全文获取类型
收费全文 | 5383篇 |
免费 | 1060篇 |
国内免费 | 856篇 |
专业分类
化学 | 2370篇 |
晶体学 | 44篇 |
力学 | 1007篇 |
综合类 | 8篇 |
数学 | 1333篇 |
物理学 | 2537篇 |
出版年
2024年 | 2篇 |
2023年 | 123篇 |
2022年 | 206篇 |
2021年 | 233篇 |
2020年 | 252篇 |
2019年 | 183篇 |
2018年 | 156篇 |
2017年 | 223篇 |
2016年 | 228篇 |
2015年 | 355篇 |
2014年 | 404篇 |
2013年 | 438篇 |
2012年 | 577篇 |
2011年 | 546篇 |
2010年 | 482篇 |
2009年 | 489篇 |
2008年 | 374篇 |
2007年 | 360篇 |
2006年 | 387篇 |
2005年 | 276篇 |
2004年 | 176篇 |
2003年 | 141篇 |
2002年 | 117篇 |
2001年 | 127篇 |
2000年 | 79篇 |
1999年 | 117篇 |
1998年 | 66篇 |
1997年 | 42篇 |
1996年 | 30篇 |
1995年 | 31篇 |
1994年 | 14篇 |
1993年 | 16篇 |
1992年 | 16篇 |
1991年 | 12篇 |
1990年 | 5篇 |
1989年 | 3篇 |
1985年 | 1篇 |
1979年 | 2篇 |
1971年 | 5篇 |
1957年 | 5篇 |
排序方式: 共有7299条查询结果,搜索用时 15 毫秒
51.
Reversible Li Plating on Graphite Anodes through Electrolyte Engineering for Fast-Charging Batteries
Xinyang Yue Jing Zhang Yongteng Dong Yuanmao Chen Zhangqin Shi Xuejiao Xu Xunlu Li Prof. Zheng Liang 《Angewandte Chemie (International ed. in English)》2023,62(19):e202302285
The difficulties to identify the rate-limiting step cause the lithium (Li) plating hard to be completely avoided on graphite anodes during fast charging. Therefore, Li plating regulation and morphology control are proposed to address this issue. Specifically, a Li plating-reversible graphite anode is achieved via a localized high-concentration electrolyte (LHCE) to successfully regulate the Li plating with high reversibility over high-rate cycling. The evolution of solid electrolyte interphase (SEI) before and after Li plating is deeply investigated to explore the interaction between the lithiation behavior and electrochemical interface polarization. Under the fact that Li plating contributes 40 % of total lithiation capacity, the stable LiF-rich SEI renders the anode a higher average Coulombic efficiency (99.9 %) throughout 240 cycles and a 99.95 % reversibility of Li plating. Consequently, a self-made 1.2-Ah LiNi0.5Mn0.3Co0.2O2 | graphite pouch cell delivers a competitive retention of 84.4 % even at 7.2 A (6 C) after 150 cycles. This work creates an ingenious bridge between the graphite anode and Li plating, for realizing the high-performance fast-charging batteries. 相似文献
52.
Ran Li Dr. Fei Yang Liying Zhang Mengzhen Li Dr. Guo Wang Prof. Weizhi Wang Prof. Yanqing Xu Prof. Wei Wei 《Angewandte Chemie (International ed. in English)》2023,62(17):e202301267
Water-soluble small organic photothermal agents (PTAs) over NIR-II biowindow (1000–1350 nm) are highly desirable, but the rarity greatly limits their applications. Based on a water-soluble double-cavity cyclophane GBox-44+ , we report a class of host–guest charge transfer (CT) complexes as structurally uniform PTAs for NIR-II photothermal therapy. As a result of its high electron-deficiency, GBox-44+ can bind different electron-rich planar guests with a 1 : 2 host/guest stoichiometry to readily tune the CT absorption band that extends to the NIR-II region. When using a diaminofluorene guest substituted with an oligoethylene glycol chain, the host–guest system realized both good biocompatibility and enhanced photothermal conversion at 1064 nm, and was then exploited as a high-efficiency NIR-II PTA for cancer cell and bacterial ablation. This work broadens the potential applications of host–guest cyclophane systems and provides a new access to bio-friendly NIR-II photoabsorbers with well-defined structures. 相似文献
53.
