DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 21
·7258-7266
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IF 4.174
Guanqun Zhang,Yaqi Fan,Ju Huang,Lijin Wang,Chengguang Yang,Meng Lyu,Haiming Liu,Yanhang Ma
The increasing demands for catalysts with improved accessibility to reactants call for a rational synthesis of nanosized zeolites. Herein we developed a facile approach for highly crystalline MFI-type (Silicalite-1 and ZSM-5) and beta zeolites with variable Si/Al ratios and high yield. This was achieved by kinetically decoupling the nucleation from the growth process of the zeolites in a highly concentrated gel system via a temperature-staged treatment. The carefully controlled low-water environment ensures only nucleation in stage I (aging), and hence the generation of abundant nuclei for the subsequent rapid crystallization within a self-confined space at stage II (growth). The method, without using expensive templates or additives, allows the syntheses of nanosized, well-isolated ZSM-5 (Si/Al = 100–∞, 36–88 nm, yield >85%) and Beta (Si/Al = 25–100, 21–66 nm, yield >95%). The ultra-small crystal size endows ZSM-5 zeolites with good catalytic activity, product selectivity and remarkably longer lifetime in methanol conversion reactions.
研究领域:
化学工程
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材料科学
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DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Ze Chen,Shengnan Wang,Zhiquan Wei,Yiqiao Wang,Zhuoxi Wu,Yue Hou,Jiaxiong Zhu,Yanbo Wang,Guojin Liang,Zhaodong Huang,Ao Chen,Donghong Wang,Chunyi Zhi
Chalcogens, especially tellurium (Te), as conversion-type cathodes possess promising prospects for zinc batteries (ZBs) with potential rich valence supply and high energy density. However, the conversion reaction of Te is normally restricted to the Te2–/Te0 redox with a low voltage plateau at ∼0.59 V (vs Zn2+/Zn) rather than the expected positive valence conversion of Te0 to Ten+, inhibiting the development of Te-based batteries toward high output voltage and energy density. Herein, the desired reversible Te2–/Te0/Te2+/Te4+ redox behavior with up to six-electron transfer was successfully activated by employing a highly concentrated Cl–-containing electrolyte (Cl– as strong nucleophile) for the first time. Three flat discharge plateaus located at 1.24, 0.77, and 0.51 V, respectively, are attained with a total capacity of 802.7 mAh g–1. Furthermore, to improve the stability of Ten+ products and enhance the cycling stability, a modified ionic liquid (IL)-based electrolyte was fabricated, leading to a high-performance Zn∥Te battery with high areal capacity (7.13 mAh cm–2), high energy density (542 Wh kgTe–1 or 227 Wh Lcathdoe+anode–1), excellent cycling performance, and a low self-discharge rate based on 400 mAh-level pouch cell. The results enhance the understanding of tellurium chemistry in batteries, substantially promising a remarkable route for advanced ZBs.
研究领域:
材料科学
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电化学
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能源存储
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Jing Li,Chen Yuan,Huiting Xu,Huibin Liu,Junjie Qi,Zhaohua Jiang,Sai Dong,Rongyu Guo,Zhijie Cui,Wenchao Peng,Jiapeng Liu
Conversion-type aqueous copper-selenium (Cu-Se) batteries have gained considerable attention due to their high theoretical capacity, safety and environmental friendliness. However, the multi-electron intermediate conversion reaction of selenium cathode generally possesses sluggish kinetics, which seriously impedes the further development of Cu-Se batteries. Herein, the porous V 2 C@VSe 2 heterostructure (P-V 2 C@VSe 2 ) with built-in electric field (BIEF) were successfully synthesized by the sacrificial template method and in situ selenization strategy, which were used as the selenium host materials for aqueous Cu-Se batteries to effectively enhance the selenium conversion reaction kinetics. The porous structure of P-V 2 C@VSe 2 not only provides faster access for the transport of polyselenide intermediates during electrochemical reactions, but also exposes more catalytic active sites, which in turn improves the catalytic activity of the material. In addition, the built-in electric field generates at the interface of the P-V 2 C@VSe 2 heterostructure facilitates the acceleration of charge transfer and thus improves the kinetics of the redox reaction of selenium. Benefiting from the synergistic effect of the porous structure and the built-in electric field, the Se/P-V 2 C@VSe 2 cathode possessed a discharge specific capacity of 1182.2 mAh g −1 at a current density of 1 A g −1 , which was much higher than those of Se/P-V 2 C (796.6 mAh g −1 ) and Se (597.0 mAh g −1 ) cathodes. In addition, it also maintained a specific capacity of 1054.6 mAh g −1 after 6000 cycles at 10 A g −1 , demonstrating excellent cycling stability. Meanwhile, a series of characterizations and density functional theory calculations were performed to systematically explore the conversion mechanism of aqueous Cu-Se batteries. This work provides promising insights into the construction of high-performance MXene-based catalytic host materials for aqueous Cu-Se batteries.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Junxian Hu,Yangyang Xie,Jingqiang Zheng,Liuyun Zhang,Hongzhong Li,Yanqing Lai,Zhian Zhang
