CeCl3和CeO2对松木屑的催化热解作用研究

以松木屑为研究对象,分别负载CeCl₃和CeO₂两种催化剂,制备松木屑原位催化热解原料,探究不同添加比例的CeCl₃和CeO₂两种催化剂在不同热解温度下对松木屑热解产物的产率和气体组分的影响。结果表明:在CeCl₃和CeO₂两种催化剂的催化作用下均能使热解气和焦炭产率增加、焦油产率减小,且随着两种催化剂添加比例的增加,松木屑热解产物的产率和气体组分均有所变化;在650℃的热解温度下,与无催化剂相比,当CeCl₃添加比为10.0%时焦油产率降低至53.05%,下降了11.70%,当CeCl₃添加比为7.5%时热解气产率达到最大值18.58%,当CeCl₃添加比为10.0%时焦炭产率为26.85%,增加了7.48%,热解气H₂和CO₂组分的百分比含量显著增加;当CeO₂添加比为7.5%时焦油产率达到最小值59.95%,下降了4.80%,当CeO₂添加比为10.0%时热解气产率增加了2.39%,当CeO₂添加比为10.0%时焦炭产率相对较大值为21.66%,增加了2.29%,各热解气组分的百分比含量变化较小;在原位催化热解中,CeCl₃催化剂的催化效果优于CeO₂催化剂。     

改性半焦烟气脱硫的机理研究

本文对海拉尔褐煤半焦及其水蒸气活化和高温氧化改性后的烟气脱硫性能进行了研究。     

Winter and Spring Thaw Measurements of N2O,NO and NOx Fluxes using a Micrometeorological Method

The impact of nitrogen fertilizers on gaseous emissions duringwinter and spring-thaw is not well understood and was the objective of this research. Using a micrometeorological method,N₂O, NO and NO_x fluxes from ryegrass were measured from November 1997 to March 1998. Three different mineralfertilizers were applied in November: urea (U), slow-release urea(SRU) and ammonium nitrate (AN). N₂O emissions during the winter were small, increasing significantly in March. Total losses of N₂O-N were significantly higher from SRU and U plots, with winter N₂O emissions accounting for 50% of annual losses. Nitric oxide fluxes from all plots weresmall during the measurement period (<0.9 ng N m^-2 s^-1). The NO fluxes from U and AN fertilized plots were significantly higher than from SRU and control plots. NO₂ fluxes were always negative (–6 ng N m^-2 s^-1)indicating deposition, but decreased to –2 ng N m^-2s^-1 when snow was present on the soil surface. Our resultsindicate that the form of inorganic N applied has an effect on NO+ N₂O emissions but not on NO₂ fluxes.Sponsored by CAPES – Brasília, Brazil     

铁铈氧化物对土壤As (Ⅴ)和P的稳定化效果

本文以铁铈氧化物(Fe-Ce,FC)为研究对象,评估其对中国3种典型砷(As)污染土壤的稳定化修复效果,并通过电子扫描显微镜能散X线分析仪(SEM-EDS)和X射线光电子能谱仪(XPS)等光谱学技术探索FC对As(Ⅴ)的微观吸附特征.结果表明,FC能使土壤毒性浸出As含量显著降低84. 1%～98. 3%,且在碱性土壤中表现出较强的高p H适应性,能显著增加吸附态As(F1+F2)向水合铁铝氧化物结合态(F3+F4)的稳定化. FC能使不同类型土壤的有效态P含量显著下降47. 13%～60. 32%,不仅能缓解P竞争土壤As(Ⅴ)吸附位点,而且能有效预防周边水体的面源污染.通过SEM-EDS和XPS分析,发现As(Ⅴ)吸附产物表面均检测到Fe、Ce和As这3种元素,且As主要吸附于Fe原子表面. FC在我国土壤砷污染稳定化修复领域具有较好地应用前景.     

A comparative investigation of NdSrCu_(1-x)Co_xO_(4-δ) and Sm_(1.8)Ce_(0.2)CU_(1-x)Co_xO_(4-δ) (x: 0-0.4) for NO decomposition

A series of single-phase T-structured NdSrCu_(1-x)Co_xO_(4-δ) with oxygen vacancies and T'-structured Sm_(1.8)Ce_(0.2)Cu_(1-x)Co_xO_(4-δ) (x:0-0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-progranuned desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCut_xCoxO4_b catalysts were of oxygen vacancies whereas the Sm_(1.8)Ce_(0.2)CU_(1-x)Co_xO_(4-δ) ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level,the oxygen vacancy density of NdSrCu_(1-x)Co_xO_(4-δ) decreased while the over-stoichiometric oxygen amount of Sm_(1.8)Ce_(0.2)CU_(1-x)Co_xO_(4-δ)increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO_(3.702) catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr~(-1), and 600-900℃, the catalytic activity of NO decomposition followed the order of NdSrCuO_(3.702)> NdSrCu_(0.8)Co_(0.2)O_(3.736) > NdSrCu_(0.6)Co_(0.4)O_(3.789) > Sm_(1.8)Ce_(0.2)Cu_(0.6)Co_(0.4)O_(4.187)> Sm_(1.8)Ce_(0.2)Cu_(0.8)Co_(0.2)O_(4.104)> Sm_(1.8)Ce_(0.2)CuO_(4.045), in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu~(3+)/Cu~(2+) redox ability of NdSrCu_(1-x)Co_xO_(4-δ) account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.     

