JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Fangshuo Jia,Yujuan Zhang,Xiutang Zhang,Tuoping Hu
Methanol oxidation reaction (MOR) and urea oxidation reaction (UOR) can be utilized as effective alternatives to the anodic oxygen evolution reaction (OER) in overall water-splitting. Nevertheless, the development of cost-effective, highly efficient and durable electrocatalysts for MOR and UOR remains a significant challenge. Herein, the Ohmic junction (Ni-CuCoN 0.6 @CC) comprising CuCoN 0.6 nanosheets and Ni nanoparticles anchored on carbon cloth (CC) was successfully synthesized via a two-step hydrothermal process followed by pyrolysis. The Ni-CuCoN 0.6 @CC demonstrates exceptional performance in both MOR (1.334 V@10 mA cm −2 ) and UOR (1.335 V@10 mA cm −2 ), coupled with outstanding durability, maintaining 88.70 % current density for MOR and 88.92 % for UOR after a rigorous 50-h stability test. Furthermore, the Ni-CuCoN 0.6 @CC demonstrates a high selectivity for oxidizing methanol to formic acid, achieving Faraday efficiencies exceeding 90 % at various current densities in the context of MOR. The outstanding performance of Ni-CuCoN0 .6 @CC in terms of MOR and UOR either surpasses or closely approaches the levels reported in previous literature, primarily due to the synergistic effect resulting from the Ohmic junction: in this system, Ni serves as the principal active component, Co augments catalytic activity and diminishes onset potential, while Cu enhances long-term durability. Moreover, CuCoN 0.6 nanosheets effectively modulate electronic structure and optimize the morphology of Ni, leading to the exposure of numerous defects that provide a wealth of active sites for the reaction. Additionally, the exceptional hydrophilic and aerophobic surface promotes enhanced mass transfer. Density functional theory (DFT) calculations show that Ni-CuCoN 0.6 @CC enhances reactant adsorption and product desorption, reducing energy barriers and expediting MOR and UOR kinetics.
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高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 36
·15093-15100
·
IF 3.5
Fang Wu,Yuhong Jiao,Jin-long Ge,Yujun Zhu,Chao Feng,Zhong Wu,Qiu Li
Facilitating the surface reconstruction of pre-catalysts has been considered an effective strategy for constructing low-cost and highly efficient OER electrocatalysts. Metal doping is a feasible way to activate the surface reconstruction, thus enhancing the OER performance. Herein, we report a facile hydrothermal method to synthesize a series of Zn-doped Ni-MOF on nickel foam (NiZn-MOF/NF) as promising pre-catalysts toward the oxygen evolution reaction (OER). The Zn leaching of NiZn-MOF/NF can promote the surface self-reconstruction of NiZn-MOF/NF into oxygen-vacancy-rich NiOOH after electrochemical activation. Benefiting from the optimized electronic structure, abundant defects, more accessible active sites, and enhanced electrical conductivity, the reconstructed metal oxyhydroxide hybrids exhibit better electrocatalytic activity than the catalysts transformed from Ni-MOF/NF without Zn doping. The optimized NiZn-MOF/NF-OH as an OER catalyst has an overpotential of 336 mV at 100 mA cm−2, and a Tafel slope of 65.9 mV dec−1, as well as stability over 12 h. This work reveals that Zn cation-doping/leaching induces the surface reconstruction of pre-catalysts for enhanced oxygen catalytic activity, which provides a new approach for the development of advanced electrocatalysts.
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Energy Technology
·
2024
·
IF 3.6
Xueli Zhang,Shan Hu,Fangyuan Zhang,Shuchen Xing,Huilin Hu,Jinhua Ye,Defa Wang
As a promising technology to mitigate global carbon emissions, photothermal catalytic CO 2 reduction remains a great challenge in increasing the conversion efficiency and regulating the product selectivity. Herein, a series of phase-separated Ni–Mo alloy catalysts for efficient photothermal CO 2 reduction with tunable CO selectivity is reported. With the increase of Mo content, the evolution rate and selectivity of CO increases. The optimal catalyst Ni 1 Mo 1 achieves 32.1% CO 2 conversion with 98.0% of CO selectivity and 71.1 mmol g cat −1 h −1 of CO evolution rate under a 300 W xenon lamp irradiation. Further increasing the Mo content reduces the CO evolution rate while maintaining the high CO selectivity. In the mechanistic study, it is revealed that the Ni–Mo alloy with an appropriate Ni/Mo ratio (e.g., Ni 1 Mo 1 ) possesses a modified electronic structure with more negative d-band center, which increases the light absorption, reduces the H 2 dissociation, and favors the CO desorption, thereby leading to efficient and selective photothermal reduction of CO 2 to CO. In this work, a viable strategy to design nickel-based catalysts is provided for efficient and selective photothermal CO 2 reduction via composition-mediated modification of electronic structure.
