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101.
Wenkai Lin Yu Liu Jinhui Wang Zhennan Zhao Kai Lu He Meng Ruiqi Luoliu Xiaojun He Jianliang Shen Zong-Wan Mao Wei Xia 《Angewandte Chemie (International ed. in English)》2023,62(43):e202310158
Despite metal-based photosensitizers showing great potential in photodynamic therapy for tumor treatment, the application of the photosensitizers is intrinsically limited by their poor cancer-targeting properties. Herein, we reported a metal-based photosensitizer-bacteria hybrid, Ir-HEcN , via covalent labeling of an iridium(III) photosensitizer to the surface of genetically engineered bacteria. Due to its intrinsic self-propelled motility and hypoxia tropism, Ir-HEcN selectively targets and penetrates deeply into tumor tissues. Importantly, Ir-HEcN is capable of inducing pyroptosis and immunogenic cell death of tumor cells under irradiation, thereby remarkably evoking anti-tumor innate and adaptive immune responses in vivo and leading to the regression of solid tumors via combinational photodynamic therapy and immunotherapy. To the best of our knowledge, Ir-HEcN is the first metal complex decorated bacteria for enhanced photodynamic immunotherapy. 相似文献
102.
Yibo Wang Pengyu Meng Zhaohui Yang Dr. Min Jiang Dr. Jian Yang Dr. Huanxin Li Prof. Jiao Zhang Prof. Baode Sun Prof. Chaopeng Fu 《Angewandte Chemie (International ed. in English)》2023,62(28):e202304229
Highly-active and low-cost bifunctional electrocatalysts for oxygen reduction and evolution are essential in rechargeable metal-air batteries, and single atom catalysts with Fe−N−C are promising candidates. However, the activity still needs to be boosted, and the origination of spin-related oxygen catalytic performance is still uncertain. Herein, an effective strategy to regulate local spin state of Fe−N−C through manipulating crystal field and magnetic field is proposed. The spin state of atomic Fe can be regulated from low spin to intermediate spin and to high spin. The cavitation of dxz and dyz orbitals of high spin FeIII can optimize the O2 adsorption and promote the rate-determining step (*O2 to *OOH). Benefiting from these merits, the high spin Fe−N−C electrocatalyst displays the highest oxygen electrocatalytic activities. Furthermore, the high spin Fe−N−C-based rechargeable zinc-air battery displays a high power density of 170 mW cm−2 and good stability. 相似文献
103.
Qingchun Xu Puning Ren Yang Peng Prof. Nengchao Luo Zhuyan Gao Caixia Meng Jian Zhang Prof. Feng Wang 《Angewandte Chemie (International ed. in English)》2023,62(30):e202301668
Photocatalytic 2-iodoethanol (IEO) coupling provides 1,4-butanediol (BDO) of particular interest to produce degradable polyesters. However, the reduction potential of IEO is too negative (−1.9 vs NHE) to be satisfied by most of the semiconductors, and the kinetics of transferring one electron for IEO coupling is slow. Here we design a catalytic Ni complex, which works synergistically with TiO2, realizing reductive coupling of IEO powered by photo-energy. Coordinating by terpyridine stabilizes Ni2+ from being photo-deposited to TiO2, thereby retaining the steric configuration beneficial for IEO coupling. The Ni complex can rapidly extract electrons from TiO2, generating a low-valent Ni capable of reducing IEO. The photocatalytic IEO coupling thus provides BDO in 72 % selectivity. By a stepwise procedure, BDO is obtained with 70 % selectivity from ethylene glycol. This work put forward a strategy for the photocatalytic reduction of molecules requiring strong negative potential. 相似文献
104.
