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1.
Liangtao Yang Liang-Yin Kuo Juan Miguel López del Amo Prasant Kumar Nayak Katherine A. Mazzio Sebastian Maletti Daria Mikhailova Lars Giebeler Payam Kaghazchi Teófilo Rojo Philipp Adelhelm 《Advanced functional materials》2021,31(38):2102939
A known strategy for improving the properties of layered oxide electrodes in sodium-ion batteries is the partial substitution of transition metals by Li. Herein, the role of Li as a defect and its impact on sodium storage in P2-Na0.67Mn0.6Ni0.2Li0.2O2 is discussed. In tandem with electrochemical studies, the electronic and atomic structure are studied using solid-state NMR, operando XRD, and density functional theory (DFT). For the as-synthesized material, Li is located in comparable amounts within the sodium and the transition metal oxide (TMO) layers. Desodiation leads to a redistribution of Li ions within the crystal lattice. During charging, Li ions from the Na layer first migrate to the TMO layer before reversing their course at low Na contents. There is little change in the lattice parameters during charging/discharging, indicating stabilization of the P2 structure. This leads to a solid-solution type storage mechanism (sloping voltage profile) and hence excellent cycle life with a capacity of 110 mAh g-1 after 100 cycles. In contrast, the Li-free compositions Na0.67Mn0.6Ni0.4O2 and Na0.67Mn0.8Ni0.2O2 show phase transitions and a stair-case voltage profile. The capacity is found to originate from mainly Ni3+/Ni4+ and O2-/O2-δ redox processes by DFT, although a small contribution from Mn4+/Mn5+ to the capacity cannot be excluded. 相似文献
2.
Wang Hay Kan Chenxi Wei Dongchang Chen Tao Bo Bao‐Tian Wang Yan Zhang Yangchao Tian Jun‐Sik Lee Yijin Liu Guoying Chen 《Advanced functional materials》2019,29(17)
Lithium‐rich disordered rock‐salt oxides have attracted great interest owing to their promising performance as Li‐ion battery cathodes. While experimental and theoretical efforts are critical in advancing this class of materials, a fundamental understanding of key property changes upon Li extraction is largely missing. In the present study, single‐crystal synthesis of a new disordered rock‐salt cathode material, Li1.3Ta0.3Mn0.4O2 (LTMO), and its use as a model compound to investigate Li concentration–driven evolution of local cationic ordering, charge compensation, and chemical distribution are reported. Through the combined use of 2D and 3D X‐ray nanotomography, it is shown that Li removal accompanied by oxygen oxidation is correlated with the development of morphological defects such as particle cracking. Chemical heterogeneity, quantified by subparticle level distribution of Mn valence state, is minimal during Mn redox, which drastically increases upon the formation of cracks during oxygen redox. Density functional theory and bond valence sum mismatch calculations reveal the presence of local short‐range ordering in the pristine oxide, which gradually disappears along with the extraction of Li. The study suggests that with cycling the transformation into true cation–disordered state can be expected, which likely impacts the voltage profile and obtainable energy density of the oxide cathodes. 相似文献
3.
The kinetics of reactions occurring at the gas-exposed surfaces of charged mixed ionic electronic conductors (MIECs) are examined
from theoretical first principles. Analysis based on the classical electrochemical potential-transition state theory model
reveals that the nature of the reactions is electrochemical in general. However, the influence of the surface potential on
the reaction rate is opposite for adsorption and incorporation reactions. Two-dimensional finite volume models of an MIEC
as working electrode in a half-cell configuration are presented. The results for a simple, two-step reduction process show
that the effect of the surface potential on the rate of reactions is minimal for incorporation-limited reactions but more
influential for adsorption-limited reactions.
An erratum to this article is available at . 相似文献
4.
