Energy Storage Materials
·
2024
·
IF 18.9
Yuhang Xin,Yingshuai Wang,Qingbo Zhou,Hexiao Zhang,Ziye Wang,Lei Liu,Kunyu Zhao,Feng Wu,Hongcai Gao
Due to the uniform distribution of sodium in the crust, the increasing demand for high specific energy and long life in terms of energy storage is placing higher requests on sodium-ion battery technology. The activation of multi-electron reactions in NASICON sodium-ion battery cathode materials can not only reduce the use of vanadium, but also effectively increase the specific energy, therefore, it has received enormous attention from researchers. In this report, the importance of the covalent proportion of metal-oxygen bond in activating the V 4+ /V 5+ redox with higher discharge voltage in Na 3 V 2 (PO 4 ) 3 has been extensively studied. Advanced characterization methods and theoretical calculations comprehensively explain the effects of Zn 2+ , Mg 2+ , and Cu 2+ on V 3+ substitution and the corresponding electrochemical behavior and structural change behavior. Moreover, a complete two-phase reaction in the high voltage reaction region (3.88 V) was observed in Na 3 V 1.5 Cu 0.5 (PO 4 ) 3 . Our results highlight the importance of the covalent proportion of metal-oxygen bonds in activating multi-electron reactions in NASICON structures.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Fangming Liu,Meng Yu,Xiang Chen,Jinhan Li,Huanhuan Liu,Fangyi Cheng
ABSTRACT High-entropy materials are emerging electrocatalysts by integrating five or more elements into one single crystallographic phase to optimize the electronic structures and geometric environments. Here, a rocksalt-type high-entropy oxide Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 O (HEO) is developed as an electrocatalyst towards the oxygen evolution reaction (OER). The obtained HEO features abundant cation and oxygen vacancies originating from the lattice mismatch of neighboring metal ions, together with enlarged Co/Ni‒O covalency due to the introduction of less electronegative Mg and Zn. As a result, the HEO exhibits superior intrinsic OER activities, delivering a turnover frequency (TOF) 15 and 84 folds that of CoO and NiO at 1.65 V, respectively. This study provides a mechanistic understanding of the enhanced OER on HEO and demonstrates the potential of high-entropy strategy in developing efficient oxygen electrocatalysts by elaborately incorporating low-cost elements with lower electronegativity.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2023
·Vol. 106
·期 10
·5822-5831
·
IF 3.9
Kang Du,Changzhi Yin,Zhengyu Zou,Mingfei Cheng,Yiyang Cai,Jiaqing Yang,Meng Zhang,Wenzhong Lu,Shengxiang Wang,Wen Lei
Novel BaCa 2 M 3 O 9 ( M = Si, Ge) microwave dielectric ceramics were prepared via solid-state reaction with sintering at 1125°C–1275°C for 5 h. Single-phase BaCa 2 M 3 O 9 ( M = Si, Ge) ceramics were obtained according to stoichiometry. The single-phase BaCa 2 Ge 3 O 9 ceramic was confirmed through Rietveld refinement and high-resolution transmission electron microscopy/selected area electron diffraction and synthesized for the first time. The BaCa 2 M 3 O 9 ( M = Si, Ge) exhibited a triclinic structure with a P 1 ¯ $\bar 1$ space group and good microwave dielectric properties. The ε r , Q × f , and τ f values of BaCa 2 M 3 O 9 ( M = Si, Ge) ceramics are mostly dominated by the relative density, ionic polarizability, relative covalence, and bond energy of M –O bond, respectively. A high Q × f value (61 800 GHz at 16.3 GHz) was obtained in BaCa 2 Ge 3 O 9 ceramic due to its high r c (Ge–O) and low intrinsic dielectric loss. The BaCa 2 Si 3 O 9 ceramic exhibited small | τ f | value (‒36.4 ppm/°C) due to its large E Si-O . Excellent microwave dielectric properties ( ε r = 8.31, Q × f = 61 800 GHz, and τ f = ‒58.7 ppm/°C) were obtained for the BaCa 2 Ge 3 O 9 ceramic.
