ACS Nano
·
2024
·
IF 15.8
Zhongxing Xu,Xinghan Chen,Wenguang Fan,Minzhi Zhan,Xulin Mu,Hongbin Cao,Xiaohu Wang,Haoyu Xue,Zhihai Gao,Yongzhi Liang,Jiajie Liu,Xinghua Tan,Feng Pan
Single-crystalline Ni-rich layered oxides are one of the most promising cathode materials for lithium-ion batteries due to their superior structural stability. However, sluggish lithium-ion diffusion kinetics and interfacial issues hinder their practical applications. These issues intensify with increasing Ni content in the ultrahigh-Ni regime (≥90%), significantly threatening the practical viability of the single-crystalline strategy for ultrahigh-Ni layered oxide cathodes. Herein, by developing a high-entropy coating strategy, we successfully constructed an epitaxial lattice-coherent high-entropy rock-salt layer (∼3 nm) via Zr and Al doping on the surface of the single-crystalline cathode LiNi0.92Co0.05Mn0.03O2 through an in situ modification process. The surface high-entropy rock-salt layer with tailored Ni valence and lattice coherence not only greatly improves lithium-ion diffusion kinetics but also suppresses interface parasitic reactions and surface structural degradations. The high-entropy surface layer-stabilized ultrahigh-Ni single-crystalline cathode (SC-Ni92-ZA) demonstrates significantly improved rate and cycling performances (127.5 mAh g–1 at 20C, capacity retention of 74.9% after 500 cycles at 1C) in a half-cell. The SC-Ni92-ZA exhibits a capacity retention of 87.1% after 600 cycles at 1C in a full-cell. This epitaxial lattice-coherent high-entropy coating strategy develops a promising avenue for developing high-capacity, long-life cathode materials.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Liang Dan,Hui Wang,Jiangwen Liu,Liuzhang Ouyang,Min Zhu
Highly fine, dispersive, and active catalysts are essential for lowering the operating temperature of MgH2, a promising high-capacity material for solid-state hydrogen storage. In this work, ultrafine Ni nanoparticles (2–6 nm) are synthesized from the precursor nickel acetylacetonate (C10H14NiO4) on the surface of MgH2 by H2 plasma reduction process, followed by further ball milling. The obtained composite could rapidly release more than 6.5 wt % H within 10 min at 275 °C. Even at a low temperature of 225 °C, up to 6 wt % H could be desorbed. The MgH2–Ni composite also exhibits excellent low-temperature hydrogenation kinetics and almost no capacity degradation over nine hydrogenation/dehydrogenation cycles. The significant improvement in the hydrogen-storage properties is attributed to the in situ formation of ultrafine and stable Mg2NiH0.3 nanocrystals during cycling. This work provides a convenient approach to synthesize ultrafine metal nanoparticles for catalytic applications in the field of high energy storage density hydride materials.
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高影响因子
ADVANCED ENGINEERING MATERIALS
·
2020
·Vol. 22
·期 11
·2000402
·
IF 3.217
Yanpeng Xue,Shuqiang Wang,Yanyan Xue,Lili Cao,Mengyan Nie,Ying Jin
Until now, superhydrophobic materials that are scale-up fabrication and application to harsh environments remain challenging because of their fragile mechanical durability. Because of their unique electronic structure, rare-earth oxides (REOs) have been proven to be intrinsically hydrophobic. Herein, cerium oxide particles (CeO 2 ) are added to the coating by coelectrodeposition. The Co–Ni/CeO 2 composite coating from the electrolyte containing 3.44 g L −1 possesses a flower-like hierarchical structure, displaying a superhydrophobic behavior after the modification by 1H,1H,2H,2H-perfluorooctyltrichlorosilane (PFTEOS). More importantly, excellent mechanical durability with critical abrasion distance of 22.5 m is achieved under a 5 kPa fixed normal pressure in the liner abrasion test before the loss of superhydrophobicity. Also, electrochemical measurements demonstrate that the superhydrophobic composite coatings display high corrosion resistance.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Wei Wang,Wenhua Cheng,Zhenjie Liu,Murong Xi,Zhouliang Tan,Yadong Wang,Weilu Zhang,Pingping Chang,Zihan Qi,Huan Zhou,Han Zhang,Juan Ding,Yudai Huang