DC cathodic polymerization of trimethylsilane (TMS) was carried out in plasma reactors with and without using anode assembly. In DC cathodic polymerization, the TMS plasma polymers are mainly deposited on the cathode (substrate) surface. As a result, fast deposition of TMS plasma polymers was easily achieved in DC cathodic polymerization as compared with AF or RF plasma polymerization. DC cathodic polymerization without using anode assembly has its advantageous features that the size and number of substrates (as cathodes) are not restricted by the size and the location of anode assembly. It was found that the maximum deposition rate on the cathode surfaces was obtained without anode assembly. The DC cathodic polymerization of TMS was conducted also in a large volume reactor with multiple cathodes (substrates). The same deposition mechanisms for DC cathodic polymerization with a single cathode also apply to the multiple cathodes. Uniform deposition on each cathode could be obtained with appropriate spacing of multiple cathodes and by adjusting the operational parameters, which are based on the current density and the system pressure. 相似文献
5.
Duan Bin Yanyan Du Beibei Yang Hongbin Lu Yao Liu Yongyao Xia 《Advanced functional materials》2023,33(8):2211765
Aqueous rechargeable zinc batteries (ARZBs) are recently prevailing devices that utilize the abundant Zn resources and the merits of aqueous electrolytes to become a competitive alternative for large-scale energy storage. Benefiting from the unique inductive effect and flexible structure, the past five years have experienced a diversiform of phosphate-based polyanion materials that are used as cathodes in ARZBs. In this review, the most recent advances in the Zn2+ storage mechanisms and electrolyte optimization of the phosphate-based cathodes of ARZBs, which mainly focus on vanadium/iron-based phosphates and their derivatives are presented. Furthermore, in addition to significant progress on polyanion phosphate-based cathode materials, the design strategies both for electrode materials and compatible electrolytes are also elaborated to improve the energy density and extend the cycling life of aqueous Zn/polyanion batteries. 相似文献
6.
Xianggang Gao Haiyan Zhang Shihao Li Shuai Zhang Chaohong Guan Xiaoping Hu Juanlang Guo Yanqing Lai Zhian Zhang 《Advanced functional materials》2023,33(43):2304065
Anionic and cationic redox chemistries boost ultrahigh specific capacities of Li-rich Mn-based oxides cathodes (LRMO). However, irreversible oxygen evolution and sluggish kinetics result in continuous capacity decay and poor rate performance, restricting the commercial fast-charging cathodes application for lithium ion batteries. Herein, the local electronic structure of LRMO is appropriately modulated to alleviate oxygen release, enhance anionic redox reversibility, and facilitate Li+ diffusion via facile surface defect engineering. Concretely, oxygen vacancies integrated on the surface of LRMO reduce the density of states of O 2p band and trigger much delocalized electrons to distribute around the transition metal, resulting in less oxygen release, enhancing reversible anionic redox and the MnO6 octahedral distortion. Besides, partially reduced Mn and lattice vacancies synchronously stimulate the electrochemical activity and boost the electronic conductivity, Li+ diffusion rate, and fast charge transfer. Therefore, the modified LRMO exhibits enhanced cyclic stability and fast-charging capability: a high discharging capacity of 212.6 mAh·g−1 with 86.98% capacity retention after 100 cycles at 1 C is obtained and to charge to its 80%, SOC is shortened to 9.4 min at 5 C charging rate. This work will draw attention to boosting the fast-charging capability of LRMO via the local electronic structure modulation. 相似文献
7.
Changmin Lee Youngjae Hong Dongho Kim Younghwan Lim Jang Wook Choi Sung-Yoon Chung 《Advanced functional materials》2023,33(44):2303763
Protons in aqueous electrolytes can perform as an additional type of charge carrier for insertion/extraction in addition to the primary carrier cations in aqueous rechargeable batteries. Despite many diverse claims regarding the effect of protons, mutually conflicting experimental results and their interpretations without direct evidence have been reported over the last decade. Systematic examinations and analyses are thus imperative to clarify the conditions of proton insertion in aqueous rechargeable batteries. Utilizing V2O5 as a model cathode and beaker-type cells with a sufficient amount of ZnSO4 aqueous electrolytes in this work, it is demonstrated that protons are inserted into the cathode prior to Zn-ions in low-pH conditions (pH ≤ 3.0). In stark contrast, the influence of protons on the discharge voltage and capacity is insignificant, when either the pH becomes higher (pH ≥ 4.0) or the electrolyte volume is considerably low in coin-type cells. Similar behavior of pH-dependent proton insertion is also verified in Na–, Mg–, and Al-ion electrolytes. Providing a resolution to the controversy regarding proton insertion, the present study emphasizes that the influence of protons substantially varies depending on the pH and relative volume of electrolytes in aqueous batteries. 相似文献
8.
