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decarbonisation of energy-intensive industries: a comparative review of techno-economic feasibility of solid looping

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1291-1317 doi: 10.1007/s11705-022-2151-5

摘要： Carbon capture and storage will play a crucial role in industrial decarbonisation. However, the current literature presents a large variability in the techno-economic feasibility of CO2 capture technologies. Consequently, reliable pathways for carbon capture deployment in energy-intensive industries are still missing. This work provides a comprehensive review of the state-of-the-art CO2 capture technologies for decarbonisation of the iron and steel, cement, petroleum refining, and pulp and paper industries. Amine scrubbing was shown to be the least feasible option, resulting in the average avoided CO2 cost of between 62.7 €·tCO2−1 for the pulp and paper and 104.6 €·tCO2−1 for the iron and steel industry. Its average equivalent energy requirement varied between 2.7 (iron and steel) and 5.1 MJth⋅kgCO2−1 (cement). Retrofits of emerging calcium looping were shown to improve the overall viability of CO2 capture for industrial decarbonisation. Calcium looping was shown to result in the average avoided CO2 cost of between 32.7 (iron and steel) and 42.9 €·tCO2−1 (cement). Its average equivalent energy requirement varied between 2.0 (iron and steel) and 3.7 MJth⋅kgCO2−1 (pulp and paper). Such performance demonstrated the superiority of calcium looping for industrial decarbonisation. Further work should focus on standardising the techno-economic assessment of technologies for industrial decarbonisation.

关键词： industrial CO2 emissions     CCS deployment     carbonate looping     net-zero industry     carbon capture benchmarks    

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Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第6期   页码 1130-1138 doi: 10.1007/s11783-015-0821-y

摘要： Chemical looping combustion is a promising technology for energy conversion due to its low-carbon, high-efficiency, and environmental-friendly feature. A vital issue for CLC process is the development of oxygen carrier, since it must have sufficient reactivity. The mechanism and kinetics of CO reduction on iron-based oxygen carriers namely pure Fe O and Fe O supported by alumina (Fe O /Al O ) were investigated using thermo-gravimetric analysis. Fe O /Al O showed better reactivity over bare Fe O toward CO reduction. This was well supported by the observed higher rate constant for Fe O /Al O over pure Fe O with respective activation energy of 41.1±2.0 and 33.3±0.8 kJ·mol . The proposed models were compared via statistical approach comprising Akaike information criterion with correction coupled with F-test. The phase-boundary reaction and diffusion control models approximated to 95% confidence level along with scanning electron microscopy results; revealed the promising reduction reactions of pure Fe O and Fe O /Al O . The boosting recital of iron-based oxygen carrier support toward efficient chemical looping combustion could be explained accurately through the present study.

关键词： chemical looping combustion     iron-based oxygen carriers     reduction kinetics     carbon monoxide     statistics    

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Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1726-1734 doi: 10.1007/s11705-022-2188-5

摘要： Chemical looping reforming of methane is a novel and effective approach to convert methane to syngas, in which oxygen transfer is achieved by a redox material. Although lots of efforts have been made to develop high-performance redox materials, a few studies have focused on the redox kinetics. In this work, the kinetics of SrFeO3−δ–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor. During the methane reduction, combustion occurs before the partial oxidation and there exists a transition between them. The weight loss due to combustion increases, but the transition region becomes less inconspicuous as the reduction temperature increased. The weight loss associated with the partial oxidation is much larger than that with combustion. The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n = 3 (A3 model) with an activation energy of 59.8 kJ∙mol‒1. The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law. The partial oxidation is half order with respect to methane pressure. The proposed rate law could well predict the reduction kinetics; thus, it may be used to design and/or analyze a chemical looping reforming reactor.

