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

2022年  第50卷  第2期

显示方式:
2022-2 目录
2022, 50(2): 1-6.
摘要:
摘要:
In order to improve the tar quality by decreasing the heavy tar content and ensuring high tar yield, in-situ catalytic upgrading of tar from the integrated process of coal pyrolysis coupled with steam reforming of methane was conducted over carbon (KD-9) based Ni catalyst. The results show that at 650 °C, the tar yield of CP-SRM over 5Ni/KD-9 is 24.4%, which is a little lower than that of without catalyst, while the light tar yield (i.e.,18.9%) is 1.4 times higher than that of without catalyst, and the content of C2, C3 and C4 alkyl used as a substitute for benzene significantly increases tar yields by 0.5, 0.6 and 4.0 times, respectively. The content of phenols and naphthalenes in tar also increases dramatically after upgrading. Isotope tracer approach combined with the mass spectra of typical components was employed in exploring the mechanism of the upgrading process. The results show that 5Ni/KD-9 catalyzes coal tar cracking and SRM at the same time. Small free radicals such as ·CHx, ·H and ·OH generated by SRM can combine with free radicals from tar cracking, thus avoiding excessive cracking of tar.
摘要:
本研究以哈密原煤和脱矿煤为原料,研究煤液化铁基催化剂对煤焦结构和气化反应性的影响。利用扫描电镜能谱仪和物理吸附仪研究煤焦表面形貌、元素分布和介孔特性,利用热重分析仪研究煤焦气化特性,采用model-fitting和model-free方法研究反应动力学。结果表明,脱矿和负载催化剂对煤焦表面附着物的影响较主体基质明显。负载催化剂的煤焦比表面积显著增加。铁基催化剂提升煤焦气化活性可归因于煤焦表面富集较多Fe和AAEMs等元素,以及比表面积的增大。负载催化剂的脱矿煤焦表现出较大的相对催化活性,且其对升温速率和碳转化率的变化不敏感。煤焦气化特性的差异将随升温速率的升高而减小。铁基催化剂可提高原煤焦的气化反应指前因子A,降低脱矿煤焦的反应活化能Ea。非等温条件下,煤焦气化反应活化能随转化率的增加而降低。根据模型拟合度和动力学补偿效应,随机孔模型是描述煤焦气化的最佳模型,且更适合于脱矿煤焦(催化)气化。
摘要:
利用热重分析仪和管式炉实验,研究了煤矸石与半焦的富氧混烧特性,考察了半焦混烧比例、O2含量和反应温度对燃烧特性和污染物排放特性的影响。结果表明,混烧半焦和提高O2含量均可显著改善混合燃料的燃烧性能,当半焦混烧比例为75%时,着火和燃尽指数最高。随半焦混烧比例增大,CO和SO2转化率均逐渐降低。提高反应温度,CO转化率降低,SO2转化率增大,NO转化率呈现先升高然后降低或缓慢增加趋势。反应温度为900 ℃时,混烧半焦可降低燃烧过程的NO排放量。其余反应温度下,混烧半焦会增大NO转化率。随O2含量升高,混合燃料富氧燃烧过程的CO转化率降低,NO转化率升高,SO2峰值释放量和转化率呈先降低后升高的趋势。当O2体积分数为20%时,SO2转化率最低。
摘要:
