本研究选取菲为模型化合物，以强化芳烃吸附为目标，采用等体积浸渍法制备了系列Pt-Ni/NiAlOx催化剂，系统考察了Pt掺杂量对催化剂结构和菲加氢饱和性能的影响。结果表明，当反应温度300 ℃、氢气压力5 MPa、重时空速52 h−1时，相比Ni/NiAlOx催化剂，掺杂0.5%Pt的0.5Pt-Ni/NiAlOx催化剂上全氢菲选择性在反应8 h后由40%提升至67%，且表观反应速率和转化频率分别由1.53 × 10−3 mol/kg/s和14.64 × 10−3/s−1提升至1.81 × 10−3 mol/kg/s/和22.16 × 10−3/s−1。这主要归因于金属Pt适宜的掺杂量提高了金属Ni缺电子结构的稳定性，促进芳烃吸附，提升了菲加氢饱和性能。

制备低成本、高活性、高稳定性的铂(Pt)基氧还原反应(ORR)催化剂是质子交换燃料电池(PEMFC)大规模商业化应用的关键。以钴(Co)等非贵金属与Pt掺杂制备二元合金PtM催化剂不仅可以减少Pt用量，还可以获得高于Pt金属催化剂的ORR催化活性和稳定性。本文使用浸渍还原法制备碳载铂钴ORR催化剂，通过控制热处理还原温度来控制纳米颗粒的结构、晶相、尺寸等，从而改善催化剂的ORR性能。XRD、TEM和电化学分析结果综合表明，热处理温度对纳米颗粒合金度和平均粒径有显著的影响，平均粒径和合金度随着热处理温度升高而增大。通过控制热处理温度可以获得粒径与合金度之间的最优值从而提高催化剂氧还原活性，实验发现800 ℃是低粒径和高合金度的平衡点，在所有制备的催化剂中有最高的质量活性(0.41 A/mgPt)和稳定性。进一步的密度泛函理论(DFT)计算表明高合金度的Pt3Co结构表面可以降低速控步反应势垒，提高ORR活性。

The characteristics of the catalytic hydrogasification of activated carbon/bituminous char/anthracite char with the different catalysts were studied in a pressurized thermogravimetry analysis (PTGA). The GC, BET were used to characterize the physical structure and chemical reaction process of carbon, and the function principle of Co to the carbon-hydrogen reaction was preliminarily obtained. The results

本文选用两种煤（白音华褐煤和鄂州煤），研究了煤中重金属砷、硒、铅的赋存形态及其在灰化过程的释放规律，并结合煤中矿物质的变化，研究了灰化条件对矿物质转化的影响。通过外推法从热失重曲线确定了煤样的燃尽温度，以此为基准并结合国标法分别对煤样进行低温和高温灰化，对所制备的灰样采用XRD、XRF、TG-DTG等方法进行表征，分析煤中矿物质在不同灰化温度下的变化特征；采用逐级化学提取法分析煤样中As、Se、Pb的形态及含量，同时利用HNO3+ HF一步法提取煤样中的重金属，提取液中重金属含量均采用电感耦合等离子体质谱法(ICP-MS) 检测。研究结果表明，白音华煤中重金属主要以硫化物结合态形式存在的As为主，且As的挥发性随温度升高而增大；鄂州煤中重金属主要为硫化物结合态的Pb，其挥发性同样极易随温度变化而改变；煤中Se主要以有机结合态和硫化物结合态形式存在。煤在灰化过程中矿物质发生了一系列的变化：如

氧化铁作为铁基费托合成主催化剂的前驱体,其还原活化过程对催化剂整体性能有着至关重要的影响.α-Fe2O3作为一种晶体材料,其暴露晶面对铁基催化剂的还原和活化过程有重要影响,但目前对此仍然缺乏必要的研究.本研究合成了六角片、立方体和菱面体三种不同形貌的α-Fe2O3单晶纳米颗粒,其对应主暴露面分别为(001)、(102)和(104)晶面,然后利用原位拉曼光谱(ORS)研究了CO还原过程中α-Fe2O3晶体结构的转变过程.结果发现,与(104)和(102)晶面相比,(001)晶面具有更好的还原活性.对于三种晶面上的CO吸附和CO2脱附,SEM、TEM和XPS等表征以及DFT理论计算结果表明,CO2

