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Catalysis Science & Technology · 2019 ·Vol. 9 ·期 20 ·5651-5659 · IF 5.726

Homogenous electrochemical water oxidation by a nickel(II) complex based on a macrocyclic N-heterocyclic carbene/pyridine hybrid ligand

Hossain M. Shahadat,Hussein A. Younus,Nazir Ahmad,Md. Abdur Rahaman,Zafar A. K. Khattak,Serge Zhuiykov,Francis Verpoort

Water-soluble homogeneous nickel catalysts have been rarely investigated for catalytic water oxidation as compared to their heterogeneous counterparts. Herein, we report homogenous electrochemical water oxidation by a nickel(II) complex, ([NiL](PF6)2 (L = bis(2-pyridyl-methylimidazolylidene)methane), based on a macrocyclic N-heterocyclic carbene/pyridine hybrid ligand under neutral and alkaline conditions. The catalyst displayed the stable catalytic current of 0.65 mA cm−2 at the overpotential of 0.80 V (∼0.55 V at GCE for CV) with a ∼93% Faradaic efficiency at pH 9.0 for oxygen evolution in long-term bulk electrolysis. The CV, UV-vis, ESI-MS, SEM, and EDX results demonstrated that the catalyst was impressively stable even after long-term controlled potential electrolysis (CPE) (11 h) and homogeneous in nature. The synthesis of this catalyst is straightforward, and its complex is air and moisture stable. To the best of our knowledge, this is the first study on the investigation of a Ni–NHC complex for water oxidation under aqueous conditions (acetate/phosphate). According to the literature, the role of the phosphate ion in homogenous nickel-catalysed water oxidation was found to vary from catalyst poisoning to activation. Interestingly, the catalytic activity of our catalyst in phosphate buffer was significantly higher than that with acetate ions at the same pH value; this might indicate the key role of phosphate ions as proton acceptors, which boosted the catalyst activity via enhanced PCET during catalysis.

研究领域: 无机化学 · 电化学 · 催化化学 · 配位化学 · 能源化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Stable selenium nickel-iron electrocatalyst for oxygen evolution reaction in alkaline and natural seawater

Jue Wang,Zhi Li,Libei Feng,Dachun Lu,Wei Fang,Qinfang Zhang,Daniel Hedman,Shengfu Tong

The development of efficient and stable catalysts for oxygen evolution reaction (OER) in seawater presents a major challenge for hydrogen production through water electrolysis. In this work, we present a stable NiFe foam catalyst with a Se-doped Ni/Fe oxide surface prepared through a combination of chemical vapor deposition and electrochemical exfoliation. This method effectively modifies the surface of the commercial NiFe foam to a rough and stable Se-doped Ni/Fe oxide surface, displaying exceptional OER performance in both freshwater and seawater with more than 54 days stability in natural seawater. Characterizations reveal Ni-Se doped Fe oxide surface, with subsurface layers consisting of Ni alloyed with a moderate concentration of Fe, optimizes the adsorption free energy of oxygen-containing intermediates. Our results demonstrate a surface engineering approach to activate NiFe foam as a robust OER catalyst for seawater electrolysis, which is beneficial for the hydrogen economy and for the environment.

研究领域: 材料科学 · 电化学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Highly durable porous NiO-derived electrodes with superior bifunctional activity for scalable alkaline water electrolysis

Shukai Diao,Tianwen Wang,Wen Kuang,Su Yan,Xiaotian Zhang,Mingxuan Chen,Ying Liu,Aidong Tan,Tianrang Yang,Jianguo Liu

Alkaline water electrolysis (AWE) is a leading “green hydrogen” production technology. Industrial electrodes use alkaline leaching to remove Al from NiAl alloy, creating pores and increasing specific surface area (SSA) but still suffer from poor electrode performance. This study presents a method for fabricating an efficient bifunctional electrode. The process involves creating a porous Ni layer with high SSA on nickel mesh (NM) by reducing NiO, which facilitates the formation of Ni(OH) 2 nanosheets. The resulting Ni/Ni(OH) 2 @NM electrode features a hydrophilic, gas-repellent and highly electrochemically active surface. It achieves low overpotentials for hydrogen and oxygen evolution reactions (164 mV and 337 mV at 100 mA/cm 2 , respectively). The electrolyzer using Ni/Ni(OH) 2 @NM electrodes only requires 1.695 V to achieve 300 mA/cm 2 at 80 °C after a 2000 h durability test. The electrode also demonstrates excellent stability under frequent start-stop cycles, making it well-suited for integration with intermittent renewable energy sources.

