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Small · 2022 ·Vol. 18 ·期 16 ·2107346 · IF 15.153

Interfacial Reviving of the Degraded LiNi0.8Co0.1Mn0.1O2 Cathode by LiPO3 Repair Strategy

Ze Feng,Shan Zhang,Xiaobing Huang,Yurong Ren,Dan Sun,Yougen Tang,Qunxuan Yan,Haiyan Wang

Nickel-rich cathode materials, owing to their high energy density and low cost, are considered to be one of the cathodes with the most potential in next-generation lithium-ion batteries. Unfortunately, this kind of cathode with highly active surface is easy to react with H 2 O and CO 2 when exposed to ambient air, resulting in the formation of lithium impurities and interfacial phase transition as well as deterioration of the electrochemical properties. In this work, the evolution mechanism of the structure and interface of LiNi 0.8 Co 0.1 Mn 0.1 O 2 during air-exposure is systematically investigated. Furthermore, a facile reviving strategy is proposed to restore the degraded LiNi 0.8 Co 0.1 Mn 0.1 O 2 by using LiPO 3 as the repair agent. The lithium impurities on the surface of the degraded sample can transform into the repair/coating layer, and part of the rock salt phase on the subsurface can revive to layered phase after repair heat treatment. As a result, the optimized cathode delivers an initial discharge capacity of 198.3 mAh g −1 at 0.1C and a capacity retention of 85.5% after 50 cycles. Although slightly lower than the bare sample (201 mAh g −1 and 88%), they are obviously higher than the exposed samples (166.5 mAh g −1 and 40.4%). The regenerated electrochemical properties should be attributed to the multifunctional repair layer that can efficiently reduce the surface lithium impurities, prevent the corrosion of electrolyte, and improve the interfacial Li + diffusion kinetics. This work can effectively reduce the waste of the degraded Ni-rich ternary materials and realize the transformation of “waste” into wealth.

研究领域: 材料科学 · 电化学 · 能源存储 · 电池技术 · 界面工程
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

“Tree blossom” Ni/NC/C composites as high-efficiency microwave absorbents

Yu Zhou,Wenjun Zhou,Chunhua Ni,Shenggang Yan,Liangmin Yu,Xia Li

Precursors of a nickel-based metal–organic framework, denoted Ni-MOF, and the loofah plant were prepared by the microwave method, and “tree blossom” Ni/Nitrogen doped Carbon (NC)/ Carbon (C) composites were prepared by in situ pyrolysis under an argon atmosphere. During pyrolysis, the morphology, specific surface area, porous structure and electromagnetic parameters of the Ni/NC/C composites were adjusted by adjusting the pyrolysis temperature. The maximum reflection loss of the corresponding Ni/NC/C composites can reach −63.1 dB at 13.84 GHz and a thickness of 2 mm when the pyrolysis temperature was 650 ℃ and the filling amount was 16 wt%. And the effective absorption bandwidth was 35.44 GHz when the thickness was adjusted from 1 mm to 5.5 mm within the range of 2–40 GHz. Excellent performance comes from conduction loss, dipole and interface polarization, magnetic resonance, multiple electromagnetic reflections and scattering, and equilibrium impedance matching.

研究领域: 材料科学 · 纳米复合材料 · 电磁功能材料 · 能源材料 · 环境功能材料
✓ 已验证 DOI 高影响因子
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JOURNAL OF CATALYSIS · 2019 · IF 7.723

A switchable-selectivity multiple-interface Ni-WC hybrid catalyst for efficient nitroarene reduction

Yuanyuan Ma,Zhongling Lang,Jing Du,Likai Yan,Yonghui Wang,Huaqiao Tan,Shifa Ullah Khan,Yang Liu,Zhenhui Kang,Yangguang Li

Selective reduction of nitroarenes is extremely valuable in industrial chemical production. The main reduced products are usually aniline derivatives obtained using single-component noble- or transition-metal catalysts; however, other important products such as hydrazobenzene derivatives always involve in harsh conditions and multiple reaction steps. Here, we realize an unexpected switchable reduction of nitroarenes into aniline or hydrazobenzene derivatives with high yield and selectivity just by controlling the molar ratio of nitroarenes to N 2 H 4 ·H 2 O with a nickel–tungsten carbide composite nanocatalyst loaded on carbon (Ni-WC/C). A series of control experiments and density functional theory (DFT) calculations indicate that the multiple interfaces between Ni and WC can induce a synergistic effect, significantly modulating the electronic structure of the Ni-WC/C catalyst, and endowing the catalyst with switchable selectivity and high activity for the reduction of nitroarenes by hydrogenation. This synergistic multi-interfacial catalyst may offer a new way to design and explore highly efficient and selective catalysts for the controllable reduction of nitroarenes and similar hydrogenation reactions.