关键词： chemical looping reforming     SrFeO3−δ/CaO·MnO nanocomposite     reduction kinetics     Avrami–Erofeyev model     pressure-dependent term    

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Polyethylene glycol-supported ionic liquid as a highly efficient catalyst for the synthesis of propylene carbonate

Rui YAO, Hua WANG, Jinyu HAN

《化学科学与工程前沿（英文）》 2012年 第6卷 第3期   页码 239-245 doi: 10.1007/s11705-012-1297-y

摘要： The coupling reaction of propylene and CO to form propylene carbonate (PC) was promoted by an ionic liquid (IL) covalently bound to polyethylene glycol (PEG). The supported ionic liquid, which has both acidic and basic components, proved to be an active catalyst for PC synthesis under mild conditions. The effects of different cations and anions, reaction temperature, CO pressure, and reaction time were investigated. It was demonstrated that the acid group in the catalyst plays an important role in the reaction. With this system, a high PC yield (95%) was achieved under mild conditions (3.0 MPa, 120°C and 4 h) without a co-solvent. In addition, the catalyst was readily recovered and reused. Based on the experimental results, a plausible mechanism for the catalyst was proposed.

关键词： ionic liquid     PEG-supported ionic liquid     carbon dioxide     propylene carbonate    

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Effect of wastewater composition on the calcium carbonate precipitation in upflow anaerobic sludge blanket

Shucheng YANG, Yanling HE, Charles CHOU, Pengxiang ZHANG, Dongqi WANG, Yonghong LIU,

《环境科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 142-149 doi: 10.1007/s11783-010-0026-3

摘要： Calcium carbonate often precipitates in anaerobic reactors treating wastewater with high calcium content. The aim of this paper is to study the effect of wastewater composition on calcium carbonate precipitation in upflow anaerobic sludge blanket (UASB) reactors. Two laboratory-scale UASB reactors were operated with calcium-containing influents using acetate and carbohydrate as substrate, respectively. There was an obvious accumulation of inorganic precipitate observed in the biogranules. Observations via scanning electron microscope (SEM) and energy dispersive spectroscopy (EDS) showed that the acclimated biogranules in the two reactors differed in microstructure. Calcium carbonate was found to have precipitated on the surface of acetate-degrading biogranules, but precipitated at the core of the carbohydrate-degrading biogranules. The results indicated that substrates had significant influence on the location of calcium carbonate precipitation in anaerobic granular sludge, which was expected due to the different methanogens distribution and pH gradient within the granular sludge degrading various substrates. Moreover, the location of calcium carbonate precipitation substantially affected the specific methanogenic activity (SMA) of the granular sludge. The SMA of the acetate-degrading biogranules dropped from 1.96 gCOD·gVSS·d to 0.61 gCOD·gVSS·d after 180-d of operation in the reactor. However, the SMA of the carbohydrate-degrading biogranules was not adversely affected by calcium carbonate precipitation.

关键词： calcium carbonate     precipitation     anaerobic granular sludge     wastewater composition     microstructure     upflow anaerobic sludge blanket (UASB)    

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化学链概念在共沸物分离中的应用 Article

高鑫, 耿雪丽

《工程（英文）》 2021年 第7卷 第1期   页码 84-93 doi: 10.1016/j.eng.2020.06.022

摘要：

为了生产高端化学品和资源回收而进行共沸物分离的必要性，促使人们对化学工业中新分离方法的开发进行了大量研究。本文基于化学链的概念，借助可逆反应辅助精馏技术，提出了一种绿色可持续的共沸物分离方法。化学链分离（CLS）方法的核心概念是选择一种既能与共沸物发生反应，又能通过逆反应进行循环利用的反应物，以闭合回路并实现共沸物分离。本文旨在从分离原理、反应物选择和案例分析（如烯烃、烷烃、芳烃和多元醇产品的分离）等的基础上，为CLS方法的基本理论和应用提供一个有益的见解。本文为产品精制和共沸体系分离过程中的化学分离工艺的过程的强化提供指导和参考，以促进化工行业的可持续发展。

关键词： 化学链     共沸物     反应精馏     反应物选择     过程强化    

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Novel eco-efficient reactive distillation process for dimethyl carbonate production by indirect alcoholysis

