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

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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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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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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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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Insight of chemical environmental risk and its management from the vinyl chloride accident

《环境科学与工程前沿（英文）》 2023年第17卷第4期 doi: 10.1007/s11783-023-1652-x

摘要： The combustion of vinyl chloride (VC) after the train derailment accident in Ohio, USA in February, 2023 has caused widespread concern around the world. This paper tried to analyze several issues concerning the accident, including the appropriateness of the VC combustion in the emergency response in this accident, the meanings of so-called “controlled combustion”, the potential environmental risks caused by VC and combustion by-products, and follow-up work. In our view, this accident had surely caused environmental and health risks to some extent. Hence, a comprehensive environmental risk assessment is necessary, and then the site with risk should be comprehensively remediated, hazardous waste should be harmlessly treated as soon as possible. Finally, this accident suggests that further efforts should be taken to bridge the gap between chemical safety management and their environmental risk management.

关键词： Vinyl chloride Combustion Chemical safety management Environmental risk Emerging contaminants

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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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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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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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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。

关键词：乙烯石脑油裂解过程强化化学循环过程模拟

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Combustion characteristics and kinetics of bio-oil

Ruixia ZHANG, Zhaoping ZHONG, Yaji HUANG

《化学科学与工程前沿（英文）》 2009年第3卷第2期页码 119-124 doi: 10.1007/s11705-009-0068-x

摘要： The combustion characteristics of bio-oils derived from rice husk and corn were studied by thermogravimetry analysis. According to the thermogravimetry (TG), differential thermogravimetry (DTG) and differential thermal analysis (DTA) curves of bio-oils in air and nitrogen atmosphere, we analyzed the combustion characteristics of different kinds of bio-oils in different atmospheres and worked out the combustion kinetics parameters of the bio-oil, providing reliable base data for the burning of bio-oil. The thermogravimetry indicated that the combustion process of bio-oil was divided into three stages. At the same time, the combustion process can be described by different order reaction models, and with the method of Coats-Redfern, the activation energy and frequency factor of different kinds of bio-oils were obtained.

关键词： bio-oil combustion characteristics combustion kinetics

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Numerical simulation of laminar premixed combustion in a porous burner

ZHAO Pinghui, CHEN Yiliang, LIU Minghou, DING Min, ZHANG Genxuan

《能源前沿（英文）》 2007年第1卷第2期页码 233-238 doi: 10.1007/s11708-007-0032-8

摘要： Premixed combustion in porous media differs substantially from combustion in free space. The interphase heat transfer between a gas mixture and a porous medium becomes dominant in the premixed combustion process. In this paper, the premixed combustion of CH

关键词： interphase mixture dominant Premixed combustion premixed combustion

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Entropy production analysis of swirling diffusion combustion processes

Deodat MAKHANLALL, Linhua LIU,

《能源前沿（英文）》 2010年第4卷第3期页码 326-332 doi: 10.1007/s11708-009-0058-1

摘要： A critical factor in the design of combustion systems for optimum fuel economy and emission performance lies in adequately predicting thermodynamic irreversibilities associated with transport and chemical processes. The objective of this study is to map these irreversibilities in terms of entropy production for methane combustion. The numerical solution of the combustion process is conducted with the help of a Fluent 6.1.22 computer code, and the volumetric entropy production rate due to chemical reaction, viscous dissipation, and mass and heat transfer are calculated as post-processed quantities with the computed data of the reaction rates, fluid velocity, temperature and radiative intensity. This paper shows that radiative heat transfer, which is an important source of entropy production, cannot be omitted for combustion systems. The study is extended by conducting a parametric investigation to include the effects of wall emissivity, optical thickness, swirl number, and Boltzmann number on entropy production. Global entropy production rates decrease with the increase in swirl velocity, wall emissivity and optical thickness. Introducing swirling air into the combustion system and operations with the appropriate Boltzmann number reduces the irreversibility affected regions and improves energy utilization efficiency.

关键词： entropy-based design radiation transfer swirl magnussen combustion-model

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Study on combustion characteristics of blended coals

LI Yonghua, WANG Chunbo, CHEN Hongwei

《能源前沿（英文）》 2007年第1卷第1期页码 96-100 doi: 10.1007/s11708-007-0010-1

摘要： Power plants in China have to burn blended coal instead of one specific coal for a variety of reasons. So it is of great necessity to investigate the combustion of blended coals. Using a test rig with a capacity of 640 MJ/h with an absolute milling system and flue gas online analysis system, characteristics such as burnout, slag, and pollution of some blended coals were investigated. The ratio of coke and slag as a method of distinguishing coal slagging characteristic was introduced. The results show that the blending of coal has some effect on NO but there is no obvious rule. SO emission can be reduced by blending low sulfur coal.

关键词： combustion capacity variety blended burnout

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Recent progress in electric-field assisted combustion: a brief review

《能源前沿（英文）》 2022年第16卷第6期页码 883-899 doi: 10.1007/s11708-021-0770-z

摘要： The control of combustion is a hot and classical topic. Among the combustion technologies, electric-field assisted combustion is an advanced techno-logy that enjoys major advantages such as fast response and low power consumption compared with thermal power. However, its fundamental principle and impacts on the flames are complicated due to the coupling between physics, chemistry, and electromagnetics. In the last two decades, tremendous efforts have been made to understand electric-field assisted combustion. New observations have been reported based on different combustion systems and improved diagnostics. The main impacts, including flame stabilization, emission reduction, and flame propagation, have been revealed by both simulative and experimental studies. These findings significantly facilitate the application of electric-field assisted combustion. This brief review is intended to provide a comprehensive overview of the recent progress of this combustion technology and further point out research opportunities worth investigation.

关键词： electric field combustion flame stabilization emission reduction flame propagation