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Scale up of reactors for carbon dioxide reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 116-122 doi: 10.1007/s11705-022-2178-7

摘要： In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds. On the other hand, the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic. Here we examine some of the major challenges, demonstrating some promising strategies towards such scale-up, including increased electrode area and stacking of electrode pairs in different configurations. We observed that increasing the electrode area from 1 to 10 cm2 led to only a 4% drop in current density, with similarly small penalties realised when stacking sub-cells together.

关键词： CO2 reduction     electrochemical cell     electrosynthesis     upscaling    

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Methanation of carbon dioxide: an overview

Wei WANG, Jinlong GONG

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 2-10 doi: 10.1007/s11705-010-0528-3

摘要： Although being very challenging, utilization of carbon dioxide (CO ) originating from production processes and flue gases of CO -intensive sectors has a great environmental and industrial potential due to improving the resource efficiency of industry as well as by contributing to the reduction of CO emissions. As a renewable and environmentally friendly source of carbon, catalytic approaches for CO fixation in the synthesis of chemicals offer the way to mitigate the increasing CO buildup. Among the catalytic reactions, methanation of CO is a particularly promising technique for producing energy carrier or chemical. This article focuses on recent developments in catalytic materials, novel reactors, and reaction mechanism for methanation of CO .

关键词： CO2 methanation     hydrogenation     catalysis     methane     environmental science    

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Enhancing the aromatic selectivity of cyclohexane aromatization by CO<sub>2sub> coupling

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1801-1808 doi: 10.1007/s11705-023-2325-9

摘要： Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes. Herein, CO2 is introduced into the cyclohexane conversion process on the HZSM-5 zeolite, which can improve the aromatic selectivity. By optimizing the reaction conditions, an improved aromatic (benzene, toluene, xylene, and C9+) selectivity of 48.2% can be obtained at the conditions of 2.7 MPa (CO2), 450 °C, and 1.7 h−1, which is better than that without CO2 (aromatic selectivity = 43.2%). In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates (e.g., carboxylic acid, anhydride, unsaturated aldehydes/ketones or ketene) would be formed during the cyclohexane conversion process in the presence of CO2. 13C isotope labeling experimental results demonstrate that CO2 can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity. This study may open a green, economic, and promising way to improve the aromatic selectivity for alkane aromatization process.

关键词： aromatics     carbon dioxide     aromatization     coupling reaction     ZSM-5 zeolite    

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Frontier science and challenges on offshore carbon storage

《环境科学与工程前沿（英文）》 2023年 第17卷 第7期 doi: 10.1007/s11783-023-1680-6

摘要：

● The main direct seal up carbon options and challenges are reviewed.

关键词： Offshore carbon storage     Direct CO2 injection     CO2-CH4 replacement     CO2-EOR     CCS hubs     CO2 transport    

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Decomposition analysis of energy-related carbon dioxide emissions in the iron and steel industry in China

Wenqiang SUN, Jiuju CAI, Hai YU, Lei DAI

《环境科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 265-270 doi: 10.1007/s11783-011-0284-8

摘要： This work aims to identify the main factors influencing the energy-related carbon dioxide (CO ) emissions from the iron and steel industry in China during the period of 1995–2007. The logarithmic mean divisia index (LMDI) technique was applied with period-wise analysis and time-series analysis. Changes in energy-related CO emissions were decomposed into four factors: emission factor effect, energy structure effect, energy consumption effect, and the steel production effect. The results show that steel production is the major factor responsible for the rise in CO emissions during the sampling period; on the other hand the energy consumption is the largest contributor to the decrease in CO emissions. To a lesser extent, the emission factor and energy structure effects have both negative and positive contributions to CO emissions, respectively. Policy implications are provided regarding the reduction of CO emissions from the iron and steel industry in China, such as controlling the overgrowth of steel production, improving energy-saving technologies, and introducing low-carbon energy sources into the iron and steel industry.

关键词： carbon dioxide (CO2) emissions     decomposition analysis     logarithmic mean divisia index (LMDI) technique     time-series analysis    

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Peak CO

Sheng ZHOU, Maosheng DUAN, Zhiyi YUAN, Xunmin OU

《能源前沿（英文）》 2020年 第14卷 第4期   页码 740-758 doi: 10.1007/s11708-018-0558-y

摘要： This paper studies the pathways of peaking CO emissions of Dezhou city in China, by employing a bottom-up sector analysis model and considering future economic growth, the adjustment of the industrial structure, and the trend of energy intensity. Two scenarios (a business-as-usual (BAU) scenario and a CO mitigation scenario (CMS)) are set up. The results show that in the BAU scenario, the final energy consumption will peak at 25.93 million tons of coal equivalent (Mtce) (16% growth versus 2014) in 2030. In the CMS scenario, the final energy will peak in 2020 at 23.47 Mtce (9% lower versus peak in the BAU scenario). The total primary energy consumption will increase by 12% (BAU scenario) and decrease by 3% (CMS scenario) in 2030, respectively, compared to that in 2014. In the BAU scenario, CO emission will peak in 2025 at 70 million tons of carbon dioxide (MtCO ), and subsequently decrease gradually in 2030. In the CMS scenario, the peak has occurred in 2014, and 60 MtCO will be emitted in 2030. Active policies including restructuring the economy, improving energy efficiency, capping coal consumption, and using more low-carbon /carbon free fuel are recommended in Dezhou city peaked CO emission as early as possible.