研究领域: 材料科学 · 能源技术
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COMPOSITES PART B-ENGINEERING · 2020 · IF 7.635

An unusual decrease in dielectric constant due to the addition of nickel hydroxide into silicone rubber

Xuan Guo,Hua Deng,Qiang Fu

Materials with low dielectric constant have drawn more and more attention due to their wide range of applications in electronic devices. Two type of methods are often used to reduce the dielectric constant of a given materials: introducing voids and replacing groups having higher polarizability with the ones having lower through copolymerization . Different from above methods, current study proposes a novel and efficient method by allow inorganic filler participating the curing process of polymer matrix , thus, consuming some of the functional groups with high polarizability. Nickel hydroxide (Ni(OH) 2 ) is selected as filler to be dispersed in room temperature vulcanized silicone rubber (SR). The addition of 1% Ni(OH) 2 into SR has resulted a decrease in dielectric constant from 3.1 to 2.1, and slightly reduced dielectric loss. With further increasing Ni(OH) 2 content, the dielectric constant increases gradually. From various characterizations, it is confirmed that Ni(OH) 2 is involved in the curing process of SR, thus, the hydroxyl group content in the final composites is reduced. Meanwhile, Ni(OH) 2 with different size and synthesized Ni(OH) 2 from hydrothermal process is also used to further confirm such observation. This method provides a novel route for the preparation of low dielectric constant materials.

研究领域: 材料科学 · 电子工程
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ENERGY & FUELS · 2020 · IF 3.421

Preparation of Bush-Like Ru/NiO-Ni Foam Catalyst and Its Performance in Hydrogen Production from Sodium Borohydride Alcoholysis

Fanghui Wang,Yimeng Luo,Yajun Zhang,Yanan Wang,Hong Zhu

A NiO–Ni foam composite carrier was prepared by the hydrothermal method. Ruthenium metal was supported on the NiO–Ni foam by electroplating, obtaining a highly active bush-like Ru/NiO–Ni foam catalyst. To investigate the effect of NiO on the structure and performance of the catalyst, a Ru/Ni foam catalyst was prepared as a reference. The structures of the carrier and both catalysts were characterized by X-ray diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy, and the performances of both catalysts were evaluated in alcoholytic hydrogen production from sodium borohydride. On the carrier with the NiO-treated surface, the active component Ru developed a three-dimensional bush-like structure that enhanced the catalytic activity. Indeed, the hydrogen production from alcoholysis of sodium borohydride was three times higher on the Ru/NiO–Ni foam catalyst than on the Ru/Ni foam catalyst, and the highest rate exceeded 6 L/g/min. The repeated-use stability of the Ru/NiO–Ni catalyst (10 times) also exceeded that of Ru/Ni foam (8 times). However, as both catalysts used the same active component (i.e., Ru), their activation energies were almost identical.

研究领域: 材料科学 · 催化化学
✓ 已验证 DOI 高影响因子
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SURFACE & COATINGS TECHNOLOGY · 2021 · IF 4.158

Effect of Al content on wear and corrosion resistance of Ni-based alloy coatings by laser cladding

Xiaoli Feng,Haifeng Wang,Xuechao Liu,Canming Wang,Hongzhi Cui,Qiang Song,Kun Huang,Neng Li,Xue Jiang

Inconel 625  + x Al ( x  = 0, 2.5, 5.0, 7.5, 10.0) alloy coatings were prepared by laser cladding. The addition of Al promoted the formation of the BCC phase, which changed the coating microstructure from an FCC + δ phase + Laves phase to FCC + BCC + δ phase + Laves phase. Inconel 625 + 2.5 Al alloy showed the greatest corrosion resistance among all samples. The formation of an Al 2 O 3 film improved the corrosion resistance of the coating, but excess Al decreased the Cr 2 O 3 content in the film, which decreased the corrosion resistance of the coating. Increasing the Al content aggravated the lattice distortion and improved the solid solution strengthening effect, while also increasing the amount of BCC phase, which improved the coating hardness. After adding Al, the Inconel 625 + x Al alloy coatings displayed strong plastic deformation resistance, and their wear resistance was improved due to the presence of a hard phase.

研究领域: 材料科学 · 表面工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Nickel complex co-catalyst confined by chitosan onto graphitic carbon nitride for efficient H2 evolution

Jun-Shuai Zhang,Wei-De Zhang

Developing earth-abundant H 2 -production heterogeneous photocatalysts with robust activity and stability has attracted great interests. Herein, a low-cost photocatalyst was prepared by binding nickel complex covalently from primary amines of chitosan (NiL) onto photosensitive carbon nitride nanosheets (CN) through electrostatic interaction. Introduction of NiL results in more efficient utilization of solar energy, photogenerated electrons’ direct transfer and lower overpotential for water reduction. The optimized NiL3-CN photocatalyst shows the highest H 2 evolution rate of 346 μmol g −1  h −1 under visible light irradiation and exhibits high stability during test. This work presents great potentials for sustainable conversion of solar energy, and sheds positive light on the development of heterogeneous photocatalysts via anchoring H 2 -evolving molecule catalysts confined by inexpensive macromolecules onto a semiconductor photosensitizer through a facile and valid method.

