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排序方式: 共有10000条查询结果,搜索用时 46 毫秒
991.
Saurav Ch Sarma Jesús Barrio Alexander Bagger Angus Pedersen Mengjun Gong Hui Luo Mengnan Wang Silvia Favero Chang-Xin Zhao Qiang Zhang Anthony Kucernak Maria-Magdalena Titirici Ifan E. L. Stephens 《Advanced functional materials》2023,33(41):2302468
The electrochemical CO2 reduction reaction (CO2RR) to value-added chemicals with renewable electricity is a promising method to decarbonize parts of the chemical industry. Recently, single metal atoms in nitrogen-doped carbon (MNC) have emerged as potential electrocatalysts for CO2RR to CO with high activity and faradaic efficiency, although the reaction limitation for CO2RR to CO is unclear. To understand the comparison of intrinsic activity of different MNCs, two catalysts are synthesized through a decoupled two-step synthesis approach of high temperature pyrolysis and low temperature metalation (Fe or Ni). The highly meso-porous structure results in the highest reported electrochemical active site utilization based on in situ nitrite stripping; up to 59±6% for NiNC. Ex situ X-ray absorption spectroscopy (XAS) confirms the penta-coordinated nature of the active sites. The catalysts are amongst the most active in the literature for CO2 reduction to CO. The density functional theory calculations (DFT) show that their binding to the reaction intermediates approximates to that of Au surfaces. However, it is found that the turnover frequencies (TOFs) of the most active catalysts for CO evolution converge, suggesting a fundamental ceiling to the catalytic rates. 相似文献
992.
Hybrid Catalyst Coupling Zn Single Atoms and CuNx Clusters for Synergetic Catalytic Reduction of CO2
Xiaosong Hu Xinyu Liu Xin Hu Chaoyue Zhao Qingxin Guan Wei Li 《Advanced functional materials》2023,33(16):2214215
Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnNx@C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N4 sites and low valence CuNx clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N4 and N4 structures, which show strong Lewis basicity and has strong adsorption for *CO2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO2. In the catalytic process, CuNx not only adsorbs and activates H2, but also cooperates with the adjacent Zn-N4 and N4 structures to jointly activate CO2 molecules and further promotes the hydrogenation of CO2. This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts. 相似文献
993.
Fenglei Lyu Bingyun Ma Xulan Xie Daqi Song Yuebin Lian Hao Yang Wei Hua Hao Sun Jun Zhong Zhao Deng Tao Cheng Yang Peng 《Advanced functional materials》2023,33(26):2214609
Cobalt phthalocyanine (CoPc) anchored on heterogeneous scaffold has drawn great attention as promising electrocatalyst for carbon dioxide reduction reaction (CO2RR), but the molecule/substrate interaction is still pending for clarification and optimization to maximize the reaction kinetics. Herein, a CO2RR catalyst is fabricated by affixing CoPc onto the Mg(OH)2 substrate primed with conductive carbon, demonstrating an ultra-low overpotential of 0.31 ± 0.03 V at 100 mA cm−2 and high faradaic efficiency of >95% at a wide current density range for CO production, as well as a heavy-duty operation at 100 mA cm−2 for more than 50 h in a membrane electrode assembly. Mechanistic investigations employing in situ Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy unravel that Mg(OH)2 plays a pivotal role to enhance the CO2RR kinetics by facilitating the first-step electron transfer to form anionic *CO2− intermediates. DFT calculations further elucidate that introducing Lewis acid sites help to polarize CO2 molecules absorbed at the metal centers of CoPc and consequently lower the activation barrier. This work signifies the tailoring of catalyst-support interface at molecular level for enhancing the turnover rate of CO2RR. 相似文献
994.
The integration of piezoelectric materials onto carbon fiber (CF) can add energy harvesting and self-power sensing capabilities enabling great potential for “Internet of Things” (IoT) applications in motion tracking, environmental sensing, and personal portable electronics. Herein, a CF-based smart composite is developed by integrating piezoelectric poly(3,4-ethylenedioxythiophene) (PEDOT)/CuSCN-coated ZnO nanorods onto the CF surfaces with no detrimental effect on the mechanical properties of the composite, forming composites using two different polymer matrices: highly flexible polydimethylsiloxane (PDMS) and more rigid epoxy. The PDMS-coated piezoelectric smart composite can serve as an energy harvester and a self-powered sensor for detecting variations in impact acceleration with increasing output voltage from 1.4 to 7.6 V under impact acceleration from 0.1 to 0.4 m s−2. Using epoxy as the matrix for a CF-reinforced plastic (CFRP) device with sensing and detection functions produces a voltage varying from 0.27 to 3.53 V when impacted at acceleration from 0.1 to 0.4 m s−2, with a lower output compared to the PDMS-coated device attributed to the greater stiffness of the matrix. Finally, spatially sensitive detection is demonstrated by positioning two piezoelectric structures at different locations, which can identify the location as well as the level of the impacting force from the fabricated device. 相似文献
995.