关键词： carbon dioxide emission     energy consumption     peak CO2 emission     low-carbon transition     Dezhou city     China    

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Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1727-8

摘要：

● Greenhouse gas mitigation by biomass-based CO2 utilization with a Fe cycle system.

关键词： Carbon dioxide utilization     Hydrothermal reactions     Biomass-based CO2 reduction     Simulation     Ex-ante LCA    

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Activated carbons and amine-modified materials for carbon dioxide capture –– a review

Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 326-340 doi: 10.1007/s11783-013-0510-7

摘要： Rapidly increasing concentration of CO in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and CO adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine (PEI) on the different porous materials were introduced in terms of preparation method and adsorption performance as well as their advantages and disadvantages for CO adsorption. In the last section, the issues and prospect of solid adsorbents for CO adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of activated carbons and amine-modified adsorbents for CO capture.

关键词： adsorption capacity     CO2 capture     activated carbon     amine-impregnated adsorbents    

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The capture of carbon dioxide by transition metal aluminates, calcium aluminate, calcium zirconate, calcium

Ganesh TILEKAR, Kiran SHINDE, Kishor KALE, Reshma RASKAR, Abaji GAIKWAD

《化学科学与工程前沿（英文）》 2011年 第5卷 第4期   页码 477-491 doi: 10.1007/s11705-011-1107-y

摘要： The capture of CO by transition metal (Mn, Ni, Co and Zn) aluminates, calcium aluminate, calcium zirconate, calcium silicate and lithium zirconate was carried out at pre- and post-combustion temperatures. The prepared metal adsorbents were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), surface area analysis and acidity/alkalinity measurements. The different experimental variables affecting the adsorbents ability to capture CO , such as the mol ratio of metal ions, the pressure of CO , the exposure time and the temperature of the adsorbent were also investigated. Calcium zirconate captured 13.85 wt-% CO at 650°C and 2.5 atm and calcium silicate captured 14.31 wt-% at 650°C. Molecular sieves (13X) and carbon can only capture a negligible amount of CO at high temperatures (300°C–650°C). However, the mixed metal oxides captured reasonable amount of CO at these higher temperatures. In addition, calcium aluminate, calcium zirconate, calcium silicate and lithium zirconate adsorbents captured CO at both pre and post-combustion temperatures. The trend for the amount of captured carbon dioxide over the adsorbents was calcium aluminate

关键词： captured CO2     pre-combustion temperature     characterization     calcium silicate     calcium zirconate    

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CO<sub>2sub>高温电解技术助力化工产业碳中和 Review

李一枫, 张龙贵, 于波, 朱建新, 吴长江

《工程（英文）》 2023年 第21卷 第2期   页码 101-114 doi: 10.1016/j.eng.2022.02.016

摘要：

化学工业是我国主要的CO<sub>2sub>排放源，为了实现我国的碳中和目标，必须重点关注化学工业的碳排放情况。基于固体氧化物电解池（SOEC）的CO<sub>2sub>高温电解技术，对于中国实现碳减排、碳达峰和碳中和目标具有重要意义。此外，该技术可以实现CO<sub>2sub>的资源化利用，从而产生可观的环境效益和潜在的经济效益。目前，CO<sub>2sub>高温电解技术已经在实验室和中试阶段取得了很大进展，但对该技术的大规模工业应用还需要进一步探索。本文综述了高温CO<sub>2sub>电解池材料的最新研究进展，讨论了SOEC技术的未来发展方向，并提出了SOEC技术与化工合成耦合实现碳中和目标的方法。

关键词： 固体氧化物电解池     二氧化碳     碳中和     镍     钙钛矿     规模化    

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MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance for carbondioxide reforming of methane

Yan LI,Zhehao WEI,Yong WANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 133-140 doi: 10.1007/s11705-014-1422-1

摘要： A Ni/MgO catalyst was prepared via novel dielectric-barrier discharge (DBD) plasma decomposition method. The combined characterization of Brunauer-Emmett-Teller measurement, X-ray diffraction, hydrogen temperature-programmed reduction and transmission electron microscopy shows that DBD plasma treatment enhances the support-metal interaction of Ni/MgO catalyst and facilitates the formation of smaller Ni particles. Sphere-like Ni particles form on plasma treated Ni/MgO catalysts. The plasma treated Ni/MgO catalyst shows a significantly improved low temperature activity and good stability for CO reforming of methane to syngas.