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ADVANCED MATERIALS
·
2023
·Vol. 36
·期 13
·2311553
·
IF 29.4
Ruyu Shi,Nengzhan Zheng,Haocheng Ji,Mengtian Zhang,Xiao Xiao,Jun Ma,Wen Chen,Junxiong Wang,Hui-Ming Cheng,Guangmin Zhou
Direct regeneration of spent lithium-ion batteries has received wide attention owing to its potential for resource reuse and environmental benefits. The repair effect of direct regeneration methods undergoing heterogeneous repair process is usually inferior, while homogenous repair process plays a vital role to achieve satisfactory repair results. However, the practical applications of current homogeneous repair methods are challenged by the complex operations and relatively high costs owing to the requirement of additional heating or pressurization. Herein, this work proposes a simple strategy to achieve homogeneous repair of spent cathode materials under relatively mild conditions by uniformly precoating lithium source at room temperature and atmospheric pressure. Followed by annealing, highly degraded LiNi 0.83 Co 0.12 Mn 0.05 O 2 with severe Li deficiency and irreversible phase transition is repaired to have an initial capacity of 181.6 mAh g -1 and capacity retention of 80.7% after 150 cycles at 0.5 C. The lithium source used in this strategy is from the spent lithium anode. Moreover, this strategy is suitable for the direct regeneration of various layer oxide cathode materials with different failure degrees. This work provides both theoretical guidance and practical examples for the straightforward, effective, and universally applicable direct regeneration methods.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Jing Zhang,Peiqi Shen,Yuchun Liu,Tianchen Wei,Xingwu Zhai,Baichuan Zhu,Jianrong Zeng,Kun Xu,Min Zhou
Lithium carbonate, the primary discharge product in Li–CO 2 batteries with high thermodynamic stability and a wide band gap, leads to significant electrochemical inertness, limiting efficiency and cycle life. The strongly delocalized p z orbital at a lower-energy HOMO level in Li 2 CO 3 causes weak coupling with the O-p z orbitals, increasing decomposition resistance owing to d-orbital degeneracy in high-local-symmetry catalysts. This study introduces metastable tetragonal-pyramidal nickel sulfide (tp-NiS) with low-symmetry NiS 5 coordination, breaking d-orbital degeneracy and bringing d z 2 , d xz , and d yz orbitals closer to the Fermi level. Enhanced orbital overlap with Li 2 CO 3 O-p z orbitals facilitates robust Ni–O bond formation. In situ spectroscopy confirms reversible Ni–O bond formation during cycling, ensuring electron transfer and complete Li 2 CO 3 decomposition. Conversely, weak interfacial interactions in octahedral NiS with highly symmetric local coordination only allow decomposition-resistant Li 2 CO 3 and interface passivation. Consequently, tp-NiS exhibits superior electrochemical performance, with the best reported reversibility and stability, a charge potential below 4.0 V, and 92.03% capacity retention after 1800 h. This metal redox-driven mechanism establishes a reversible geometric conversion pathway, emphasizing the critical role of symmetry-engineered Ni–O interactions in bifunctional catalysts.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Dexin Chen,Yunxuan Ding,Xing Cao,Licheng Sun
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) offers a sustainable pathway for biomass valorization and green H 2 generation, yet its multi-electron transfer process demands efficient catalysts to overcome kinetic bottlenecks. Herein, we demonstrate that the spatial configuration of Co species in Ni hydroxides (Ni(OH) 2 ) dictates alcohol oxidation activity by modulating interfacial electron transfer dynamics. Engineered heterostructured Co 3 O 4 -Ni(OH) 2 outperforms planar NiCo layered double hydroxide (LDH), achieving 106 % higher current density with nearly 100 % yields and Faradaic efficiencies of the target product. Experimental and theoretical results reveal that the heterointerface optimizes alcohol adsorption and accelerates electron transfer kinetics via interfacial charge distribution. Engineering of interfacial electronic properties enables the catalyst to be versatile for the electrooxidation of variant substituted alcohol substrates. Those insightful results establish a paradigm for catalyst design methodology in biomass upgrading through regulating charge transfer pathways.
