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INORGANIC CHEMISTRY · 2024 · IF 4.3

Phase-Modified Strongly Coupled δ/ε-MnO2 Homojunction Cathode for Kinetics-Enhanced Zinc-Ion Batteries

Fu Wan,Ruiqi Liu,Yaoyang Xia,Kaida Hu,Yu Lei,Changding Wang,Sida Zhang,Shufan Li,Da Yang,Yujie Zheng,Weigen Chen

Rechargeable Zn-MnO2 batteries using mild water electrolytes have garnered significant interest owing to their impressive theoretical energy density and eco-friendly characteristics. However, MnO2 suffers from huge structural changes during the cycles, resulting in very poor stability at high charge–discharge depths. Briefly, the above problems are caused by slow kinetic processes and the dissolution of Mn atoms in the cycles. In this paper, a 2D homojunction electrode material (δ/ε-MnO2) based on δ-MnO2 and ε-MnO2 has been prepared by a two-step electrochemical deposition method. According to the DFT calculations, the charge transfer and bonding between interfaces result in the generation of electronic states near the Fermi surface, giving δ/ε-MnO2 a more continuous distribution of electron states and better conductivity, which is conducive to the rapid insertion/extraction of Zn2+ and H+. Moreover, the strongly coupled Mn–O–Mn interfacial bond can effectively impede dissolution of Mn atoms and thus maintain the structural integrity of δ/ε-MnO2 during the cycles. Accordingly, the δ/ε-MnO2 cathode exhibits high capacity (383 mAh g–1 at 0.1 A g–1), superior rate performance (150 mAh g–1 at 5 A g–1), and excellent cycling stability over 2000 cycles (91.3% at 3 A g–1). Profoundly, this unique homojunction provides a novel paradigm for reasonable selection of different components.

研究领域: 材料科学 · 能源存储与转换
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Structural Regulation Enables High Interfacial Functionality for Ni-Rich Single-Crystalline Cathodes

Pei Liu,Haoran Wei,Tao Huang,Zhencheng Huang,Lingli Chen,Xuanlong He,Yuying Liu,Hongkai Yang,Mijie Liu,Shenghua Ye,Xuming Yang,Zhanhua Wu,Yaming Liu,Qingqing Jia,XiaoBai Ma,Jing Chen,Xiangzhong Ren,Xiaoping Ouyang,Jianhong Liu,Qianling Zhang,Jiangtao Hu

Ni-rich single-crystalline layered cathodes have garnered significant attention due to their high energy density and thermal stability. However, they experience severe capacity degradation caused by lattice strain and interfacial side reactions during practical applications. In this study, an effective yttrium modification method is employed to stabilize the structure of Ni-rich single-crystalline LiNi0.83Mn0.05Co0.12O2 (SC-NMC83) to solve these issues. This innovative approach successfully immobilizes oxygen within the material, preventing crack formation while simultaneously broadening the diffusion path of Li+. The yttrium-modified sample (SC-NMC83-Y) exhibits a superior capacity retention compared to the SC-NMC83 sample, with values of 90% and 76.1% after 100 cycles, respectively. This work demonstrates the promising potential of a doping strategy for Ni-rich single-crystalline cathodes and paves a pathway for its practical implementation, such as all-solid-state batteries.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学
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CHINESE CHEMICAL LETTERS · 2025 · IF 8.9

Cu/Sb induced minimal lattice distortion for the development of high-performance sodium-ion battery cathode materials

Weijie Yi,Huijun Li,Mingyang Gao,Zirun Chai,Xiaomin Wang

O3-layered oxides are considered promising for various applications due to their high capacity. However, these O3-type materials are prone to undergo an irreversible O3-P3 phase transition, which adversely impacts their structural stability. Elemental doping has been identified as an effective strategy to mitigate this issue. However, substituting Cu at the redox center reduces the capacity of the pristine material. The unique introduction of the Sb element reduces the lattice oxygen ratio, leading to a significant increase in initial capacity. Thus, the Cu/Sb co-doped material NaNi 0.37 Mn 0.49 Cu 0.13 Sb 0.01 O 2 (NNMCS) with unique O3-dominated phase transition process, was successfully prepared using the high temperature solid-phase method. Cu/Sb doping increases Mn⁴⁺ concentration through the charge compensation mechanism at transition metal sites, mitigating the negative structural effects of the dual simplicial state e g orbitals in the high-spin Mn³⁺ state. Doping with Cu/Sb increases the electron cloud density at the transition metal sites, enhancing the electron shielding effect and ultimately causing the distance between the transition metal sites to expand. The increased distance between the transition metal sites indirectly promotes flexibility during transition metal migration, resulting in electrode materials with a smaller rate of lattice parameter change during cycling and ultimately enhancing phase transition reversibility. As a result, NNMCS demonstrates a high initial specific capacity of 188 mAh/g and 78% capacity retention after 200 cycles at 1 C within a 2.0–4.3 V window. This work provides valuable insights into the coupling mechanism between capacity and structural stability in layered oxides for sodium-ion batteries.

