RARE METALS
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2025
·
IF 11
He Shuai,Zhao Man,Zhao Peipei,Ma Jiamin,Liu Chunmei,Xiao He,Zhang Li,Zhang Junming,Hu Tianjun,Wang Shengxiang,Pang Huan,Jia Jianfeng
Nickel-based catalysts display promising potential in integrated hydrogen production through methanol electrooxidation (MOR). The unavoidable self-oxidation from Ni(OH) 2 to NiOOH severely restricts their MOR performance. To inspire the progress of MOR before self-oxidation of Ni species by altering reaction pathways, a heterostructured Ni–WO 2 catalyst is constructed to follow the direct electrooxidation pathway of methanol. In-situ/ex-situ characterization techniques combined with density functional theory calculations reveal the constructed Ni–WO 2 heterostructure alters the electronic structure of Ni site. It’s found Ni–Ni bond in Ni–WO 2 becomes longer and the electrons transfer from Ni sites to W sites. This results in upshifted d band center of Ni site and its closing to the Fermi energy level, which optimizes the CH 3 OH adsorption and the deprotonation of *CH 3 O into *CH 2 O in potential-determining step. Moreover, the formed asymmetric adsorption sites increase the polarity of the methanol and the intermediate. As expected, CH 3 OH molecule is highly converted into HCOOH via direct electrooxidation pathway. This obtained Ni–WO 2 exhibits superior MOR activity with high peak current density of 325.26 mA cm −2 and performs long term of 90 h at 10 mA cm −2 in hydrogen production. This work provides an important guidance for designing efficient Ni-based samples for direct electrooxidation of methanol. Graphical abstract
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FUEL PROCESSING TECHNOLOGY
·
2025
·
IF 7.7
Yi Lin,Zaixing Wang,Lina Tang,Shi Jiang,Yu Guo,Xiaoqin Liu
Ni-based catalysts supported on composite metal oxides (NiO-Al 2 O 3 , MgO-Al 2 O 3 , Co 3 O 4 -Al 2 O 3 ) were synthesized via coprecipitation followed by Ni impregnation to investigate the influence of support composition on catalyst stability in methane steam reforming. Accelerated deactivation protocols (methane decomposition, high-temperature sintering, hydrothermal oxidation) revealed hydrothermal oxidation as the primary cause of irreversible deactivation. The 10Ni/NiAl catalyst (10 wt% Ni/10 wt% NiO-Al 2 O 3 ) showed remarkable regenerability after 923 K hydrothermal treatment, fully restoring its activity. This was attributed to coexisting reduced Ni species and readily reducible NiO, facilitating rapid reactivation. Other catalysts formed thermally stable NiAl 2 O 4 , leading to permanent deactivation. Methane cracking at 973 K had negligible effect, and 10Ni/NiAl catalyst exhibited the lowest carbon deposition (17.02 %). Under extreme hydrogen purged at 1223 K, only the 10Ni/CoAl catalyst exhibited a minor activity decline. The superior stability of 10Ni/NiAl was attributed to an in situ-formed NiAl composite metal oxides during 973 K calcination, which effectively anchored Ni particles, suppressed sintering, and prevented extensive oxidation.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Lei Zhao,Zilong Zhang,Tianyuan Zhang,Xiang Wang,Huanjun Peng,Jingdong Peng
The Fenton reaction in advanced oxidation processes is an ideal pathway for the generation of highly reactive hydroxyl radicals (•OH). However, its application in organic wastewater treatment is limited due to the requirement for acidic pH conditions and the additional introduction of H2O2 and Fe2+. In this study, FeOOH–CN/Ni(OH)2 composites were constructed as photocatalysis-self-Fenton catalysts by the amorphous FeOOH, which was uniformly anchored onto the surface of pure g-C3N4 (carbon nitride (CN)), and Ni(OH)2 was assembled on top. In this process, FeOOH–CN/Ni(OH)2 achieved self-sufficiency in H2O2 production while enabling efficient degradation of tetracycline hydrochloride (TCH) over a wide pH range, with a degradation ratio of up to 98.82%, and a first-order reaction rate constant (k) was determined to be 0.04925 min–1, representing a 10.15 times enhancement compared to the pristine CN. A reasonable S-scheme heterojunction charge migration mechanism was demonstrated based on valence-band X-ray