以正己烷为模型化合物,通过产物分布分析,探讨HZSM-5分子筛上烷烃酸催化裂解反应路径及机理.研究结果表明,反应温度为300℃,不存在热裂解过程的条件下,只有基于碳正离子机理的酸催化反应.催化剂裂化活性与B酸(Br?nsted acid)量成正相关.由裂解产物的分布特点,其中,丙烯的选择性与催化剂硅铝比和剂油比正相关,而乙烷、乙烯和丙烷的选择性呈负相关性,证实了低酸密度有利于单分子裂解路径的进行.值得注意的是,正己烷直接裂解所得C4产物的总选择性明显高于C 2产物,结合量化计算,证实正己烷裂解生成的C2H+5碳正离子难以通过氢转移反应生成乙烯和乙烷,而是更倾向于与正己烷分子形成新的碳_离子(C

直接乙醇燃料电池作为便携式移动电源受到越来越多的关注,如乙醇能量密度高、可再生、无毒、清洁、便于储存和运输等优点.然而,乙醇燃料电池的研究也面临一些严重问题,其中C?C键断裂是最为挑战的问题之一.近年来有报道表明,乙醇的完全氧化(包含C?C键断裂过程)并没有显示出燃料电池效率的增加,相反乙醇不完全氧化的催化剂会导致更明显的催化电流增加.同时金属Bi掺杂会对催化剂产生电子效应和几何效应并有效增加碱性体系中催化剂的活性位中心和抗CO中毒能力.因此,本工作将铋掺杂在铂和钯中制备出PtBi/C和PdBi/C作为乙醇燃料电池催化剂,同时研究Bi掺杂催化剂对乙醇燃料电池性能以及乙醇的不完全氧化产物醋酸盐的

采用巨正则蒙特卡洛(GCMC)模拟方法研究了CO2、CH4和N2在MER型沸石中的吸附性能,模拟结果与实验结果吻合证明模型和力场是可靠的.在此基础上,以纯硅MER型沸石作为对照,采用分子动力学(MD)模拟方法研究了CO2、CH4和N2在K-MER型沸石中的扩散和分离性能.结果表明,CO2、CH4和N2在MER型沸石中存在亚扩散现象,扩散方式为构型扩散,在沸石三维通道中的扩散存在各向异性.沸石与气体之间的作用力和沸石骨架外阳离子均影响气体分子的扩散能力,而沸石骨架外阳离子是影响气体分子扩散能力的主要因素.CO2和N2的自扩散系数随吸附浓度的增加而减小;CH4的自扩散系数随吸附浓度的增大先增加后减

以硝酸钴与硝酸锌为原料,加入尿素和氟化钠在反应釜120℃下均匀生长在碳纸上得到Zn-Co(OH)2复合前驱体,通过在室温下用5 mol/L NaOH和1 mol/L Na2S溶液将前驱体刻蚀并部分硫化合成了CoSOH/Co(OH)2复合材料,考察其在电解水析氧反应(OER)中的催化性能.利用XRD、SEM、TEM、XPS对催化剂的微观结构及物理化学性质进行了表征.结果表明,该方法可以刻蚀Zn原子,留下氧空位并引入掺杂S元素,氧空位和S掺杂对OER反应起到积极促进作用.同时,非晶的CoSOH也有较好的OER活性.CoSOH与Co(OH)2的协同作用使得材料表现出最优催化效果(过电位η=310 m

研究了K、Ru和La助剂对碳化和未碳化的熔铁催化剂在结构、比表面积、晶相和催化行为上的影响,运用了XRD、XPS、TPD和N2物理吸附-脱附等分析手段对所制备的催化剂进行表征.实验结果表明,无论是否碳化,K助剂的添加都提高了C5+的选择性.助剂Ru使碳化后催化剂活性明显下降,但对未碳化的催化剂影响极小.La助剂的加入由于其包覆了碳化铁,因此,严重抑制了催化剂的碳化和活性.在产物分布上,Ru和La促进了氢气的吸附,提高了甲烷的选择性.K改性后未碳化的催化剂产物分布最优,其中,甲烷选择性为4.04％,C5+选择性为75.84％.