Kuan Wang Haoxiang Zhuo Jiantao Wang Fanny Poon Xueliang Sun Biwei Xiao 《Advanced functional materials》2023,33(13):2212607
Branded with low cost and a high degree of safety, with an ambitious aim of substituting lithium-ion batteries in many fields, sodium-ion batteries have received fervid attention in recent years after being dormant for decades. Layered materials are a major focus of study owing to the extensive experience already gained in lithium-ion batteries, and the pursuit of a Mn-rich composition is critical to reduce the cost while retaining the performance. This review provides a timely update of the recent progress of Mn-rich layered materials for sodium-ion batteries based on the understandings of the phase forming principles, structure transformation upon cycling and charge compensation mechanisms and discusses potential ambiguities in the pursuit of high-performance materials. 相似文献
9.
Xiangyu Meng Yuzhao Liu Le Yu Jieshan Qiu Zhiyu Wang 《Advanced functional materials》2023,33(11):2211062
Anode-free batteries can maximize the energy density but their development is hindered by a lack of Li-rich cathodes for compensating the irreversible Li loss. Li2S cathode is particularly appealing to this desire due to 2.6–4.7 folds more Li content and 4.2–6.8 times higher capacity than conventional intercalation cathodes. But its practical application is hindered by poor stability against moisture attacking in the air. Herein, a facile expendable polymer sheathing strategy toward air-stable Li2S cathodes with high capacities for developing high-performance quasi-solid-state anode-free batteries without risk of cell leakage is reported. Tight protection by dense polymer barrier dramatically prolongs the lifetime of Li2S cathode by 2,000 times at least in the air. Such air-stable Li2S cathode allows for high compatibility of anode-free battery production with commercial schemes. More attractively, the polymer protective layer can in situ transform to multifunctional gel polymer electrolyte for releasing ionic pathways and enhancing cell performance by inhibiting LiPS loss and smoothing Li plating. With air-stable Li2S cathode, the quasi-solid-state anode-free cells are assembled in ambient environment to deliver superb volumetric energy density of 1093 Wh L−1. This study may shed new light to push the commercialization of high-energy and reliable anode-free batteries forward. 相似文献
10.
Zhicheng Wang Ran Han Haiyang Zhang Dan Huang Fengrui Zhang Daosong Fu Yang Liu Yumeng Wei Haiqi Song Yanbin Shen Jingjing Xu Jieyun Zheng Xiaodong Wu Hong Li 《Advanced functional materials》2023,33(24):2215065
Nex-generation high-energy-density storage battery, assembled with lithium (Li)-metal anode and nickel-rich cathode, puts forward urgent demand for advanced electrolytes that simultaneously possess high security, wide electrochemical window, and good compatibility with electrode materials. Herein an intrinsically nonflammable electrolyte is designed by using 1 M lithium difluoro(oxalato)borate (LiDFOB) in triethyl phosphate (TEP) and N-methyl-N-propyl-pyrrolidinium bis(trifluoromethylsulfonyl)imide [Pyr13][TFSI] ionic liquid (IL) solvents. The introduction of IL can bring plentiful organic cations and anions, which provides a cation shielding effect and regulates the Li+ solvation structure with plentiful Li+-DFOB− and Li+-TFSI− complexes. The unique Li+ solvation structure can induce stable anion-derived electrolyte/electrode interphases, which effectively inhibit Li dendrite growth and suppress side reactions between TEP and electrodes. Therefore, the LiNi0.9Co0.05Mn0.05O2 (NCM90)/Li coin cell with this electrolyte can deliver stable cycling even under 4.5 V and 60 °C. Moreover, a Li-metal battery with thick NCM90 cathode (≈ 15 mg cm−2) and thin Li-metal anode (≈ 50 µm) (N/P ≈ 3), also reveals stable cycling performance under 4.4 V. And a 2.2 Ah NCM90/Li pouch cell can simultaneously possess prominent safety with stably passing the nail penetration test, and high gravimetric energy density of 470 Wh kg−1 at 4.4 V. 相似文献