研究领域:
材料科学
·
无机化学
✓ 已验证
DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 1
·162-169
·
IF 8.897
Zhong Dazhong,Li Tan,Wang Dong,Li Lina,Wang Jiancheng,Hao Genyan,Liu Guang,Zhao Qiang,Li Jinping
Oxygen evolution reaction (OER) is crucial for hydrogen production as well as other energy storage technologies. CoFe-layered double hydroxide (CoFe-OH) has been widely considered as one of the most efficient electrocatalysts for OER in basic aqueous solution. However, it still suffers from low activity in neutral electrolyte. This paper describes partially oxidized CoFe-OH (PO-CoFe-OH) with enhanced covalency of M-O bonds and displays enhanced OER performance under mild condition. Mechanism studies reveal the suitably enhanced M-O covalency in PO-CoFe-OH shifts the OER mechanism to lattice oxygen oxidation mechanism and also promotes the rate-limiting deprotonation, providing superior OER performance. It just requires the overpotentials of 186 and 365 mV to drive the current density densities of 1 and 10 mA·cm −2 in 0.1 M KHCO 3 aqueous solution (pH = 8.3), respectively. It provides a new process for rational design of efficient catalysts for water oxidation in mild conditions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Yinlong Zhu,Qian Lin,Zhenbin Wang,Dongchen Qi,Yichun Yin,Yu Liu,Xiwang Zhang,Zongping Shao,Huanting Wang
The oxygen evolution reaction (OER) plays a crucial role in many electrochemical energy technologies, and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency. Here, we highlight a new halogen-chlorine (Cl)-anion doping strategy to boost the OER activity of perovskite oxides. As a proof-of-concept, proper Cl doping at the oxygen site of LaFeO 3 (LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER, including rich oxygen vacancies , increased electrical conductivity and enhanced Fe-O covalency . Benefiting from these factors, the LaFeO 2.9-δ Cl 0.1 (LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO. This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts .
研究领域:
材料科学
·
电催化
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 48
·23296-23303
·
IF 6.97
Yibin Yang,Yingqing Ou,Yang Yang,Xijun Wei,Di Gao,Lin Yang,Yuli Xiong,Hongmei Dong,Peng Xiao,Yunhuai Zhang
The development of efficient and stable non-noble-metal electrocatalytic materials for the oxygen evolution reaction (OER) is a huge and important challenge at present. Herein, we report the prominent enhancement of OER activity via doping vanadium into CoFe-based layered double hydroxide (LDH) electrocatalysts. Electrochemical characterization shows that the Co2Fe0.5V0.5 LDH grown on carbon papers (CPs) has an enormous electrochemical surface area (ECSA) and exhibits the smallest overpotential of 242 mV at 10 mA cm−2, which only requires a small Tafel slope of 41.4 mV dec−1 in 1 M KOH solution. The X-ray photoelectron spectroscopy (XPS) peak position of Co, Fe and O moves slightly to higher binding energy, elucidating the improved covalency of the metal–oxygen bond after V doping. DFT+U simulation indicates that the outstanding electrocatalytic activity of Co2Fe0.5V0.5 could be ascribed to the increased metal–oxygen covalency in LDH after V element doping, and facilitates the charge-transfer from oxygen to the metal. This finely tuned strategy by V doping into the CoFe-based LDH matrix can adjust the covalency of metal–oxygen bridges and enhance its electrocatalytic activity for the OER. In this work, we also present a general method to study various highly efficient metal hydroxide catalysts for the OER.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Kexin Wei,Fan Yang,Yang Sun,Chunhui Yu,Junpu An,Kaiyi Chen,Shijia Li,Jiabao Guo,Yongfeng Li
The development of efficient and low-cost non-precious metal bifunctional oxygen electrocatalysts remains a critical challenge for advancing zinc-air batteries. In this study, we designed and synthesized three-dimensional carbon nanofiber catalysts integrated with sulfur- and nitrogen-doped carbon anchoring FeS/MnS heterostructures, leveraging an interfacial engineering approach. Originating from this strategy, the optimized FeS/MnS@CNFs shows a higher half-wave potential (E 1/2 ) of 0.88 V for ORR and a lower overpotential (E j=10 ) of 230 mV at 10 mA cm −2 for OER. The theoretical studies elucidate that the significant work function difference (0.43 eV) between FeS and MnS induces a built-in electric field at their heterointerface. This field drives electron transfer from MnS to FeS, which consequently strengthens the covalency of Fe S bonds and significantly enhances the adsorption capability for the *OOH intermediate species. When employed as the air-cathode catalyst, the FeS/MnS@CNFs-based zinc-air battery achieved a remarkable peak power density of 223 mW cm −2 and maintained stable operation for over 280 h at 10 mA cm −2 . Further theoretical modeling of the heterostructure elucidated that the built-in electric field modulates Fe S bond energies through electronic rearrangement, providing a fundamental explanation for the enhanced oxygen electrocatalytic performance and improved structural stability.
