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Simultaneous CO

Jie ZHU,Wei WANG,Xiuning HUA,Zhou XIA,Zhou DENG

《环境科学与工程前沿（英文）》 2015年第9卷第6期页码 1117-1129 doi: 10.1007/s11783-015-0812-z

摘要： The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe O 60 wt.% and Fe O 55 wt.%/CuO 5 wt.% supported by Al O , were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO capture and H production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H ·g Fe O compared with Fe-Al of 2300 μmol H ·g Fe O . The overall CO capture efficiency remained 98%–98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, H , CH and CO were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu-Al in the reduction stage. The intensity of hydrogen production and the overall CO capture efficiency were in the range of 2000–2400 μmol H ·g Fe O and 89%–95%, respectively.

关键词： CO₂ capture chemical looping hydrogen generation iron based oxygen carriers single packed bed reactor long-term test complex gases fuel

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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 SrFeO_3−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 SrFeO_3−δ/CaO·MnO nanocomposite reduction kinetics Avrami–Erofeyev model pressure-dependent term

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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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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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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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Metal-based direct hydrogen generation as unconventional high density energy

Shuo XU, Jing LIU

《能源前沿（英文）》 2019年第13卷第1期页码 27-53 doi: 10.1007/s11708-018-0603-x

摘要： Metals are unconventional hydrogen production materials which are of high energy densities. This paper comprehensively reviewed and digested the latest researches of the metal-based direct hydrogen generation and the unconventional energy utilization ways thus enabled. According to the metal activities, the reaction conditions of metals were generalized into three categories. The first ones refer to those which would violently react with water at ambient temperature. The second ones start to react with water after certain pretreatments. The third ones can only react with steam under somewhat harsh conditions. To interpret the metal-water reaction mechanisms at the molecular scale, the molecule dynamics simulation and computational quantum chemistry were introduced as representative theoretical analytical tools. Besides, the state-of-the-art of the metal-water reaction was presented with several ordinary metals as illustration examples, including the material treatment technologies and the evaluations of hydrogen evolution performances. Moreover, the energy capacities of various metals were summarized, and the application potentials of the metal-based direct hydrogen production approach were explored. Furthermore, the challenges lying behind this unconventional hydrogen generation method and energy strategy were raised, which outlined promising directions worth of further endeavors. Overall, active metals like Na and K are appropriate for rapid hydrogen production occasions. Of these metals discussed, Al, Mg and their alloys offer the most promising hydrogen generation route for clean and efficient propulsion and real-time power source. In the long run, there exists plenty of space for developing future energy technology along this direction.

关键词： metal hydrogen generation hydrolysis metal water reaction clean energy

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Exergy analysis and performance enhancement of isopropanol-acetone-hydrogen chemical heat pump

Min XU, Jun CAI, Xiulan HUAI

《能源前沿（英文）》 2017年第11卷第4期页码 510-515 doi: 10.1007/s11708-017-0508-0

摘要： Exergy loss analysis was conducted to identify the irreversibility in each component of the isopropanol-acetone-hydrogen chemical heat pump (IAH-CHP). The results indicate that the highest irreversibility on a system basis occurs in the distillation column. Moreover, the effect of operating parameters on thermodynamic performances of the IAH-CHP was studied and the optimal conditions were obtained. Finally, the potential methods to reduce the irreversibility of the IAH-CHP system were investigated. It is found that reactive distillation is apromising alternative. The enthalpy and exergy efficiency of the IAH-CHP with reactive distillation increases by 24.1% and 23.2%, respectively.

关键词： waste heat reuse chemical heat pump exergy analysis isopropanol

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Nano-confined ammonia borane for chemical hydrogen storage

M. A. WAHAB, Huijun ZHAO, X. D. YAO

《化学科学与工程前沿（英文）》 2012年第6卷第1期页码 27-33 doi: 10.1007/s11705-011-1171-3

摘要： There is a great demand for a sufficient and sustainable energy supply. Hence, the search for applicable hydrogen storage materials is extremely important owing to the diversified merits of hydrogen energy. In this regard, ammonia borane (NH BH , AB) containing 19.6 wt-% hydrogen has been considered as a promising material for hydrogen storage applications to realize the “hydrogen economy”, but with limits from slow kinetics of hydrogen release and by-product of trace gases such as ammonia and borazine. In this review, we introduce the recent research on AB, regarding to the nanoconfinement effect on improving the kinetics at a relatively low temperature and the prevention/reduction of undesirable gas formation.

关键词： ammonia borane hydrogen storage

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Mature

Giorgia De Guido, Matteo Compagnoni, Laura A. Pellegrini, Ilenia Rossetti

《化学科学与工程前沿（英文）》 2018年第12卷第2期页码 315-325 doi: 10.1007/s11705-017-1698-z

摘要： Carbon capture and storage (CCS) have acquired an increasing importance in the debate on global warming as a mean to decrease the environmental impact of energy conversion technologies, by capturing the CO produced from the use of fossil fuels in electricity generation and industrial processes. In this respect, post-combustion systems have received great attention as a possible near-term CO capture technology that can be retrofitted to existing power plants. This capture technology is, however, energy-intensive and results in large equipment sizes because of the large volumes of the flue gas to be treated. To cope with the demerits of other CCS technologies, the chemical looping combustion (CLC) process has been recently considered as a solution for CO separation. It is typically referred to as a technology without energy penalty. Indeed, in CLC the fuel and the combustion air are never mixed and the gases from the oxidation of the fuel (i.e., CO and H O) leave the system as a separate stream and can be separated by condensation of H O without any loss of energy. The key issue for the CLC process is to find a suitable oxygen carrier, which provides the fuel with the activated oxygen needed for combustion. The aim of this work is to explore the feasibility of using perovskites as oxygen carriers in CLC and to consider the possible advantages with respect to the scrubbing process with amines, a mature post-combustion technology for CO separation.