研究领域: 催化化学 · 有机合成 · 纳米材料 · 表面科学 · 工业化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Controlled synthesis of a high-performance α-NiS/Ni3S4 hybrid by a binary synergy of sulfur sources for supercapacitor

Qin Hu,Shengtao Zhang,Feng Chen,Wenpo Li,Hao Jiangyu,Xinyue Liang,Bin Xiang,Chao Chen,Xuefeng Zou

Nickel sulfide possesses ultra-high theoretical energy storage capacity. Though it is easily obtained, it is very difficult to exert its intrinsic strong capacity. In this work, a new strategy based on a binary synergy of sulfur sources is introduced. By regulating the molar ratio of two sulfur sources, a high-performance α-NiS/Ni 3 S 4 binary hybrid is successfully synthesized. Interestingly, it is found that changing the molar ratio of two sulfur sources in hydrothermal process can efficiently regulate the components of product but cannot visibly affect its morphology. The electrochemical results indicate that this strategy is highly effective for improving the performance of nickel sulfide. As a result, a highest specific capacity of 214.9 mAh g −1 at 2 A g −1 was reached. In addition, the fabricated S3//rGO hybrid supercapacitor displays a highest energy density of 41.9 Wh kg −1 at a power density of 799.0 kW kg −1 . Moreover, the device delivers an excellent cycle stability with 103% capacity retention rate after 10,000 cycles. These findings open a new avenue for the controlled synthesis of high-performance nickel sulfides or other metal sulfides.

研究领域: 材料科学 · 电化学 · 纳米技术 · 储能
✓ 已验证 DOI 高影响因子
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Journal of Energy Storage · 2022 · IF 8.907

Facile synthesis and incomplete sulfidation of nickel-cobalt-aluminum ternary layered hydroxide binder-free electrode with enhanced supercapacitor properties

Kailin Li,Changqing Yin,Xingjian Dai,Jiayun Zhang,Shuang Yi,Jinsong Rao,Yuxin Zhang

Layered transition metal hydroxide, a clay-like material, possessing characteristics of large specific surface area, adjustable fraction, and plentiful active components make it a potential energy storage material , especially in the background of energy and environment crisis. Herein, comprehensive applications of cobalt-aluminum-based LDHs for supercapacitors are proposed. Binder-free electrodes were successfully synthesized such as Co 3 Al 1 -LDH/Ni, Ni 2 Co 1 Al 1 -LDH/Ni and Ni 1 Co 2 Al 1 -LDH/Ni using a rapid green hydrothermal approach. Subsequently, further sulfuration was carried out to obtain a heterostructure of sulfide/layered hydroxide. The electrochemical energy storage properties of binder-free electrodes were investigated, which show that the performance of ternary LDH electrode is better than that of binary one, and the incompletely sulfuration Ni 1 Co 2 S/Ni has the optimal electrochemical performance among all electrodes, with a specific capacitance of 2186 F g −1 at 1 A g −1 . The Ni 1 Co 2 S//AG hybrid supercapacitor (HSC) device assembled with Ni 1 Co 2 S as positive electrode and active graphene as negative electrode delivers an energy density of 13 Wh kg −1 at a power density of 749 W kg −1 , good rate capability and cycling stability.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 功能材料 · 电化学储能
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Synergistically regulating the structural tolerance of Co-free Ni-rich cathode materials at high-rate through multi-heteroatoms substitution

Bao Zhang,Heng Wen,Keyi Xian,Na Lu,Chao Zheng,Zhiming Xiao,Xinyou He,Long Ye,Jiexi Wang,Lei Ming,Chunhui Wang,Xing Ou