Iulian Patraşcu, Costin S. Bîldea, Anton A. Kiss

《化学科学与工程前沿（英文）》 2022年 第16卷 第2期   页码 316-331 doi: 10.1007/s11705-021-2047-9

摘要： Dimethyl carbonate is an eco-friendly essential chemical that can be sustainably produced from CO , which is available from carbon capture activities or can even be captured from the air. The rapid increase in dimethyl carbonate demand is driven by the fast growth of polycarbonates, solvent, pharmaceutical, and lithium-ion battery industries. Dimethyl carbonate can be produced from CO through various chemical pathways, but the most convenient route reported is the indirect alcoholysis of urea. Previous research used techniques such as heat integration and reactive distillation to reduce the energy use and costs, but the use of an excess of methanol in the trans-esterification step led to an energy intensive extractive distillation required to break the dimethyl carbonate-methanol azeotrope. This work shows that the production of dimethyl carbonate by indirect alcoholysis of urea can be improved by using an excess of propylene carbonate (instead of an excess of methanol), a neat feat that we showed it requires only 2.64 kW·h·kg dimethyl carbonate in a reaction-separation-recycle process, and a reactive distillation column that effectively replaces two conventional distillation columns and the reactor for dimethyl carbonate synthesis. Therefore, less equipment is required, the methanol-dimethyl carbonate azeotrope does not need to be recycled, and the overall savings are higher. Moreover, we propose the use of a reactive distillation column in a heat integrated process to obtain high purity dimethyl carbonate (>99.8 wt-%). The energy requirement is reduced by heat integration to just 1.25 kW·h·kg dimethyl carbonate, which is about 52% lower than the reaction-separation-recycle process. To benefit from the energy savings, the dynamics and control of the process are provided for ±10% changes in the nominal rate of 32 ktpy dimethyl carbonate, and for uncertainties in reaction kinetics.

关键词： dimethyl carbonate     reactive distillation     process design     plantwide control    

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地下水碳酸平衡检查系统

刘建刚,郑克勋,傅伟宁,吴顺华

《中国工程科学》 2003年 第5卷 第9期   页码 61-64

摘要：

文章主要研究地下水在不同温度和CO2分压条件下碳酸三种存在形式与pH值的关系，以便更有效地对地下水水质资料进行可靠性检查。分析认为HCO3-出现峰值的分界pH0值，纯水在CO2分压1～105Pa，温度0～30℃时的变化范围为7.92～8.60，碳酸盐岩地下水的变化范围为8.28～8.57。pH0值随温度的升高而降低。石灰岩和白云岩的pH0十分接近，碳酸盐岩地区的平衡特性将取决于方解石成分。

关键词： 碳酸盐岩     地下水     碳酸平衡     pH值    

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Multi-objective optimization of molten carbonate fuel cell system for reducing CO

Ramin ROSHANDEL,Majid ASTANEH,Farzin GOLZAR

《能源前沿（英文）》 2015年 第9卷 第1期   页码 106-114 doi: 10.1007/s11708-014-0341-7

摘要： The aim of this paper is to investigate the implementation of a molten carbonate fuel cell (MCFC) as a CO separator. By applying multi-objective optimization (MOO) using the genetic algorithm, the optimal values of operating load and the corresponding values of objective functions are obtained. Objective functions are minimization of the cost of electricity (COE) and minimization of CO emission rate. CO tax that is accounted as the pollution-related cost, transforming the environmental objective to the cost function. The results show that the MCFC stack which is fed by the syngas and gas turbine exhaust, not only reduces CO emission rate, but also produces electricity and reduces environmental cost of the system.