随着经济发展和能源需求不断增加,资源合理配置显得尤为重要.以天然气为原料的甲醇制烯烃(MTO)技术的发展,为弥合日益扩大的低碳烯烃供需矛盾提供了一条可替代传统石油化工路线、有广阔应用前景的合成路径.酸性调节对MTO催化剂的催化性能及积炭问题的解决至关重要.本研究通过改变Ca含量调节催化剂的酸性并测定系列Ca改性HZSM-5催化剂(9≤Ca/Al≤54)的甲醇转化率和低碳烯烃选择性以及催化剂稳定性,研究了Ca含量对150 nm Si/Al比为230的HZSM-5纳米颗粒催化甲醇制烯烃性能及积炭生成的影响.利用阳离子引入策略调节Lewis酸和Bronsted酸的比例及酸强度,研究了不同Ca离子含量

为了获得较多高活性II型MoS2活性相,采用四硫代钼酸铵原位热分解法制备了MoS2基催化剂,对比分析了Ni源引入方式和热分解气氛对MoS2活性相微观结构、表面元素化学状态和加氢脱氮脱硫性能等的影响.结果表明,同时引入Mo源和Ni源原位沉淀生成无定形NiMoS4后,再热分解有利于Ni取代MoS2片晶边缘的Mo原子,被修饰后的MoS2片晶保持较高的分散度、适宜的长度(3?5 nm)和堆叠层数(2?4层),从而在边缘暴露较多具有加氢和氢解活性的rim和corner活性位点.热分解气氛H2比N2更有利于Ni在热分解过程中取代MoS2边缘的Mo原子,形成更多II型Ni-Mo-S活性结构,有利于喹啉和二苯

采用硝酸溶液在不同温度和时间下对钠基蒙脱土进行处理,制备了一系列酸活化蒙脱土(Acid-MMT),并以其为固体酸与商品化的Cu/ZnO/Al2O3物理混合组成双功能催化剂用于二甲醚水蒸气重整(SRD)反应.结果表明,与钠基蒙脱土相比,酸活化蒙脱土的结构、织构及酸性均发生了明显的变化,且变化的程度与酸处理条件密切相关.酸活化蒙淹恋慕峁购退嵝悦飨杂跋焖δ艽呋恋腟RD反应性能.其中,在80℃处理12 h的酸活化蒙脱土(Acid-MMT-80/12)与Cu/ZnO/Al2O3组成双功能催化剂表现出较好的SRD性能,在p=0.1 MPa,t=350℃,GHSV=3000 h?1的反应条件下,二甲醚

采用水热合成法制备了甲醇合成甲缩醛的新型Mo-Sn催化剂.该催化剂可以在低Mo含量时实现甲醇低温氧化高选择性制取甲缩醛.通过考察Mo含量对催化剂结构及甲醇低温氧化制甲缩醛性能的影响,发现Mo1Sn10催化剂在甲醇氧化中表现出了较好的催化性能,在140℃、常压反应条件下,甲醇转化率为14.2％,甲缩醛选择性达到了88.9％,并且反应过程中无COx生成.采用XRD、Raman、FT-IR、XPS、NH3-TPD及H2-TPR等表征手段对催化剂进行深入研究.结果表明,不同Mo含量的催化剂结构性能存在着明显的差别,较低含量Mo的存在更有利于Mo5+及MoOx的生成,而由此引起的酸性及氧化还原性的变化是

采用柠檬酸溶胶凝胶法制备了Zn掺杂和Zn-Al共掺杂的La2O3催化剂,运用原位表征技术研究了该催化剂在甲烷氧化偶联(OCM)反应中的构效关系.原位XRD表征结果发现,La2O3晶体在高温下沿c轴发生热膨胀.H2-TPR结果显示,La2O3基催化剂中含有两种类型的氧物种,即强结合氧和弱结合氧;XPS结果表明,强结合氧归属于为O?.Zn掺杂的La2O3催化剂在高温下形成更多的氧空位,能活化氧气产生更多的强结合氧,因而在OCM反应中表现出较好的催化性能.Al的共掺杂能促进Zn在La2O3中的分散,进一步增加强结合氧数量,提升OCM反应C2+烃的选择性.