Zhenjie Mu Yuhao Zhu Yufeng Zhang Anwang Dong Chunyan Xing Ziru Niu Prof. Dr. Bo Wang Prof. Dr. Xiao Feng 《Angewandte Chemie (International ed. in English)》2023,62(17):e202300373
Pore environment and aggregated structure play a vital role in determining the properties of porous materials, especially regarding the mass transfer. Reticular chemistry imparts covalent organic frameworks (COFs) with well-aligned micro/mesopores, yet constructing hierarchical architectures remains a great challenge. Herein, we reported a COF-to-COF transformation methodology to prepare microtubular COFs. In this process, the C3-symmetric guanidine units decomposed into C2-symmetric hydrazine units, leading to the crystal transformation of COFs. Moreover, the aggregated structure and conversion degree varied with the reaction time, where the hollow tubular aggregates composed of mixed COF crystals could be obtained. Such hierarchical architecture leads to enhanced mass transfer properties, as proved by the adsorption measurement and chemical catalytic reactions. This self-template strategy was successfully applied to another four COFs with different building units. 相似文献
54.
Tianchen Qin Prof. Dr. Dezhou Guo Juanjuan Xiong Xingyu Li Lei Hu Weishan Yang Zijie Chen Yulun Wu Dr. Honghe Ding Dr. Jun Hu Qian Xu Dr. Tao Wang Prof. Dr. Junfa Zhu 《Angewandte Chemie (International ed. in English)》2023,62(43):e202306368
The electrical and mechanical properties of graphene-based materials can be tuned by the introduction of nanopores, which are sensitively related to the size, morphology, density, and location of nanopores. The synthesis of low-dimensional graphene nanostructures containing well-defined nonplanar nanopores has been challenging due to the intrinsic steric hindrance. Herein, we report the selective synthesis of one-dimensional (1D) graphene nanoribbons (GNRs) containing periodic nonplanar [14]annulene pores on Ag(111) and two-dimensional (2D) porous graphene nanosheet containing periodic nonplanar [30]annulene pores on Au(111), starting from a same precursor. The formation of distinct products on the two substrates originates from the different thermodynamics and kinetics of coupling reactions. The reaction mechanisms were confirmed by a series of control experiments, and the appropriate thermodynamic and kinetic parameters for optimizing the reaction pathways were proposed. In addition, the combined scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations revealed the electronic structures of porous graphene structures, demonstrating the impact of nonplanar pores on the π-conjugation of molecules. 相似文献
55.
Yu-Xing Yao Dr. Xiang Chen Nan Yao Jin-Hui Gao Dr. Gang Xu Jun-Fan Ding Chun-Liang Song Dr. Wen-Long Cai Prof. Chong Yan Prof. Qiang Zhang 《Angewandte Chemie (International ed. in English)》2023,62(4):e202214828
Extreme fast charging (XFC) of high-energy Li-ion batteries is a key enabler of electrified transportation. While previous studies mainly focused on improving Li ion mass transport in electrodes and electrolytes, the limitations of charge transfer across electrode–electrolyte interfaces remain underexplored. Herein we unravel how charge transfer kinetics dictates the fast rechargeability of Li-ion cells. Li ion transfer across the cathode–electrolyte interface is found to be rate-limiting during XFC, but the charge transfer energy barrier at both the cathode and anode have to be reduced simultaneously to prevent Li plating, which is achieved through electrolyte engineering. By unlocking charge transfer limitations, 184 Wh kg−1 pouch cells demonstrate stable XFC (10-min charge to 80 %) which is otherwise unachievable, and the lifetime of 245 Wh kg−1 21700 cells is quintupled during fast charging (25-min charge to 80 %). 相似文献
56.
Feini Hao Chao Yang Ximeng Lv Fangshuai Chen Prof. Shengyao Wang Prof. Gengfeng Zheng Prof. Qing Han 《Angewandte Chemie (International ed. in English)》2023,62(50):e202315456
Herein, the exposure of highly-active nitrogen cation sites has been accomplished by photo-driven quasi-topological transformation of a 1,10-phenanthroline-5,6-dione-based covalent organic framework (COF), which contributes to hydrogen peroxide (H2O2) synthesis during the 2-electron O2 photoreduction. The exposed nitrogen cation sites with photo-enhanced Lewis acidity not only act as the electron-transfer motor to adjust the inherent charge distribution, powering continuous and stable charge separation, and broadening visible-light adsorption, but also providing a large number of active sites for O2 adsorption. The optimal catalyst shows a high H2O2 production rate of 11965 μmol g−1 h−1 under visible light irradiation and a remarkable apparent quantum yield of 12.9 % at 400 nm, better than most of the previously reported COF photocatalysts. This work provides new insights for designing photo-switchable nitrogen cation sites as catalytic centers toward efficient solar to chemical energy conversion. 相似文献
57.