关键词： molten carbonate fuel cell (MCFC)     multi-objective optimization (MOO)     Pareto curve     genetic algorithm     CO2 separation    

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Effect of potassium carbonate on catalytic synthesis of calcium carbide at moderate temperature

Dejun SHI, Ke QIAO, Zifeng YAN

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 372-375 doi: 10.1007/s11705-010-0570-1

摘要： Calcium carbide was successfully synthesized by carbothermal reduction of lime with coke at 1973 K for 1.5 h. The effect of potassium carbonate as additive on the composition and morphology of the product was investigated using X-ray diffraction and scanning electron microscope. Addition of potassium carbonate increased the yield of calcium carbide. The sample in the presence of potassium carbonate generated acetylene gas of 168.3 L/kg, which was 10% higher than that in the absence of potassium carbonate. This result confirmed the catalytic effect of potassium carbonate on the synthesis of calcium carbide. A possible mechanism of the above effects was that the additive, which was melted at the reduction temperature, dissolved CaO and so promoted the contact between CaO and carbon, which was essential for the solid-solid reaction to form calcium carbide.

关键词： calcium carbide     synthesis     catalysis    

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Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate

Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 415-422 doi: 10.1007/s11705-012-1214-4

摘要： The catalysts supported on LiAl O (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H . Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl O (spinel) was formed at 800°C, while LiAl O (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO , also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl -PdCl /LiAl O (spinel) with better electron transfer ability and low Pd reduction temperature exhibited a better catalytic ability.

关键词： Wacker-type catalyst     dimethyl carbonate     methyl nitrite     spinel    

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Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substituted

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 59-64 doi: 10.1007/s11705-007-0012-x

摘要： The perovskite-type compound LaMnO was substituted for the part of La in position A and for the part of Mn in position B by citrate method. The phases were detected by X-ray diffraction. Powder morphologies were scanned by scanning electron microscopy. The valence of atoms was determined by X-ray photoelectron spectroscopy. It was found that the perovskite can form crystal defect and increase the proportion of high valence B element by doping. Active component Pd was loaded on various perovskite supports for synthesis of diphenyl carbonate. The results showed that the activities of catalysts in which supports have crystal defect by substitution were higher. It can be concluded that perovskite with defect structure by doping could lead to the formation of oxygen vacancy where the lattice oxygen became exchangeable with the oxygen gas. Also, this improved the redox process of the carrier by transferring electrons and activities of catalysts.

关键词： photoelectron spectroscopy     diphenyl carbonate     proportion     diffraction     perovskite    

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 对化学链系统中氧载体材料发展的新认识 Review

Zhuo Cheng, Lang Qin, Jonathan A. Fan, Liang-Shih Fan

《工程（英文）》 2018年 第4卷 第3期   页码 343-351 doi: 10.1016/j.eng.2018.05.002

摘要：

化学循环燃烧（CLC）和化学循环重整（CLR）是通过循环氧化还原反应将清洁和有效的碳氢化合物转化为动力、燃料和化学品的创新技术。金属氧化物材料在化学循环氧化还原过程中起着重要作用。在还原过程中，氧载体提供所需量的氧离子用于烃转化和产物合成。在氧化步骤中，耗尽的金属氧化物氧载体从空气中补充分子氧，同时释放热量。近年来，用于各种化学循环应用的氧载体材料已经取得了显着进步。在这些金属氧化物材料中，铁基氧载体由于其高载氧能力、成本效益和化学循环反应应用的多功能性而具有吸引力。它们的反应性也可以通过结构设计和改进来增强。本文讨论了氧载体材料开发的最新进展以及这些材料上烃转化的机制。这些进步将促进氧载体材料的开发，以实现更有效的化学循环技术应用。

