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2022年 第24卷 第2期    刊出日期:2022-06-30
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2022, 24(2):  0. 
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Review
非晶态催化剂用于电解水制氢的研究进展
张聪 王帅洋 荣峻峰 米万良
2022, 24(2):  1-13. 
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Hydrogen production by water electrolysis is an important route for generating green hydrogen. However, the development of efficient and inexpensive electrocatalysts is crucial for future industrial applications. Amorphous catalysts possess a large specific surface area with abundant structural defects. In addition, their structures can be tuned to provide more efficient active sites, leading to superior water electrolysis activity compared with their crystalline counterparts. In this review, we summarize recent progress on amorphous electrocatalysts for water splitting, with a focus on the reaction mechanisms under both acidic and alkaline conditions, catalyst synthesis, and the application of these catalysts to the hydrogen and oxygen evolution reactions. Moreover, we highlight the current challenges and promising opportunities relating to amorphous catalysts for electrochemical water splitting.
Process Research
双功能催化剂上四氢萘加氢裂化生成单环芳烃的反应网络研究
鞠雪艳
2022, 24(2):  14-22. 
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Conversion of LCO (light cycle oil) to BTX (benzene, toluene, and xylene) is an economically valuable method for refineries. However, this approach still faces difficulties as the main reactions are not clearly understood. Here we study the detailed hydrocracking pathway of typical reactants, 1-methylnaphthalene and tetralin, through molecular simulations and experiments to improve our understanding of the conversion process of LCO to BTX. Molecular simulations demonstrate that the rate-determining step is the isomerization pathway of six-membered ring to five-membered ring in tetralin as its activation energy (ΔEa) is the highest among all the reactions and the order of ΔEa of reactions is isomerization > ring-opening ≈ side-chain cleavage. The results of experiments show that with the increase in reaction depth, i.e., through a high temperature (350 – 370 °C) and low LHSV (4.5 – 6.0 h−1), isomerization, ring-opening, and side-chain  cleavage reactions occurred, thus improving the selectivity and yield of alkyl aromatics.
水力空化改质对重质原油沥青质及性质的影响
李康 韩海波 雷杰 王有和 李德坤 Mark J. Rood Fazle Subhan 阎子峰
2022, 24(2):  23-33. 
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利用水力空化过程产生局部的高温、高压、高射流以及强大的剪切力等极端化学物理条件改质处理沙特重质原油,试验结果表明:沙特重质原油经过水力空化改质后粘度由13.61降低至7.22mm2/s,残碳由7.16%降低至6.48%,实沸点蒸馏后减压渣油降低1个百分点。进一步采用APPI FT-IR MS、XRD、FT-IR、SEM和粒度分布等技术研究了水力空化改质对沙重原油分子组成,沥青质团聚体微晶结构、沥青质胶束粒径分布、沥青质官能团、沥青质形貌等方面的影响,从分子角度阐述空化改质重油的机理。研究结果表明:水力空化改质后沙重原油分子量分布、芳烃类化合物缔合作用变小;沥青质对低DBE化合物吸附性能降低;沥青质团聚体微晶结构更加松散;沥青质胶束粒度分布降低;沥青质分子相互团聚作用力减弱。进一步考察了水力空化改质前后减压渣油延迟焦化性能,改质处理后焦炭产率降低1.85个百分点,液体收率和气体产率分别增加1.52和0.33个百分点,水力空化改质对沥青质性质、结构特点的改善能够有效的提高其加工性能。
Acid Desulfurization Exploration of High-Sulfur Petroleum Coke Intensified by Pre-calcination, H2O2 treatment, and Ultrasound
王港 毛秋云 刘伟 周宇 仲奇凡
2022, 24(2):  34-45. 
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The present investigation reported the acid desulfurization of high sulfur petroleum coke (petcoke) powder intensified by pre-calcination, H2O2, and ultrasound combing X-ray photoelectron spectroscopy, thermal gravity/ derivative thermogravimetry, pore distribution, specific surface area, energy-dispersive X-ray spectroscopy, transmission electron microscopy, and Fourier transform infrared spectroscopy analyses. Results showed that pre-calcination at 800 °C for 6 h, mixing with HNO3 (8 mol/L) + H2O2 (2 mol/L) solution at a liquid-to-solid ratio of 10 ml/g, 60 °C, and 40 kHz ultrasound power of 400 W assisted for at least 6 h, and over 45% of sulfur atoms in Tianjin coke and Qilu coke (particle size < 0.1 mm) were removed efficiently. Besides, the specific surface area of petcoke particles increased from 0.7 m2/g to 301.49 m2/g. After desulfurization, the pore distribution of petcoke particles was concentrated more on smaller pores with micropores formed. This allowed desulfurized petcoke to be superior to the preparation of activated carbon and petcoke gasification. Reactive molecular dynamics (ReaxFF) simulation results revealed HNO3 continuously oxidized the carbon atoms adjacent to S in petcoke macromolecules, and promoted S to be removed from petcoke via destroying the stable structure between C and S. The transformation behavior of thiophene S could be summarized as follows: thiophene S → carbon branched chain S → CO2S → C2O2S → C2O3NS → C2O4S → CO2S.
