MnCeOx/沸石催化剂对工业典型VOCs的催化性能

以沸石为载体制备了锰铈复合氧化物催化剂（记为:MnCeO_x/沸石催化剂）,探究了催化剂对工业典型VOCs的二元催化性能,并对催化剂进行BET、XRD及SEM表征。结果表明:Ce的加入,促进了Mn的分散,提高了MnCeO_x/沸石催化剂的活性;当n（Mn）∶n（Ce）为1∶1,负载率为20%,焙烧温度为500℃时,催化剂的活性最高,其对甲苯的起燃温度（T₅₀）和完全燃烧温度（T₉₀）分别为155,255℃;单组分实验中,催化剂对3种有机物均表现出较高活性,转化率达到90%时的反应温度均在275℃以下,其活性顺序为乙酸乙酯>甲苯>丙酮,主要受反应活化能大小及分子极性的影响;二元催化实验中,由于竞争吸附的影响,3种物质的T₅₀和T₉₀较单组分均分别提高了8~13,14~38℃。     

有机废物厌氧发酵生物合成己酸研究进展

厌氧发酵处理有机废物并合成高价值羧酸盐的技术日趋成熟。尤其是己酸作为产物之一,因其附加值高,易于分离,用途广泛,越来越受到关注。微生物合成己酸需要电子供体及受体。详细介绍了乙醇、乙酸分别作为电子供体、受体合成己酸的机理——逆β氧化反应,总结合成己酸底物以及影响合成的因素（温度、pH值、水力停留时间、竞争路径、氢气分压、底物比例、氮源等）。目前采用科氏梭菌以乙醇为电子供体来合成己酸的技术较成熟,探索了利用乳酸为电子供体合成己酸的代谢机理,并指出开发乳酸转化合成己酸的技术可成为未来发展方向。     

稻田NO3-还原耦合As(III)氧化过程及微生物群落特征

以华南稻田土壤为研究对象通过构建微宇宙体系,研究了淹水稻田自养硝酸盐还原耦合As（III）氧化过程及其微生物群落结构组成.结果表明,NO₃^-的添加促进了稻田土壤中As（III）的氧化,在未添加NO₃^-的处理（Soil+As（III））以及灭菌处理（Sterilized soil+As（III）+NO₃^-）中As（III）未发生明显的氧化;在Soil+As（III）+NO₃^-处理中,NO₃^-有少量被还原,而在Soil+NO₃^-处理中,NO₃^-没有被还原.通过16S rRNA高通量分析在NO₃^-还原耦合As（III）氧化体系中微生物群落结构特征,在Soil+As（III）+NO₃^-处理中shannon指数相对较低为8.19,土壤微生物群落多样性降低,其中在门水平上主要优势菌群为变形菌门Proteobacteria（33%）、绿弯菌门Chloroflexi（11%）、浮霉菌门Planctomycetes（12%）;在属水平上主要的优势菌属为Gemmatimonas（7.4%）以及少量的Singulisphaera、Thermomonas、Bacillus.NO₃^-的添加能够促进稻田土壤中自养As（III）氧化,并且影响着稻田土壤中微生物群落组成.     

二乙烯三胺五甲叉膦酸酸解磷尾矿的实验探究

为减少磷尾矿堆积带来的环境污染问题,实现磷尾矿的钙、镁、磷元素的分离,以高镁磷尾矿为原料,采用二乙烯三胺五甲叉膦酸(DTPMP)进行酸解,探究磷尾矿中主要物相在DTPMP中的分解机制,并通过单因素实验探究pH、反应时间、反应温度及投料比对磷尾矿中MgO、CaO和P_2O_5分解率的影响。实验结果表明:pH对P_2O_5的分解率影响较大,高温更有利于尾矿中镁的溶出,在pH为2. 5,反应时间为60 min,反应温度为80℃,投料比为1. 56时,MgO、CaO和P_2O_5的分解率分别达到61. 05%、38. 23%和9. 67%。     

Tuning the fill percentage in the hydrothermal synthesis process to increase catalyst performance for ozone decomposition

The performance of Ce-OMS-2 catalysts was improved by tuning the fill percentage in the hydrothermal synthesis process to increase the oxygen vacancy density. The Ce-OMS-2 samples were prepared with different fill percentages by means of a hydrothermal approach (i.e. 80%, 70%, 50% and 30%). Ce-OMS-2 with 80% fill percentage (Ce-OMS-2-80%) showed ozone conversion of 97%, and a lifetime experiment carried out for more than 20?days showed that the activity of the catalyst still remained satisfactorily high (91%). For Ce-OMS-2-80%, Mn ions in the framework as well as K ions in the tunnel sites were replaced by Ce⁴⁺, while for the others only Mn ions were replaced. O₂-TPD and H₂-TPR measurements proved that the Ce-OMS-2-80% catalyst possessed the greatest number of mobile surface oxygen species. XPS and XAFS showed that increasing the fill percentage can reduce the AOS of Mn and augment the amount of oxygen vacancies. The active sites, which accelerate the elimination of O₃, can be enriched by increasing the oxygen vacancies. These findings indicate that increasing ozone removal can be achieved by tuning the fill percentage in the hydrothermal synthesis process.     