关键词： CO2 reforming     methane     dielectric-barrier discharge (DBD)     plasma     Ni/MgO    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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Molecular level understanding of CO<sub>2sub> capture in ionic liquid/polyimide composite membrane

Linlin You, Yandong Guo, Yanjing He, Feng Huo, Shaojuan Zeng, Chunshan Li, Xiangping Zhang, Xiaochun Zhang

《化学科学与工程前沿（英文）》 2022年 第16卷 第2期   页码 141-151 doi: 10.1007/s11705-020-2009-7

摘要： Ionic liquid (IL)/polyimide (PI) composite membranes demonstrate promise for use in CO separation applications. However, few studies have focused on the microscopic mechanism of CO in these composite systems, which is important information for designing new membranes. In this work, a series of systems of CO in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide composited with 4,4-(hexafluoroisopropylidene) diphthalic anhydride (6FDA)-based PI, 6FDA-2,3,5,6-tetramethyl-1,4-phenylene-diamine, at different IL concentrations were investigated by all-atom molecular dynamics simulation. The formation of IL regions in PI was found, and the IL regions gradually became continuous channels with increasing IL concentrations. The analysis of the radial distribution functions and hydrogen bond numbers demonstrated that PI had a stronger interaction with cations than anions. However, the hydrogen bonds among PI chains were destroyed by the addition of IL, which was favorable for transporting CO . Furthermore, the self-diffusion coefficient and free energy barrier suggested that the diffusion coefficient of CO decreased with increasing IL concentrations up to 35 wt-% due to the decrease of the fractional free volume of the composite membrane. However, the CO self-diffusion coefficients increased when the IL contents were higher than 35 wt-%, which was attributed to the formation of continuous IL domain that benefitted the transportation of CO .

关键词： carbon dioxide     ionic liquid     6FDA-TeMPD     composite membrane     molecular dynamics simulation    

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Capture of carbon dioxide over porous solid adsorbents lithium silicate, lithium aluminate and magnesium

P. V. Korake, A. G. Gaikwad

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 215-226 doi: 10.1007/s11705-010-1012-9

摘要： The capturing process for carbon dioxide over porous solid adsorbents such as lithium silicate, lithium aluminate, and magnesium aluminate at pre- combustion temperatures was studied. Lithium silicate was prepared by the sol gel and solid fusion methods. The lithium silicate adsorbent was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), nuclear magnetic resonance (NMR), and surface area. The capturing of carbon dioxide over lithium silicate, lithium aluminate, and magnesium aluminate was explored at different experimental conditions such as exposure time, temperature variation, and exposure carbon dioxide pressure. The capturing process for carbon dioxide was investigated over these adsorbents with variation of their metal mole ratios. The effect of the addition of (promoter) sodium, potassium, and cesium in the lithium silicate adsorbent was explored to investigate the variation of the capture of carbon dioxide over these adsorbents.

关键词： capturing CO2     lithium silicate     lithium aluminate     magnesium aluminate    

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CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion     nickel catalysts     CO2 methanation     co-methanation of CO and CO2    

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标题 作者 时间 类型 操作

Scale up of reactors for carbon dioxide reduction

期刊论文

Methanation of carbon dioxide: an overview

Wei WANG, Jinlong GONG

期刊论文

Enhancing the aromatic selectivity of cyclohexane aromatization by CO<sub>2sub> coupling

期刊论文

Frontier science and challenges on offshore carbon storage

期刊论文

Decomposition analysis of energy-related carbon dioxide emissions in the iron and steel industry in China

Wenqiang SUN, Jiuju CAI, Hai YU, Lei DAI

期刊论文

Peak CO

Sheng ZHOU, Maosheng DUAN, Zhiyi YUAN, Xunmin OU

期刊论文

Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

期刊论文

Activated carbons and amine-modified materials for carbon dioxide capture –– a review

Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU

期刊论文

The capture of carbon dioxide by transition metal aluminates, calcium aluminate, calcium zirconate, calcium

Ganesh TILEKAR, Kiran SHINDE, Kishor KALE, Reshma RASKAR, Abaji GAIKWAD

期刊论文

CO<sub>2sub>高温电解技术助力化工产业碳中和

李一枫, 张龙贵, 于波, 朱建新, 吴长江

期刊论文

MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance for carbondioxide reforming of methane

Yan LI,Zhehao WEI,Yong WANG

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

期刊论文

Molecular level understanding of CO<sub>2sub> capture in ionic liquid/polyimide composite membrane

Linlin You, Yandong Guo, Yanjing He, Feng Huo, Shaojuan Zeng, Chunshan Li, Xiangping Zhang, Xiaochun Zhang

期刊论文

Capture of carbon dioxide over porous solid adsorbents lithium silicate, lithium aluminate and magnesium

P. V. Korake, A. G. Gaikwad

期刊论文

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文