Junwei Xiang Chuanzhou Han Jianhang Qi Yanjie Cheng Kai Chen Yongming Ma Jiayu Xie Yue Hu Anyi Mei Yinhua Zhou Hongwei Han 《Advanced functional materials》2023,33(25):2300473
Due to the low cost and excellent potential for mass production, printable mesoscopic perovskite solar cells (p-MPSCs) have drawn a lot of attention among other device structures. However, the low open-circuit voltage (VOC) of such devices restricts their power conversion efficiency (PCE). This limitation is brought by the high defect density at perovskite grain boundaries in the mesoporous scaffold, which results in severe nonradiative recombination and is detrimental to the VOC. To improve the perovskite crystallization process, passivate the perovskite defects, and enhance the PCE, additive engineering is an effective way. Herein, a polymeric Lewis base polysuccinimide (PSI) is added to the perovskite precursor solution as an additive. It improves the perovskite crystallinity and its carbonyl groups strongly coordinate with Pb2+, which can effectively passivate defects. Additionally, compared with its monomer, succinimide (SI), PSI serves as a better defect passivator because the long-chained macromolecule can be firmly anchored on those defect sites and form a stronger interaction with perovskite grains. As a result, the champion device has a PCE of 18.84%, and the VOC rises from 973 to 1030 mV. This study offers a new strategy for fabricating efficient p-MPSCs. 相似文献
996.
Andy Shar Phillip Glass Sung Hyun Park Daeha Joung 《Advanced functional materials》2023,33(5):2211079
3D printing of conductive elastomers is a promising route to personalized health monitoring applications due to its flexibility and biocompatibility. Here, a one-part, highly conductive, flexible, stretchable, 3D printable carbon nanotube (CNT)-silicone composite is developed and thoroughly characterized. The one-part nature of the inks: i) enables printing without prior mixing and cures under ambient conditions; ii) allows direct dispensing at ≈100 µm resolution printability on nonpolar and polar substrates; iii) forms both self-supporting and high-aspect-ratio structures, key aspects in additive biomanufacturing that eliminate the need for sacrificial layers; and iv) lends efficient, reproducible, and highly sensitive responses to various tensile and compressive stimuli. The high electrical and thermal conductivity of the CNT-silicone composite is further extended to facilitate use as a flexible and stretchable heating element, with applications in body temperature regulation, water distillation, and dual temperature sensing and Joule heating. Overall, the facile fabrication of this composite points to excellent synergy with direct ink writing and can be used to prepare patient-specific wearable electronics for motion detection and cardiac and respiratory monitoring devices and toward advanced personal health tracking and bionic skin applications. 相似文献
997.
Yuki Akinaga Tokuhisa Kawawaki Hinano Kameko Yuki Yamazaki Kenji Yamazaki Yuhi Nakayasu Kosaku Kato Yuto Tanaka Adie Tri Hanindriyo Makito Takagi Tomomi Shimazaki Masanori Tachikawa Akira Yamakata Yuichi Negishi 《Advanced functional materials》2023,33(33):2303321
Single-atom (SA) catalysts exhibit high activity in various reactions because there are no inactive internal atoms. Accordingly, SA cocatalysts are also an active research fields regarding photocatalytic hydrogen (H2) evolution which can be generated by abundant water and sunlight. Herein, it is investigated whether 10 transition metal elements can work as an SA on graphitic carbon nitride (g-C3N4; i.e., gCN), a promising visible-light-driven photocatalyst. A method is established to prepare SA-loaded gCN at high loadings (weight of ≈3 wt.% for Cu, Ni, Pd, Pt, Rh, and Ru) by modulating the photoreduction power. Regarding Au and Ag, SAs are formed with difficulty without aggregation because of the low binding energy between gCN and the SA. An evaluation of the photocatalytic H2-evolution activity of the prepared metal SA-loaded gCN reveals that Pd, Pt, and Rh SA-loaded gCN exhibits relatively high H2-evolution efficiency per SA. Transient absorption spectroscopy and electrochemical measurements reveal the following: i) Pd SA-loaded gCN exhibits a particularly suitable electronic structure for proton adsorption and ii) therefore they exhibit the highest H2-evolution efficiency per SA than other metal SA-loaded gCN. Finally, the 8.6 times higher H2-evolution rate per active site of Pd SA is achieved than that of Pd-nanoparticles cocatalyst. 相似文献
998.