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Sun Yuanmiao,Wang Jiarui,Xi Shibo,Shen Jingjing,Luo Songzhu,Ge Jingjie,Sun Shengnan,Chen Yubo,Hanna John V.,Li Shuzhou,Wang Xin,Xu Zhichuan J.
Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the M T –O–M O backbone. A stronger M O –O covalency relative to M T –O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
Energy & Environmental Science
·
2017
·Vol. 10
·期 7
·1590-1599
·
IF 29.518
Guang-Kun Ren,Shan-Yu Wang,Ying-Cai Zhu,Kyle J. Ventura,Xing Tan,Wei Xu,Yuan-Hua Lin,Jihui Yang,Ce-Wen Nan
BiCuSeO oxyselenides are promising thermoelectric materials at intermediate temperatures, primarily due to their ultralow lattice thermal conductivity (κL) and high Seebeck coefficient. The intrinsically low carrier mobility in these materials, normally below ∼20 cm2 V−1 s−1 at 300 K, however, largely limits further improvements of their thermoelectric properties. In this study, by introducing less electronegative Te into the conductive Cu–Se layers, we demonstrate that the enhanced chemical bond covalency results in smaller effective mass and thus improved carrier mobility, through the weakening of carrier-phonon coupling. The improved carrier mobility by Te-doping largely retains the electrical conductivity values and thus high power factors even with decreased carrier concentrations. Meanwhile, the hierarchical structural features including dual point defects, nanoinclusions, grain boundaries, etc., originating from the nonequilibrium self-propagating high-temperature synthesis (SHS) processes, further reduce κL close to the amorphous limit. Ultimately, a maximum ZT value of ∼1.2 at 873 K is achieved in Bi0.96Pb0.04CuSe0.95Te0.05O, ∼35% improvement as compared with that of Te-free Bi0.96Pb0.04CuSeO and ∼2.4 times higher than that of the pristine sample. Furthermore, our study elucidates that weakening of carrier–phonon coupling through regulating chemical bonding within the conductive functionalities can be an effective avenue for further improving the thermoelectric performance of BiCuSeO.