The commercialization of Ni-rich layered oxide cathode materials has been severely hampered by rapid capacity degradation and safety issues. Here, we demonstrate a lattice reconstruction strategy to improve the structural and thermal stability of LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM83) via calcium. The enhanced stability of NCM83 is ascribed to the formation of Ca-O bond, which is stronger than TM-O (TM=Ni, Mn, Co) bond. The lattice reconstruction enables metal-O (M-O) bond more stable which mitigates the loss of lattice oxygen, thus improving the reversibility of the H2-H3 phase transition in NCM83. Moreover, Ca 2+ acts as a pillar, facilitating the transport of Li + . The lattice-reconstructed Ni-rich cathode material with 0.5 % Ca can maintain a capacity retention ratio of 97.3 % at 1 C after 150 cycles. As compared with the pristine NCM83 cathode, the high-voltage cycling stability at 4.5 V and high-temperature performance at 55 °C are increased by 17.9 % and 12.2 %, respectively. This work actually proposes a new approach to design and construct high-performance Ni-rich cathode materials for practical lithium-ion batteries.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Lifan Wang,Rui Wang,Jingyue Wang,Rui Xu,Xindong Wang,Chun Zhan
To satisfy the increasing energy density requirements for electric vehicles and grid-scale energy storage systems, Ni-rich layered oxide cathode materials are often fabricated as micron-sized secondary spherical particles consisting of nanosized single crystals. Unfortunately, the hierarchical structure inevitably induces intergranular cracks and parasitic reactions at the cathode–electrolyte interphase, aggravating chemomechanical instability and seriously hindering their practical application. Here, we propose a nanowelding strategy to build consolidation points at the grain boundary of the primary particles, which dramatically enhances the capacity retention and chemomechanical stability. Meanwhile, the oxygen vacancies in the ceria-based solid electrolyte possessing oxygen adsorbing and storage capability can restrain the active oxygenates in the surficial lattice to avoid oxygen evolution. Experimental characterization further confirms that this unique architecture can effectively prevent the liquid electrolyte from penetrating into the active material along the grain boundary and consequently eliminate the adverse effects, including intergranular cracks, cathode electrolyte interface formation and growth, and the layered structure-rock salt phase irreversible transition. This finding provides a promising approach to realize the rapid commercialization of highly stabilized nickel-rich cathode materials for high-performance lithium-ion batteries.
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高影响因子
Energy Technology
·
2018
·Vol. 7
·期 3
·1800533
·
IF 3.175
Shiliang Zhang,Qilu Yao,Qingyang Li,Gang Feng,Zhang-Hui Lu
The synthesis of noble-metal-free recyclable catalysts with prominent catalytic performance for the complete hydrogen production from hydrazine borane (N 2 H 4 BH 3 , HB) is of great significance in achieving a hydrogen economy-based society. Herein, Raney Ni is synthesized using a rapidly quenched aluminum–nickel alloy under a typical alkali leaching condition and is used to catalytically convert hydrogen of N 2 H 4 BH 3 to H 2 via hydrolyzing BH 3 groups and decomposing the N 2 H 4 moiety in alkaline conditions. It is the first report of a noble-metal-free catalyst achieving a complete production of hydrogen from N 2 H 4 BH 3 at room temperature. This noble-metal-free catalyst might tremendously broaden the actual utilization of HB as a promising chemical hydrogen storage material. In addition, such a simple strategy can also be expanded to design and synthesize other porous metals for more applications.
