全文获取类型
收费全文 | 4439篇 |
免费 | 689篇 |
国内免费 | 1044篇 |
专业分类
化学 | 3957篇 |
晶体学 | 19篇 |
力学 | 118篇 |
综合类 | 116篇 |
数学 | 732篇 |
物理学 | 1230篇 |
出版年
2024年 | 5篇 |
2023年 | 272篇 |
2022年 | 194篇 |
2021年 | 180篇 |
2020年 | 345篇 |
2019年 | 231篇 |
2018年 | 133篇 |
2017年 | 158篇 |
2016年 | 154篇 |
2015年 | 141篇 |
2014年 | 478篇 |
2013年 | 447篇 |
2012年 | 345篇 |
2011年 | 420篇 |
2010年 | 327篇 |
2009年 | 374篇 |
2008年 | 284篇 |
2007年 | 211篇 |
2006年 | 159篇 |
2005年 | 160篇 |
2004年 | 116篇 |
2003年 | 140篇 |
2002年 | 115篇 |
2001年 | 112篇 |
2000年 | 92篇 |
1999年 | 99篇 |
1998年 | 72篇 |
1997年 | 77篇 |
1996年 | 55篇 |
1995年 | 60篇 |
1994年 | 38篇 |
1993年 | 37篇 |
1992年 | 27篇 |
1991年 | 22篇 |
1990年 | 19篇 |
1989年 | 7篇 |
1988年 | 11篇 |
1987年 | 10篇 |
1986年 | 4篇 |
1985年 | 21篇 |
1984年 | 2篇 |
1983年 | 4篇 |
1982年 | 2篇 |
1980年 | 1篇 |
1979年 | 1篇 |
1978年 | 3篇 |
1976年 | 1篇 |
1975年 | 1篇 |
1974年 | 2篇 |
1959年 | 3篇 |
排序方式: 共有6172条查询结果,搜索用时 15 毫秒
1.
Hanghang Zhou Dr. Ying Luo Dr. Jun Xu Dr. Lidan Deng Prof. Dr. Zheng Wang Prof. Dr. Hong He 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(68):e202202044
Cubic-like CaTaO2N photocatalysts with high crystallinity and uniform particle size were successfully prepared by the flux-assisted nitridation method. The growth of CaTaO2N single crystals under different synthesis conditions was systematically investigated to understand the effects of the crystallinity and optical property on photocatalytic performance of CO2 reduction. Moreover, the modification of CaTaO2N single crystals with core-shell Ni−Ag bicomponent cocatalyst by two-step decoration process gave a 2.4 times higher amount of CO evolution than the deposition of sole Ag cocatalyst, because of the synergistic effects of bicomponent cocatalyst on the interfacial electron transfer and surface catalytic process. This study provides a valuable way to construct high-crystalline photocatalysts with effective bicomponent cocatalyst for visible-light-driven CO2 reduction with H2O. 相似文献
2.
Photocatalytic CO2 reduction to C1 fuels is considered to be an important way for alleviating increasingly serious energy crisis and environmental pollution. Due to the environment-friendly, simple preparation, easy formation of highly-stable metal-nitrogen(M-Nx) coordination bonds, and suitable band structure, polymeric carbon nitride-based single-atom catalysts(C3N4-based SACs) are expected to become a potential for CO2 reduction under visible-light irradiation. In this review, we summarize the recent advancement on C3N4-based SACs for photocatalytic CO2 reduction to C1 products, including the reaction mechanism for photocatalytic CO2 reduction to C1 products, the structure and synthesis methods of C3N4-based SACs and their applications toward photocatalytic CO2 reduction reaction(CO2RR) for C1 production. The current challenges and future opportunities of C3N4-based SACs for photoreduction of CO2 are also discussed. 相似文献
3.
Dong Gun Oh Prof. Hristiyan A. Aleksandrov Haneul Kim Dr. Iskra Z. Koleva Dr. Konstantin Khivantsev Prof. Georgi N. Vayssilov Prof. Ja Hun Kwak 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(49):e202200684
Pd-based catalysts are the most widely used for CO oxidation because of their outstanding catalytic activity and thermal stability. However, fundamental understanding of the detailed catalytic processes occurring on Pd-based catalysts under realistic conditions is still lacking. In this study, we investigated CO oxidation on metallic Pd clusters supported on Al2O3 and SiO2. High-angle annular dark-field scanning transmission electron microscopy revealed the formation of similar-sized Pd clusters on Al2O3 and SiO2. In contrast, CO chemisorption analysis indicated a gradual change in the dispersion of Pd (from 0.79 to 0.2) on Pd/Al2O3 and a marginal change in the dispersion (from 0.4 to 0.24) on Pd/SiO2 as the Pd loading increased from 0.27 to 5.5 wt %; these changes were attributed to differences in the metal-support interactions. Diffuse reflectance infrared Fourier-transform spectroscopy revealed that fewer a-top CO species were present in Pd supported on Al2O3 than those in Pd supported on SiO2, which is related to the morphological differences in the metallic Pd clusters on these two supports. Despite the different dispersion profiles and surface characteristics of Pd, O2 titration demonstrated that linearly bound CO (with an infrared signal at 2090 cm−1) reacted first with oxygen in the case of CO-saturated Pd on Al2O3 and SiO2, which suggests that a-top CO on the terrace site plays an important role in CO oxidation. The experimental observations were corroborated by periodic density functional calculations, which confirmed that CO oxidation on the (111) terrace sites is most plausible, both kinetically and thermodynamically, compared to that on the edge or corner sites. This study will deepen the fundamental understanding of the effect of Pd clusters on CO oxidation under reaction conditions. 相似文献
4.
