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1.
《环境科学学报(英文版)》2023,35(2):491-504
Ce1-xZrxO2 composite oxides (molar, x = 0-1.0, interval of 0.2) were prepared by a cetyltrimethylammonium bromide-assisted precipitation method. The enhancement of silver-species modification and catalytic mechanism of adsorption-transformation-desorption process were investigated over the Ag-impregnated catalysts for low-temperature selective catalytic oxidation of ammonia (NH3-SCO). The optimal 5 wt.% Ag/Ce0.6Zr0.4O2 catalyst presented good NH3-SCO performance with >90% NH3 conversion at temperature (T) ≥ 250°C and 89% N2 selectivity. Despite the irregular block shape and underdeveloped specific surface area (∼60 m2/g), the naked and Ag-modified Ce0.6Zr0.4O2 solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer (SEM-EDS) (mapping), N2 adsorption-desorption test and X-ray diffraction (XRD). H2 temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO2 reducibility and synergistic Ag0/Ag+ and Ce4+/Ce3+ redox cycles. Besides, Ag+/Ag2O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia. NH3-temperature programmed desorption (NH3-TPD) showed more adsorption-desorption capacity to ammonia were provided by physical, weak- and medium-strong acid sites. Diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure, during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction (i-SCR) reactions were proposed. 相似文献
2.
以沉淀-回流方法于磷酸银(Ag3PO4)中掺杂氮化碳(g-C3N4)制备新型复合光催化剂,同时采用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射图(XRD)等手段对合成催化剂的形态特征、晶型结构以及物理化学性质进行表征.以碘帕醇(IPM)作为目标污染物,通过改变催化剂的使用条件考察了氙灯光照下催化剂对水溶液中含碘类造影剂(ICMs)的光催化降解性能,并且分析了催化氧化过程中可能的污染物降解途径以及转化产物.结果表明,合成后的催化剂结构稳定,相对于使用单一催化剂(Ag3PO4或g-C3N4)条件下,复合催化剂对ICMs的光降解性能都得到大幅度提升,经条件优化后,确定Ag3PO4与g-C3N4的质量比例为0.15∶0.1时降解效果最佳,但不可超过0.2∶0.1,且降解性能与催化剂的投加浓度呈正相关,浓度在0.75 ... 相似文献
3.
Zhen Bi Deqing Wanyan Xiang Li Yong Huang 《Frontiers of Environmental Science & Engineering》2020,14(3):38
4.
The effect of pyrolysis and oxidation characteristics on the explosion sensitivity and severity parameters, including the minimum ignition energy MIE, minimum ignition temperature MIT, minimum explosion concentration MEC, maximum explosion pressure Pmax, maximum rate of pressure rise (dP/dt)max and deflagration index Kst, of lauric acid and stearic acid dust clouds was experimentally investigated. A synchronous thermal analyser was used to test the particle thermal characteristics. The functional test apparatuses including the 1.2 L Hartmann-tube apparatus, modified Godbert-Greenwald furnace, and 20 L explosion apparatus were used to test the explosion parameters. The results indicated that the rapid and slow weight loss processes of lauric acid dust followed a one-dimensional diffusion model (D1 model) and a 1.5 order chemical reaction model (F1.5 model), respectively. In addition, the rapid and slow weight loss processes of stearic acid followed a 1.5 order chemical reaction model (F1.5 model) and a three-dimensional diffusion model (D3 model), respectively, and the corresponding average apparent activation energy E and pre-exponential factor A were larger than those of lauric acid. The stearic acid dust explosion had higher values of MIE and MIT, which were mainly dependent on the higher pyrolysis and oxidation temperatures and the larger apparent activation energy E determining the slower rate of chemical bond breakage during pyrolysis and oxidation. In contrast, the lauric acid dust explosion had a higher MEC related to a smaller pre-exponential factor A with a lower amount of released reaction heat and a lower heat release rate during pyrolysis and oxidation. Additionally, due to the competition regime of the higher oxidation reaction heat release and greater consumption of oxygen during explosion, the explosion pressure Pm of the stearic acid dust was larger in low concentration ranges and decayed to an even smaller pressure than with lauric acid when the concentration exceeded 500 g/m3. The rate of explosion pressure rise (dP/dt)m of the stearic acid dust was always larger in the experimental concentration range. The stearic acid dust explosion possessed a higher Pmax, (dP/dt)max and Kst mainly because of a larger pre-exponential factor A related to more active sites participating in the pyrolysis and oxidation reaction. Consequently, the active chemical reaction occurred more violently, and the temperature and overpressure rose faster, indicating a higher explosion hazard class for stearic acid dust. 相似文献
5.