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高影响因子
EES Catalysis
·
2023
·Vol. 2
·期 1
·365-378
·
IF 0
Yaqi Hu,Zhong Liang,Yabin Zhang,Yaping Du,Hongbo Zhang
Hydrogen production with high efficiency and low CO selectivity in methanol steam reforming (MSR) is of pivotal importance. However, there is limited understanding of the active sites and reaction mechanisms during catalysis. In this study, we maximized the interfacial site, known as the active component in MSR, of Ni–CeOx by atomically dispersed Ni and Ce over the carbon–nitrogen support to generate the Ni and Ce dual-atomic catalyst (DAC), which achieved 6.5 μmolH2 gcat.−1 s−1 H2 generation rate and 0.8% CO selectivity at 99.1% methanol conversion at 513 K. The finely dispersed Ni and Ce structure was confirmed by systematic characterization of AC HAADF-STEM and EXAFS. Electron transfer from Ce to Ni was confirmed simultaneously by quasi-in situ XPS analysis. Moreover, the reaction mechanism of methanol steam reforming was clarified by combining kinetic studies with isotope-tracing/exchange analysis (i.e., KIEs and steady-state isotopic transient kinetic analysis (SSITKA)), which suggests that the steam reforming consists of two tandem reaction processes: methanol decomposition (MD) and water–gas shift (WGS) reaction, with methanol and water activation at independent active sites (e.g., Ni and oxygen vacancy over CeOx), and that hydrogen generation was primarily determined by both C–H bond rupture and OL–H (OL represents the lattice oxygen) cleavage within methoxy and hydroxyl groups, respectively, with the catalytic surface mainly covered by CO and methoxy groups. A shift of WGS involvement in hydrogen generation from negligibly influenced to significantly promoted was selectively observed once modifying the reaction from differential conditions to a high methanol conversion regime, and two quantification methods have been established by comparing the molecule ratio between CO and CO2 or H2.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Zicheng Wang,Shenggui Ma,Jundong Guo,Hongying Liu,Mingwu Tan,Xia Jiang
High-performance Ni/CeO 2 catalyst achieves ∼ 100% m-cresol conversion. • The Ni doping reduces oxygen vacancy formation energy and modulates electronic structure. • The methylcyclohexane as the thermodynamically favored pathway. The conversion of waste biomass into biofuels via fast pyrolysis followed by hydrodeoxygenation (HDO) represents a promising route for sustainable energy production. This study examines the selective HDO of bio-oil, using m-cresol as a model compound, over a Ni/CeO 2 catalyst to enhance the yield and stability of hydrocarbon fuels. Experimental investigations coupled with density functional theory (DFT) calculations were employed to elucidate the reaction mechanism and identify active sites. Under optimized conditions (300 °C, 3 MPa H 2 ), the Ni/CeO 2 catalyst achieved nearly complete conversion of m-cresol, with methylcyclohexane as the dominant product. DFT results indicate that Ni doping lowers the oxygen vacancy formation energy and modifies the electronic structure of CeO 2 , thereby enhancing catalytic activity. A detailed reaction network was established, revealing that elevated H 2 pressures favor methylcyclohexane formation, whereas higher temperatures promote toluene and benzene production. This work underscores the efficacy of Ni/CeO 2 catalysts in bio-oil upgrading, contributing to the development of efficient renewable fuel processes. Download: Download high-res image (188KB) Download: Download full-size image
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高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Guorong Hu,Manfang Zhang,Lili Wu,Zhongdong Peng,Ke Du,Yanbing Cao
A facile solution route was employed for the preparation of an Al doped ZnO (AZO) coating layer, which was composed of many AZO nanoparticles. These nanoparticles have an average particle size of 50 nm and have been successfully decorated on the surface of NCM523. As cathode material for lithium ion batteries, the AZO-decorated NCM523 exhibits superior lithium storage improvements according to good cyclic performance, enhanced rate performance (134.2 mAhg–1 after 200 cycles at 10 C), and high-temperature performance (148.9 mAhg–1 at 10 C at 60 °C). Such significant improvement could be attributed to the structural superiority of the AZO decoration on the surface of NCM523, which would stabilize the surface structure of the bulk, suppress the undesirable side reaction at the interface of the electrodes, and lead to the enhancement of the conductivity. The preparation of AZO-decorated NCM523 provides an effective method for the high-performance lithium ion batteries and has a certain reference for other materials.
