed that 1% Ni–PbO 2 electrode had the highest electrochemical stability. In addition, nickel modified PbO 2 electrodes were used to degradation aspirin in aqueous solution, which gave the direct evidence of the electrocatalytic capabilities of these electrodes. The results showed that 1% Ni–PbO 2 electrode obtained the highest kinetic rate constant, chemical oxygen demand (COD) and total organic carbon (TOC) removals, which were 1.41, 1.22, 1.20 times than those of undoped PbO 2 electrode, respectively. Moreover, the energy required for the treatment of 1 m 3 aspirin solution significantly decreased and the hydroxyl radical utilization rate was enhanced after appropriate nickel doping. As a result, the 1% Ni–PbO 2 electrode is a promising anode for the treatment of organic pollutants.
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Nanomaterials
·
2020
·Vol. 11
·期 1
·31
·
IF 4.324
Qianqian Shen,Yu Zhang,Xuesha Li,Li Xiang,Chaoyin Nie
In order not to sacrifice nitrided layer thickness and reduce brittle compound layer thickness, Ni-coated pretreatment was carried out with electrodeposition on a pure iron surface, followed by gas nitriding. The brittle compound layer thickness of duplex surface treated samples was reduced, and the nitrided layer thickness increased to 320 μm. The microhardness was 4 times harder, and the wear loss was reduced by 68% compared with the original material. The results indicate that Ni-coated pretreatment could effectively improve microhardness and wear resistance and realize the controlled microstructure of a brittle compound layer of pure iron without compromising nitrided layer thickness. Ni coating plays an important role in ammonia adsorption and decomposition, and in the transfer of active nitrogen atoms during nitriding.
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