Cobalt-free, nickel-rich layered oxides are attracting extensive interest as cathodes to construct high-energy and sustainable lithium-ion batteries, but the intrinsic structure instability and weakened reaction kinetics deteriorate their application. Nowadays, doping engineering, especially multielement doping, has become an effective modification method for obtaining high-performance Ni-rich materials. Herein, the designed doping strategy with high oxidation states element (Zr 4+ , Mo 6+ ) substituting transition metal element and Mg 2+ replacing Li + in LiNi 0.9 Mn 0.1 O 2 (NM-ZMM) has been designed to enhance its electrochemical properties. The introduced doping elements with high oxidation states can generate the strong metal-O bond, which contributes to suppress the structural collapse induced by internal stress, and then maintain unblock ion channels for NM-ZMM. Meanwhile, the presence of Mg 2+ can also be employed as the pillar ions to reinforce the structure stability, and occupy the Li-sites to inhibit lattice distortion during charging/discharging process. Thus, benefitting from the synergistic reinforcement of co-doping strategy, as-prepared NM-ZMM materials exhibit the prominent capacity retention (87.5 %, 210 cycles, 1C; 85.5 %, 2C, 150 cycles). Thereof, this creative strategy is crucial in strengthening the electrochemical performance of Ni-rich Co-free materials, which contributes to promote the development of high-performance and cost-effective Li-ion storage technology.

研究领域: 材料科学 · 电化学 · 能源存储 · 锂离子电池 · 固态化学 · 纳米材料 · 电极材料
✓ 已验证 DOI 高影响因子
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ACS Catalysis · 2017 · IF 10.614

TiO2–x-Modified Ni Nanocatalyst with Tunable Metal–Support Interaction for Water–Gas Shift Reaction

Ming Xu,Shan He,Hao Chen,Guoqing Cui,Lirong Zheng,Bin Wang,Min Wei

The modulation of strong metal–support interaction (SMSI) plays a key role and remains a challenge in achieving the desired catalytic performance in many important chemical reactions. Herein, we report a TiO2–x-modified Ni nanocatalyst with tunable Ni–TiO2–x interaction via a two-step procedure: preparation of Ni/Ti mixed metal oxide (NiTi–MMO) from NiTi-layered double hydroxide (NiTi–LDH) precursor, followed by a further reduction treatment at different temperatures. A combination study (XRD, TEM, H2-TPR, XPS, and in situ EXAFS) verifies that a high reduction temperature enhances the Ni–TiO2–x interaction, which results in an increased coverage degree of Ni nanoparticles by TiO2–x as well as electron density of interfacial Ni (Niδ−). Moreover, the creation of a Niδ−–Ov–Ti3+ interface site (Ov denotes oxygen vacancy) induced by strong Ni–TiO2–x interaction serves as dual-active site to efficiently catalyze the water–gas shift reaction (WGSR). The optimized catalyst (Ni@TiO2–x(450)) via tuning Ni–TiO2–x interaction gives a TOF value of 3.8 s–1, which is ∼7 times larger than the conventional 15%Ni/TiO2(450) catalyst. Such a high catalytic efficiency is attributed to the interfacial site (Niδ−–Ov–Ti3+) with medium strength of metal–support interaction, as revealed by in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS), which promotes the synergic catalysis between Niδ− and oxygen vacancy toward WGSR.

研究领域: 催化化学 · 材料科学 · 表面科学 · 能源化学 · 纳米催化
✓ 已验证 DOI 高影响因子
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2018 · IF 3.235

Facile synthesis of mesoporous NiCo2O4 nanoneedle arrays on three dimensional graphene thin film grown on Ni foam for a high-performance binder-free lithium-ion battery anode

Xu Wang,Peng Zhang,Tong Wang,Osamu Yamamoto,Nobuyuki Imanishi,Miao Wang

Mesoporous NiCo 2 O 4 nanoneedle arrays on graphene film grown directly on a three-dimensional Ni foam have been fabricated by a facile hydrothermal method , accompanied by annealing under air atmosphere. The BET specific surface area of NiCo 2 O 4 @graphene film@Ni foam is as high as 47.65 m 2  g −1 . The porous composites served as a binder-free anode material for lithium-ion batteries display an excellent and stable electrochemical performance with high specific capacities of 1232 mAh g −1 at the current density of 500 mA g −1 over 100 cycles and 1493 mAh g −1 at the current density of 1500 mA g −1 after 230 cycles with Coulombic efficiency higher than 97%. Moreover, a fairly high rate capacity of 586 mAh g −1 retained even at a high current density of 8000 mA g −1 . The outstanding electrochemical performance should be attributed to synergetic effect of NiCo 2 O 4 nanoneedle arrays with mesoporous nature and high specific area as well as graphene substrate supporting, which can accommodate the volume variation during the electrochemical reactions and facilitate the ion and electron transmission.

