全文获取类型
收费全文 | 2268篇 |
免费 | 473篇 |
国内免费 | 359篇 |
专业分类
化学 | 1055篇 |
晶体学 | 5篇 |
力学 | 239篇 |
综合类 | 29篇 |
数学 | 993篇 |
物理学 | 779篇 |
出版年
2024年 | 13篇 |
2023年 | 54篇 |
2022年 | 106篇 |
2021年 | 118篇 |
2020年 | 162篇 |
2019年 | 133篇 |
2018年 | 118篇 |
2017年 | 113篇 |
2016年 | 146篇 |
2015年 | 121篇 |
2014年 | 169篇 |
2013年 | 209篇 |
2012年 | 154篇 |
2011年 | 141篇 |
2010年 | 94篇 |
2009年 | 114篇 |
2008年 | 118篇 |
2007年 | 101篇 |
2006年 | 135篇 |
2005年 | 89篇 |
2004年 | 78篇 |
2003年 | 60篇 |
2002年 | 75篇 |
2001年 | 67篇 |
2000年 | 46篇 |
1999年 | 46篇 |
1998年 | 51篇 |
1997年 | 45篇 |
1996年 | 38篇 |
1995年 | 27篇 |
1994年 | 24篇 |
1993年 | 17篇 |
1992年 | 19篇 |
1991年 | 14篇 |
1990年 | 12篇 |
1989年 | 14篇 |
1988年 | 3篇 |
1987年 | 3篇 |
1986年 | 6篇 |
1985年 | 5篇 |
1984年 | 5篇 |
1983年 | 7篇 |
1982年 | 8篇 |
1981年 | 3篇 |
1980年 | 4篇 |
1979年 | 4篇 |
1978年 | 3篇 |
1977年 | 3篇 |
1976年 | 2篇 |
1975年 | 2篇 |
排序方式: 共有3100条查询结果,搜索用时 46 毫秒
101.
Construction of Shallow Surface States through Light Ni Doping for High‐Efficiency Photocatalytic Hydrogen Production of CdS Nanocrystals
下载免费PDF全文
![点击此处可从《Chemistry (Weinheim an der Bergstrasse, Germany)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Shuo Li Lijing Zhang Tengfei Jiang Liping Chen Prof.Dr. Yanhong Lin Prof. Dr. Dejun Wang Prof. Dr. Tengfeng Xie 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(1):311-316
Ni‐doped CdS nanowires were synthesized by a simple one‐step method. X‐ray diffraction, X‐ray photoelectron spectroscopy, and photoluminescence spectroscopy confirmed that light Ni doping can form shallow surface states due to the presence of substitutional Ni ions, and heavy Ni doping can form deep surface states due to the presence of interstitial Ni ions. Surface photovoltage spectroscopy and transient photovoltage measurements revealed that the shallow surface states can prolong the lifetime of the photogenerated charge carriers, whereas the deep surface states lead to recombination of the photogenerated charge carriers. The relationship between different surface states and the photocatalytic performance of CdS nanocrystals are discussed. The enhanced density of shallow surface states due to light Ni doping significantly promotes photocatalytic H2 production. 相似文献
102.
Dr. Jungki Ryu Dong Heon Nam Dr. Sahng Ha Lee Prof.Dr. Chan Beum Park 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(38):12020-12025
Efficient harvesting of unlimited solar energy and its conversion into valuable chemicals is one of the ultimate goals of scientists. With the ever‐increasing concerns about sustainable growth and environmental issues, numerous efforts have been made to develop artificial photosynthetic process for the production of fuels and fine chemicals, thus mimicking natural photosynthesis. Despite the research progress made over the decades, the technology is still in its infancy because of the difficulties in kinetic coupling of whole photocatalytic cycles. Herein, we report a new type of artificial photosynthesis system that can avoid such problems by integrally coupling biocatalytic redox reactions with photocatalytic water splitting. We found that photocatalytic water splitting can be efficiently coupled with biocatalytic redox reactions by using tetracobalt polyoxometalate and Rh‐based organometallic compound as hole and electron scavengers, respectively, for photoexcited [Ru(bpy)3]2+. Based on these results, we could successfully photosynthesize a model chiral compound (L ‐glutamate) using a model redox enzyme (glutamate dehydrogenase) upon in situ photoregeneration of cofactors. 相似文献
103.