Metal phosphates are attracting great attention as anode materials for alkali-ion batteries due to their chemical stability, low working voltage, and high theoretical capacity. However, there are few reports on the application of metal phosphate as potassium-ion batteries (PIBs) anode material, and the potassium storage mechanism remains mysterious. Herein, a core–shell chromium phosphate@N-doped carbon (denoted as CrPO 4 @NC) composite is newly synthesized and demonstrated as conversion-type anode material for PIBs. The N-doped carbon coating layer effectively relieves the mechanical strain and improves electrical conductivity during repetitive cycling. The formed P–C bonding between CrPO 4 core and nitrogen-doped carbon shell can help to maintain structural integrity and accelerate charge transfer. As a consequence, the CrPO 4 @NC composite exhibits a decent capacity (304.6 mAh g −1 at 50 mA g −1 ), good rate capability (135.1 mAh g −1 at 500 mA g −1 ), and superior stability (133.2 mAh g −1 at 200 mA g −1 after 100 cycles). Particularly noteworthy, we also provide experimental evidence that a conversion reaction occurs at CrPO 4 @NC electrode with metallic Cr and K 3 PO 4 formed during the potassiation process. This work illustrates that CrPO 4 may be a kind of anode material for applications in energy storage systems.
研究领域:
材料科学
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能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
H. Chen,S. Cai,Y. Wu,W. Wang,M. Xu,S.-J. Bao
Rechargeable aqueous zinc-manganese oxide (Zn/MnO 2 ) batteries using Mn 2+ as the electrolyte additive have recently attracted remarkable attention owing to their largely improved cycling stability. Herein, we find that the Zn/MnO 2 batteries with Mn 2+ additive still exhibit rapid capacity fading when cycling between 0.8 and 1.6 V vs. Zn/Zn 2+ , its improved performance is only observed when charged to a higher slope region (>1.6 V), which suggests that the improved performance of Mn 2+ added Zn/MnO 2 is not caused by suppressing the dissolution of MnO 2 cathode. Inspired by this discovery, successive electrochemcial conversion reactions are scrutinized and proved for evaluating the performance of the Zn/MnO 2 batteries after using Mn 2+ as the electrolyte additive. By adding a certain amount of Mn 2+ into the electrolyte, the battery can improve the capacity and cycling abilitily through converted electrodepostion of Mn 2+ . Specifically, the zinc sulfate hydroxide hydrate (Zn 4 SO 4 ·(OH) 6 ·4H 2 O) large-flake can initiate the generation of zinc vernadite nanosheets (Zn x MnO(OH) y ) during the charge process (around 1.5 V vs. Zn/Zn 2+ ), and then the zinc vernadite nanosheets can reversibly re-back to Zn 4 SO 4 ·(OH) 6 ·4H 2 O during the discharge process. Importantly, part of zinc vernadite nanosheets irreversibly transform into tunnel-like MnO 2 nanocrystalline material when charging higher than 1.6 V vs. Zn/Zn 2+ , which can improve the specific capacity of Zn/MnO 2 batteries in subsequent cycles and then make the Zn/MnO 2 batteries exhibit excellent cycles stability. Finally, through a special zinc/carbon nanotube (Zn/CNT) battery, this successive electrochemcial conversion reactions are further verified.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 35
·期 16
·2211611
·
IF 29.4
Chunyan Zhu,Weiqing Yu,Shuxian Zhang,Jianchao Chen,Qingyuan Liu,Qingyu Li,Shijie Wang,Minghao Hua,Xiaohang Lin,Longwei Yin,Rutao Wang
Group IIIA–VA metal sulfides (GMSs) have attracted increasing attention because of their unique Na-storage mechanisms through combined conversion and alloying reactions, thus delivering large theoretical capacities and low working potentials. However, Na + diffusion within GMSs anodes leads to severe volume change, generally representing a fundamental limitation to rate capability and cycling stability. Here, monodispersed In 6 S 7 /nitrogen and sulfur co-doped carbon hollow microspindles (In 6 S 7 /NSC HMS) are produced by morphology-preserved thermal sulfurization of spindle-like and porous indium-based metal organic frameworks. The resulting In 6 S 7 /NSC HMS anode exhibits theoretical-value-close specific capacity (546.2 mAh g −1 at 0.1 A g −1 ), ultrahigh rate capability (267.5 mAh g −1 at 30.0 A g −1 ), high initial coulombic efficiency (≈93.5%), and ≈92.6% capacity retention after 4000 cycles. This kinetically favored In 6 S 7 /NSC HMS anode fills up the kinetics gap with a capacitive porous carbon cathode, enabling a sodium-ion capacitor to deliver an ultrahigh energy density of 136.3 Wh kg −1 and a maximum power density of 47.5 kW kg −1 . The in situ/ex situ analytical techniques and theoretical calculation both show that the robust and fast Na + charge storage of In 6 S 7 /NSC HMS arises from the multi-electron redox mechanism, buffered volume expansion, negligible morphological change, and surface-controlled solid-state Na + transport.