研究领域: 材料科学 · 电化学
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Journal of Energy Storage · 2025 · IF 9.8

Tailored core-shell PW@PB cathodes for enhanced sodium-ion battery stability and rate capability

Yuan Wang,Qinfeng Zheng,Yuepeng Pang,Yixiao Zhang,Tao Yuan,Shiyou Zheng

Prussian blue and its analogues (PBA) are promising cathode materials for economical large-scale sodium-ion batteries (SIBs). Manganese-based PBA, abbreviated as “PW”, offers advantages such as high voltage, high capacity, and good cost-effectiveness but faces challenges with manganese dissolution and structural distortion during cycling. In contrast, iron-based PBA, abbreviated as “PB”, maintains more stable structural integrity but exhibits relatively lower capacity. In this study, we introduce an ion-exchange technique to create core-shell structural cathode materials with PW as the main active ingredient and PB as the protective shell (PW@PB). This approach achieves more than doubled capacity retention after 500 cycles compared to naked PW. Furthermore, PW@PB demonstrates notable rate capability enhancements, retaining 80 % of its capacity at 0.1C when subjected to a high rate of 10C, proving its potential for use in fast-charging SIBs. The improved performance is primarily attributed to the reduced lattice and bound water in the structure of PW@PB. Additionally, the stable outer layer of PB inhibits the leaching of Mn and Fe, minimizing lattice distortion during the charge-discharge process.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Correlations and Mechanisms between Temperature Stability and Structural Stability of PNN–PHT Piezoceramics

Xi Ouyang,Manwen Yao,Tongqing Yang,Xi Yao

The significance of temperature stability in piezoelectric materials is crucial as it directly impacts their reliability and consistency in piezoelectric performance under varying temperature conditions. However, the relationship between structural stability and temperature stability remains ambiguous. In this study, we aim to address this issue by constructing piezoceramics with low and high structural stability using the “high configurational entropy” (Pb (Ni0.11Hf0.33Ti0.34Nb0.22) O3) strategy and “tolerance factor” (Pb (Ni0.11Hf0.21Ti0.46Nb0.22) O3) strategy. The relationship between structural stability and temperature stability was then explored through temperature-dependent XRD, Raman, and piezoelectric property tests in the range of 25–250 °C. Our results successfully demonstrate a positive correlation between structural stability and temperature stability. The microstructure information analyzed by temperature-dependent XRD and Raman showed that Pb (Ni0.11Hf0.33Ti0.34Nb0.22) O3 has a more abundant phase structure transition and higher ion disorder, which is directly reflected in its poor temperature stability in the piezoelectric property tests. On the other hand, Pb (Ni0.11Hf0.21Ti0.46Nb0.22) O3 exhibited excellent temperature stability due to its stable phase structure and lower ion disorder. Specifically, the unipolar strain of piezoceramics with low structural stability decreases from 1.63% at 25 °C to 0.24% at 200 °C, while the unipolar strain of piezoceramics with high structural stability only changes from 0.78% at 25 °C to 0.79% at 225 °C. Additionally, our understanding of the high energy barrier imposed by a wide band gap, as well as the hindrance of domain switching and stabilization of domains through the pinning effect of defect dipoles, reveals the underlying mechanism of temperature stability. These findings provide a promising approach to the development of piezoceramics that can effectively function across a wide range of temperatures.

CAS / MDL: 12055-23-1 1313-99-1
研究领域: 材料科学 · 物理学
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Energy Storage Materials · 2022 · IF 20.831

Interlocking biphasic chemistry for high-voltage P2/O3 sodium layered oxide cathode

Lianzheng Yu,Zhiwei Cheng,Kang Xu,Yu-Xin Chang,Yi-Hu Feng,Duo Si,Mengting Liu,Peng-Fei Wang,Sailong Xu

Biphasic hybridization of layered cathode materials for sodium-ion batteries (SIBs) is crucial to enhance storage performances. The synergistic effect of biphases is generally considered to underlie the enhancement, yet the in-depth mechanism underneath remains unclear, in particular at high-voltages (> 4.2 V, vs Na + /Na). Herein, a unique high-voltage-stable P2/O3 composite layered oxide-Na 0.85 Ni 0.34 Mn 0.33 Ti 0.33 O 2 with a specific proportion (P2:O3 = 24.8%:75.2%) is reported via tuning the amounts of Ti substitution in Na 0.85 Ni 0.34 Mn 0.66-x Ti x O 2 . Operando X-ray diffraction reveals that the biphasic Na 0.85 Ni 0.34 Mn 0.33 Ti 0.33 O 2 cathode successfully restrains the formation of O2 phase and undergoes completely reversible structural evolution of P2/O3–P2/P3–OP4/OP2 upon being charged to a high voltage of 4.4 V. Moreover, the interlocking effect between the phase boundaries is revealed to effectively mitigate the severe structural strain and large lattice volume change, thus further raising its structural stability under the high-voltage regions. Consequently, the obtained biphasic P2/O3-Na 0.85 Ni 0.34 Mn 0.33 Ti 0.33 O 2 cathode exhibits an excellent capacity retention of 80.6% at 1C after 200 cycles. More importantly, the full cell fabricated with hard carbon anode achieves a high energy density of 294.6 Wh kg −1 . These results highlight the excellent electrochemical performance of biphasic cathode materials and also grasp new insight into designing composite structure materials for SIBs.

