留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

2017年  第45卷  第7期

显示方式:
论文
摘要:
Coal and char are essential energy sources for the process industry. Insightful understanding of those molecules is useful to explore reactivities of coal and char. Therefore, coal and char molecular structures were investigated at atomic level using Materials Studio 7.0 software. Firstly, coal and char initial structures were constructed based on reported literatures. Secondly, those structures were improved by molecular mechanics, where functional group fragments were added to satisfy the property of coal or char. Then, the subsequent structures were optimized by annealing dynamics simulation to adjust density and elementary composition. Finally, the potential energies of coal and char were calculated using energy minimization method. It was pointed out that the estimated densities and elementary composition were agreements with the published literatures, which indicated that those structures were valid and reasonable. From the simulated results, it was shown that the Coulomb energy and van der Waals energy played a much more important role than other energies during the stabilizing molecular construction process. Thus, it was inferred that the weak bond was predominant in the thermal processing of coal or char. In addition, this work demonstrated that the molecular simulation technology was meaningful to construct the complex macromolecular structure.
摘要:
利用分选结合逐级酸洗的方法制备出不同灰含量和矿物组成的褐煤煤样,使用沉降管反应器(DTR)和热重分析仪(TGA)研究内在矿物在1 000-1 200℃对褐煤CO2气化的影响。结果表明,内在矿物对褐煤CO2气化具有促进作用,且促进机制具有温度敏感性。低温时(1 000℃),内在矿物可通过增加初生半焦微晶结构的无序度,间接提高气化碳转化率。高温时(1 100-1 200℃),内在矿物通过催化煤焦气化,直接促进气化碳转化率的上升。碱性指数不适用于表征本研究的褐煤内在矿物的催化作用。Ca是内在矿物中影响整体催化能力的主要成分,而且羧酸盐形式的Ca是其中的活性组分。不同的催化机制是导致煤焦中钙的催化活性因其化学形式而异的根本原因。羧酸盐形式的Ca可降低煤焦气化反应的活化能,而CaO则提高反应的表观频率因子。
摘要:
利用固定床反应器、红外光谱仪、吸附仪、X射线衍射仪、电感耦合等离子原子发射光谱仪、偏光显微镜等对比研究了原生生物质(原生物质)及水洗脱钾生物质(脱钾生物质)在N2及富一氧化碳(CO)气氛下所得半焦的产率、官能团及其他物化结构的变化规律。研究表明,与脱钾生物质相比,热解温度低于750℃时,原生物质的半焦产率降低、比表面积增大、芳环结构减少而烷基、脂肪族结构等增加;与N2相比,富CO气氛下所得半焦产率降低、比表面积增大,芳香结构、脂肪族结构、烷基减小。而热解温度高于750℃时,生物质中的钾和热解气氛中的CO均使生物质半焦产率增加、官能团数量和比表面积减少。利用偏光显微镜对生物质半焦表面矿物质的研究表明,热解温度低于750℃时,所得半焦表面矿物组分较少且高度分散;热解温度高于750℃时,所得半焦表面矿物组分较多,分布密集且熔融团聚现象随温度升高而增多。而对于半焦石墨化程度的研究表明,半焦石墨化程度随温度升高而增加,但低热解温度所得半焦的石墨化程度较差。温度高于750℃时,CO气氛使石墨化程度增加,而钾使石墨化程度降低。
摘要:
通过控制溶出温度(160、180和200℃),制备了三种毛竹乙醇木质素EOL(EOL-160、EOL-180和EOL-200),并采用红外光谱仪(FT-IR)、凝胶渗透色谱(GPC)和热重分析(TG)分别对乙醇木质素的官能团、分子量分布及热稳定性进行了分析;采用微型高温高压反应釜,在超临界乙醇体系,进行三种乙醇木质素的解聚实验,通过气相色谱/质谱联用仪(GC/MS)及FT-IR对解聚产物进行分析,探讨乙醇木质素特性对其超临界乙醇环境解聚产物组成的影响规律。结果表明,随着溶出温度的升高,乙醇木质素溶出率呈上升趋势。EOL-160、EOL-180和EOL-200三种乙醇木质素在超临界条件解聚液相产物主要成分分别为对乙基苯酚、2,6-二甲氧基苯酚和4-羟基-3-甲氧基-苯甲酸酯。
摘要:
This work presents a synthesis of bimetallic NiMo and NiW modified ZSM-5/MCM-41 composites and their heterogeneous catalytic conversion of crude palm oil (CPO) to biofuels. The ZSM-5/MCM-41 composites were synthesized through a self-assembly of cetyltrimethylammonium bromide (CTAB) surfactant with silica-alumina from ZSM-5 zeolite, prepared from natural kaolin by the hydrothermal technique. Subsequently, the synthesized composites were deposited with bimetallic NiMo and NiW by impregnation method. The obtained catalysts presented a micro-mesoporous structure, confirmed by XRD, SEM, TEM, EDX, NH3-TPD, XRF and N2 adsorption-desorption measurements. The results of CPO conversion demonstrate that the catalytic activity of the synthesized catalysts decreases in the series of NiMo-ZSM-5/MCM-41 > NiW-ZSM-5/MCM-41 > Ni-ZSM-5/MCM-41 > Mo-ZSM-5/MCM-41 > W-ZSM-5/MCM-41 > NiMo-ZSM-5 > NiW-ZSM-5 > ZSM-5/MCM-41 > ZSM-5 > MCM-41. It was found that the bimetallic NiMo-and NiW-ZSM-5/MCM-41 catalysts give higher yields of liquid hydrocarbons than other catalysts at a given conversion. Types of hydrocarbon in liquid products, identified by simulated distillation gas chromatography-flame ionization detector (SimDis GC-FID), are gasoline (150-200 ℃; C5-12), kerosene (250-300 ℃; C5-20) and diesel (350 ℃; C7-20). Moreover, the conversion of CPO to biofuel products using the NiMo-and NiW-ZSM-5/MCM-41 catalysts offers no statistically significant difference (P > 0.05) at 95% confidence level, evaluated by SPSS analysis.