利用小试精馏装置对生物油模型化合物进行蒸馏实验,通过调节系统的真空度将生物油模型化合物分别在常压和减压状态下进行蒸馏,分析并总结了馏分中各组分的变化规律。结果表明,随着系统内真空度的不断升高,生物油模型化合物的总馏出率不断增加且结焦率不断降低,水分更容易被蒸出,馏分中有机物的初馏温度降低而馏出率增加。因此,增大真空度可有效分离生物油模型化合物的组分并降低蒸馏的能量损耗;当真空度为−0.08 MPa时,生物油模型化合物的蒸馏效果最好,其中,乙酸和糠醛的馏出率分别可达99.50%和65.88%、苯酚和愈创木酚的馏出率为25.19%和26.17%,均超过25%。
摘要:
二甲醚羰基化反应是在二甲醚分子中定向插入一氧化碳的重要增碳反应,在工业生产中具有重要意义。近年来,研究发现廉价的丝光沸石可催化二甲醚羰基化反应,且具有较高的反应活性和十分优异的羰基化产物选择性,因此,得到了广泛的研究。本文对丝光沸石催化二甲醚羰基化的研究进行综述,介绍了羰基化反应的机理,并总结丝光沸石内部酸性位点调控的各种方法以及对羰基化反应的影响。
摘要:
在煤矿开采及燃气轮机等工业应用或移动源领域存在甲烷大体量排放,且传统高温焚烧法会导致二次污染,因此,在低温下实现甲烷高效转化成为亟待解决的问题。从能源利用和环境保护角度,催化燃烧技术是实现甲烷废气高效净化的有效措施。本文综述了近年来催化机理和催化剂的研究进展。首先,在实验和理论基础上,总结概括了甲烷氧化机理,其中,重点阐述了“Two-term”模型;其次,系统介绍了各催化剂的性能优缺点和改性技术;最后,对甲烷催化未来研究提出展望,即采用结构优化方法来暴露更多活性位点或产生多组分协同催化效果、利用非贵金属掺杂等强化手段制备高效催化剂、进一步通过多重外场共同激发催化性能。此外,各类催化机理的自身完善和新型机理描述符的开发也是未来研究的重要方向。
摘要:
随着现代社会的快速发展,人们对能源的需求与日俱增,目前,发展中国家仍以化石燃料为主要能源投入,其燃烧产生的二氧化碳排放带来的温室效应和环境问题已引起举世关注。因此,通过对二氧化碳进行捕集、封存与转化利用,实现碳减排和碳中和目标成为目前研究的热点。其中,二氧化碳基高分子材料的制备在实现二氧化碳资源化利用的同时,也为聚合物的绿色生产提供了新思路。基于此,本文综述了二氧化碳在聚氨酯中的资源化利用现状,着重对其在材料中的物理、化学应用进行了阐述,并详细介绍了在转化利用过程中的制备技术和方法。
摘要:
H-[B,Al]-ZSM-5 zeolites were synthesized with glucose as assistant template to catalyze methanol converting toward propylene. The superior catalytic performance in terms of the propylene selectivity and the activity longevity was related to high ratio of weak acid to strong acid for favorable production of propylene and to high mesoporosity for improved diffusion of reactants and prevention from fast coking. More framework Al siting in the straight or sinusoidal channels of the MFI zeolite could also enhance the propylene/ethylene ratio due to the promotional effect on propylene formation. Low weak acid density was conducive to the production of high propylene/ethylene ratio. With the B/Al ratio of 2 and the (Al2+B2)/Si ratio of 0.01, HZ5-G-2B was applied in the methanol to propylene reaction at CH3OH/H2O (1∶1.2) WHSV of 1.8 h−1 and 480 °C. Propylene selectivity of 51.6%, the ${\rm{C}}_{{2-4}}^ {=} $ selectivity of 83.7% and complete conversion of methanol were achieved. The propylene/ethylene ratio was 2. The catalytic activity kept stable for 580 h.