photoelectron spectroscopy (VB-XPS), atomic force microscopy (AFM) equipped with a Kelvin probe force microscope, and density functional theory (DFT) theoretical calculations. Furthermore, degradation experiments demonstrated that the catalyst possesses remarkable degradation efficiency for other contaminants as well. On one hand, this significant improvement can be attributed to the formation of an S-scheme heterojunction between Ni(OH)2 and CN, which not only increased the specific surface area of the composite but also remarkably enhanced the separation and transfer efficiency of photogenerated charges. On the other hand, the synergistic effect between Ni and Fe effectively facilitated the activation of H2O2 and promoted the cycling of Fe3+/Fe2+. This study provided an efficient visible-light-driven photocatalysis-self-Fenton system, offering novel perspectives for enhancing Fenton-based processes and advancing the application of Fenton reactions in the treatment of organic wastewater.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Shuang Wu,Zheni Wang,Lei Wan,Chenghui Luo,Shams Ali Baig,Xinhua Xu
In the present study, Pd/Ni foam electrode was prepared by improved impregnation method for electrocatalytic hydrodechlorination (ECH) of clofibric acid (CA). The effects of complexing agent addition into the impregnation solution for the formation of Ni(OH) 2 and the ECH activity of Pd/Ni foam electrode were investigated. Results revealed that the introduction of sodium acetate (the complexing agent) greatly enhanced the ECH activity as compared to common impregnation liquid. Characterizations analyses demonstrated that the addition of sodium acetate did not change the phase of the electrode’s surface, but effectively reduced the deposition of Ni(OH) 2 . The surface morphology of the electrode was changed simultaneously by the addition of sodium acetate and the interlacing structure of Ni(OH) 2 and Pd catalyst was formed. NaAc before -Pd/Ni and NaAc after -Pd/Ni foam electrodes were used to perform ECH experiments on CA, and the combined Pd/Ni foam 15 min electrode was compared with the Pd/Ni foam 6 h electrode. After 2 h of electrolysis, the NaAc after -Pd/Ni foam electrode was found to remove the CA (∼100%) in the solution, which was 1.3 times the removal rate of the Pd/Ni foam 6 h electrode to CA and exceeded the Pd/Ni foam 15 min electrode. Findings from the present study demonstrated that adding the complexing agent into the impregnation solution can improve the ECH activity of Pd/Ni foam electrode and achieve a faster and more efficient dechlorination effect of CA.
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Catalysts
·
2026
·Vol. 16
·期 5
·409
·
IF 4.5
Linhao Zhang,Hong Liu,Jianming Zhang,Fagen Wang
Harnessing low-grade thermal energy from industrial processes and the environment represents an attractive route toward sustainable chemical production. In this work, we report a thermoelectrocatalytic (TE-Catal) system capable of converting small temperature gradients into chemical energy for hydrogen peroxide (H2O2) generation. A hybrid catalyst composed of nickel-based metal–organic frameworks (Ni-MOFs) nanoparticles integrated with carbon nanotubes (CNTs), Ni-MOFs/CNTs, was synthesized through a facile one-pot strategy. Under a temperature gradient, the thermoelectric response of the Ni-MOFs induces charge carrier generation through the Seebeck effect, enabling interfacial redox reactions that produce H2O2. However, rapid recombination of thermally generated carriers typically limits catalytic efficiency. By coupling Ni-MOFs with conductive CNTs networks, charge separation and transport are significantly enhanced due to the strong interfacial interaction and the high electrical conductivity of CNTs. As a result, the Ni-MOFs/CNTs nanohybrids exhibit greatly improved H2O2generation rate of ~111.7 µmol g−1h−1compared with pristine Ni-MOFs (31.8 µmol g−1h−1). Thermoelectric electrochemical measurements confirm that the CNT incorporation effectively promotes carrier migration and suppresses recombination. This study demonstrates the potential of MOF-based thermoelectric nanostructures for transforming waste heat into valuable chemical products.