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高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 8
·e202202128
·
IF 8.4
Shuang Wang,Zhengrong Li,Tao Shen,Deli Wang
Graphical Electrocatalytic HERo in the making : Synthesis of Ru 7 Ni 3 nanoalloys encapsulated within N-doped carbon shells (Ru 7 Ni 3 @NC/C) is achieved for the alkaline HER. It exhibits a current density of 10 mA cm −2 at 16 mV with a Tafel slope of 29.9 mV dec −1 , and robust durability over 10 000 cycles in 1 m KOH. The high HER activity of Ru 7 Ni 3 @NC/C can be attributed to the strong synergistic interaction, N-doped carbon shells structure with high surface area and electrical conductivity. The alkaline hydrogen evolution reaction (HER) is of great significance for the large-scale green H 2 production. Currently, pressing challenges in the fabrication of cost-effective HER electrocatalysts are related to their sluggish water dissociation kinetics. Herein, a facile strategy to accelerate the desorption of HER intermediates and water dissociation is proposed. RuNi nanoalloy confined within N-doped carbon shells (Ru 7 Ni 3 @NC/C) with optimized Ru/Ni ratio and the dicyandiamide dosage was prepared. It displays an overpotential ( η 10 ) of 16 mV, Tafel slope of 29.9 mV dec −1 , and long-term stability over 10 000 cycles. The decent HER performance on Ru 7 Ni 3 @NC/C stems from the core-shell structure that is favoring the exposure of dispersed active sites, and the synergistic effect to promote water capture and dissociation. This work provides insight into the relationship between the HER performance and the electrochemical behavior of the intermediate adsorbed state, and paves an avenue toward rational design efficient electrocatalysts for HER.
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高影响因子
Nano Research
·
2014
·Vol. 7
·期 9
·1337-1343
·
IF 6.963
Xiang Ji,Li Peng,Chong Hanbao,Feng Li,Fu Fangyu,Wang Zhuang,Zhang Shilin,Zhu Manzhou
A simple and efficient solution-based method for the synthesis of Pd-Ni bimetallic nanoparticles (NPs) has been developed. A series of Pd-Ni bimetallic NPs were readily achieved by reduction of PdCl 2 and Ni(acac) 2 (acac = acetylacetonate) in the presence of oleylamine (OAm), oleic acid (OA) and benzyl alcohol. Furthermore, by using high-resolution transmission electron microscopy (HRTEM), energy-dispersive spectrometry (EDS) mapping and X-ray diffraction (XRD), we demonstrate that the as-prepared Pd-Ni bimetallic NPs have core-shell structures with a Pd-rich core and a Ni-rich shell. In addition, the as-obtained Pd-Ni bimetallic NPs with varying compositions show excellent catalytic activities in the Miyaura-Suzuki reaction. When the nickel molar percentage was 0.23 to 0.65, the conversion with the as-obtained Pd-Ni bimetallic catalysts was above 90%. It is believed that this strategy can be employed to produce a variety of other well-defined core-shell type multimetallic nanostructures.
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高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 35
·16810-16817
·
IF 9.931
Dazhong Zhong,Lei Zhang,Chengcheng Li,Dandan Li,Congcong Wei,Qiang Zhao,Jinping Li,Jinlong Gong
Electrochemical water splitting into hydrogen and oxygen is one of the most promising strategies for the utilization and storage of solar energy. However, the sluggish kinetics of the oxygen evolution reaction (OER) hinder its larger-scale application. NiFe-based catalysts are some of the most efficient oxygen evolution catalysts (OECs). High-valence Ni is considered as an active site or conductive framework in NiFe-based OECs. However, the oxidation of Ni is usually hindered in the presence of Fe. This paper describes an effective strategy to produce NiFe (oxy)hydroxide with easily oxidized Ni and a hierarchical nanosheet structure as the most efficient OEC. High valence Ni may provide frameworks with good conductivity and facilitate OERs in Fe active sites. In addition, the hierarchical structure can increase the electrochemical surface area, resulting in more active sites for the OER. The as-prepared Fe–O–Ni(OH)2 supported on nickel foam needs overpotentials of 185, 220 and 261 mV to drive current densities of 10, 100 and 500 mA cm−2, respectively. The catalyst also shows excellent stability at the current densities of 100 and 500 mA cm−2 for 50 hours.
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高影响因子