Dr. Chi Zhang Dr. Meiling Shao Dr. Dongqing Wu Dr. Zhongyi Li Muzhi Zhao Xiangfei Zhang Prof. Bin Zhai Prof. Yunjun Luo Prof. Xiaoyu Li 《Angewandte Chemie (International ed. in English)》2023,62(52):e202314052
Azide compounds are widely used and especially, polymers bearing pendant azide groups are highly desired in numerous fields. However, harsh reaction conditions are always mandatory to achieve full azidation, causing severe side reactions and degradation of the polymers. Herein, we report the design and preparation of two azide ionic liquids (AILs) with azide anion and triethylene glycol (E3)-containing cation, [P444E3][N3] and [MIME3][N3]. Compared with the traditional sodium azide (NaN3) approach, both AILs showed much higher reaction rates and functional-group tolerance. More importantly, they could act as both reagents and solvents for the quantitative azidation of various polymeric precursors under mild conditions. Theoretical simulations suggested that the outstanding performance of AILs originated from the existence of ion pairs during the reaction, and the E3 moieties played a crucial role. Lastly, after the reaction, the AILs could be easily regenerated, presenting a safer, greener, and highly efficient synthesis route for azide polymers. 相似文献
58.
Using cheap n‐butylamine as template, ZSM‐5 zeolites have been successfully synthesized and coated on monolithic interconnected macroporous Al2O3 by the secondary growth method. The use of cheap n‐butylamine could significantly reduce the synthesis cost. Hierarchical monolithic ZSM‐5 zeolites were prepared from synthetic mixtures with different H2O/Na2O or SiO2/Al2O3 ratio. The synthesized samples were characterized by scanning electron microscopy (SEM), X‐ray diffraction (XRD), Fourier transform infrared spectroscopy (FT‐IR) and N2 adsorption‐desorption. The results show that the hierarchical monolithic zeolites were obtained with cheap n‐butylamine template as template. During the hydrothermal reaction process, the morphology of the micrometer‐sized support was well maintained. The irregular crystals were formed in a wide range of the H2O/Na2O or SiO2/Al2O3 ratio of synthetic mixtures and coated on monolithic Al2O3. The relative crystallinity of the zeolites was highest at H2O/Na2O=250 or SiO2/Al2O3=160. This type of composites exhibited hierarchical porous structures and relatively high specific surface areas. 相似文献
59.
Yahui Zhang Lingwei Kong Jianbing Shi Bin Tong Junge Zhi Xiao Feng Yuping Dong 《中国化学》2015,33(7):701-704
A new type of AIE molecules based on hexaphenyl‐1,3‐butadienes was reported with respect to the synthesis and characterization. This material exhibited different maximum emission wavelength and enhanced emission intensity at different aggregate state (amorphous and crystalline state). 相似文献
60.
MoS2 Nanosheets Supported on 3D Graphene Aerogel as a Highly Efficient Catalyst for Hydrogen Evolution 下载免费PDF全文
Yufei Zhao Xiuqiang Xie Jinqiang Zhang Dr. Hao Liu Hyo‐Jun Ahn Prof. Kening Sun Prof. Guoxiu Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(45):15908-15913
The development of efficient catalysts for electrochemical hydrogen evolution is essential for energy conversion technologies. Molybdenum disulfide (MoS2) has emerged as a promising electrocatalyst for hydrogen evolution reaction, and its performance greatly depends on its exposed edge sites and conductivity. Layered MoS2 nanosheets supported on a 3D graphene aerogel network (GA‐MoS2) exhibit significant catalytic activity in hydrogen evolution. The GA‐MoS2 composite displays a unique 3D architecture with large active surface areas, leading to high catalytic performance with low overpotential, high current density, and good stability. 相似文献