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《环境科学学报(英文版)》2023,35(4):408-422
A series of organic compounds were successfully immobilized on an N-doped graphene quantum dot (N-GQD) to prepare a multifunctional organocatalyst for coupling reaction between CO2 and propylene oxide (PO). The simultaneous presence of halide ions in conjunction with acidic- and basic-functional groups on the surface of the nanoparticles makes them highly active for the production of propylene carbonate (PC). The effects of variables such as catalyst loading, reaction temperature, and structure of substituents are discussed. The proposed catalysts were characterized by different techniques, including Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy/energy dispersive X-ray microanalysis (FESEM/EDX), thermogravimetric analysis (TGA), elemental analysis, atomic force microscopy (AFM), and ultraviolet–visible (UV-Vis) spectroscopy. Under optimal reaction conditions, 3-bromopropionic acid (BPA) immobilized on N-GQD showed a remarkable activity, affording the highest yield of 98% at 140°C and 106 Pa without any co-catalyst or solvent. These new metal-free catalysts have the advantage of easy separation and reuse several times. Based on the experimental data, a plausible reaction mechanism is suggested, where the hydrogen bonding donors and halogen ion can activate the epoxide, and amine functional groups play a vital role in CO2 adsorption. 相似文献
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Carbon Management in Agricultural Soils 总被引:11,自引:0,他引:11
R. Lal 《Mitigation and Adaptation Strategies for Global Change》2007,12(2):303-322
World soils have been a major source of enrichment of atmospheric concentration of CO2 ever since the dawn of settled agriculture, about 10,000 years ago. Historic emission of soil C is estimated at 78 ± 12 Pg
out of the total terrestrial emission of 136 ± 55 Pg, and post-industrial fossil fuel emission of 270 ± 30 Pg. Most soils
in agricultural ecosystems have lost 50 to 75% of their antecedent soil C pool, with the magnitude of loss ranging from 30
to 60 Mg C/ha. The depletion of soil organic carbon (SOC) pool is exacerbated by soil drainage, plowing, removal of crop residue,
biomass burning, subsistence or low-input agriculture, and soil degradation by erosion and other processes. The magnitude
of soil C depletion is high in coarse-textured soils (e.g., sandy texture, excessive internal drainage, low activity clays
and poor aggregation), prone to soil erosion and other degradative processes. Thus, most agricultural soils contain soil C
pool below their ecological potential. Adoption of recommend management practices (e.g., no-till farming with crop residue
mulch, incorporation of forages in the rotation cycle, maintaining a positive nutrient balance, use of manure and other biosolids),
conversion of agriculturally marginal soils to a perennial land use, and restoration of degraded soils and wetlands can enhance
the SOC pool. Cultivation of peatlands and harvesting of peatland moss must be strongly discouraged, and restoration of degraded
soils and ecosystems encouraged especially in developing countries. The rate of SOC sequestration is 300 to 500 Kg C/ha/yr
under intensive agricultural practices, and 0.8 to 1.0 Mg/ha/yr through restoration of wetlands. In soils with severe depletion
of SOC pool, the rate of SOC sequestration with adoption of restorative measures which add a considerable amount of biomass
to the soil, and irrigated farming may be 1.0 to 1.5 Mg/ha/yr. Principal mechanisms of soil C sequestration include aggregation,
high humification rate of biosolids applied to soil, deep transfer into the sub-soil horizons, formation of secondary carbonates
and leaching of bicarbonates into the ground water. The rate of formation of secondary carbonates may be 10 to 15 Kg/ha/yr,
and the rate of leaching of bicarbonates with good quality irrigation water may be 0.25 to 1.0 Mg C/ha/yr. The global potential
of soil C sequestration is 0.6 to 1.2 Pg C/yr which can off-set about 15% of the fossil fuel emissions. 相似文献
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生物矿化已受到化学、物理、生物、材料、医学、生命及环境等多学科的广泛关注,其中,以尿素为底物的MICP(微生物诱导碳酸盐沉淀)技术是生物矿化领域的研究热点之一.在分析MICP过程中的酶解机理和生物大分子在微生物矿化过程中的作用基础上,通过对重金属离子的矿化产物和碳酸盐矿化菌的成矿因素分析,揭示MICP矿化产物的特征及形成条件.碳酸盐矿化菌主要产生脲酶分解尿素,增加土壤CO32-饱和度,其代谢产生的胞外聚合物具有多种功能团组合和键能连接,起着调控生物矿化的作用.MICP技术可用于固定土壤和水体中的Cu、Pb、Zn、Cd、Cr、As等重金属,重金属主要以共沉淀的形式被固定,阴阳离子型重金属以类质同象置换方式分别占据方解石中的CO32-位和Ca2+位,从而促使污染土壤中的可交换态重金属向碳酸盐结合态转移.但是,MICP技术主要针对减少重金属的生物可利用性,不能满足以全量来计算的现行土壤环境质量标准,且MICP技术在长期有效性、生物安全性和土壤理化性质等方面存在诸多隐患.因此,由试验条件转向实际应用具有一定挑战.建议寻找更稳定的方法以阻止碳酸盐矿物中的重金属溶出,且有必要将开发高效的土著微生物复合菌剂作为未来MICP研究的方向之一. 相似文献
77.