研究领域: 材料科学 · 电化学 · 纳米能源材料 · 储能技术 · 功能材料
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2016 · IF 3.014

Synthesis of Li2Si2O5-coated LiNi0.6Co0.2Mn0.2O2 cathode materials with enhanced high-voltage electrochemical properties for lithium-ion batteries

Shengjie Liu,Hao Wu,Ling Huang,Mingwu Xiang,Heng Liu,Yun Zhang

Ni-rich ternary layered oxides , (LiNi x [M] 1−x O 2 , x ≥ 0.5, M = Co and Mn), have become one of the mainstream cathode materials for next-generation lithium-ion batteries due to their high capacity and cost efficiency compared with LiCoO 2 . However, the high-voltage operation of the Ni-rich oxides (>4.3 V) required for high capacity is inevitably accompanied with a rapid capacity decay over numerous cycles. In this work, we reported a surface coating of LiNi 0.6 Co 0.2 Mn 0.2 O 2 with Li 2 Si 2 O 5 via a facile and efficient synthetic approach, which involves the employment of silicic acid (H 2 SiO 3 ) as remover to react with the surface residual lithium compounds ( e.g. Li 2 CO 3 and LiOH) of LiNi 0.6 Co 0.2 Mn 0.2 O 2 and consequent formation of a robust and complete Li + -conductive Li 2 Si 2 O 5 protective coating layer . The structure and morphology of the coated cathode materials are fully characterized by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). Compared with the pristine LiNi 0.6 Co 0.2 Mn 0.2 O 2 , coating with the Li + -conductive Li 2 Si 2 O 5 is found to be very effective for improving the rate capability of the LiNi 0.6 Co 0.2 Mn 0.2 O 2 when evaluated at a high cut-off voltage up to 4.5 V. Specifically, 1 wt. % H 2 SiO 3 -treated LiNi 0.6 Co 0.2 Mn 0.2 O 2 electrode exhibits high discharge specific capacities of 213.9 and 121.6 mAh g −1 at 0.1 and 10 C, respectively, whereas the pristine electrode only shows 196.8 and 92.1 mAh g −1 . Besides, the surface-modified LiNi 0.6 Co 0.2 Mn 0.2 O 2 electrode also manifests an enhanced long-term cycling stability (67% capacity retention after 200 cycles at 5 C), much better than the pristine electrode (52% retention) due to the robust protective effect of the Li 2 Si 2 O 5 coating layer. All these results indicate that the Li 2 Si 2 O 5 -coated LiNi 0.6 Co 0.2 Mn 0.2 O 2 will be a promising cathode material for lithium-ion batteries with fascinating electrochemical energy storage capabilities.

研究领域: 电化学 · 材料科学 · 能源存储 · 锂离子电池技术 · 固态化学 · 表面改性
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 46 ·24579-24589 · IF 11.301

Implanting an electrolyte additive on a single crystal Ni-rich cathode surface for improved cycleability and safety

Yongkang Han,Jinmei Xu,Wei Wang,Fu Long,Qunting Qu,Yan Wang,Honghe Zheng

Interfacial modification is one of the most important technologies to improve the overall electrochemical properties of Ni-rich cathodes. Herein, a novel strategy of in situ planting of an electrolyte film-forming additive on a single crystal NCM811 surface is proposed by consuming the residual lithium to develop a functional Al(Li)BOB nano-layer. Different from traditional physical coating, this approach cleverly consumed the undesirable residual lithium on the NCM811 surface. The in situ grown 30–50 nm Al(Li)BOB layer on the single crystal NCM811 cathode surface contributes to its much enhanced electrochemical performances. At a high operating voltage (charge voltage limit of 4.5 V vs. Li/Li+), the capacity retention is greatly increased from 57.0% to 83.5% after 295 cycles. Meanwhile, the incorporation of aluminum is effective in improving the thermal stability of the Ni-rich cathode. The novel interfacial strategy by in situ implanting of an electrolyte additive is of important significance for solving the critical interfacial issue for Ni-rich cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储 · 锂离子电池 · 界面工程 · 纳米材料 · 固态化学
✓ 已验证 DOI 高影响因子
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Journal of the American Chemical Society · 2024 · IF 14.4