Rong Zhang Xiujun Wang Zhen Zhang Wendi Zhang Junqi Lai Siqi Zhu Yunfei Li Yong Zhang Kecheng Cao Song Qiu Qi Chen Lixing Kang Qingwen Li 《Advanced functional materials》2023,33(41):2301864
High current carrying capacity and high conductivity are two important indicators for materials used in microscale electronics and inverters. However, it is challenging to obtain high conductivity and high current carrying capacity at the same time since high conductivity requires a weakly bonded system to provide free electrons, while high current carrying capacity requires a strongly bonded system. In this paper, CuI@SWCNT networks by filling the single-walled carbon nanotubes (SWCNTs) with CuI is ingeniously prepared. CuI@SWCNT shows good stability due to the confinement protection of SWCNTs. Through the host-guest hybridization, CuI@SWCNT networks exhibit a current carrying capacity of 2.04 × 107 A cm−2 and a conductivity of 31.67 kS m−1. Their current carrying capacity and conductivity are significantly improved compared with SWCNT. The Kelvin probe force microscopy measurements show a drop of surface potential energy after SWCNT filled with CuI, indicating that the CuI guest molecules regulate the position of the Fermi level of SWCNTs, increasing carrier concentration, achieving high conductivity and high current carrying capacity. This study offers ideas and solutions for the regulation of high-performance carbon tube networks, which hold great promise for future applications in carbon-based electronic devices. 相似文献
999.
Boshi Tian Shaohua Liu Chenghao Yu Shikai Liu Shuming Dong Lili Feng Narisu Hu Piaoping Yang 《Advanced functional materials》2023,33(25):2300818
As a less O2-dependent photodynamic therapy (PDT), type I PDT is an effective approach to overcome the hypoxia-induced low efficiency against solid tumors. However, the commonly used metal-involved agents suffer from the long-term biosafety concern. Herein, a metal-free type I photosensitizer, N-doped carbon dots/mesoporous silica nanoparticles (NCDs/MSN, ≈40 nm) nanohybrid with peroxidase (POD)-like activity for synergistic PDT and enzyme-activity treatment, is developed on gram scale via a facile one-pot strategy through mixing carbon source and silica precursor with the assistance of template. Benefiting from the narrow bandgap (1.92 eV) and good charge separation capacity of NCDs/MSN, upon 640 nm light irradiation, the excited electrons in the conduction band can effectively generate O2•− by reduction of dissolved O2 via a one-electron transfer process even under hypoxic conditions, inducing apoptosis of tumor cells. Moreover, the photoinduced O2•− can partially transform into more toxic •OH through a two-electron reduction. Moreover, the POD-like activity of NCDs/MSN can catalyze the endogenous H2O2 to •OH in the tumor microenvironment, further synergistically ablating 4T1 tumor cells. Therefore, a mass production way to synthesize a novel metal-free type I photosensitizer with enzyme-mimic activity for synergistic treatment of hypoxic tumors is provided, which exhibits promising clinical translation prospects. 相似文献
1000.
Kun Guo Zhimin He Song Lu Pengjun Zhang Ning Li Lipiao Bao Zhixin Yu Li Song Xing Lu 《Advanced functional materials》2023,33(29):2302100
Carbon nano-onions (CNOs) as a novel form of carbon materials hold peculiar structural features but their electrocatalytic applications are largely discouraged by the demanding synthesis conditions (e.g., ≥1500 °C and vacuum). Using C60 fullerene molecules as the sacrificial seeds and melamine as the main feedstock, herein, a novel strategy for the facile construction of CNOs nanoparticles is presented with ultrafine sizes (≈5 nm) at relatively low temperatures (≤900 °C) and atmospheric pressure. During the calcination, in-depth characterizations reveal that C60 can retain the melamine-derived graphitic carbon nitride from complete sublimation at high temperatures (≥700 °C). Owing to the N removal and subsequent pentagon generation, severely deformed graphitic fragments together with the disintegrated C60 molecules merge into larger sized nanosheets with high curvature, eventually leading to the formation of N-doped defect-rich CNOs. Owing to the integration of multiple favorable structural features of pentagons, edges, and N dopants, the CNOs obtained at 900 °C present superior oxygen reduction half-wave potential (0.853 VRHE) and zinc–air cathode performance to the commercial Pt/C (0.838 VRHE). Density functional theory calculation further uncovers that the carbon atoms adjacent to the N-doped edged pentagons are turned into the ORR-active sites with O2 protonation as the rate-determining step. 相似文献