大气中二氧化碳(CO2)浓度的急剧增加引起了人们的关注,并提出了许多将CO2转化为高价值化学品的策略.金属有机框架材料(MOFs)由于其独特的孔隙率、大的比表面积、丰富的孔结构、多活性中心、良好的稳定性和可回收性,可用于二氧化碳的捕获和催化转化.基于晶体多孔材料的金属有机骨架(MOF)设计和合成的各种功能纳米材料可以作为多相催化剂或载体/前体来应对这些挑战.在本文中,笔者将主要关注MOFs在催化二氧化碳加氢领域的最新研究进展,包括催化加氢制备一氧化碳、甲烷、甲酸、甲醇和烯烃,分析了基于MOFs的催化剂的合成方法和提高催化活性的原因.介绍了提高新型MOF材料的催化活性和探索新的CO2转化可行的策

通过对生长在石墨相氮化碳两侧的镍基沸石咪唑酸盐骨架材料进行热分解,制备了一种新型的高活性氮掺杂多孔炭负载的镍基催化剂Ni@N-PC,并将其用于高温煤焦油异丙醇超声萃取物的催化加氢转化.催化剂的镍纳米颗粒主要包裹在碳纳米管的顶端,部分分散在碳纳米薄片表面.以1-萘酚为模型化合物,考察了催化剂在不同反应条件下的催化加氢转化活性,揭示了其催化反应机理.并利用GC/MS分析了高温煤焦油异丙醇超声萃取物及其加氢转化产物.结果表明,1-萘酚在120℃反应2 h有70％转化,在200℃反应2 h后完全转化,高温煤焦油异丙醇超声萃取物经加氢后得到大幅改质.高温煤焦油异丙醇超声萃取物中共检测到180种有机物,其

通过催化热解农业废弃物甘蔗渣(SCB),采用两步工艺生产具有显著应用价值的碳纳米管(CNTs).主要研究沸石催化剂(HZSM-5、HMOR和HY)、热解温度(450?700℃)和SCB/ZSM-5的比例(3?12)对SCB催化热解的影响,确定最佳工艺参数.随后,将第一步产生富含碳的热解产物用于第二步由Co-Mo/MgO催化生长CNTs.通过简单的两步工艺催化热解SCB生产CNTs.SCB的催化热解在半间歇式反应器(外径=4 cm,长度=90 cm)中进行,CNTs的生长在水平反应器(外径=2.5 cm,长度=100 cm)中进行.两个反应器通过玻璃管(直径0.6 cm,长度12 cm)连接并将

采用二硫化碳、甲醇、丙酮和二硫化碳/丙酮(等体积混合溶剂)对淖毛湖褐煤(NL)进行逐级超声萃取,得到各级萃取物(E1?E4)和最终萃余物(ER).采用GC-MS对各级萃取物E1?E4中的化合物组成和结构进行分析,发现E1中主要为烷烃、芳烃、醇类化合物和酯类化合物;E2中以烷烃、醇类化合物和酯类化合物为主.醇类化合物、酚类化合物以及酯类化合物是E3中的主要物质,且酯类化合物主要为邻苯二甲酸二酯类化合物.受到CS2和丙酮这两种溶剂协同作用的影响,E4中的烯烃类化合物的相对含量也比较高.采用FT-IR对NL、E1?E4和ER中所含官能团进行表征分析,结果发现,超声萃取过程只是将淖毛湖褐煤大分子骨架中

镶嵌结构沥青焦作为一种特种人造炭材料,是制备高品质各向同性石墨和核石墨的重要原料.镶嵌结构沥青焦的性质在很大程度上决定了其石墨制品的质量.为进一步明确重相沥青中QI含量对其镶嵌结构沥青焦的结构及性质的影响,本研究以九种QI含量迥异的重相沥青为原料,制备了系列镶嵌结构沥青焦.利用偏光显微镜、扫描电镜、XRD、Raman光谱及分峰拟合的方法对镶嵌结构焦的微观结构进行了判定,并对九种镶嵌结构沥青焦的显微强度进行了研究.结果表明,重相沥青中QI含量越高,在液相炭化过程中越有利于镶嵌结构的生成.并且,随着重相沥青QI含量的增加,镶嵌结构沥青焦中趋于规整炭微晶含量逐渐降低,无定型炭含量逐渐增加,强度越大.