关键词： 化学循环     氧载体     烃类转化     离子扩散     机制    

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碱硅酸反应与碱碳酸盐反应

唐明述

《中国工程科学》 2000年 第2卷 第1期   页码 34-40

摘要：

碱集料反应（AAR）可分为两类，即碱硅酸反应（ASR）与碱碳酸盐反应（ACR）。二者的共同点是与碱发生的化学反应可导致混凝土中集料的体积增大，从而可能使混凝土甚至整个建筑物或构筑物发生膨胀开裂。文章着重从膨胀过程和机理以及岩石的结构特征探讨二者的特性与差异。ASR类型岩石具有碱活性的前提条件是较低的二氧化硅结晶完整度。只有隐晶质、微晶质、玻璃质或发生过应变的二氧化硅才会具有较高的化学活性，导致混凝土破坏。通过系统研究证实，对碱碳酸盐反应，虽然结晶的完整程度以及白云石（CaCO3·MgCO3）分子式中Ca/Mg比也将影响其与碱反应的速率，但起决定作用的是白云石晶体的尺寸及其在岩石中的分布状态和被基质包围的紧密程度。从微观结构得出的这些特征将有助于加深对碱集料反应膨胀机理的认识。文中还介绍了形成活性白云石的地质环境和碱硅酸反应与碱碳酸盐反应的区分方法。

关键词： 碱     集料     硅酸     碳酸盐     混凝土开裂     机理    

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Direct synthesis of dimethyl carbonate over rare earth oxide supported catalyst

JIANG Qi, CHENG Jiye, GAO Zhiqin

《化学科学与工程前沿（英文）》 2007年 第1卷 第3期   页码 300-303 doi: 10.1007/s11705-007-0055-z

摘要： Solid base catalysts for the direct synthesis of dimethyl carbonate (DMC) from carbon dioxide, methanol, and propylene oxide were prepared by loading KCl and KCO on the surface of LaO, YO, CeO and NdO. The catalysts were characterized by thermogravimetric analysis (TGA) and X-ray diffraction (XRD) techniques. The catalytic activities were efficiently influenced by the preparation conditions. The optimal loading amount of KCO is 17.6% (mass) for KCl-KCO/YO and 22.2% for other catalysts. Supports affected the activity of catalyst. KCl-KCO/NdO exhibited the highest activity. The activity of KCl-KCO/YO increased with the increase of calcination temperature in the range of 800ºC–900ºC. The formation of KYO, YOCl or YO species probably promoted the catalysts.

关键词： thermogravimetric analysis     increase     KCl-KCO/NdO     catalytic     KCl-KCO/YO    

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标题 作者 时间 类型 操作

decarbonisation of energy-intensive industries: a comparative review of techno-economic feasibility of solid looping

期刊论文

Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

期刊论文

Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

期刊论文

Polyethylene glycol-supported ionic liquid as a highly efficient catalyst for the synthesis of propylene carbonate

Rui YAO, Hua WANG, Jinyu HAN

期刊论文

Effect of wastewater composition on the calcium carbonate precipitation in upflow anaerobic sludge blanket

Shucheng YANG, Yanling HE, Charles CHOU, Pengxiang ZHANG, Dongqi WANG, Yonghong LIU,

期刊论文

化学链概念在共沸物分离中的应用

高鑫, 耿雪丽

期刊论文

Novel eco-efficient reactive distillation process for dimethyl carbonate production by indirect alcoholysis

Iulian Patraşcu, Costin S. Bîldea, Anton A. Kiss

期刊论文

地下水碳酸平衡检查系统

刘建刚,郑克勋,傅伟宁,吴顺华

期刊论文

Multi-objective optimization of molten carbonate fuel cell system for reducing CO

Ramin ROSHANDEL,Majid ASTANEH,Farzin GOLZAR

期刊论文

Effect of potassium carbonate on catalytic synthesis of calcium carbide at moderate temperature

Dejun SHI, Ke QIAO, Zifeng YAN

期刊论文

Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate

Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA

期刊论文

Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substituted

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

期刊论文

 对化学链系统中氧载体材料发展的新认识

Zhuo Cheng, Lang Qin, Jonathan A. Fan, Liang-Shih Fan

期刊论文

碱硅酸反应与碱碳酸盐反应

唐明述

期刊论文

Direct synthesis of dimethyl carbonate over rare earth oxide supported catalyst

JIANG Qi, CHENG Jiye, GAO Zhiqin

期刊论文