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JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Kun Lang,Yuanyingxue Gao,Panzhe Qiao,Xudong Xiao,Mingyang Liu,Bin Wang,Xinrui Li,Wei Wu,Jingping Ge,Huiyuan Meng,Baojiang Jiang
Air calcination stabilizes LaMnO 3 but can promote particle coarsening and oxidation-driven Mn-valence elevation, reducing Mn e g -electron availability for nitrite-to-ammonia conversion. Here, B-site Ni regulation yields a more dispersed LaMnO 3 nanoperovskite, LaMn 0.95 Ni 0.05 O 3 (LMNO), while coupling oxygen-defect formation with Mn-valence rebalancing without disrupting the LaMnO 3 -type lattice. Combined structural and spectroscopic analyses show stronger oxygen-defect signatures, enhanced lattice-oxygen reducibility, lower average Mn valence, and altered Mn-centered coordination after Ni incorporation. These changes suggest electron compensation of neighboring high-valent Mn species and a more electron-rich Mn–O environment for nitrite activation and hydrogenation. In situ infrared spectroscopy and density functional theory calculations further indicate stepwise intermediate hydrogenation, favorable H 2 O dissociation and initial NO 2 stabilization at Ni sites, Ni 3d and Mn 3d/O 2p states near the Fermi level, and more favorable overall conversion thermodynamics at Ni-regulated Mn sites. LMNO delivers an NH 3 yield rate of 8996 μg h −1 cm −2 with 97.3% Faradaic efficiency and remains stable for 400 h. Downstream acid trapping enables crystalline NH 4 Cl recovery, while tests with pretreated landfill leachate show a shift in nitrogen speciation toward NH 4 + and reduced seedling-growth inhibition.
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Journal of Physical Chemistry C
·
2019
·
IF 4.309
Wen Wu,Ying Li,Limin Liang,Qiuyan Hao,Jun Zhang,Hui Liu,Caichi Liu
Antimony selenide (Sb2Se3) semiconductor with a narrow band gap is regarded as an ideal candidate for the next-generation broadband photodetectors. However, the photodetectors based on the binary Sb2Se3 semiconductor suffer from low responsivity (Rλ) and external quantum efficiency due to the intrinsic low electrical conductivity. To address the issue, we introduce a low-valence Ni cation (Ni2+) into the binary Sb2Se3 ((Sb1–xNix)2Se3) nanorods synthesized by a facile hot-injection process. With increasing Ni-doping concentration, the (Sb1–xNix)2Se3 nanorods exhibit a significant increase of electrical conductivity from 4.983 × 10–5 to 4.011 × 10–4 Ω–1 m–1. The photodetector based on (Sb0.995Ni0.005)2Se3 nanorod film exhibits an excellent responsivity of 18.9 mA/W under white light illumination of 45 mW/cm2 at an applied bias voltage of 3 V, which is an approximately 19-fold higher than that of the pristine Sb2Se3 nanorod photodetector. Moreover, the density functional theory calculation has demonstrated that the Ni2+ doped into Sb2Se3 will preferentially occupy the Sb site and introduce a shallow energy level of acceptor, resulting in the enhancement of electrical conductivity, which is consistent with the experimental result. Therefore, the work proves the substitution of Sb site with a low-valence metal cation into Sb2Se3 is an effective strategy to improve the performance of the Sb2Se3-based photodetector.
研究领域:
材料科学
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光电子学
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半导体物理
·
纳米技术
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RSC Advances
·
2022
·Vol. 12
·期 45
·29177-29186
·
IF 4.036
Zhao Qin,Yanqin Xu,Lin Liu,Min Liu,Hanjun Zhou,Liyue Xiao,Yuan Cao,Changguo Chen
Electrodes for supercapacitors made from metal–organic frameworks (MOFs) are still hindered by electron transfer properties. Therefore, an electrode composite material Ni-MOF@PPy was synthesized from a Ni-based metal–organic framework (Ni-MOF) doped with poly-pyrrole (PPy) using a simple chemical oxidation method to improve its electron transfer property. After introducing the electrochemically active substance K4Fe(CN)6 into the electrolyte, the composite material had a specific capacitance of 1815.4 F g−1 at a current density of 1 A g−1. Ni-MOF@PPy and active carbon (AC) as the positive and negative electrodes have been used, respectively, to assemble asymmetric supercapacitors (ASCs) in the KOH and K4Fe(CN)6 mixed electrolyte. This novel Ni-MOF@PPy//AC ASC energy storage device can provide 38.5 W h kg−1 energy density, 7001 W kg−1 power density, and 90.2% capacitance retention after 3000 cycles. Therefore, Ni-MOF@PPy//AC ASC is an excellent energy storage device with practical and economic value. The synergistic effect strategy proposed in this work can be easily applied to develop other MOFs with unique crystal structures as well as other redox active additives, providing new avenues and research ideas for exploring novel energy storage devices.