研究领域: 材料科学 · 催化化学 · 可再生能源
✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY · 2022 · IF 5.436

Modulating Electronic Characteristics of Nickel Molybdate via an Effective Manganese-Doping Strategy to Enhance Oxidative Desulfurization Performance

Xin An,Wei Jiang,Jing He,Linhua Zhu,Lingchao Xu,Hongping Li,Wenshuai Zhu,Huaming Li

Modulating the electronic characteristics of catalysts plays a significant role in optimizing their catalytic activity. Herein, Mn-doped nickel molybdate (MNMO) nanorods are synthesized via replacing the partial Ni sites by the Mn element, engineering a bimetallic synergistic effect to enhance the activation of oxygen (O2). Compared with the extremely low catalytic activity of pristine nickel molybdate (NiMoO4), complete desulfurization can be achieved by MNMO under the same reaction conditions. Characterization results show that the electronic structure and surface atomic composition of pure NiMoO4 will be modulated owing to the introduction of Mn atoms, leading to the enhancement of the oxygen vacancy content and stronger O2 activation capacity. Besides, the optimized catalyst MNMO-20 also displays satisfactory cycle performance, and the sulfur removal of dibenzothiophene still maintains 96.1% after six times of recycling. The distinctive engineering strategy and simple synthesis method provide a new insight in designing and developing oxidative desulfurization catalysts with high stability and effectivity.

研究领域: 催化材料 · 环境化学 · 能源化学
✓ 已验证 DOI 高影响因子
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International Journal of Minerals Metallurgy and Materials · 2022 ·Vol. 30 ·期 1 ·54-62 · IF 3.85

Effects of highly dispersed Ni nanoparticles on the hydrogen storage performance of MgH2

Xu Nuo,Yuan Zirui,Ma Zhihong,Guo Xinli,Zhu Yunfeng,Zou Yongjin,Zhang Yao

MgH 2 with a large hydrogen capacity is regarded as a promising hydrogen storage material. However, it still suffers from high thermal stability and sluggish kinetics. In this paper, highly dispersed nano-Ni has been successfully prepared by using the polyol reduction method with an average size of 2.14 nm, which significantly improves the de/rehydrogenation properties of MgH 2 . The MgH 2 —10wt% nano-Ni sample starts releasing H 2 at 497 K, and roughly 6.2wt% H 2 has been liberated at 583 K. The rehydrogenation kinetics of the sample are also greatly improved, and the adsorption capacity reaches 5.3wt% H 2 in 1000 s at 482 K and under 3 MPa hydrogen pressure. Moreover, the activation energies of de/rehydrogenation of the MgH 2 —10wt% nano-Ni sample are reduced to (88 ± 2) and (87 ± 1) kJ·mol −1 , respectively. In addition, the thermal stability of the MgH 2 —10wt% nano-Ni system is reduced by 5.5 kJ per mol H 2 from that of pristine MgH 2 . This finding indicates that nano-Ni significantly improves both the thermodynamic and kinetic performances of the de/rehydrogenation of MgH 2 , serving as a bi-functional additive of both reagent and catalyst.

研究领域: 材料科学 · 化学工程 · 能源存储
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Small · 2022 ·Vol. 18 ·期 26 ·2201996 · IF 15.153

Dual-Atom Nickel Moieties of Ni(II)2N4(µ2-N)2 Anchored on Alfalfa-Derived Developed Porous N-Doped Carbon for High-Performance Li–S Battery

Tengfei Zhang,Hong Xiao,Xiao Liang,Fanchao Zhang,Huifeng Zhuang,Qiuming Gao,Lirong Zheng