摘要:
采用化学还原法在不同单一和复配溶剂体系中制备了一系列NiCoB非晶态合金催化剂,对其液相糠醛加氢性能进行了考察,并采用N2吸附-脱附等温线、ICP、FE-SEM、HRTEM、XRD、XPS等手段进行了表征。结果表明,在相同反应条件下,制备溶剂的表面张力、黏度、极性大小和溶解度常数等对NiCoB非晶态合金催化剂的组成、形貌和结构及其糠醛加氢反应性能均产生重要影响。由甲醇/乙二醇复配溶剂(MEG,体积比1:1)制备的NiCoB-MEG催化剂具有最理想的糠醛液相加氢制糠醇性能,糠醛转化率达到96.4%,糠醇选择性达到83.49%,这可归因于甲醇和乙二醇之间的协同作用促进了金属组分的分散和还原。
摘要:
采用NaOH溶液对HZSM-5分子筛进行碱处理,利用XRD、SEM、BET、Py-FTIR四种方法表征改性HZSM-5分子筛,对生物原油有机相、未改性HZSM-5制得生物油有机相与改性HZSM-5制得生物油有机相进行理化特性及成分分析,研究了碱处理HZSM-5分子筛对生物油有机相产物的影响;对使用了120 min的三种失活催化剂进行了热重分析,并对焦炭峰面积进行了积分计算。结果表明,经过碱处理后的HZSM-5分子筛保留了典型的MFI拓扑结构,形成了一定数量的介孔;同时,经碱处理1 h的HZSM-5分子筛催化制得的生物油有机相产物的产率有所增加且理化特性得到提高,其产物中烃类物质的含量显著增加,达到了37.67%,且以单环芳香烃为主;同时改性HZSM-5分子筛对生物油有机相中的酸、醛及酮类物质均有较好的脱除效果,有效地降低了生物油的腐蚀性并提升了生物油的稳定性,热值达到了35.32 MJ/kg;经1 h碱处理的HZSM-5分子筛的总结焦量明显降低。
摘要:
Polyoxymethylene dimethyl ethers (H3CO(CH2O)nCH3, PODEn or DMMn, n ≥ 2) with unique physical and chemical properties are a potential additive for diesel fuels, which can effectively enhance the combustion efficiency and reduce the emission of pollutants. In this work, a series of pure PODEn components (n=2-5) were synthesized from methylal and trioxymethylene and obtained with high purity through collaborative separation; their structure and properties were characterized by NMR, FT-IR, Raman, and DFT calculation and a detailed assignment of the expressions in the spectrogram to the various groups was performed. The density and viscosity of PODEn were measured at 298.15-323.15 K. The results indicate that the density and viscosity of PODEn decrease gradually with the increase of temperature. Meanwhile, with the increase in the number of -CH2O-units (n) from 2 to 5, the density, viscosity, flash point, pour point, and the heat of fusion and solidification of PODEn are all increased. These results are valuable for the practical synthesis and application of PODEn.