研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Low-Dose and Stable X-Ray Imaging Enabled by Low-Dimensional Dion-Jacobson Perovskites

Deyu Xin,Min Zhang,Zhenghui Fan,Yujie Yang,Siyin Dong,Lin Lei,Wei Zhao,Qianqian Lin,Xiaojia Zheng

Metal halide perovskites have emerged as highly promising candidates for next-generation X-ray detectors due to their facile and low-cost processability, high attenuation coefficient, and tunable optoelectrical properties. In this work, quasi-2D Dion-Jacobson (DJ) perovskites are introduced in a flat panel X-ray imager (FPXI) for X-ray imaging. This study demonstrates that the diammonium interlayers in DJ perovskites play a key role in enhancing structural stability, suppressing ion migration, and improving charge transport. As a result, DJ perovskite-based X-ray FPXIs achieve a sensitivity of 18000 µC Gy air −1 cm −2 , a low detection limit of 5.7 nGy air s −1 , representing performance comparable to that of state-of-the-art 3D perovskite FPXIs. Thanks to the decrease in the signal crosstalk effect of the FPXIs, a high spatial resolution of 0.54 line-pair-per-pixel is achieved, which is higher than that of 3D perovskite FPXIs. Remarkably, high-quality X-ray imaging is achieved at a total dose of 20 µGy air , which is only 1/5 of the dose typically used in commercial equipment. This work not only provides valuable insights and guidance for the fabrication of 2D DJ perovskite X-ray detectors but also lays the groundwork for the adoption of high-performance, stable DJ perovskite imagers as novel flat-panel X-ray detectors.

研究领域: 材料科学 · 医学影像 · 电子工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Modulating electrochemical properties by Fe3+ doping for cobalt-free Li1.2Ni0.26Mn0.54O2 cathode material

Qiuming Liang,Aoping He,Huan He,Tianquan Liang

The widespread application of Li-rich cathode material is restricted due to capacity attenuation and poor rate capability caused by crystal structure transformation and irreversible lattice oxygen escape during cycling. The Fe 3+ -doped effects on lattice structures and electrochemical properties of Li 1.2 Ni 0.26−x Mn 0.54 Fe x O 2 (x = 0, 0.03, 0.05 and 0.08) cathode materials fabricated by a sol-gel method are systematically studied in this paper. Doped materials exhibit good electrochemical performance such as high discharge specific capacity and capacity retention at high current density rates. Li 1.2 Ni 0.21 Mn 0.54 Fe 0.05 O 2 can supply a specific capacity of 190.7 mAh g −1 with 73.6 % capacity retention after 100th cycle at 2 C, and rate capacities of 230.6, 208.5, 193.1, 172.1 and 105.6 mAh g −1 at 0.1, 0.5, 1, 2 and 5 C, respectively. It is attributed to the enhanced structural stability, enlarged Li layer spacing, intensive interaction between transition metals and oxygen, less manganese disproportionation and oxygen release and increased Li + diffusion coefficient by Fe 3+ doping.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

An orderly arrangement of layered carbon Nanosheet/TiO2 nanosheet stack with superior artificially interfacial lithium pseudocapacity

Wenwu Fu,Yaoting Li,Mao-sung Chen,Yanjie Hu,Bingheng Liu,Kai Zhang,Chenyang Zhan,Ming Zhang,Zhongrong Shen

Poor rate capability and cyclability are the major barriers to using TiO 2 as the next generation anode material for high-performance lithium-ion batteries. In this study, a sandwich-like composite consisting of atomically defined two-dimensional (2D) carbon nanosheet is constructed by the confined synthesis in the galleries of layered TiO 2 nanosheet with the superior cycling and rate performances as the anode material for lithium-ion batteries. It is first experimentally revealed that the interfacial charge storage between unilamellar TiO 2 nanosheet and carbon nanosheet in the Carbon/TiO 2 nanosheet stack and the excellent structure stability during the discharge/charge process contribute to the superior performance of the composites. The resultant composite exhibits a high specific capacity (568 mAh g −1 ) with a specific energy of 407.4 Wh kg −1 at a specific power of 71.7 W kg −1 , and remains 88.0 Wh kg −1 at a specific power of 9.0 kW kg −1 . Apart from promising lithium-ion battery anode, this 2D Carbon/TiO 2 composite also has immense potential for applications in other areas such as sodium/potassium-ion batteries, supercapacitor , and catalysis.