Removal of Heteroaromatic Sulfur Compounds by a Non-noble Metal Fe Single-atom Adsorbent
吕燕军 文婕
2022, 24(2):  46-57. 
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Sulfur-containing compounds (SCCs) need to be removed from fuels due to their negative effects on the environment and catalytic stability. In this study, a novel non-noble metal Fe single-atom adsorbent (SA-Fe/CN) was synthesized using a core-shell strategy and applied to the adsorptive removal of benzothiophene (BT) and dibenzothiophene (DBT). Simultaneously, the adsorption isotherms, thermodynamics, and kinetics of DBT and BT on SA-Fe/CN were studied. SA-Fe/CN exhibited a strong adsorption affinity to DBT, and the isothermal equilibrium was well described by the Langmuir isotherm model. Thermodynamic analysis showed that the Gibbs free energy values were negative (ΔG0 <0), illustrating that the adsorption process for DBT and BT was favorable and spontaneous. Adsorption kinetics was analyzed using pseudo-first-order and pseudo-second-order, the results displayed that the adsorption process conformed to the pseudo-second-order kinetic model with higher R2 values (0.9994, 0.9987). The adsorption results also indicated that the adsorption capacity of SA-Fe/CN for DBT and BT reached 163.21 mg-S/g and 93.82 mg-S/g, respectively, which might be attributed to the highly active sites of the single atom and the electrostatic interaction with the sulfide. Therefore, this study proves SA-Fe/CN is a promising adsorbent for DBT removal.
Scientific Research
High-performance composite epoxy coating based on 2D Co2(OH)2BDC and electrospinning-made PAN nanofiber membrane
程志林
2022, 24(2):  58-67. 
摘要 ( 19 )   PDF (1312KB) ( 49 )  
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Based on a two-dimensional (2D) Co–MOF (Co2(OH)2BDC) with a self-contained organic interface and low conductivity, a composite epoxy coating (2D Co2(OH)2BDC-PAN/EP) was constructed by a two-step preparation. First, a polyacrylonitrile (PAN) nanofiber membrane was electrospuned on the surface of Q235 steel, followed by coating using the epoxy coating (EP) containing 2D Co2(OH)2BDC. The 2D Co2(OH)2BDC-PAN/EP composite epoxy coatings showed robust mechanical performance and excellent corrosion resistance capacity.
乙醇的添加对汽油喷射自燃性质的影响及其与辛烷值的关系
王俊 杨鹤 胡晓明 宋海清 张然 田华宇
2022, 24(2):  68-75. 
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In this study, the spray auto-ignition properties of binary primary reference fuels (PRFs) of 2,2,4-trimethylpentane and n-heptane with different research octane numbers (RONs) were measured according to the industry standard NB/SH/T 6035 to determine their ignition delay times at various initial temperatures. Furthermore, the auto-ignition properties were investigated after blending the PRFs with various amounts of ethanol. The results revealed a very good correlation between the derived cetane number and the RON for the PRFs in both the presence and absence of ethanol. In addition, a concept of ignition delay sensitivity was developed for ethanol-containing fuels that exhibited a close relationship with the octane sensitivity, which is defined as the RON minus the motor octane number (MON). Finally, the developed method was applied to conveniently estimate the RON and MON values of several ethanol-containing fuels by simply measuring their autoignition properties.
Kinetic Study of Homogeneous Carbonylation of Ethanol Containing Bisdiphenylphosphinomethane Disulfide Ligands
龙浩宇 徐林 宋建华 王小平 王唯充 刘殿华
2022, 24(2):  76-84. 