摘要:
为进一步提高镍基催化剂的抗积炭能力,增强其甲烷二氧化碳重整反应性能,采用沉积沉淀法(DP)、共沉淀法(CP)和共浸渍法(CI)制备了NiCo/MgO催化剂。结合现代仪器分析表征技术,研究了制备方法对NiCo/MgO催化剂结构和抗积炭能力的影响。结果表明,与共沉淀法相比,沉积沉淀法制备过程为Ni2+和Co2+的完全水解沉淀提供了碱性环境,粒子的成核和生长速率相对较快,不存局部过饱和现象,所制备的催化剂具有良好的还原性、较小的颗粒粒径(9.7 nm)、良好的Ni/Co分散度(10.4%)和大的比表面积(68.1 m2/g),从而具有优良的抗积炭性能。对于甲烷二氧化碳重整,DP催化剂上CH4和CO2转化率保持在88%和92%,与800℃下的热力学平衡转化率相近;同时,H2收率比CP和CI催化剂分别高约10%和43%,CO收率比CP和CI催化剂分别高约13%和42%,且稳定性更好。
摘要:
通过共沉淀法制备了ZrO2和Al2O3载体,采用等体积浸渍法制备了MoO3质量分数为5%的Mo/ZrO2和Mo/Al2O3催化剂,并用于甲烷化反应。在三种反应气氛下对两种预硫化的Mo基催化剂进行评价,发现ZrO2载体均可显著促进甲烷化反应,同时能够促进水汽变换(WGS)反应。通过XRD、H2-TPR、XPS和TEM等表征发现,两种载体上Mo物种的硫化程度以及暴露的活性位数量不同,从而导致两种催化剂上催化性能差异显著。与Mo/Al2O3相比,Mo/ZrO2催化剂上的MoO3更易被还原,硫化程度也更高,并且Mo4+的含量更高,Mo6+的含量更低。虽然ZrO2载体上MoS2尺寸较大,边位置的Mo比例有所降低,但是由于MoS2沿ZrO2颗粒表面弯曲生长,使得MoS2基面成为反应的活性位;因此,Mo/ZrO2催化剂在甲烷化与WGS反应中表现出更优异的催化性能。
摘要:
以TEAOH和TMAOH为有机模板剂,酸处理的UZM-9分子筛为晶种,采用水热法在48 h内合成出分子筛UZM-9,并对其CO2/CH4/N2的吸附分离性能进行了研究。采用XRD、ICP、TG、SEM与气体吸附等手段对晶种法合成的UZM-9分子筛结构、耐水稳定性与吸附性能进行了研究。结果表明,晶种法可以在2 d内合成出硅铝原子比在3以上、收率达到65%的UZM-9分子筛;所得分子筛的CO2吸附容量可以达到5 mmol/g以上,吸附热为34 kJ/mol,CO2/CH4、CO2/N2与CH4/N2的平均分离因子分别为100、240与2.4,CO2分离性能优良且具有一定耐水性能。
摘要:
Utilizing microbial fuel cells (MFCs) is a promising technology for energy-efficient domestic wastewater treatment, but it still faces practical barriers such as low power generation. In this study, the LaMnO3 perovskite-type oxide nanoparticles and nickel oxide/carbon nanotube/polyaniline (NCP) nanocomposite (the cathode and anode catalysts, respectively) have been prepared and used to enhance power density of MFC. The prepared La-based perovskite oxide catalysts were characterized by X-ray diffraction (XRD) and scanning electron microscopies (SEM). The electrocatalytic properties of the prepared catalysts were investigated through cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) and Tafel plot at ambient temperature. Results show the exchange current densities of LaMnO3/carbon cloth cathode and NCP nanocomposite/carbon cloth anode were 1.68 and 7 times more compared to carbon cloth cathode, respectively. In comparison to the bare carbon cloth anode, the MFC with the modified electrodes shows 11 times more enhancement in power density output which according to electrochemical results, it can be due to the enhancement of the electron transfer capability. These cathodic and anodic catalysts were examined in batch and semi-continuous modes to provide conditions close to industrial conditions. This study suggests that utilizing these low cost catalysts has promising potential for wastewater treatment in MFC with high power generation and good COD removal efficiency.
摘要:
以离子交换树脂(D001)为载体,四乙烯五胺(TEPA)为改性剂,采用三种不同的方法制备了一系列固态胺吸附剂。采用N2吸附-脱附、傅里叶变换红外光谱(FT-IR)、热重分析(TGA)等手段对吸附剂进行表征。在固定床反应器中考察了TEPA负载量、吸附温度、进气流量和CO2分压等因素对CO2吸附性能的影响。结果表明,配位法制得的固态胺吸附剂分散性和稳定性较好,且在TEPA负载量为40%,吸附温度为65℃,进气流量为40 mL/min时有最大CO2吸附量达4 mmol/g。经过10次吸附-脱附循环实验后,CO2吸附量下降3.98%。热力学、动力学研究结果表明,CO2吸附是物理吸附和化学吸附的结果。
摘要:
搭建燃煤热态实验系统,研究脱硫废水蒸发对电除尘和脱硫系统的影响;考察脱硫废水蒸发前后细颗粒粒径的变化、电除尘出口PM2.5和SO3浓度变化;分析增强电除尘脱除PM2.5和SO3机理。结果表明,脱硫废水蒸发后,蒸发室出口细颗粒粒径峰值由0.1 μm增大到1.1 μm,观察脱硫废水蒸发前后扫描电镜,明显观察到废水蒸发后颗粒团聚长大,颗粒间存在絮状物;采用脱硫废水烟道蒸发后,电除尘细颗粒脱除效率提高5%左右,PM2.5数量浓度脱除效率提高25%左右;SO3脱除效率为60%-80%,烟气中SO3浓度对增强电除尘脱除PM2.5和SO3均有影响;脱硫废水蒸发对脱硫系统的效率和脱硫浆液的pH值没有影响。