干湿法结合工艺回收废弃SCR脱硝催化剂中的钛、钒和钨

利用干湿法结合工艺实现废弃SCR脱硝催化剂中Ti、V和W元素的高效分离和浸出,提出成套废弃SCR脱硝催化剂中Ti、V和W的回收技术。以废弃SCR脱硝催化剂为研究对象,优选Ti、V和W元素最佳浸出工况,研究硫酸溶解法回收TiO₂和有机萃取法回收V₂O₅和WO₃的回收率与纯度。结果表明:酸浸还原浸钒最优工艺条件为温度140℃,液固比30∶1;钠化焙烧浸钨最优工艺条件为煅烧温度750℃,反应物与Na₂CO₃配比（质量比）为1∶1.5,在以上条件下V、W浸出率分别达到97.6%、93.6%。利用硫酸溶解法回收得到的TiO₂产物主要以锐钛矿晶型存在形式,在最佳焙烧温度750℃下,TiO₂回收率达到97.17%,纯度为95.35%。利用有机萃取法回收得到的V₂O₅和WO₃产物的回收率和纯度分别为72.47%、75.43%和93.25%、78.26%。     

核桃壳生物炭对土壤中镉的钝化修复

通过室内模拟试验,研究了核桃壳生物炭（BC400、BC500、BC600）对人工Cd污染土壤（20 mg/kg）pH、Cd赋存形态分布的影响,并探究可能的修复机理。结果显示:经56 d修复后,与空白对照组相比,10%添加量的核桃壳生物炭BC400、BC500、BC600分别使土壤pH升高了1.07、1.31、1.38,弱酸可提取态Cd含量减少了17.02%、20.20%、24.53%,可还原态Cd含量减少了8.9%、19.1%、38.2%,可氧化态Cd含量增加了44.83%、78.45%、100%,残渣态Cd含量增加了66.03%、71.43%、89.21%。同时,土壤pH与土壤中弱酸可提取态Cd含量呈显著负相关（P<0.01）。综上,核桃壳生物炭能够对Cd污染土壤起到钝化修复作用。     

Role of glycine on sulfuric acid-ammonia clusters formation: Transporter or participator

Glycine(Gly) is ubiquitous in the atmosphere and plays a vital role in new particle formation(NPF).However,the potential mechanism of its on sulfuric acid(SA)-ammonia(A)clusters formation under various atmospheric conditions is still ambiguous.Herein,a(Gly)_x·(SA)_y·(A)_z(z≤x+y≤3) multicomponent system was investigated by using density functional theory(DFT) combined with Atmospheric Cluster Dynamics Code(ACDC) at different temperatures and precursor concentrations.The results show that Gly,with one carboxyl(-COOH) and one amine(-NH_2) group,can interact strongly with SA and A in two directions through hydrogen bonds or proton transfer.Within the relevant range of atmospheric concentrations,Gly can enhance the formation rate of SA-A-based clusters,especially at low temperature,low [SA],and median [A].The enhancement(R) of Gly on NPF can be up to 340 at T=218.15 K,[SA]=10~4,[A]=10~9,and [Gly]=10~7 molecules/cm~3.In addition,the main growth paths of clusters show that Gly molecules participate into cluster formation in the initial stage and eventually leave the cluster by evaporation in subsequent cluster growth at low [Gly],it acts as an important "transporter" to connect the smaller and larger cluster.With the increase of [Gly],it acts as a "participator" directly participating in NPF.     

Adsorption of 17β-estradiol from aqueous solution by raw and direct/pre/post-KOH treated lotus seedpod biochar

Five biochars derived from lotus seedpod(LSP) were applied to examine and compare the adsorption capacity of 17β-estradiol(E2) from aqueous solution.The effect of KOH activation and the order of activation steps on material properties were discussed.The effect of contact time,initial concentration,p H,ionic strength and humic acid on E2 adsorption were investigated in a batch adsorption process.Experimental results demonstrated that the pseudo second-order model fitted the experimental data best and that adsorption equilibrium was reached within 20 hr.The efficiency of E2 removal increased with increasing E2 concentration and decreased with the increase of ionic strength.E2 adsorption on LSP-derived biochar(BCs) was influenced little by humic acid,and slightly affected by the solution p H when its value ranged from 4.0 to 9.0,but considerably affected at p H 10.0.Low environmental temperature is favorable for E2 adsorption.Chemisorption,π–π interactions,monolayer adsorption and electrostatic interaction are the possible adsorption mechanisms.Comparative studies indicated that KOH activation and the order of activation steps had significant impacts on the material.Post-treated biochar exhibited better adsorption capacity for E2 than direct treated,pretreated,and raw LSP biochar.Pyrolyzed biochar at higher temperature improved E2 removal.The excellent performance of BCs in removing E2 suggested that BCs have potential in E2 treatment and that the biochar directly treated by KOH would be a good choice for the treatment of E2 in aqueous solution,with its advantages of good efficiency and simple technology.     

Effects of SO2 and H2O on low-temperature NO conversion over F-V2O5-WO3/TiO2 catalysts

F-V_2 O_5-WO3/Ti02 catalysts were prepared by the impregnation method.As the content of F ions increased from 0.00 to 0.35 wt.%,the NO conversion of F-V_2 O_5-WO_3/TiO_2 catalysts initially increased and then decreased.The 0.2 F-V_2 O_5-WO_3/TiO_2 catalyst(0.2 wt.% F ion)exhibited the best denitration(De-NOx) performance,with more than 95% NO conversion in the temperature range 160-360℃,and 99.0% N2 selectivity between 110 and 280℃.The addition of an appropriate amount of F ions eroded the surface morphology of the catalyst and reduced its grain size,thus enhancing the NO conversion at low temperature as well as the sulfur and water resistance of the V_2 O_5-WO3/Ti02 catalyst.After selective catalytic reduction(SCR) reaction in a gas flow containing SO_2 and H_2 O,the number of NH3 adsorption sites,active component content,specific surface area and pore volume decreased to different degrees.Ammonium sulfate species deposited on the catalyst surface,which blocked part of the active sites and reduced the NO conversion performance of the catalyst.On-line thermal regeneration could not completely recover the catalyst activity,although it prolonged the cumulative life of the catalyst.In addition,a mechanism for the effects of S02 and H_2 O on catalyst NO conversion was proposed.