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Homogeneous rhodium-catalyzed carbonylation of ethanol is a potential route for the preparation of propionic acid, but its industrialization is hindered by the low reaction rate. In order to improve the reaction rate, a batch of bisdiphenylphosphine ligands were tested in the rhodium-catalyzed reaction system. By comparing the space-time yield (SYT) of the catalytic system, the effects of ligands, components, and process conditions in the catalytic system were studied. In the presence of 1,1-bis(diphenylthiophosphinyl)methane (dppmS2), the activity and stability of the catalysts were improved significantly. The effects of temperature, carbon monoxide pressure, and the content of ligand, Rh, EtI, and lithium iodide on the reaction rate were investigated in a Hastelloy autoclave. The results show that dppmS2 and Rh are preferably added in a molar ratio of 1:2, and the optimal catalytic system is composed of 10wt% EtI, 1000ppm rhodium iodide, and 10% lithium iodide. The most suitable reaction temperature is 463k, the optimal CO pressure is 3.0MPa and the maximum STY is 4.30 mol·h-1·L-1. A macroscopic kinetic model was established in the temperature range of 442K-463K. The model data was regressed and validated. The activation energy of the reaction was 28.01 kJ mol-1. Residual analysis and statistical tests showed that the kinetic experiments were reasonable and acceptable.
Catalyst Research
Industrial Preparation and Acid Resistance of Ultra-stable Y Zeolite with Small Cell Size Produced by Gas-phase Method
张婧 贾继顺 沙昊 卢冠群 严加松 王生吉 周灵萍
2022, 24(2):  85-90. 
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The zeolite HSY-S with small cell size prepared by gas-phase ultra-stable method had been researched and developed, and industrial preparation tests of HSY-S had been successfully carried out for the first time in the world. The acid resistance of HSY-S prepared in industrial was investigated by acid solutions with different pH values. The structures and properties of HSY-S and its acid-treated samples were characterized by XRD, XRF,BET and IR. The results showed that the zeolite HSY-S has the characteristics of high crystallinity, good stability, large specific surface area and good acid resistance.
纳米棒状NiMoO4催化剂的可控制备及其在碱性电解液以及模拟海水电解液中析氢性能的研究
蒋博龙 史顺杰 崔艳艳 姜楠
2022, 24(2):  91-100. 
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本研究通过水热法将NiMoO4纳米棒直接负载于碳布(CC)表面,制备了不同过渡双金属Ni-Mo负载量的一系列NiMoO4-NRs/CC-x (x代表负载量)析氢(HER)催化剂。所制备的催化剂用于碱性电解液以及模拟海水HER过程的研究。结果表明,所制备的NiMoO4-NRs/CC-10催化剂具有较高的HER活性,在碱性电解液中,其电流密度10 mA/cm2所对应过电势以及塔菲尔斜率分别为244.8 mV和95 mV/dec。除此之外,该催化剂同样具有极好的电导性(Rct<1Ω)以及稳定性。即便在模拟海水电解液中,NiMoO4-NRs/CC-10催化剂同样展现出了高HER活性及高稳定性。导致该催化剂高活性的主要原因为NiMoO4纳米棒结构内部过渡金属Ni与Mo之间以及CC与NiMoO4纳米棒之间的协同作用。两种作用的存在不仅提高了催化剂的电导性,同时也加快了产氢速率。
Simulation and Optimization
A multi-objective optimization approach for the design of heat exchanger network (HEN) in process industries
谭强 陈玉婷 徐燕燕 叶爽 肖浩 黄伟光
2022, 24(2):  101-111. 
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To simultaneously improve the quantity and quality of heat recovery in a heat exchanger network (HEN), this study conducts a theory analysis based on the first and second laws of thermodynamics. Under the premise of maximizing the heat recovery quantity of HEN, ?diss is used as an evaluation index to optimize the quality of heat recovery. Meanwhile, the total annual cost (TAC) is considered as another optimization objective to ensure the economic feasibility of the HEN. A superstructure-based multi-objective mixed integer non-linear programming approach is put forward to solve the trade-off between minimizing ?diss and minimizing TAC. This allows for the optimum HEN structure to be obtained. A well-studied example is solved to highlight the benefits of the proposed method.
Modeling of C8 Aromatics Isomerization in a Radial Bed Reactor
高宁晗 唐晓津 周震寰 徐建
2022, 24(2):  112-117. 
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Reactor models were developed to describe the isomerization reaction process of C8 aromatics by applying a sixcomponent sequential reaction network. Lab-scale experimental data were used in an axial bed reactor model, and dynamic parameters were fitted by simulated annealing algorithm. In addition, industrial data and calculated dynamic parameters were used to determine the six-component concentration distributions using a radial reactor model. The influence of backmixing on reaction performance was investigated. It was found that the model considering back-mixing was much closer to the real industrial reaction process.
