Porous FeOx/BiVO4-δS0.08：Highly efficient photocatalysts for the degradation of Methylene Blue under visible-light illumination

Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide （y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40） photocatalysts were fabricated using the dodecylamine-assisted alcohol-hydrothermal and incipient wetness impregnation methods, respectively. It is shown that the y wt.% FeOx/BiVO4-δS0.08 photocatalysts contained a monoclinic scheetlite BiVO4 phase with a porous olive-like morphology, a surface area of 8.8-9.2 m^2/g, and a bandgap energy of 2.38-2.42 eV. There was co-presence of surface Bi^5＋, Bi^3＋, V^5＋, V^3＋, Fe^3＋, and Fe^2＋ species in y wt.% FeOx/BiVO4-δS0.08. The 1.40 wt.% FeOx/BiVO4-δS0.08 sample performed the best for Methylene Blue degradation under visible-light illumination. The photocatalytic mechanism was also discussed. We believe that the sulfur and FeOx co-doping, higher oxygen adspecies concentration, and lower baudgap energy were responsible for the excellent visible-light-driven catalytic activity of 1.40 wt.% FeOx/BiVO4-δS0.08.     

废物管理活动中N_2O产生及排放研究进展

N_2O是一种重要的温室气体,并且对臭氧层有严重的破坏作用,因而在全球气候变化研究中受到广泛关注。随着人类活动的加剧,全球废物排放量呈上升趋势,且废物管理活动中产生的N_2O显著增加了全球温室气体的排放。废物管理活动中N_2O排放源主要包括废水处理、动物粪肥管理及生活垃圾处理处置系统。目前对废物管理活动中N_2O排放缺乏全面认识,文章综述了废物管理活动中N_2O排放机理及产生规律,指出应加强废物管理活动中N_2O减量化方向的研究。     

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.     

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。     

负载镍锌氧体木质素基活性炭吸附磺胺噻唑

以碱木素为原料热解制备碱木素基活性炭（LAC）,在此基础上添加硝酸镍、硝酸锌等,用水热合成法成功制备出负载镍锌氧体的木质素基活性炭（NiZn-DO/LAC）.通过SEM、BET、XRD等仪器对木质素基活性炭性能结构进行表征,并研究其在水溶液中对于磺胺噻唑（ST）的吸附.结果表明,所制得的木质素基活性炭具有明显的三维多孔结构与稳定的晶体结构,其具备较大的比表面积（759.1m²/g）.在吸附ST的过程中,NiZn-DO/LAC表现出较好的吸附性能,最大吸附容量可达328.2mg/g,优于其他报道的吸附剂.在NaOH溶液中,ST易从活性炭材料中脱附,在循环利用4次后,解吸率仍可达79.43%.NiZn-DO/LAC对ST的吸附主要通过静电作用、π-π堆积作用、络合作用、氢键作用及疏水性作用的协同,从而使吸附性能得到很大提高.     

施加Fe3O4/桑树杆生物炭对土壤砷形态和水稻砷含量的影响

以桑树杆为生物炭原料,制备Fe₃ O₄/桑树杆生物炭(Fe-MBC).通过土壤培养试验,研究不同炭化温度下制备的Fe-MBC对土壤有效态As含量的钝化效果,筛选出钝化效果好的Fe-MBC-800(800℃下炭化制备)并对其进行表征.通过盆栽试验,研究Fe-MBC-800添加比例为1%~7%(质量分数)时,其对种植水稻后土壤pH值、土壤电导率(EC)、土壤As形态、水稻生物量和水稻总As含量的影响.结果表明:①Fe-MBC-800成功负载了Fe₃ O₄,其主要官能团有C=O双键、O-H键、C-O键和Fe-O键; Fe-MBC-800、MBC-800和Fe₃ O₄的比表面积分别为209.659、517.714和68.025 m² ·g^-1.②添加Fe-MBC-800可提高土壤pH值,降低土壤EC值,提高土壤残渣态As含量,降低土壤水溶态As含量和土壤有效态As含量; 土壤中添加7%的Fe-MBC-800后,水溶态As含量和土壤有效态As含量分别降低了81.6%和56.33%.③土壤中Fe-MBC-800的添加比例为5%~7%时,能促进水稻植株的生长,提高水稻生物量,使水稻植株As的累积降低了62.5%~68.75%.     