利用密度泛函理论和过渡态理论,在分子水平上研究了循环流化床锅炉再燃过程中生物质气CO对CaO催化N2O脱除的影响.构建了N2O分子在CaO(100)表面的吸附模型,同时对N2O分子在CaO(100)表面的分解及还原过程进行了探究.结果表明,N2O在CaO(100)表面的异相分解相比于N2O的均相分解所需的能垒更低,CaO的存在有利于N2O的分解;CaO(100)表面的O活性位点被N2O分解产生的原子O毒化,而再燃过程中生物质气CO促进了CaO(100)表面活性位点的再生,有利于CaO对N2O分解的催化作用.

Abstract CeO2 aerogel (CeO2-A), nanorod (CeO2-R) and nanoflake (CeO2-F) were prepared via sol-gel, hydrothermal and coprecipitation methods, respectively. The effect of morphology and structure of CeO2 on the catalytic performance in toluene combustion reaction was investigated based on structure analysis provided by characterization. The results revealed that the activity of both CeO2-R and CeO2-F

Abstract Ru-Co3O4 catalyst was prepared by the co-precipitation method. Its catalytic performance in liquid-phase hydrogenation of CO2 into methane was investigated, and compared with those of the conventional Ru-based catalysts (Ru/SiO2, Ru/CeO2, Ru/ZrO2, Ru/TiO2) prepared by impregnation method. The solvents including H2O, n-butanol, 1,4-butyrolactone, DMF, n-nonane, decalin, cyclohexane and isooctane

Abstract The preparation of efficient catalysts in hydrogen evolution reaction (HER) is an urgent task at present. In this work, Ni(OH)2/Ni/g-C3N4 composite catalyst was prepared through liquid phase impregnation with in-situ reduction, which was used to compose the cathode with carbon paper (CP) for the microbial electrolysis cell (MEC). With the help of SEM, TEM, XRD, XPS and electrochemical analysis

Abstract The carbon content in fine slag during entrained-flow gasification is very high, at present, most of the fine slag was disposed by landfill. It is expected to provide a favorable technology by adding the fine slag to the circulating fluidized bed boilers to participate in combustion reaction. In this study, the gasification fine slags generated from GE, OMB and GSP gasifier, which are typical

Abstract The carbon deposition and sintering of Ni-based catalysts, used in CO methanation, are the main problems to be solved. In this paper, supported LaNiO3/Al2O3-ZrO2 catalyst was prepared by neutralization hydrolysis-citric acid complexation method. The effects of La-Ni loading and calcination temperature of support on the structure and catalytic activity of the catalyst were investigated. The

Abstract AseriesofK-CuZrO2catalysts with different Cu contents were prepared. The catalytic performance and reaction mechanism of 2-pentanone from ethanol condensation were investigated. The structure and properties of the catalysts were studied by N2 sorption, XRD, H2-TPR, CO2-TPD, TEM and XPS. The results showed that when the content of Cu was 9%, the conversion of ethanol reached the maximum (99

Abstract The effect of lead on the catalytic performance of Mn-Ce/TiO2 catalysts in the selective catalytic reduction (SCR) of NOx with ammonia at low temperature was investigated; with the help of nitrogen sorption, XRD, FT-IR spectroscopy, H2-TPR and NH3-TPD characterization, the causes of lead poisoning and acid regeneration were clarified. The results indicate that the doping of Pb in Mn-Ce/TiO2

Abstract Five dispersed molybdenum, nickel and cobalt oil soluble homogeneous catalysts were synthesized. The hydrogenation of coal tar pitch was under the conditions of 370°C, 10MPa hydrogen pressure, and 4 h reaction time in an autoclave reactor. The effects of molybdenum naphthenate addition, molybdenum nickel and molybdenum cobalt bimetallic ratios on hydrogenation were investigated. The catalytic

Abstract A series of Ti(SO4)2/activated carbon spheres (CS) bifunctional catalysts were designed and prepared by impregnation method, and the effect of calcination temperature of the catalysts on direct oxidation of dimethyl ether (DME)to polyoxymethylene dimethyl ethers (DMMx) was investigated. The results showed that the performance of Ti(SO4)2/CS catalysts was closely related to the calcination