摘要:
采用油酸铁热分解法制备出不同尺寸(4−19 nm)的γ-Fe2O3纳米颗粒,在350 ℃下,于5%CO/He、5%CO/10%H2/He和5%CO/20%H2/He的三种气氛中,使用原位XRD反应装置研究了γ-Fe2O3纳米颗粒的碳化过程与物相变化规律,同时结合Raman、CO-TPR和TEM等手段对样品进行了表征。结果表明,γ-Fe2O3纳米颗粒完全碳化后会形成稳定比例的χ-Fe5C2θ-Fe3C的混合相;在相同碳化气氛下,随γ-Fe2O3颗粒尺寸增大完全碳化所需时间缩短,尺寸较小的γ-Fe2O3颗粒表面残留炭较多,会抑制碳化反应进程,碳化相中θ-Fe3C相对含量随γ-Fe2O3纳米颗粒尺寸增大而增高;相同尺寸的γ-Fe2O3颗粒在不同气氛下碳化,完全碳化所需时间随H2分压增大先缩短后略有延长,碳化相中θ-Fe3C相对含量随H2分压增大而增高。通过调节γ-Fe2O3颗粒尺寸和碳化气氛可定向制得合适比例的χ-Fe5C2θ-Fe3C混合相,这一结果有益于费托合成铁基催化剂中的铁碳化物活性相结构的优化。
摘要:
The dehydrogenation performance of vanadyl catalysts was closely related to the form of surface vanadyl species. To enhance the vanadium dispersion, phosphorus was adopted to modify V-MCM-41 catalysts by using organic vanadium and phosphorus precursors. The influence of phosphorus introduction to the mesoporous structure and vanadyl species were investigated by various characterization techniques. The results showed that the catalysts could maintain ordered hexagonal mesoporous structures though the specific surface area slowly decreased along with the increase of phosphorus content. Both the reducibility and dispersion of the surface vanadyl species were improved. The proportion of polymerized vanadyl species obviously decreased due to the presence of phosphorus species. The propane dehydrogenation reaction results showed that both the catalytic performance and the catalyst stability were improved. Both the maximum surface vanadyl site density and optimum propane dehydrogenation performance were obtained over the sample with Si/P molar ratio of 30.
摘要:
分别以1,3,5-三异丙苯和正辛烷为不同分子尺寸催化裂解原料,以1-己烯为叠合原料,评估了合成的多级孔ZSM-5分子筛催化剂上催化裂化反应和烯烃叠合反应的耦合机制。模型化合物催化裂解反应结果表明,在合成的多级孔ZSM-5分子筛上不同尺寸分子裂解性能受到抑制,1,3,5-TIPB裂解能力下降,正辛烷裂解初始转化率由70%降低到20%。而多级孔ZSM-5分子筛的1-己烯叠合催化活性得到提升,高于工业ZSM-5分子筛,叠合产物以二聚物为主。分子筛中强酸酸量的降低可抑制催化裂化反应的进行,促进C6烯烃低聚为二聚物和三聚物(航空煤油的理想成分)的能力。因此,从抑制催化裂化的角度进行催化剂设计,可有效提高催化剂的烯烃叠合反应性能。
摘要:
Recently, a new carbon nitride (C3N5) photocatalyst has attracted much attention due to its excellent light harvesting and unique 2D structure. However, high recombination rates of electron-hole pairs of bulk C3N5 serious affect the photocatalytic performance. Herein, nickel oxide (NiO) modified C3N5 p-n junctions photocatalyst was synthesized by a facile hydrothermal method. Results indicated that the 9-Ni/C3N5 nanosheet photocatalyst showed excellent hydrogen production efficiency under visible light. The hydrogen production rate reached 357 μmol/(g·h), which was 107-fold higher than that of pristine C3N5. The high catalytic performace was attributed to the 9-Ni/C3N5 p-n junctions which could efficiently promote photogenerated electron-hole pair separation and thus promote the hydrogen evolution reaction.
摘要:
采用水热法和溶剂热法制备BiOBr、Bi3O4Br和Bi4O5Br2三种光催化剂,通过X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)与紫外-可见漫反射光谱(UV-vis DRS)表征光催化剂的晶体结构、表面形貌和光学性能,利用密度泛函理论计算光催化剂的能带结构和态密度,在可见光照射下,通过降解RhB考察光催化剂的活性。结果表明,Bi的含量会影响光催化剂的导带位置和禁带宽度,Bi4O5Br2光催化剂降解效果最好,能够在50 min内将RhB完全降解。自由基捕获实验证明,超氧自由基(·${\rm{O}}_2^- $)是光催化降解RhB的主要活性物质。