Craig J. Richmond Roc Matheu Dr. Albert Poater Dr. Laura Falivene Dr. Jordi Benet‐Buchholz Dr. Xavier Sala Prof. Luigi Cavallo Prof. Antoni Llobet 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(52):17282-17286
Extremely slow and extremely fast new water oxidation catalysts based on the Ru–bda (bda=2,2′‐bipyridine‐6,6′‐dicarboxylate) systems are reported with turnover frequencies in the range of 1 and 900 cycles s?1, respectively. Detailed analyses of the main factors involved in the water oxidation reaction have been carried out and are based on a combination of reactivity tests, electrochemical experiments, and DFT calculations. These analyses give a convergent interpretation that generates a solid understanding of the main factors involved in the water oxidation reaction, which in turn allows the design of catalysts with very low energy barriers in all the steps involved in the water oxidation catalytic cycle. We show that for this type of system π‐stacking interactions are the key factors that influence reactivity and by adequately controlling them we can generate exceptionally fast water oxidation catalysts. 相似文献
104.
A Cost‐Effective 3D Hydrogen Evolution Cathode with High Catalytic Activity: FeP Nanowire Array as the Active Phase
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Dr. Ping Jiang Qian Liu Yanhui Liang Dr. Jingqi Tian Prof. Abdullah M. Asiri Prof. Xuping Sun 《Angewandte Chemie (International ed. in English)》2014,53(47):12855-12859
Iron is the cheapest and one of the most abundant transition metals. Natural [FeFe]‐hydrogenases exhibit remarkably high activity in hydrogen evolution, but they suffer from high oxygen sensitivity and difficulty in scale‐up. Herein, an FeP nanowire array was developed on Ti plate (FeP NA/Ti) from its β‐FeOOH NA/Ti precursor through a low‐temperature phosphidation reaction. When applied as self‐supported 3D hydrogen evolution cathode, the FeP NA/Ti electrode shows exceptionally high catalytic activity and good durability, and it only requires overpotentials of 55 and 127 mV to afford current densities of 10 and 100 mA cm2, respectively. The excellent electrocatalytic performance is promising for applications as non‐noble‐metal HER catalyst with a high performance–price ratio in electrochemical water splitting for large‐scale hydrogen fuel production. 相似文献
105.
Photocatalytic Water Oxidation by a Pyrochlore Oxide upon Irradiation with Visible Light: Rhodium Substitution Into Yttrium Titanate
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Borbala Kiss Dr. Christophe Didier Timothy Johnson Dr. Troy D. Manning Dr. Matthew S. Dyer Dr. Alexander J. Cowan Dr. John B. Claridge Prof. James R. Darwent Prof. Matthew J. Rosseinsky 《Angewandte Chemie (International ed. in English)》2014,53(52):14480-14484
A stable visible‐light‐driven photocatalyst (λ≥450 nm) for water oxidation is reported. Rhodium substitution into the pyrochlore Y2Ti2O7 is demonstrated by monitoring Vegard′s law evolution of the unit‐cell parameters with changing rhodium content, to a maximum content of 3 % dopant. Substitution renders the solid solutions visible‐light active. The overall rate of oxygen evolution is comparable to WO3 but with superior light‐harvesting and surface‐area‐normalized turnover rates, making Y2Ti1.94Rh0.06O7 an excellent candidate for use in a Z‐scheme water‐splitting system. 相似文献
106.
Nanocomposites of Tantalum‐Based Pyrochlore and Indium Hydroxide Showing High and Stable Photocatalytic Activities for Overall Water Splitting and Carbon Dioxide Reduction
下载免费PDF全文
![点击此处可从《Angewandte Chemie (International ed. in English)》网站下载免费的PDF全文](/ch/ext_images/free.gif)
Meng‐Chun Hsieh Guan‐Chang Wu Dr. Wei‐Guang Liu Prof. William A. Goddard III Prof. Dr. Chia‐Min Yang 《Angewandte Chemie (International ed. in English)》2014,53(51):14216-14220
Nanocomposites of tantalum‐based pyrochlore nanoparticles and indium hydroxide were prepared by a hydrothermal process for UV‐driven photocatalytic reactions including overall water splitting, hydrogen production from photoreforming of methanol, and CO2 reduction with water to produce CO. The best catalyst was more than 20 times more active than sodium tantalate in overall water splitting and 3 times more active than Degussa P25 TiO2 in CO2 reduction. Moreover, the catalyst was very stable while generating stoichiometric products of H2 (or CO) and O2 throughout long‐term photocatalytic reactions. After the removal of In(OH)3, the pyrochlore nanoparticles remained highly active for H2 production from pure water and aqueous methanol solution. Both experimental studies and density functional theory calculations suggest that the pyrochlore nanoparticles catalyzed the water reduction to produce H2, whereas In(OH)3 was the major active component for water oxidation to produce O2. 相似文献
107.