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Water
·
2022
·Vol. 14
·期 9
·1420
·
IF 3.53
Juan Peng,Yameng Ma,Xiao Huang,Jianghua Yu,Fengjiao Yu,Jingsi Gao
Ni-ethylenediaminetetraacetic acid (Ni-EDTA) poses serious threats to the ecological environment and human health, due to its acute toxicity and low biodegradability. The decomplexation efficiency of Ni-EDTA through the conventional Fenton process has been constrained to pH; thus, other appropriate approaches are required to destroy the stable chelate structure at a neutral pH. In this study, the effect of operating parameters such as the pH, Fe2+concentration, particle electrode dosage, current density, and coexisting ions was studied. The results revealed that the 3D-EF system owned advantages for the removal of Ni-EDTA in the broadening of the pH application window. The Ni-EDTA removal efficiency in the 3D-EF system reached 84.89% after 120 min at a pH of 7. In addition, the presence of coexisting ions slightly affected the decomplexation efficiency of Ni-EDTA.Keywords:Ni-EDTA;three-dimensional electro-Fenton;neutral pH;decomplexation
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Xingang Luan,Qinghua Zhao,Shaomin Gu,Xichao Dong,Laifei Cheng,Ralf Riedel
Wireless passive sensors based on surface acoustic wave (SAW) provide a good solution for the measurement demand under high temperature and harsh conditions. SiBCN ceramics have excellent mechanical properties at high temperature and semiconductor behavior, making them potential for electrode of SAW sensors. To achieve the target conductivity, a series of SiBCN and SiNiBCN coatings are prepared by polymer derived ceramics (PDC) method and the influence of microstructure on the conductivity of the coatings is discussed. The results show that the conductivity of the SiBCN coatings is affected by both the content of free carbon and the degree of graphitization. The introduction of Ni leads to the formation of Ni 2 Si conductive microcrystals at lower temperatures and catalyzes the graphitization of the carbon phase, so that the SiNiBCN coatings show lower electrical resistivity. The amount of the metal conductive phase and the graphitization degree of the carbon phase increase with the pyrolysis temperature, resulting in decrease of the SiNiBCN coatings resistivity.
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Nanoscale
·
2018
·Vol. 11
·期 3
·1058-1064
·
IF 7.233
Yu Ding,Ying Li,Yuanyuan Xue,Boqiang Miao,Shuni Li,Yucheng Jiang,Xien Liu,Yu Chen
Atomically thick ultrathin nanomeshes (NMs) possessing the inherent advantages of both two-dimensional nanomaterials and porous nanomaterials are attracting increasing interest in catalysis and electrocatalysis. Herein, we report a direct chemical synthesis of atomically thick Ni(OH)2-NMs by a NaBH4 assisted cyanogel hydrolysis method, which overcomes the shortcoming of the post-etching method for NM synthesis. Various physical characterization methods show that the as-synthesized Ni(OH)2-NMs have 1.7 nm thickness, a big surface area, abundant nanoholes, and numerous surface/edge atoms with low-coordination numbers. The as-synthesized Ni(OH)2-NMs show a better electrocatalytic performance for the urea oxidation reaction than conventional Ni(OH)2 nanoparticles without holes in the alkaline electrolyte, including a lower onset oxidation potential, faster reaction kinetics, and higher mass activity.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Zhihao Liu,Yachao Li,Kangzhou Wang,Yan Li,Yurong He,Jie Liang,Jianli Zhang,Tian-sheng Zhao,Noritatsu Tsubaki,Xinhua Gao
The design and preparation of highly active and stable Ni-based catalysts has attracted extensive attention. In this study, a series of embedded Ni@C catalysts were synthesized by a facile sol-gel method. After reduction at 400 °C, the optimized Ni@C-400 catalyst showed excellent performance in CO 2 methanation at a low temperature of 300 °C, with a CO 2 conversion of 74.3 % and good stability for 70 h. The characterization results indicated that after reduction treatment, the carbon species in the precursor were transformed into graphite carbon with more disorder defects. This structure facilitated the anchoring effect of the nickel components in the Ni@C catalyst, thereby forming a distinctive embedded structure that ensured the preservation of the nickel active phase in the catalyst following prolonged reaction. Therefore, the Ni@C catalyst prevented severe sintering and loss of loaded nickel. In addition, the interaction between Ni and C facilitated charge transfer, enhancing the CO 2 activation.
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