MON-3超声辅助化学电位法制备氧化石墨烯

目的得到关于氧化石墨烯制备的最佳工艺条件。方法以绿色四氧化二氮推进剂和石墨为原料,开展基于化学电位法和超声法制备氧化石墨烯的实验研究,结合对氧化石墨烯产物进行扫描电子显微镜(SEM)和X-射线衍射仪(XRD)表征。结果对于氧化石墨的制备,最佳初始ORP区间为1700～1800 mV。石墨与N2O4配料比为1︰10、低温预处理工艺H2O2用量为18 mL、KMnO4用量为1.5 g、氧化温度为30℃、氧化时间为120 min是最佳工艺条件。对于氧化石墨烯的制备,分散溶剂pH为11,分散功率为150 W,分散时间为40 min是超声分散的最佳工艺条件。结论采用该工艺条件制备氧化石墨烯,既有利于解决大批量报废硝基氧化剂的转化处理难题,也制备得到了氧化石墨烯这种高附加值的民用工业产品。     

以淀粉为模板多孔纳米氧化铈的制备及其催化性能研究

为获得多孔纳米CeO₂（氧化铈）,以淀粉为生物模板,以Ce（NO₃）₃·6H₂O为铈源,在温和条件下制备出海绵状的多孔纳米CeO₂,同时考察了焙烧温度、碱液、铈源投加量对样品形貌的影响.利用XRD（X射线衍射光谱）、SEM（扫描电镜）、N₂吸附-脱附等表征手段对合成的多孔纳米CeO₂进行物相组成、微观形貌及孔径大小分布的分析.通过湿式催化过氧化试验,探究其对腈纶废水中有机物COD_Cr的催化降解性能.结果表明:①所制备的多孔纳米CeO₂具有多孔结构,孔径分布范围为2~4 nm,孔容为0.225 cm3/g,BET比表面积为256.426 m2/g;②多孔纳米CeO₂的最佳制备条件为1 g淀粉溶解于20 mL水中,加入0.02 mol Ce（NO₃）₃·6H₂O,以5%的氨水调节前驱体混合液pH,以1℃/min升至400℃,焙烧4 h,得到海绵状的多孔纳米CeO₂.③以不同形貌的CeO₂作为湿式催化反应中的催化剂,催化降解腈纶废水中有机物,其中以制备的多孔纳米CeO₂催化性能最佳,COD_Cr去除率可达82.5%.研究显示,焙烧温度、碱液、铈源投加量均可影响样品的形貌,在湿式催化过氧化处理腈纶废水试验中,多孔纳米CeO₂能显著提高废水COD_Cr的去除率.      

Facile synthesis of graphitic carbon-nitride supported antimony-doped tin oxide nanocomposite and its application for the adsorption of volatile organic compounds

Antimony-doped tin oxide(ATO) nanoparticles with an average size of ～ 6 nm were prepared by co-precipitation and subsequent heat treatment. Graphitic carbon nitride(g-CN)/ATO hybrid nanocomposite was designed by the combination of thermally synthesized g-CN and ATO nanoparticles by ultrasonication. The materials were characterized using N2 adsorption/desorption(BET), X-ray diffraction(XRD), scanning electron microscopy(SEM), energy dispersive spectroscopy(EDS), transmission electron microscopy(TEM) and Fourier transform infrared spectroscopy(FTIR). A mixture of five volatile organic compounds(VOCs, chloroform, benzene, toluene, xylene and styrene) was used to compare the adsorption capacity of the samples. The adsorption capacity of ATO nanoparticles was improved by the addition of g-CN. Experimental data showed that, among the five VOCs,chloroform was the least adsorbed, regardless of the samples. The g-CN/ATO showed nearly three times greater adsorption capacity for the VOC mixture than pure ATO. The unchanged efficiency of VOC adsorption during cyclic use demonstrated the completely reversible adsorption and desorption behavior of the nanocomposite at room conditions. This economically and environmentally friendly material can be a practical solution for outdoor and indoor VOC removal.     

A novel graphene oxide-carbon nanotubes anchored α-FeOOH hybrid activated persulfate system for enhanced degradation of Orange II

Persulfate activation has been applied as one of the efficient advanced oxidation processes(AOPs) to remediate polluted environments. In this study, a novel α-FeOOH anchored by graphene oxide(GO)-carbon nanotubes(CNTs) aerogel(α-FeOOH@GCA) nanocomposite activated persulfate system(α-FeOOH@GCA + K_2S_2O_8) was applied for decolorization of Orange Ⅱ(OⅡ). The decolorization of OⅡ was remarkably enhanced to a level of ～ 99% in this system compared with that of pristine α-FeOOH(～ 44%) or GO-CNTs(～18%). The enhanced catalytic activity of α-FeOOH@GCA was due to the formation of a heterojunction byα-FeOOH and GO-CNTs as confirmed by the presence of Fe–O–C chemical bonds. The degradation intermediates of OⅡ were comprehensively identified. The proposed degradation pathway of OⅡ begins with the destruction of the conjugated structures of OⅡ by the dominant reactive oxygen species, surface-bound SO_4~(·-). The decolorization efficiency of OⅡ by the α-FeOOH@GCA activated persulfate system decreased from the first to third cycle of recycling. Ultraviolet(UV) irradiation or introduction of a small amount of Fe~(2+) could restore the activation of this system. The results show that the α-FeOOH@GCA persulfate activation system promises to be a highly efficient environmental remediation method for organic pollutants.