研究领域:
材料科学
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电化学
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储能技术
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DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Guanglu Tang,Mingrui Li,Bin Wang,Yunming Fang,Tianwei Tan
The n -butanol to hydrocarbon (BTH) reaction can produce a series of valuable chemicals and clean fuel precursors. The BTH reaction over different zeolite catalysts (ZSM-5, ZSM-22, Meso-ZSM-22, and ZSM-35) with an emphasis on the production of liquid branched olefins which can be used as precursors for clean gasoline was investigated in this paper. It was found that the structure and acidity of zeolite significantly influences the product distribution in BTH reaction. ZSM-5 zeolite with medium micropore size and large intersections, which are not present in ZSM-22, led to aromatic-rich products and had a long lifetime. ZSM-22 and Meso-ZSM-22 zeolites with unidirectional 10-ring structure achieved a high selectivity to isobutylene and C5+ branched hydrocarbons. Moreover, the Meso-ZSM-22 obtained by desilication with a higher acidity density and improved diffusion property resulted in more liquid organic products than the parent ZSM-22. ZSM-35 exhibited a high product-shape-selectivity for producing isobutylene because of its unique irregular sheet structure and is not suitable for liquid olefin production.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 16
·7088-7098
·
IF 9.931
Chao Cui,Zengxi Wei,Gang Zhou,Weifeng Wei,Jianmin Ma,Libao Chen,Chengchao Li
Developing electrode materials with a full conversion reaction is an effective route to break through the capacity barriers, but this goal remains a great challenge. In this work, we report the synthesis of CoSe2 anodes with a quasi-reversible conversion reaction by uniformly encapsulating CoSe2 nanoparticles in nitrogen-doped carbon nanofibers (CoSe2/N-CNFs). The space-confined effect of CNFs effectively inhibits pulverization and amorphization of CoSe2 during charge and discharge and thus remarkably ensures the integrity of the crystal structure. Meanwhile, pseudocapacitive contributed by the size effect of CoSe2 nanodots and excellent conductivity due to doped nitrogen heteroatoms give the electrode outstanding electrochemical properties. When used as an anode, the CoSe2/N-CNFs achieved a reversible capacity of 371.8 mA h g−1 after 500 cycles at 0.2 A g−1. Even at a high current density of 2 A g−1, the discharge capacity of the CoSe2/N-CNFs still reached 308 mA h g−1 after 1000 cycles with excellent rate performance. The first principles calculations demonstrate that the heterointerfaces between CoSe2 and nitrogen-doped carbon can significantly enhance the stability of the structure and improve the storage/diffusion capability of Na+. Moreover, ex situ high-resolution transmission electron microscopy (HRTEM) and selected area electron diffraction (SAED) reveal that the unique structure enables quasi-reversible crystalline-phase transformation of CoSe2, which leads to the superior cycling stability of the battery with high capacity retention.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 13
·2101955
·
IF 6.389
Anping Tang,Ziqin Liang,Hezhang Chen,Guorong Xu,Haishen Song
A new type of cathodic active material for lithium-ion batteries based on a composite of Li 3 PO 4 and V 2 O 3 is proposed in this work. Although the V 2 O 3 component is almost inactive in the voltage range of 2–4.5 V versus Li + /Li, the mixture of the two components can deliver a larger reversible specific capacity of ≈190 mA h g −1 in the voltage range of 2–4.5 V at a current density of 15 mA g −1 . X-ray photoelectron spectroscopy data and cyclic voltammetry data suggest that the vanadium ions are probably oxidized and reduced repetitively upon cycling and that the V 3+ ions are partially oxidized to V 4+ and even V 5+ ions during charging to 4.5 V. This distinctive lithium-ion uptake and release phenomenon, in which Li 3 PO 4 functions as a lithium source of surface conversion reaction, will introduce a new path for designing unique cathodic active materials for lithium-ion batteries.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
IONICS
·
2025
·Vol. 31
·期 9
·8961-8969
·
IF 2.6