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Energy Storage Materials
·
2022
·
IF 20.831
Tong Zhou,Xinrun Yu,Fan Li,Jianwei Zhang,Bowen Liu,Longlong Wang,Yuan Yang,Zhiwei Hu,Jun Ma,Chao Li,Guanglei Cui
Nickel-rich layered transition metal oxide is limited by the poor structural stability during cycling as cathode materials for next-generation lithium-based automotive batteries . In the past, the poor electrochemical performance was mainly attributed to cracks and formation of rock-salt phase on the particle surface at high potentials. Rarely is the effect of bulk phase structure evolution on properties discussed. Here, we report a bulk oxygen release induced dynamic accumulative electrochemical–mechanical coupling failure mechanism. Domain-like rock salt phases are generated due to the oxygen release and transition metals migration in the bulk region of LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) particles at the first cycle high cutoff voltage. Then, reversible compressive/tensile lattice strain alternately dominate around the domain boundary and accumulate with cycling, leading to capacity fading and becoming the origin of intracrystalline cracks. The results suggest that, in addition to the side effects from the surface, the structural transformation of the bulk plays an important role in the capacity fading. The stabilization of lattice oxygen in bulk region is a feasible solution to suppress the structural transition and the inhomogeneous stress distribution.
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Russian Journal of Physical Chemistry A
·
2023
·Vol. 97
·期 13
·2966-2975
·
IF 0.7
Liu Kun,Zhu TianHan,Li Feng,Wang Jing,Song Hua
A series of Ni/SiO 2 –Al- x catalysts ( x is the initial mass ratio of SiO 2 to Al(NO 3 ) 3 ) with different aluminum contents was prepared by impregnation method using nickel nitrate as the Ni source. The prepared Ni/SiO 2 –Al- x catalysts were characterized by XRD, BET, TPR, TEM, XPS, NH 3 -TPD, and Py-FTIR methods. Taking m -cresol as a model compound, the effects of aluminum content and reaction conditions on the HDO performance were investigated. Results showed that addition of appropriate amount of aluminum can generate acid sites and improve the metal Ni dispersion by increasing the surface area of catalyst. Furthermore, the selectivity to deoxygenated methyl-cyclohexane product over aluminum modified Ni/SiO 2 –Al- x catalysts increased significantly as compared to that of Ni/SiO 2 , which confirmed the importance of aluminum addition on the dehydration of 3-methyl-cyclohexanol to methyl-cyclohexane. Among the prepared Ni/SiO 2 –Al- x catalysts, the Ni/SiO 2 –Al-5 catalyst exhibits the best HDO performance. A 100% m -cresol conversion with the selectivity to MCH of 100% was achieved under the conditions of T = 250°C, p = 2 MPa, t = 75 min with catalyst (mg)/ m -cresol solution = 2.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 7
·1-9
·
IF 2.8
Li Wei,Dai Bo,Li Zhao,Yang Hongwei,Liu Guixiang,Xu Fang
A series of Ni x Zn 1− x Fe 2 O 4 ( NiZn, x = 0.15, 0.25, 0.35, 0.45, 0.65, 0.7, 0.8, 0.85) ferrites were prepared via a solid-phase sintering method. The microstructure, phase, and gyromagnetic properties of the NiZn samples were studied in depth. It was found that the lattice constants, density, and hardness of the samples gradually decreased with increasing Ni 2+ content. X-ray diffraction confirmed that all of the samples were in the spinel phase. Scanning electron microscopy indicated that the grain sizes were more uniformly distributed when x = 0.65. Raman analysis showed that the variation of Ni 2+ content affected the occupancy distribution of ferrite ions. The results indicated that Zn 2+ mainly occupied the A-site and that Ni 2+ mainly occupied the B-site. The coercivity ( H c ) of NiZn increased with increasing Ni 2+ content. Meanwhile, the saturation magnetization ( M s ) initially increased and then decreased. When x = 0.65, the total molecular magnetic moment started decreasing because of the decrease in the net A-site magnetic moment. The sample that had a composition of Ni 0.65 Zn 0.35 Fe 2 O 4 had the highest M s intensity with a value of 78.68 emu/g and a maximum value of 4 πM s = 4780 Gs.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2012
·Vol. 19
·期 2
·501-508
·
IF 5.925
Jianwei Nai,Zhengbo Chen,Haopeng Li,Fangyuan Li,Yang Bai,Lidong Li,Lin Guo