崇明东滩芦苇湿地氧化亚氮排放

采用静态箱-气相色谱法,研究了崇明东滩芦苇带氧化亚氮(N2O)的排放通量.结果表明,在生长季,高潮滩无植被覆盖沉积物与芦苇根际土中NO3--N的含量变化趋势基本一致,而两者的NH4+-N的含量变化趋势则有所不同;芦苇对高潮滩沉积物N2O排放有较强的促进作用,特别是7月份,使高潮滩沉积物的排放量由0.71μg·m-·2h-1增加到566.28μg·m-·2h-1.而在1月份,芦苇根际土N2O的通量也存在小幅排放,由-4.02mg·m-·2h-1增加到67.54μg·m-·2h-1.对于芦苇根际沉积物而言,除NO3--N、NH4+-N、温度和水分以外,植物的生理过程也是控制N2O排放通量的主要因子.     

不同耕作方式对稻田净增温潜势和温室气体强度的影响

免耕技术近年来在南方稻区被广泛推广应用,但该项技术是否有利于减缓稻田综合温室效应目前并不清楚.因此,本文以双季稻-紫云英为研究对象,利用静态箱-气相色谱法分别研究不同耕作方式对稻田CH4和N2O排放、双季稻产量、土壤固碳、稻田净综合增温潜势(GWP)和温室气体强度(GHGI)的影响.试验处理包括常规翻耕(CT)、旋耕(RT)和免耕(NT).结果表明,稻田周年CH4累积排放量为233.5~404.0kg·hm-2·a-1,NT和RT处理分别比CT增加73.1%和35.1%.晚稻生长季CH4排放量占周年CH4排放量的53.7%~66.5%,其中,晚稻移栽至烤田期间CH4累积排放通量占晚稻季排放总量的77.0%~81.3%.稻田N2O累积排放量为4.00~4.82 kg·hm-2·a-1(以N计),但各处理之间没有显著差异.稻田年固碳量为0.36~1.31 t·hm-2·a-1(以C计),其中,NT处理比CT和RT处理分别增加148.4%和261.0%.双季稻周年产量为15.2~17.1 t·hm-2,耕作方式对产量没有显著影响.稻田净GWP为5095.4~7788 kg·hm-2(以CO2当量计),其中,RT和NT处理分别比CT增加52.8%和32.2%.稻田GHGI为0.30~0.46 kg·kg-1(以每kg粮食产量产生的CO2当量计),其中,RT和NT处理分别显著高于CT处理50.1%和45.3%.综上所述,免耕在短期内会增加稻田温室效应,但可以促进土壤固碳量的显著增加,因此,其固碳减排的长期效应还有待观测.     

程序升温条件下铁及其氧化物在CO存在时对N2O的还原机理

应用热综合分析仪（TG－FTIR）研究了在还原性气氛下Fe及其氧化物对N2O的催化还原 作用。研究发现铁氧化物对氮氧化物的催化还原能力相当弱，而Fe可以高效地降低N2O分解的初始温度和提高N2O向N2的转化率。在Fe和CO的作用下，N2O的初始分解温度为920K和1000K。在1123K时，N2O的转化率达到95％和805。TG／DSC曲线表明了在Fe与N2O反应过程中CO的作用表现为通过与N2O在反应表面的竞争吸附使铁氧化物还原为金属铁，X射线衍射证明Fe与N2O反应后的氧化物为Fe2O3；扫描电镜对反应后Fe表面物理形态的研究发展，在CO作用下，Fe的表面呈松散结构，可以保证Fe对氮氧化物反应的连续进行。     

中国燃煤N2O排放量监测和总量估算

对我国不同行业典型燃煤设备－电站锅炉,工业锅炉,工业窑炉和用民灶具燃煤烟气中Ｎ２Ｏ的排放量进行了实际监测,测定的Ｎ２Ｏ浓度为１．５－５７．４ｍｇ／ｍ＾３,通过对燃煤煤质分析和烟灰,炉渣中Ｃ含量测定,计算了不同炉具燃煤煤的氧化和烟气量,进而得到了各种炉具燃煤Ｎ２Ｏ的排放因子。     

氮肥运筹对稻田CH4和N2O排放的影响

开展了连续2 a（2019～2020年）的田间试验,通过设置不施肥（CK）、农户习惯施肥（CF）、二次追肥（TT）和有机肥替代20%化肥（OF）这4个处理,用静态箱-气相色谱法研究施肥对稻田CH₄和N₂O排放的影响,并综合水稻产量和综合温室效应（GWP）对单位水稻产量温室气体排放强度（GHGI）进行分析,探讨长江中下游典型水稻种植区增产减排的施肥方式.结果表明：（1）与CK相比,两年间各施肥处理均降低了CH₄排放,降幅为14.6%～25.1%;增加了N₂O排放,增幅为610%～1 836%;（2）与CF相比,TT和OF处理均呈现增加CH₄排放和降低N₂O排放的趋势,TT和OF处理两年CH₄累积排放量年均值的增幅分别为1.8%（P>0.05）和14.0%（P<0.05）; TT和OF处理两年N₂O累积排放量年均值的降幅分别为63.3%（P<0.05）和49.2%（P<0.05）;（3）与CK...