Ning Liping,Sui Zhixing,Tang Anping,Liang Ziqin,Chen Hezhang,Song Haishen,Xu Guorong
Conversion reactions have made LiF-metal oxide (MO) composites with attractive specific capacities compelling candidates for the next generation of lithium-ion battery cathode materials. However, it is necessary for the high charge voltage (> 4.5 V) to drive the redox reaction of MOs and break a strong ionic bond between Li + and F − upon charge. It is a crucial way for decrease in the charge voltage to lower the activation energy barrier of the redox process between LiF and MOs. A novel conversion cathode LiF-V 2 O 3 system is proposed in this study. Unlike most of the previously reported LiF-MOs systems, the LiF-V 2 O 3 system can work at the lower charge cut off voltage of 4.3 V. It delivers a reversible specific capacity of 197 mAh g −1 at C/20 rate in the voltage range of 2–4.3 V. Cyclic voltammetry data suggest a dominant contribution of pseudocapacitance effect in the conversion reaction of the LiF-V 2 O 3 sample.
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高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 32
·期 23
·1908027
·
IF 27.398
Shuai Dong,Dandan Yu,Jie Yang,Li Jiang,Jiawei Wang,Liwei Cheng,Yan Zhou,Honglei Yue,Hua Wang,Lin Guo
Currently, exploring high-volumetric-capacity electrode materials that allow for reversible (de-)insertion of large-size K + ions remains challenging. Tellurium (Te) is a promising alternative electrode for storage of K + ions due to its high volumetric capacity, confirmed in lithium-/sodium-ion batteries, and the intrinsic good electronic conductivity. However, the charge storage capability and mechanism of Te in potassium-ion batteries (KIBs) have not been unveiled until now. Here, a novel K–Te battery is constructed, and the K + -ion storage mechanism of Te is revealed to be a two-electron conversion-type reaction of 2K + Te ↔ K 2 Te, resulting in a high theoretical volumetric capacity of 2619 mAh cm −3 . Consequently, the rationally fabricated tellurium/porous carbon electrodes deliver an ultrahigh reversible volumetric capacity of 2493.13 mAh cm −3 at 0.5 C (based on Te), a high-rate capacity of 783.13 mAh cm −3 at 15 C, and superior long-term cycling stability for 1000 cycles at 5 C. This excellent electrochemical performance proves the feasibility of utilizing Te as a high-volumetric-capacity active material for storage of K + ions and will advance the practical application of KIBs.
研究领域:
储能
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材料科学
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电化学
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电池技术
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DOI
高影响因子
Energy & Environmental Science
·
2020
·Vol. 13
·期 9
·2924-2937
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IF 30.289
Dongjiang Chen,Chao Feng,Yupei Han,Bo Yu,Wei Chen,Ziqi Zhou,Ning Chen,John B. Goodenough,Weidong He
Transition metal carbides (TMCs), known to deliver extra capacity beyond the theoretical limit, are proposed as emerging high-capacity anodes for next-generation lithium ion batteries (LIBs). Nevertheless, the underlying mechanism for the extra lithium storage in TMCs has not been revealed clearly due to the electrochemical inertness of TMCs to Li in cycling. Here, for the first time, by employing in situ Raman and X-ray photoelectron spectroscopies, we corroborate that the capacity enhancement of Fe3C anodes originates from the physiochemical evolution of solid electrolyte interphase (SEI) and surface carbonaceous materials through three mechanisms: (i) Fe3C catalyzes the reversible conversion between esters and ethers to store extra lithium ions in the SEI; (ii) Fe and inorganic components embedded in the SEI form a reversible surface-conversion reaction of Fe + 3LiF ⇌ FeF3 + 3Li+ + 3e− to contribute additional capacity; and (iii) surficial carbon delivers capacity through surface capacitive effects and Li+ inter/deintercalation processes. With the extra lithium ion storage in the SEI and carbon, the C@Fe3C/Fe anode delivers a high reversible capacity of 808 mA h g−1 after 700 cycles at 1 A g−1. This study provides a fundamental basis for emerging high-capacity TMC anodes to be efficiently explored for next-generation LIBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）