研究领域:
材料科学
·
热电材料
·
凝聚态物理
·
无机功能材料
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Huang Jun,Yang Qirui,Hu Anyi,Liao Zhu,Zhang Zhengxi,Zheng Qinfeng,Ren Zhouhong,Zheng Shun,Zhang Yixiao,Yang Xiaolong,Xu Zhenming,Zhang Le,Zhu Daming,Wen Wen,Liu Xi,Orita Akihiro,Saito Nagahiro,Wang Liguang,Xia Yongyao,Chen Liwei,Lu Jun,Yang Li
Developing lithium-ion batteries with high specific energy and fast-charging capability requires overcoming the potential-capacity trade-off in negative electrodes. Conventional fast-charging materials (e.g., Li 4 Ti 5 O 12 , TiNb 2 O 7 ) operate at high potentials (>1.5 V vs. Li + /Li) to circumvent lithium plating, yet this compromises specific energy. A viable strategy for enhancing the specific energy is to reduce the potential while avoiding the lithium plating risk; however, the underlying mechanisms remain unclear. Here we demonstrate that enhancing Titanium-Oxygen covalency through pseudo-Jahn-Teller Effect distortion in Ruddlesden-Popper perovskites enables low-potential operation. The Li 2 La 2 Ti 3 O 10 negative electrode exhibits a working potential of 0.5 V vs. Li + /Li with initial 139.3 mAh g −1 at 5 A g −1 and 72.9% capacity retention after 5000 cycles. Full cells with LiNi 0.8 Co 0.1 Mn 0.1 O 2 positive electrodes deliver 3.45 V average discharge voltage-50% higher than conventional Li 4 Ti 5 O 12 | |LiNi 0.8 Co 0.1 Mn 0.1 O 2 systems-achieving 100 mAh g −1 at 4 A g −1 . Mechanistic analysis reveals low Li⁺ migration barriers and stable Ruddlesden-Popper perovskite frameworks enable rapid ion transport.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Hanlin Wang,Jiajia An,Wenxi Zhao,Binkai Yu,Ye Li,Jinqiao Hu,Shikang Jiang,Qinfen Gu,Junwu Zhu,He Zhu,Jingwen Sun,Limin Zhou,Shengjie Peng,Yuping Wu,Hui Xia,Mingzhe Chen
Revealing the mechanism of Mn doping in polyanionic NaFePO4 materials advances our fundamental understanding of electrochemical reactions. Herein, we propose the concept of heterotransition metal ligand field clusters (H-TMLFC) as a framework to investigate the structural evolution of transition metal (TM) ligand fields at the microscopic level. The introduced [MnO6] octahedra exhibit a distinctive half-filled frontier orbital configuration, thereby strengthening σ-bonding interactions and modulating the charge distribution between adjacent [FeO6] units. The redistribution of charge density around the edge-sharing oxygen atoms in [FeO6]–[MnO6] pairs enhances Fe–O covalency and mitigates Fe/Na antisite defects. As a result, H-TMLFC-derived NaFe0.95Mn0.05PO4 achieves an exceptional capacity of 148.9 mAh·g–1 (96.7% of the theoretical capacity) and exhibits superior long-term cycling stability. This work introduces a novel approach for designing high-performance sodium-ion batteries through TM doping, offering atomic-scale insights into the optimization of polyanionic cathode materials.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Chao Huang,Qiang Li,Liping Sun,Lihua Huo,Hui Zhao,Fourcade Sebastien,Bassat Jean-Marc
High entropy oxides are one of the research topicalities in the field of SOFC. However, the relationship between configuration entropy and the electrochemical properties of these materials is not well understood. Here, a medium entropy material (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Eu 0.2 ) 2 CuO 4 ((Ln 0.2 ) 2 CuO 4 ) derived from Nd 2 CuO 4 material is designed. It was found that increasing the configuration entropy of the A-site promotes the production of highly reactive/concentrated non-stoichiometric oxygen and increases the covalency of the Cu3d-O2p orbital. The polarization impedance of (Ln 0.2 ) 2 CuO 4 is 0.92 Ω cm 2 at 700 °C, which is smaller than that of Nd 2 CuO 4 (1.8 Ω cm 2 at 700 °C). The peak power density of single cells NiO-YSZ|YSZ|GDC|cathode is 526 mW cm −2 at 700 °C within 60 h of stable operation at 0.5 V. First-principles calculations demonstrate that (Ln 0.2 ) 2 CuO 4 has lower charge transfer energy, which promotes the electronic conduction. Furthermore, the dissociation energy of adsorbed oxygen (O ad ) on the surface of (Ln 0.2 ) 2 CuO 4 is 2.24 eV, which is smaller than that of Nd 2 CuO 4 (2.26 eV). These results suggest that the entropy-increasing strategy can enhance the electrocatalytic performance.
研究领域:
材料科学
·
电化学
·
能源材料
·
固态离子学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）