By using angle resolved photoemission spectroscopy, we investigate the electronic structures of Pt-skin layer of Pt–Co and Pt–Ni alloys with CO molecules on the surface. Measured Fermi surface maps and band dispersions reflect the signatures of chemical bonding between Pt-skin layer and CO molecules. Furthermore, the degree of chemical bonding strength of CO molecules, estimated from the energy shift of the participating bands, is found to be reduced on both Pt bimetallic alloys. Our results show how the surface band structure of Pt bimetallic alloys is modified with molecular orbitals of CO molecules on the surface, revealing the important role of the electronic structure in the determination of chemical properties of bimetallic alloys. 相似文献
5.
6.
以氧化石墨烯为载体,单原子铂(Pt)为活性组分,利用化学还原法制备了单原子Pt/rGO催化剂,用在催化氧化一氧化碳(CO)反应中。通过透射电子显微镜、扫描电子显微镜、球差电镜、傅里叶红外光谱仪对单原子Pt催化剂进行表征。考察了金属负载量、反应温度对催化剂性能的影响,利用气相色谱对CO氧化反应性能进行评价。此次实验包含催化剂的制备、表征和性能测试,实验难度适中,贴近科研前沿,可以让学生体验一个综合的科研过程,激发学生的科研兴趣,培养学生的科研能力。 相似文献
7.
构建了CO高压溶解的进气系统,在连续式反应系统中对超临界水条件下CO的转化规律进行了研究;针对生物质超临界水气化中钾盐的多样性,选择KHCO3、K2CO3和KOH等三种钾盐成分,研究了它们在不同工艺条件(450-600℃、23-29 MPa、停留时间3-6 s)下对超临界水中水煤气转化过程的影响。结果表明,在无催化条件下,提高反应温度、延长停留时间均提高了CO的转化率,而压力对其影响在低压下(23-25 MPa)比较大,高压下(25-29 MPa)比较小,水煤气转化的反应动力学方程为k=103.75×exp(-0.66×105/RT)(s-1)。碱性钾盐均能显著提高CO转化率,其催化促进程度从大到小依次为:KHCO3>K2CO3>KOH。添加碱性钾盐时,提高反应温度、延长停留时间均提高CO转化率,而压力的影响比较复杂。碱性盐对水煤气转化反应的催化是通过草酸盐(HC2O4-)和甲酸盐(HCOO-)作为中间产物进行的。 相似文献
8.
Hongjian Yu Jieyuan Li Yihe Zhang Songqiu Yang Keli Han Fan Dong Tianyi Ma Hongwei Huang 《Angewandte Chemie (International ed. in English)》2019,58(12):3880-3884
A facile and controllable in situ reduction strategy is used to create surface oxygen vacancies (OVs) on Aurivillius‐phase Sr2Bi2Nb2TiO12 nanosheets, which were prepared by a mineralizer‐assisted soft‐chemical method. Introduction of OVs on the surface of Sr2Bi2Nb2TiO12 extends photoresponse to cover the whole visible region and also tremendously promotes separation of photoinduced charge carriers. Adsorption and activation of CO2 molecules on the surface of the catalyst are greatly enhanced. In the gas‐solid reaction system without co‐catalysts or sacrificial agents, OVs‐abundant Sr2Bi2Nb2TiO12 nanosheets show outstanding CO2 photoreduction activity, producing CO with a rate of 17.11 μmol g?1 h?1, about 58 times higher than that of the bulk counterpart, surpassing most previously reported state‐of‐the‐art photocatalysts. Our study provides a three‐in‐one integrated solution to advance the performance of photocatalysts for solar‐energy conversion and generation of renewable energy. 相似文献
9.
Abdillah Sani Bin Mohd Najib Xiaobo Peng Ayako Hashimoto Shusaku Shoji Takayuki Iida Yunxing Bai Hideki Abe 《化学:亚洲杂志》2019,14(16):2802-2805
Mesoporous precious metals with abundant active sites and high surface area have been widely recognized as high‐performance catalytic materials. However, the templated synthesis is complex and costly. Herein, we report a mesoporous rhodium (m‐Rh) that can be readily synthesized from entangled nanofibres of Rh and Y2O3 without templates. The entangled nanofibres, prepared from uniform Rh‐Y alloys under redox atmosphere, were the key precursor in the synthesis processes. Moreover, the m‐Rh efficiently catalyzed carbon dioxide reforming of methane (DRM) at a low reaction temperature of 683 K. Further, electrochemical methods of CO electro‐oxidation were innovatively used to demonstrate the stability of CO and oxygen species for the DRM reaction. 相似文献
10.
固体氧化物电解池可高效地电解H2O/CO2制备燃料,越来越受到人们的重视. 本文对近年来在燃料电极(阴极)材料方面的研究进展进行了全面综述,指出各种阴极材料的优缺点及发展趋势,强调亟待解决的关键科学与技术问题. 相似文献