采用溶胶-凝胶法制备了Mn掺杂钙钛矿型催化剂LaFexMn1-xO3,并以其为催化剂催化湿式双氧水氧化处理煤气化废水纳滤浓缩液。采用XRD,SEM,FTIR技术对催化剂进行了表征。表征结果显示:制备的催化剂均具有标准的钙钛矿型结构,其中,LaFe0.9Mn0.1O3的结构稳定,比表面积大。实验结果表明:制备的催化剂中LaFe0.9Mn0.1O3的催化活性最高,且稳定性好,连续使用5次后催化活性未见明显减弱;在H2O2投加量3.0 g/L、n(H2O2)∶n(LaFe0.9Mn0.1O3)=12∶1、反应温度160 ℃、反应压力1 MPa、浓缩液pH 3、反应时间60 min的最优条件下,COD、UV254和TOC的去除率分别达到80.9%、95.2%和68.0%,BOD5/COD由0.02提升至0.40,可生化性大幅提高。 相似文献
6.
以颗粒活性炭(GAC)为载体、铜为活性组分、铈为助剂组分、草酸钠为沉淀剂,采用浸渍焙烧法制得CuO_x-CeO_2/GAC催化剂。以H_2O_2为氧化剂,微波强化催化湿式过氧化氢氧化(CWPO)处理二甲亚砜(DMSO)初始质量浓度为1 000 mg/L的废水,处理3 min后DMSO去除率达93.8%。催化剂第7次使用时DMSO去除率仍保持在75%以上。初始废水pH在3~9范围内,DMSO去除率均在85%以上。助剂Ce的加入提高了催化剂表面活性组分的分散性和稳定性,使催化剂的活性稳定性和使用寿命显著提高。 相似文献
7.
采用臭氧氧化—湿式钙法吸收工艺对模拟烟气进行同时脱硫脱硝处理。O3于150 ℃下具有较高的热稳定性,可将NO氧化为高价态氮氧化物,且NO氧化率随n(O3)∶n(NO)的增大而逐渐提高。烟气中SO2和H2O的存在对NO氧化率的影响不大。O3对SO2的氧化率较低,约为5%。3%(w)石灰石浆液对SO2的吸收率接近100%,NOx吸收率随n(O3)∶n(NO)的增大而逐渐提高,当n(O3)∶n(NO)为1.6时NOx吸收率可达约65%。SO2能促进吸收液对NOx的脱除。石灰石浆液中加入0.2%(w)的(NH4)2SO3或Na2SO3后NOx吸收率可达约85%或82%,且吸收率随添加剂加入量的增加而提高,添加(NH4)2SO3的NOx吸收率略高于添加Na2SO3。 相似文献
8.
采用三维电极电Fenton氧化法处理实际染料废水,探究了染料废水处理效果的影响因素。实验结果表明:以钌铱镀层钛电极为阳极、不锈钢板为阴极、粉末活性炭为颗粒电极,在粉末活性炭投加量为2.0 g/L、电流密度为0.5 mA/mm2、极板间距为3 cm、pH为2.0、硫酸亚铁投加量为0.50 g/L的最优工艺条件下,反应2 h后COD、TOC、氨氮、色度的去除率达到最大,分别为62.80%、41.15%、42.48%和95.00%;粉末活性炭作为颗粒电极可使染料废水COD去除率提高18个百分点;重复使用10次的处理效果与第2次基本持平。 相似文献
9.
利用矿化垃圾层预防和控制渗滤液导排系统堵塞 总被引:1,自引:0,他引:1
在卫生填埋场中,垃圾渗滤液导排系统堵塞普遍存在,悬浮固体形成的物理堵塞、有机物降解和金属离子沉淀导致的生物-化学堵塞是引起导排系统堵塞的关键因素.本文构建了"矿化垃圾+砾石层导排"的渗滤液下渗装置,通过矿化垃圾预处理渗滤液中悬浮固体和有机物以控制导排系统发生的物理和生物-化学堵塞.结果表明,在矿化垃圾层,渗滤液中化学需氧量(COD)和悬浮固体(SS)去除较多,去除率分别达到了85%和87%,并且Ca2+浓度也出现了波动较大的现象;然而,渗滤液在砾石层下渗过程中,其COD、SS和Ca2+浓度保持稳定.并且,砾石层可排水孔隙率在长期运行的过程中没有明显变化,表明渗滤液在砾石导排层没有形成明显的沉淀.与此同时,在没有添加矿化垃圾的对照组发现,砾石层可排水孔隙率减少最多的区段是渗滤液的进水点位(可排水孔隙率减少达到了53%),即渗滤液有机负荷最大处的饱和砾石层堵塞最为严重,其无机堵塞物主要是碳酸钙等.因此,在渗滤液流入砾石层前,采用矿化垃圾层部分饱和的方式对渗滤液中有机物和悬浮固体进行预处理,可以预防和控制渗滤液在砾石层形成沉淀堵塞.研究为填埋场的运行管理渗滤液导排系统堵塞提供了新的思路和方法. 相似文献
10.