Dr. Xianzhong Yang Weiping Li Ziyan Chen Dr. Meng Tian Jun Peng Jinrong Luo Yiwen Su Yuhan Zou Gao Weng Prof. Yuanlong Shao Prof. Shixue Dou Prof. Jingyu Sun 《Angewandte Chemie (International ed. in English)》2023,62(10):e202218454
Despite conspicuous merits of Zn metal anodes, the commercialization is still handicapped by rampant dendrite formation and notorious side reaction. Manipulating the nucleation mode and deposition orientation of Zn is a key to rendering stabilized Zn anodes. Here, a dual electrolyte additive strategy is put forward via the direct cooperation of xylitol (XY) and graphene oxide (GO) species into typical zinc sulfate electrolyte. As verified by molecular dynamics simulations, the incorporated XY molecules could regulate the solvation structure of Zn2+, thus inhibiting hydrogen evolution and side reactions. The self-assembled GO layer is in favor of facilitating the desolvation process to accelerate reaction kinetics. Progressive nucleation and orientational deposition can be realized under the synergistic modulation, enabling a dense and uniform Zn deposition. Consequently, symmetric cell based on dual additives harvests a highly reversible cycling of 5600 h at 1.0 mA cm−2/1.0 mAh cm−2. 相似文献
105.
Xiao-Yu Li Dr. Tao Wang Yu-Chen Cai Zhao-Dong Meng Jing-Wen Nan Dr. Jin-Yu Ye Prof. Dr. Jun Yi Prof. Dr. Dong-Ping Zhan Prof. Dr. Na Tian Prof. Dr. Zhi-You Zhou Prof. Dr. Shi-Gang Sun 《Angewandte Chemie (International ed. in English)》2023,62(14):e202218669
Proton transfer is crucial for electrocatalysis. Accumulating cations at electrochemical interfaces can alter the proton transfer rate and then tune electrocatalytic performance. However, the mechanism for regulating proton transfer remains ambiguous. Here, we quantify the cation effect on proton diffusion in solution by hydrogen evolution on microelectrodes, revealing the rate can be suppressed by more than 10 times. Different from the prevalent opinions that proton transport is slowed down by modified electric field, we found water structure imposes a more evident effect on kinetics. FTIR test and path integral molecular dynamics simulation indicate that proton prefers to wander within the hydration shell of cations rather than to hop rapidly along water wires. Low connectivity of water networks disrupted by cations corrupts the fast-moving path in bulk water. This study highlights the promising way for regulating proton kinetics via a modified water structure. 相似文献
106.
Pengzhou Li Dr. Meng Liao Dr. Shuquan Cui Jiaxin Li Dr. Lei Ye Yibei Yang Chuang Wang Prof. Bingjie Wang Prof. Huisheng Peng 《Angewandte Chemie (International ed. in English)》2023,62(17):e202300705
Flexible batteries based on gel electrolytes with high safety are promising power solutions for wearable electronics but suffer from vulnerable electrode-electrolyte interfaces especially upon complex deformations, leading to irreversible capacity loss or even battery collapse. Here, a supramolecular sol-gel transition electrolyte (SGTE) that can dynamically accommodate deformations and repair electrode-electrolyte interfaces through its controllable rewetting at low temperatures is designed. Mediated by the micellization of polypropylene oxide blocks in Pluronic and host-guest interactions between α-cyclodextrin (α-CD) and polyethylene oxide blocks, the high ionic conductivity and compatibility with various salts of SGTE afford resettable electrode-electrolyte interfaces and thus constructions of a series of highly durable, flexible aqueous zinc batteries. The design of this novel gel electrolyte provides new insights for the development of flexible batteries. 相似文献
107.