Abstract The Ni/SiO2 catalysts were prepared by ammonia evaporation method, with nickel nitrate as Ni source and silica sol as the SiO2 source, for synthesis of 2-MTHF from 2-MF hydrogenation. The catalytic performance of catalysts prepared at different calcination temperatures were tested on a fixed-bed reactor. XRD, N2 adsorption-desorption isothermal, H2-TPR, NH3-TPD, XPS and TG were employed to

Abstract Alignite-based porous carbon was prepared by KOH solution extraction and subsequently by an activation of the extractant with Baoqing lignite as the raw material, and the composite capacitive materials combining the porous carbon with CoNi2S4 were fabricated by a facile hydrothermal method. The effect of different carbon material ratios on the electrochemical performance of lignite-based porous

Abstract Sulfated zirconia (SZ) and two promoted 1%Mn/SZ catalysts which have been prepared via sol gel (Mn/SZ-S) and impregnation (Mn/SZ-I) methods were studied. The morphology of the catalysts was characterized by XRD, BET, NH3-TPD, ICP, SEM and FT-IR analysis. The conversion of methanol to dimethyl ether and hydrocarbons was carried out in the temperature range of 120–300°C. The Mn/SZ-S showed the

Abstract To enhance the catalytic effect of dolomite, La/Dol catalyst was prepared by impregnation modification of dolomite with La (NO3)3 as additive. The catalyst was characterized by BET, SEM and XRD. With pine rods as raw materials and La/Dolas reforming catalysts, the effects of gasification temperature and La amount of catalysts on the catalytic gasification of pine were compared and analyzed

Abstract Distribution of rare earth elements (REEs) in six speciations extracted from coal and coal gangue and their combustion products (slag and fly ash) generated by three different power plants in China were determined by sequential extraction procedure combined with inductively coupled plasma mass spectrometry method. The results show that the REEs mainly occurred as acid soluble and silicate

Abstract The spent fluid catalytic cracking (SFCC) catalysts were activated by an “internal instant vaporization (IIV)” method and used in the removal of Hg0 from a simulated flue gas in a fixed bed reactor; the effect of various operation parameters such as the SFCC activation conditions, adsorption temperature, and flue gas components on the Hg0 removal efficiency was investigated. The results indicate

Abstract The MnOx/PG catalysts were prepared by supporting Mn oxides to palygorskite (PG) and used to remove Hg0 in simulated flue gas, which were analyzed and characterized by the specific surface area analysis (BET), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The results show that the co-effect of MnOx and PG significantly enhances the Hg0 removal performance; the MnOx/PG

Abstract Simultaneous removal of SO2, NOx and Hg0 using O3 and corn stalk bio-charcoal (CR)/coconut shell activated carbon (CS) was compared in a fixed bed. The effects of temperature, adsorption time and ratio of O3/NO on the removal efficiency of NO, Hg0 and SO2 by CR/CS were studied, and the CR and CS was characterized and analyzed. The results indicated that the oxidation rate of NO and Hg0 increased

Abstract During coal and coal gangue combustion, many heavy metal pollutants are emitted and cause serious environmental problems. In this paper, the environmental effect values of As and Pb emission during coal gangue and coal combustion in the 330 MW pulverized coal boiler, 50 kW circulated fluidized bed boiler and laboratory were calculated by ReCiPe2016. The results show that when coal combustion

Abstract The speciations of Arsenic (As) in coal will inevitably convert during the combustion process. The As speciations in coal and its by-products are closely related to human health and environmental safety which is urgent to be identified. However, there is a lack of pretreatment procedure and analysis method on the As species in coal-related products in power plants. In this study, the As species

Abstract Alkali/alkaline earth metals (AAEMs) are widely present in various solid fuels. During the combustion process, the AAEMs undergo complex physical and chemical reactions with heavy metals and other minerals in the fuel, thereby affecting the migration and transformation of heavy metals. This paper mainly introduced the influence of AAEMs on the migration and transformation of As, Se, Pb and

Abstract Blended coal combustion technology was extensively used in coal-fired power plants in China. In order to investigate the in-situ reaction between trace elements and minerals in fly ash during blended coal combustion, a bituminous (HLH), anthracite (ZW) and the blended coal of these two parent coals were combusted in a drop tube furnace at 1150°C. The ash gathered at high temperature segment