As the properties of nanomaterials are strongly dependent on their size, shape and nanostructures, probing the relations between macro-properties and nanostructures is challenging for nanoscientists. Herein, we deliberately chose three types of Ni(OH) 2 with hexagonal, truncated trigonal, and trigonal hourglass-like nanostructures, respectively, as the electrode modifier to demonstrate the correlation between the nanostructures and their electrocatalytic performance towards L -histidine. It was found that the hexagonal hourglass-like Ni(OH) 2 sample had the best electrocatalytic activity, which can be understood by a cooperative mechanism: on one hand, the hexagonal sample possesses the largest specific surface area and the tidiest nanostructure, resulting in the most orderly packing on the electrode surface; on the other hand, its internal structure with the most stacking faults would generate a lot of unstable protons, leading to an enhanced electronic conductivity. The findings are important because they provide a clue for materials design and engineering to meet a specific requirement for electrocatalysis of L -histidine, possibly even for other biomolecules. In addition, the hexagonal Ni(OH) 2 -based biosensor shows excellent sensitivity and selectivity in the determination of L -histidine and offers a promising feature for the analytical application in real biological samples. Graphical Structure-dependent performance : Three different types of Ni(OH) 2 with hexagonal, truncated trigonal, and trigonal hourglass-like nanostructures, respectively, were deliberately chosen as electrode modifiers to demonstrate the correlation between the structures and their electrocatalytic performance toward L -histidine (see figure). The electrocatalytic activity of these unique nanostructures depends not only their external architecture, but also on their relevant internal degree of crystallinity.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 6
·1504-1511
·
IF 2.726
He Kai,Liu Shijia,Zhao Guiyan,Qin Yucai,Bi Yanfeng,Song Lijuan
A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(Ni x W/SBA-15, Ni-5%, x =1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), transmission electronic microscopy(TEM), H 2 -temperature programmed reduction(H 2 -TPR), and X-ray photoelectron spectroscopy(XPS). High-resolution TEM images, XPS measurements, H 2 -TPR experiments coupled with PXRD results determined the evolution of Ni and W species. It is found that a trace amount of W from H 2 WO 4 can significantly improve Ni dispersion on SBA-15 (Ni 50 W/SBA-15) with Ni 0 and non-stoichiometric WO x species as small as ca . 3.6 nm. The prepared Ni x W/SBA-15 was utilized for CO 2 hydrogenation, which showed that a higher W content restrained the CO 2 hydrogenation while a lower W ratio promoted both conversion rate and selectivity for methane compared with Ni/SBA-15. The Ni 50 W/SBA-15 catalyst showed the best performance with a 93.3% CO 2 conversion rate and 99.7% selectivity for methane at 400 o C under 0.1 MPa and maintained ca . 97% initial performance for 24 h. Tracking product evolution experiments by in-situ Fourier transform infrared spectrascopy(FTIR) indicated that a small amount of W can modify the surface of Ni particles by geometric coverage and electronic modification, which facilitates the adsorption of the CO intermedia and results in the formation of CH 4 . This work provides a new clue to fabricating efficient CO 2 conversion bimetallic materials.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 18
·5130-5141
·
IF 5.726
Shuang Song,Qiuxiang Liu,Jinhui Fang,Weiting Yu
The reductive dechlorination of chlorinated organic compounds (COCs) is very important to reduce the toxicity of waste effluents produced from pharmaceutical, electronics, dyestuff, pesticide, paper, and plastics industries. Electrochemical dechlorination as a green technology under mild reaction conditions is widely used in the reductive dechlorination of COCs using Pd as the electrode. Currently, the challenges of this method are the need to use large Pd loadings and the low dechlorination efficiency. Efforts were made in this work to reduce the loading of Pd and improve the efficiency using 2,4-dichlorophenoxyacetic acid (2,4-D) as a probe molecule for COCs in dechlorination. In this study, Pd-anchored Ni(OH)2/Ni-foam bifunctional electrodes were prepared in situ and for the first time applied in the reductive dechlorination of COCs. The results indicate that the dechlorination efficiency of 2,4-D can be enhanced on Pd-anchored Ni(OH)2/Ni-foam bifunctional electrodes even at a low Pd loading (<2 mg cm−2). A synergistic effect is found for 2,4-D dechlorination: H* formation on Ni(OH)2 and dechlorination steps on Pd. The enhanced dechlorination efficiency might be related to the shortened transport route between Ni(OH)2 and Pd active centers for H*.
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