Min Wang Jia-Qi Wang Cong Xi Chuan-Qi Cheng Cheng-Qin Zou Rui Zhang Ya-Meng Xie Zhong-Lu Guo Prof. Cheng-Chun Tang Dr. Cun-Ku Dong Prof. Yong-Jun Chen Prof. Xi-Wen Du 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(28):11607-11612
Developing highly efficient and low-cost photocatalysts for overall water splitting has long been a pursuit for converting solar power into clean hydrogen energy. Herein, we demonstrate that a nonstoichiometric nickel–cobalt double hydroxide can achieve overall water splitting by itself upon solar light irradiation, avoiding the consumption of noble-metal co-catalysts. We employed an intensive laser to ablate a NiCo alloy target immersed in alkaline solution, and produced so-called L-NiCo nanosheets with a nonstoichiometric composition and O2−/Co3+ ions exposed on the surface. The nonstoichiometric composition broadens the band gap, while O2− and Co3+ ions boost hydrogen and oxygen evolution, respectively. As such, the photocatalyst achieves a H2 evolution rate of 1.7 μmol h−1 under AM 1.5G sunlight irradiation and an apparent quantum yield (AQE) of 1.38 % at 380 nm. 相似文献
108.
Dr. Linzhou Zhuang Dr. Yi Jia Hongli Liu Zhiheng Li Dr. Mengran Li Dr. Longzhou Zhang Dr. Xin Wang Prof. Dongjiang Yang Prof. Zhonghua Zhu Prof. Xiangdong Yao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14772-14778
The oxygen vacancies of defective iron–cobalt oxide (FeCoOx-Vo) nanosheets are modified by the homogeneously distributed sulfur (S) atoms. S atoms can not only effectively stabilize oxygen vacancies (Vo), but also form the Co−S coordination with Co active site in the Vo, which can modulate the electronic structure of the active site, enabling FeCoOx-Vo-S to exhibit much superior OER activity. FeCoOx-Vo-S exhibits a mass activity of 2440.0 A g−1 at 1.5 V vs. RHE in 1.0 m KOH, 25.4 times higher than that of RuO2. The Tafel slope is as low as 21.0 mV dec−1, indicative of its excellent charge transfer rate. When FeCoOx-Vo-S (anode catalyst) is paired with the defective CoP3/Ni2P (cathode catalyst) for overall water splitting, current densities of as high as 249.0 mA cm−2 and 406.0 mA cm−2 at a cell voltage of 2.0 V and 2.3 V, respectively, can be achieved. 相似文献
109.
Jin Su Takashi Hisatomi Tsutomu Minegishi Kazunari Domen 《Angewandte Chemie (International ed. in English)》2020,59(33):13800-13806
Most CdTe photoanodes and photocathodes show positive and negative photocurrent onset potentials for water oxidation and reduction, respectively, and are thus unable to drive photoelectrochemical (PEC) water splitting without external applied biases. Herein, the activity of a CdTe photoanode having an internal p‐n junction during PEC water oxidation was enhanced by applying a CdCl2 annealing treatment together with surface modifications. The resulting CdTe photoanode generated photocurrents of 1.8 and 5.4 mA cm?2 at 0.6 and 1.2 VRHE, respectively, with a photoanodic current onset potential of 0.22 VRHE under simulated sunlight (AM 1.5G). The CdCl2 annealing increased the grain sizes and lowered the density of grain boundaries, allowing more efficient charge separation. Consequently, a two‐electrode tandem PEC cell comprising a CdTe‐based photoanode and photocathode split water without any external bias at a solar‐to‐hydrogen conversion efficiency of 0.51 % at the beginning of the reaction. 相似文献
110.
Shijia Feng Tuo Wang Bin Liu Congling Hu Lulu Li Zhi‐Jian Zhao Jinlong Gong 《Angewandte Chemie (International ed. in English)》2020,59(5):2044-2048
A facile photoetching approach is described that alleviates the negative effects from bulk defects by confining the oxygen vacancy (Ovac) at the surface of BiVO4 photoanode, by 10‐minute photoetching. This strategy could induce enriched Ovac at the surface of BiVO4, which avoids the formation of excessive bulk defects. A mechanism is proposed to explain the enhanced charge separation at the BiVO4 /electrolyte interface, which is supported by density functional theory (DFT) calculations. The optimized BiVO4 with enriched surface Ovac presents the highest photocurrent among undoped BiVO4 photoanodes. Upon loading FeOOH/NiOOH cocatalysts, photoetched BiVO4 photoanode reaches a considerable water oxidation photocurrent of 3.0 mA cm?2 at 0.6 V vs. reversible hydrogen electrode. An unbiased solar‐to‐hydrogen conversion efficiency of 3.5 % is realized by this BiVO4 photoanode and a Si photocathode under 1 sun illumination. 相似文献