关键词： CO₂ capture monoethanolamine chemical looping combustion oxygen carrier perovskites

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面向低碳未来的化学链清洁能源技术

程卓, Anuj Joshi, 范良士

《工程（英文）》 2023年第29卷第10期页码 42-44 doi: 10.1016/j.eng.2023.08.008

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Alkali-thermal gasification and hydrogen generation potential of biomass

Alexander B. Koven, Shitang S. Tong, Ramin R. Farnood, Charles Q. Jia

《化学科学与工程前沿（英文）》 2017年第11卷第3期页码 369-378 doi: 10.1007/s11705-017-1662-y

摘要： Generating hydrogen gas from biomass is one approach to lowering dependencies on fossil fuels for energy and chemical feedstock, as well as reducing greenhouse gas emissions. Using both equilibrium simulations and batch experiments with NaOH as a model alkaline, this study established the technical feasibility of converting various biomasses (e.g., glucose, cellulose, xylan and lignin) into H -rich gas via catalyst-free, alkali-thermal gasification at moderate temperatures (as low as 300 °C). This process could produce more H with less carbon-containing gases in the product than other comparable methods. It was shown that alkali-thermal gasification follows , with carbonate being the solid product which is different from the one suggested in the literature. Moreover, the concept of hydrogen generation potential (H -GP)—the maximum amount of H that a biomass can yield, was introduced. For a given biomass C H O , the H -GP would be moles of H . It was demonstrated experimentally that the H -GP was achievable by adjusting the amounts of H O and NaOH, temperature and pressure.

关键词： hydrogen generation potential biomass lignocellulose alkali-thermal gasification sodium hydroxide

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风氢互补发电系统构建初探

徐晔,陈晓宁

《中国工程科学》 2010年第12卷第11期页码 83-88

摘要：

为了解决风力发电输出功率的不平稳性和电压的波动性，以解决并网的瓶颈问题，提出风氢互补发电系统，将风力发电输出“波谷”对应的可控出力作为风电场能保证恒定输出的功率，“波峰”至“波谷”之间对应的不可控的出力，采用“波峰”制氢进行“削峰”、“波谷”氢气发电进行“填谷”的方式进行平衡。并以如东风电场为例进行了实例分析与计算，结果证明采用该风氢互补系统基本能保证发电输出平衡，是解决风电并网有效可行的途径。

关键词：风力发电氢能发电制氢储氢

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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

€·t CO 2 − 1

for the pulp and paper and 104.6

€·t CO 2 − 1

for the iron and steel industry. Its average equivalent energy requirement varied between 2.7 (iron and steel) and 5.1

MJ th ⋅ kg CO 2 − 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

€·t CO 2 − 1

(cement). Its average equivalent energy requirement varied between 2.0 (iron and steel) and 3.7

MJ th ⋅ kg CO 2 − 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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Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

《能源前沿（英文）》 2022年第16卷第5期页码 734-746 doi: 10.1007/s11708-022-0840-x

摘要： This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal–organic framework (MOF)-based systems toward the photocatalytic hydrogen evolution (PHE) reaction through specific strategies: tailoring the photocatalytic activity of bare MOFs and guest@MOF composites, formation of heterojunctions based on MOFs and various photocatalysts, and inorganic photocatalysts derived from MOFs. According to the data reported in this mini-review, the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units (SBUs). Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view, many of these studies relate this activity to the physicochemical and catalytic properties of MOFs. However, they did not consider the interactions between the components of the photocatalytic material. This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE. A thorough review and comparison of the results established that metal–nanoparticle@MOF composites have weak van der Waals forces between components, whereas heterostructures only interact with MOFs at the surface of bare materials. Regarding material derivatives from MOFs, we found that pyrolysis destroyed some beneficial properties of MOFs for PHE. Thus, we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.

关键词： metal–organic frameworks (MOFs) photocatalytic hydrogen evolution MOF heterojunctions materials derived from MOFs bandgap recombination

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氧化还原氧化裂解石脑油制乙烯的过程模拟与分析 Article

Vasudev Pralhad Haribal,Yun Chen,Luke Neal,Fanxing Li

《工程（英文）》 2018年第4卷第5期页码 714-721 doi: 10.1016/j.eng.2018.08.001

摘要：

石脑油热裂解制乙烯（C₂H₄）是一种能源密集型工艺（每吨C₂H₄ 高达40 GJ 热量），会形成大量焦炭和氮氧化物（NO_x），而且每产生1 kg C₂H₄就有1.8~2 kg 的二氧化碳（CO₂）排放量。我们提出了石脑油氧化还原氧化裂解（redox oxy-cracking，ROC）的替代方法。在该两步法中，石脑油裂解产生的氢气（H₂）首先在氧化还原催化剂的作用下与其晶格氧选择性地燃烧。随后氧化还原催化剂被空气再次氧化并释放热量，以满足裂解反应对热量的需求。这个强化过程减少了附加能量的消耗以及CO₂ 和NO_x 的排放。此外，由于H₂ 的选择性燃烧，C₂H₄和丙烯（C₃H₆）的形成可以被增强。在本研究中，我们基于最近开发氧化还原催化剂的实验数据，使用ASPEN Plus® 模拟ROC工艺。与传统的石脑油裂解相比，ROC 工艺可将能耗和CO₂ 排放量降低52%。该工艺的上游部分少消耗约67% 的能量，同时每千克石脑油原料多产生28% 的C₂H₄ 和C₃H₆。