沥青质-二甲苯体系中结构组成对沥青质自扩散系数的影响
杨海洋 王春璐 任强 王丽新 颜学敏
2022, 24(2):  118-125. 
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以沥青质-二甲苯体系模拟稠油体系,采用分子模拟方法考察沥青质致黏机理。沥青质-二甲苯平衡体系中沥青质的自扩散主要受沥青质分子间相互作用的影响。沥青质分子间相互作用能越大,沥青质自扩散的越慢,对应的稠油黏度越大。而沥青质分子间相互作用主要包括芳香环之间的π-π作用和含有较强电负性杂原子基团间氢键两方面。这将为稠油降黏提供理论指导。
Environmental Protection
Effects of combined stress from salt and herbicide on microbial remediation of soil contaminated by n-Hexadecane and phenanthrene
刘炳琨 张秀霞 李茹月 郝博宇 李婧 尹凌皓 白雨昊 宋佳宇 顾莹莹 孙娟
2022, 24(2):  126-137. 
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In this study, physicochemical analysis, cluster analysis, high throughput sequencing were used to investigate the effects of combined salt and herbicide stress on microbial remediation of soil contaminated by n-Hexadecane and phenanthrene. Based on the physical and chemical properties of the soil, the differences in microbial quantity and enzyme activities were analyzed among the samples, and the influence on the distribution of soil community structure was mainly discussed. After 120 days of indoor simulated remediation, the cumulative degradation rate of n-hexadecane decreased by 94.92% (blank control), 96.96% (low concentration of salt and herbicide glyphosate stress), 65.07% (high concentration of salt and herbicide glyphosate stress), and that of phenanthrene decreased by 87.33% (blank control), 86.25% (low concentration of salt and herbicide glyphosate stress), 58.45% (high concentration of salt and herbicide glyphosate stress), respectively. The analysis of physical and chemical properties indicated that the combined stress of salt and herbicides could decrease the reduction efficiency of organic matter, total nitrogen, and total phosphorus, and also restrict the growth of microorganisms and enzyme activities. Cluster analysis implied that the non-stress group was similar to the low-concentration compound stress group during different repair periods, while the high-concentration compound stress group was quite different. High-throughput sequencing showed that dominant bacteria phyla changed from Firmicutes to Actinobacteria within 120 days of remediation.
二氧化钛纳米棒在可见光下的光催化活性及其在降解有机污染物中的应用
贺婕 史超杰 杨正春 侯强 张瑞 朱田佳 潘鹏 张平
2022, 24(2):  138-146. 
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The FTO/TiO2 seed layer/TiO2 nanorods were prepared by ion beam deposition and hydrothermal methods. Under UV light, the photocurrent density of FTO/TiO2 seed layer/TiO2 nanorods can reach 1.39 mA/cm2, which is higher than that without seed layer and nanorods structure. Not only that, the FTO/TiO2 seed layer/TiO2 nanorods can also adsorb visible light, which overcomes the defect that traditional TiO2 can not absorb visible light. The photocurrent density of FTO/TiO2 seed layer/TiO2 nanorods can reach 0.21 mA/cm2 under visible light. The increased performance resulted from the deposition of the TiO2 seed layer, which can reduce the band gap of TiO2. FTO/TiO2 seed layer/TiO2 nanorods also exhibited high photodegradation ability for organic pollutant methylene blue (MB). Within 120 min, 77.3% MB can be degraded, and the degradation rates remained almost unchanged after four cycles. Not only that, compared with powdered photocatalysts, FTO/TiO2 seed layer/TiO2 nanorods is easy to recover, and it can be reused by rinsing it with water several times and drying it naturally after the reaction.
超细颗粒Bi3TaO7与二维Fe2O3纳米片组装:增强水中残留四环素的净化作用
刘晓庆
2022, 24(2):  147-158. 
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Composites of 2D/0D Fe2O3-Bi3TaO7 (FO-BTO) prepared by a hydrothermal method in which superfine Bi3TaO7 particles were mounted onto lamellae of Fe2O3 sheets could efficiently remove aqueous tetracycline (TC) residues. The optimal composite FO-3BTO had a TC removal rate of 95% in 120 min under solar light, and its overall properties were better than those of reported photocatalysts. According to XRD, HRTEM, XPS, SEM, PL, EIS, and photocurrent tests, Fe2O3 and Bi3TaO7 composites formed on effective S-scheme heterojunctions, and the tight contact structure contributed to the increase in efficiency of aqueous TC residue removal.