Single-Atom Ni Supported on TiO2 for Catalyzing Hydrogen Storage in MgH2

Jiyue Zhang,Wenda Wang,Xiaowei Chen,Jinlong Jin,Xiaojun Yan,Jianmei Huang

As an efficient and clean energy carrier, hydrogen is expected to play a key role in future energy systems. However, hydrogen-storage technology must be safe with a high hydrogen-storage density, which is difficult to achieve. MgH2 is a promising solid-state hydrogen-storage material owing to its large hydrogen-storage capacity (7.6 wt %) and excellent reversibility, but its large-scale utilization is restricted by slow hydrogen-desorption kinetics. Although catalysts can improve the hydrogen-storage kinetics of MgH2, they reduce the hydrogen-storage capacity. Single-atom catalysts maximize the atom utilization ratio and the number of interfacial sites to boost the catalytic activity, while easy aggregation at high temperatures limits further application. Herein, we designed a single-atom Ni-loaded TiO2 catalyst with superior thermal stability and catalytic activity. The optimized 15wt%-Ni0.034@TiO2 catalyst reduced the onset dehydrogenation temperature of MgH2 to 200 °C. At 300 °C, the H2 released and absorbed 4.6 wt % within 5 min and 6.53 wt % within 10 s, respectively. The apparent activation energies of MgH2 dehydrogenation and hydrogenation were reduced to 64.35 and 35.17 kJ/mol of H2, respectively. Even after 100 cycles of hydrogenation and dehydrogenation, there was still a capacity retention rate of 97.26%. The superior catalytic effect is attributed to the highly synergistic catalytic activity of single-atom Ni, numerous oxygen vacancies, and multivalent Tix+ in the TiO2 support, in which the single-atom Ni plays the dominant role, accelerating electron transfer between Mg2+ and H– and weakening the Mg–H bonds. This work paves the way for superior hydrogen-storage materials for practical unitization and also extends the application of single-atom catalysis in high-temperature solid-state reactions.

研究领域: 储能技术 · 催化化学 · 材料科学 · 纳米技术 · 氢能技术 · 固态化学
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ChemSusChem · 2024 ·Vol. 17 ·期 24 ·e202400840 · IF 7.5

A Plastic-Crystal Electrolyte Layer Promotes Interfacial Stability of Ni-Rich Oxide Cathode in Li6PS5Cl-Based All-Solid-State Rechargeable Li Batteries

Ruojian Ma,Yaning Liu,Ruyi Fang,Jun Zhang,Ya-Hui Wang,Hui Huang,Yongping Gan,Xinping He,Xinhui Xia,Wenkui Zhang,Yang Xia,Sen Xin

Unfavorable parasitic reactions between the Ni-rich layered oxide cathode and the sulfide solid electrolyte have plagued the realization of all-solid-state rechargeable Li batteries. The accumulation of inactive by-products (P 2 S x , S, PO x n − and SO x n − ) at the cathode-sulfide interface impedes fast Li-ion transfer, which accounts for sluggish reaction kinetics and significant loss of cathode capacity. Herein, we proposed an easily scalable approach to stabilize the cathode electrochemistry via coating the cathode particles by a uniform, Li + -conductive plastic-crystal electrolyte nanolayer on their surface. The electrolyte, which simply consists of succinonitrile and Li bis(trifluoromethanesulphonyl)imide, serves as an interfacial buffer to effectively suppress the adverse phase transition in highly delithiated cathode materials, and the loss of lattice oxygen and generation of inactive oxygenated by-products at the cathode-sulfide interface. Consequently, an all-solid-state rechargeable Li battery with the modified cathode delivers high specific capacities of 168 mAh g −1 at 0.1 C and a high capacity retention >80 % after 100 cycles. Our work sheds new light on rational design of electrode-electrolyte interface for the next-generation high-energy batteries. Graphical A uniform plastic-crystal electrolyte nanolayer is coated onto the surface of Ni-rich oxide cathode particles and serves as a buffer to effectively suppress the adverse phase transition, loss of lattice oxygen and interfacial parasitic reactions with a sulfide solid electrolyte at highly delithiated cathode, which contributes improved electrochemical performance of an all-solid-stare rechargeable Li battery.

研究领域: 材料科学 · 电化学 · 能源存储 · 固体离子学 · 电池技术
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