A universal strategy is established for preparing the carbonaceous matrix-based atomically distributed metal catalysts M-BPC (M=Ni, Co, Fe, Cu, and Mn, and biomass-derived porous carbon (BPC)) by one-step pyrolysis of mixed metal salts and biomass alfalfa. The optimized Ni-BPC has dual-atom Ni(II) 2 N 4 (µ 2 -N) 2 moieties, which are chemically anchored on the alfalfa-derived developed porous N-doped carbon BPC matrix. An ultrahigh specific surface area of 3133 m 2 g −1 with huge total pore volume of 3.02 cm 3 g −1 is obtained for Ni-BPC. The Ni-BPC could greatly promote the redox kinetics and effectively prevent the shuttle effect of lithium polysulfides in a Li–S battery. The Li–S battery assembled with the Ni-BPC modified separator exhibits prominent rate performance with the reversible specific capacities of 1279, 1119, 1037, 948 and 787 mAh g −1 at the current densities of 0.1, 0.2, 0.5, 1 and 2 C, respectively. The battery presents an ultra-long life with low capacity decay of 0.028% per cycle up to 2100 cycles at 1 C. Even under high areal S loadings of 3.9 mg cm −2 , the high discharge capacity of 976.6 mAh g −1 is obtained at 0.2 C and excellent cycling stability with 61.1% capacity retention is achieved after 490 cycles.

研究领域: 材料科学 · 能源存储
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Scientific Reports · 2019 ·Vol. 9 ·期 1 ·1-16 · IF 4.011

S-containing and Si-containing compounds as highly effective electrolyte additives for SiOx -based anodes/NCM 811 cathodes in lithium ion cells

An Fuqiang,Zhao Hongliang,Zhou Weinan,Ma Yonghong,Li Ping

Recently, high-energy density cells containing nickel-rich cathodes and silicon-based anodes have become a practical solution for increasing the driving range of electric vehicles. However, their long-term durability and storage performance is comparatively poor because of the unstable cathode-electrolyte-interphase (CEI) of the high-reactivity cathode and the continuous solid-electrolyte-interphase (SEI) growth. In this work, we study several electrolyte systems consisting of various additives, such as S-containing (1,3,2-dioxathiolane 2,2-dioxide (DTD), DTD + prop-1-ene-1,3-sultone (PES), methylene methanedisulfonate (MMDS)) and Si-containing (tris(trimethylsilyl) phosphate (TTSP) and tris(trimethylsilyl) borate (TMSB)) compounds, in comparison to the baseline electrolyte (BL = 1.0 M LiPF 6  + 3:5:2 w-w:w EC: EMC: DEC + 0.5 wt% lithium difluoro(oxalato)borate (LiDFOB) + 2 wt% lithium bis(fluorosulfonyl)imide (LiFSI) + 2 wt% fluoroethylene carbonate (FEC) + 1 wt% 1,3-propane sultone (PS)). Generally, electrolytes with Si-containing additives, particularly BL + 0.5% TTSP, show a lower impedance increase in the full cell, better beginning-of-life (BOL) performance, less reversible capacity loss through long-term cycles and better storage at elevated temperatures than do electrolytes with S-containing additives. On the contrary, electrolytes with S-containing additives exhibit the advantage of low SEI impedance but yield a worse performance in the full cell than do those with Si-containing additives. The difference between two types of additives is attributed to the distinct function of the electrodes, which is characterized by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS), which was performed on full cells and half cells with fresh and harvested electrodes.

研究领域: 材料科学 · 电化学 · 能源存储
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ChemistrySelect · 2022 ·Vol. 7 ·期 45 ·e202203339 · IF 2.307

Balancing Ni0 and Ni2+ on γ-Al2O3 for Efficient Steam Methane Reforming

Junjie Zhang,Zhourong Xiao,Li Wang,Xiangwen Zhang,Guozhu Li

Graphical The key role of Ni valence state on the catalytic SMR performance of Ni/Al 2 O 3 is reported. Ni 0 /Ni 2+ ratio on Ni/Al 2 O 3 is individually regulated by changing the reduction temperature while maintaining the states of nickel particles and support. A deep understanding is gained on how the Ni valence state of Ni/Al 2 O 3 affects the catalytic SMR performance. Steam methane reforming (SMR) is the most mature technology for hydrogen production in industry, and alumina supported nickel (Ni/Al 2 O 3 ) is the most widely used catalyst. Herein, the key role of Ni valence state on the catalytic SMR performance of Ni/Al 2 O 3 is reported. The ratio of Ni 0 /Ni 2+ on Ni/Al 2 O 3 is individually and effectively tuned by changing the reduction temperature after wet impregnation. Catalytic performance of Ni/Al 2 O 3 is greatly dependent on the surface concentration of Ni 0 and Ni 2+ . The catalyst reduced at 675 °C possesses balanced Ni 0 and Ni 2+ sites and exhibits superior catalytic performance, on which 60 % of methane is stably converted at 600 °C. CH 4 -TPD and CO-TPD profiles demonstrate that appropriate Ni 0 /Ni 2+ ratio can promote the adsorption of CH 4 and inhibit the moderate-strength adsorption of CO, which leads to increased SMR activity and selectivity.

研究领域: 化学工程 · 材料科学
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