Juan Qin Chuanmeng Yang Chong Cui Jiantao Huang Ahmad Hussain Hailong Ma 《环境科学学报(英文版)》2016,28(9):91-99
Lime mud is a kind of solid waste in the papermaking industry, which has been a source of serious environmental pollution. Ceramsites containing anorthite and gehlenite were prepared from lime mud and fly ash through the solid state reaction method at 1050°C. The objective of this study was to explore the efficiency of Ca2 + and OH− release and assess the phosphorus and copper ion removal performance of the ceramsites via batch experiments, X-ray diffraction (XRD) and scanning electron microscopy (SEM). The results show that Ca2 + and OH− were released from the ceramsites due to the dissolution of anorthite, gehlenite and available lime. It is also concluded that gehlenite had stronger capacity for Ca2 + and OH− release compared with anorthite. The Ca2 + release could be fit well by the Avrami kinetic model. Increases of porosity, dosage and temperature were associated with increases in the concentrations of Ca2 + and OH− released. Under different conditions, the ceramsites could maintain aqueous solutions in alkaline conditions (pH = 9.3–10.9) and the release of Ca2 + was not affected. The removal rates of phosphorus and copper ions were as high as 96.88% and 96.81%, respectively. The final pH values of both phosphorus and copper ions solutions changed slightly. The reuse of lime mud in the form of ceramsites is an effective strategy. 相似文献
78.
Gasification is considered to be an effective process for energy conversion from various sources such as coal, biomass, and waste. Cleanup of the hot syngas produced by such a process may improve the thermal efficiency of the overall gasification system. Therefore, the cleanup of hot syngas from biomass gasification using molten carbonate is investigated in bench-scale tests. Molten carbonate acts as an absorbent during desulfurization and dechlorination and as a thermal catalyst for tar cracking. In this study, the performance of molten carbonate for removing H2S was evaluated. The temperature of the molten carbonate was set within the range from 800 to 1000 °C. It is found that the removal of H2S is significantly affected by the concentration of CO2 in the syngas. When only a small percentage of CO2 is present, desulfurization using molten carbonate is inadequate. However, when carbon elements, such as char and tar, are continuously supplied, H2S removal can be maintained at a high level.To confirm the performance of the molten carbonate gas-cleaning system, purified biogas was used as a fuel in power generation tests with a molten carbonate fuel cell (MCFC). The fuel cell is a high-performance sensor for detecting gaseous impurities. When purified gas from a gas-cleaning reactor was continuously supplied to the fuel cell, the cell voltage remained stable. Thus, the molten carbonate gas-cleaning reactor was found to afford good gas-cleaning performance. 相似文献
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本文以广西大厂锡石-硫化物矿区巴里尾矿库的富碳酸盐尾矿(堆放了20余年)作为研究对象,采用BCR三步提取法研究Zn、Cd、Pb和As的化学形态分量以及其总含量在该尾矿铅垂剖面中的分布,并结合尾矿的结构构造、次生和原生矿物成分及其变化等分析,探讨在氧化/酸化条件下富碳酸盐尾矿中重金属的释放机制。研究结果表明:(1)尾矿下层原尾矿中重金属主要以稳定或较稳定的残渣态(As、Pb、Zn、Cd)、氧化物结合态(Pb)及硫化物结合态(Zn、Cd)形式赋存。在酸水淋滤作用下,原尾矿中重金属的释放顺序为Cd≈ZnPbAs;(2)尾矿上部厚层状氧化硬层(厚度1~1.5m)中,Zn、Cd以酸可溶态大量富集,具有较强的迁移性;As、Pb主要以残渣态以及氧化物结合态赋存,其迁移性较差。因此,富含碳酸盐的硫化物尾矿经过氧化作用具有释放多种重金属的潜能。由于这类尾矿中各重金属的赋存状态存在差异性,因此对其迁移性及环境效应须具体分析。 相似文献