研究领域: 材料科学 · 能源存储
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Nano Research · 2018 ·Vol. 11 ·期 12 ·6375-6383 · IF 7.994

Integration of two-dimensional morphology and porous surfaces to boost methanol electrooxidation performances of PtAg alloy nanomaterials

Shang Changshuai,Guo Yaxiao,Wang Erkang

As an attempt to minimize the usage amounts of noble metals in catalysis, PtAg alloy nanocrystals with a porous nanosheet morphology were fabricated through a galvanic replacement reaction. During the reaction, ascorbic acid was added to the solution to protect the Ag triangular nanoplates from being totally etched. Structural characterizations indicated that the obtained nanocrystals had thin porous basal planes and winding edges with abundant bulges. Such unique two-dimensional porous architectures endowed this nanomaterial with plenty of catalytically active sites and structural benefits in electron and mass moving, as well as morphology stability. Electrochemical tests proved that the PtAg porous nanosheets had superior catalytic activity and durability towards methanol electrooxidation in basic media. Specifically, the mass and specific activities of the PtAg porous nanosheets were 4.5 and 2.7 times higher than those of a commercial Pt/C catalyst. In addition to the special structures, the introduction of Ag enhanced the catalytic performances of the PtAg porous nanosheets.

研究领域: 材料科学 · 电化学
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Nano Energy · 2021 · IF 17.881

Insight into the coordinating mechanism of multi-electron reaction and structural stability induced by K+ pre-intercalation for magnesium ions batteries

Shiqi Ding,Xin Dai,Yuxin Tian,Bo Song,Lei Wang,Guicun Li,Shaoxiang Li,Jianfeng Huang,Zhenjiang Li,Alan Meng

Multi-electron reaction as the appealing alternative can offer higher specific capacity, however, it delivers a tendency to collapse the structure causing cycling instability. Herein, K + pre-intercalation strategy is applied to modify VS 4 /N-TG as cathode for MIBs . As opposed to the structural breakdown caused by multi-electron reaction, pre-intercalated K + not only modulate electronic state, making V 2+ present as instead of partial V 4+ achieving multi-electron reaction, but also act as pillar ions for coordinating the interaction of guest-ions with adjacent host ions to strengthen the framework to maintain structural stability, therefore, K 0.20 VS 4 /N-TG delivers high specific capacity of 190 mAh g –1 , and excellent cycling stability with about near 100% capacity retention after 2000 cycles. This finding gives insights into enabling multi-electron transfer reaction while achieving high structural stability via K + pre-intercalation, shed light on designing viable multi-electron reaction in intercalation type cathode without destroying stable structure for high performance magnesium ions batteries.

CAS / MDL: 7803-55-6
研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Unveiling the role of Ni doping in the electrochemical performance improvement of the LiMn2O4 cathodes

Wangqiong Xu,Qiling Li,Fengrui Sui,Shimei Guo,Ruijuan Qi,Cuiqiong Yan,Lijuan Chen,Shubiao Xia,Junming Guo,Zhe Li,Rong Huang,Feixiang Cheng

Ni doping is a commonly used strategy to improve the electrochemical performance of LiMn 2 O 4 . Uncovering the structural changes of Ni-doped LiMn 2 O 4 during electrochemical cycling, particularly at the atomic level, is important to understand the mechanism of the relationship between Ni doping and performance improvement. Herein, we investigate the chemical and structural evolutions of the Ni-doped LiMn 2 O 4 electrodes before and after 1000 cycles at 10 C with atomic resolution and correlate them with changes in the electrochemical properties . We found that Ni 2+ ions doped into the Mn 16d sites to form a more steady LiNi x Mn 2-x O 4 phase construction, which can effectively stabilize the spinel structure by hindering Jahn − Teller distortion. Comprehensive atomic imaging demonstrated that Ni doping can suppress the formation of the unexpected Mn 3 O 4 , and rock-salt MnO phases on the surface and subsurface of LiMn 2 O 4 during cycling, which is conducive to stabilizing the MnO 6 octahedron and inhibiting the migration of Mn. Resultantly, splendid long cycling stability of 88.92 % after 1000 cycles at 10 C (1 C = 148 mAh g −1 ) for the optimized LiNi 0.05 Mn 1.95 O 4 sample is presented. Our study provides an ingenious avenue for regulating the surface optimization and reconstruction of electrode materials .

CAS / MDL: 1317-35-7 1313-99-1
研究领域: 材料科学 · 电化学
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