Weijie Yu Shengchun Wang Meng He Zhou Jiang Yi Yu Jinping Lan Jin Luo Pengjie Wang Prof. Xiaotian Qi Prof. Tao Wang Prof. Aiwen Lei 《Angewandte Chemie (International ed. in English)》2023,62(17):e202219166
Precisely introducing two similar functional groups into bulk chemical alkenes represents a formidable route to complex molecules. Especially, the selective activation of two electrophiles is in crucial demand, yet challenging for cross-electrophile-coupling. Herein, we demonstrate a redox-mediated electrolysis, in which aryl nitriles are both aryl radical precursors and redox-mediators, enables an intermolecular alkene 1,2-diarylation with a remarkable regioselectivity, thereby avoiding the involvement of transition-metal catalysts. This transformation utilizes cyanoarene radical anions for activating various aryl halides (including iodides, bromides, and even chlorides) and affords 1,2-diarylation adducts in up to 83 % yield and >20 : 1 regioselectivity with more than 80 examples, providing a feasible approach to complex bibenzyl derivatives. 相似文献
108.
Xinlin Huang Chuang Wang Dr. Chuanfa Li Dr. Meng Liao Jiaxin Li Haibo Jiang Yao Long Xiangran Cheng Kun Zhang Pengzhou Li Prof. Bingjie Wang Prof. Huisheng Peng 《Angewandte Chemie (International ed. in English)》2023,62(24):e202303616
Fiber lithium-ion batteries represent a promising power strategy for the rising wearable electronics. However, most fiber current collectors are solid with vastly increased weights of inactive materials and sluggish charge transport, thus resulting in low energy densities which have hindered the development of fiber lithium-ion batteries in the past decade. Here, a braided fiber current collector with multiple channels was prepared by multi-axial winding method to not only increase the mass fraction of active materials, but also to promote ion transport along fiber electrodes. In comparison to typical solid copper wires, the braided fiber current collector hosted 139 % graphite with only 1/3 mass. The fiber graphite anode with braided current collector delivered high specific capacity of 170 mAh g−1 based on the overall electrode weight, which was 2 times higher than that of its counterpart solid copper wire. The resulting fiber battery showed high energy density of 62 Wh kg−1. 相似文献
109.
Hongyuan Zhao Qiujie Wang Ziying Wen Haibo Sun Sujun Ji Xuan Meng Ruiling Zhang Junke Jiang Zhe Tang Feng Liu 《Angewandte Chemie (International ed. in English)》2023,62(52):e202316336
The achievement of significant photoluminescence (PL) in lanthanide ions (Ln3+) has primarily relied on host sensitization, where energy is transferred from the excited host material to the Ln3+ ions. However, this luminous mechanism involves only one optical antenna, namely the host material, which limits the accessibility of excitation wavelength-dependent (Ex-De) PL. Consequently, the wider application of Ln3+ ions in light-emitting devices is hindered. In this study, we present an organic–inorganic compound, (DMA)4LnCl7 (DMA+=[CH3NH2CH3]+, Ln3+=Ce3+, Tb3+), which serves as an independent host lattice material for efficient Ex-De emission by doping it with trivalent antimony (Sb3+). The pristine (DMA)4LnCl7 compounds exhibit high luminescence, maintaining the characteristic sharp emission bands of Ln3+ and demonstrating a high PL quantum yield of 90–100 %. Upon Sb3+ doping, the compound exhibits noticeable Ex-De emission with switchable colors. Through a detailed spectral study, we observe that the prominent energy transfer process observed in traditional host-sensitized systems is absent in these materials. Instead, they exhibit two independent emission centers from Ln3+ and Sb3+, each displaying distinct features in luminous color and radiative lifetime. These findings open up new possibilities for designing Ex-De emitters based on Ln3+ ions. 相似文献
110.
Meiyun Su Lina Guo Peiyu Mao Meng Xiao Prof. Dr. Wenjie Liu Prof. Dr. Shaohua Wang 《European journal of organic chemistry》2023,26(29):e202300268
The catalyst-free electrochemical halogenation and trifluoromethylation of 4H-pyrido[1,2-a]pyrimidin-4-ones was realized under external-oxidant-free conditions. This strategy provides an easy and green access to functionalized new 4H-pyrido[1,2-a]pyrimidin-4-one derivatives with broad scope, good functional group tolerance and high regioselectivity. 相似文献