CO2 sequestration utilizing basic-oxygen furnace slag: Controlling factors, reaction mechanisms and V–Cr concerns

Basic-oxygen furnace slag(BOF-slag) contains 35%CaO,a potential component for CO_2sequestration.In this study,slag-water-CO_2 reaction experiments were conducted with the longest reaction duration extending to 96 hr under high CO_2 pressures of 100-300 kg/cm2 to optimize BOF-slag carbonation conditions,to address carbonation mechanisms,and to evaluate the extents of V and Cr release from slag carbonation.The slag carbonation degree generally reached the maximum values after 24 hr slag-water-CO_2 reaction and was controlled by slag particle size and reaction temperature.The maximum carbonation degree of 71%was produced from the experiment using fine slag of0.5 mm under 100℃and a CO_2 pressure of 250 kg/cm~2 with a water/slag ratio of 5.Vanadium release from the slag to water was significantly enhanced(generally 2 orders) by slag carbonation.In contrast,slag carbonation did not promote chromium release until the reaction duration exceeded 24 hr.However,the water chromium content was generally at least an order lower than the vanadium concentration,which decreased when the reaction duration exceeded 24 hr.Therefore,long reaction durations of 48-96 hr are proposed to reduce environmental impacts while keeping high carbonation degrees.Mineral textures and water compositions indicated that Mg-wustite,in addition to CaO-containing minerals,can also be carbonated.Consequently,the conventional expression that only considered carbonation of the CaO-containing minerals undervalued the CO_2 sequestration capability of the BOF-slag by~20%.Therefore,the BOF-slag is a better CO_2 storage medium than that previously recognized.     

Two-step accelerated mineral carbonation and decomposition analysis for the reduction of CO2 emission in the eco-industrial parks

Carbon dioxide（CO2） emissions are a leading contributor to the negative effects of global warming. Globally, research has focused on effective means of reducing and mitigating CO2 emissions. In this study, we examined the efficacy of eco-industrial parks（EIPs） and accelerated mineral carbonation techniques in reducing CO2 emissions in South Korea.First, we used Logarithmic Mean Divisia Index（LMDI） analysis to determine the trends in carbon production and mitigation at the existing EIPs. We found that, although CO2 was generated as byproducts and wastes of production at these EIPs, improved energy intensity effects occurred at all EIPs, and we strongly believe that EIPs are a strong alternative to traditional industrial complexes for reducing net carbon emissions. We also examined the optimal conditions for using accelerated mineral carbonation to dispose of hazardous fly ash produced through the incineration of municipal solid wastes at these EIPs. We determined that this technique most efficiently sequestered CO2 when micro-bubbling, low flow rate inlet gas, and ammonia additives were employed.     

Co-utilisation of CO2 and steelmaking slags for production of pure CaCO3 – legislative issues

The steel industry is characterised by large amounts of CO₂ emissions, but there is no easy means to reduce these emissions. One interesting option for the reduction of CO₂ emissions could be the utilisation of steelmaking slags for carbon dioxide mineralisation. In this option CO₂ is bound with the calcium of the slag material, producing stable carbonate as an end product. The utilisation of steelmaking slags as the raw material for carbon dioxide mineralisation will change the quality of the slags. If, however, this change degrades the slags it could prevent the use of slags in carbon dioxide mineralisation or make it very expensive.The purpose of the research presented here is to evaluate this issue with the help of a case study where the quality of the residual slag from the recently suggested carbonation method was experimentally investigated. The CO₂ mineralisation method, based on steelmaking slags and ammonium salt solutions, was found to change the quality of the slags: the calcium content was reduced, the CaO and Ca(OH)₂ phases were completely dissolved, and the solubility of the V and Cr increased notably. This residual slag would presumably have to be handled as waste. Currently, the steelmaking slag used in the case study is defined as a by-product, but if it is used for CO₂ mineralisation instead of liming its legal status will be re-evaluated. Subsequently, the CO₂ mineralisation process could possibly be defined as an end-of-waste procedure.     

基于生命周期评价的钢铁厂碱渣固碳技术比较研究

本研究以3种钢铁厂碱渣直接法固碳技术为研究对象,该技术将钢渣进行碳酸化处理,可快速永久地将CO2固化储存在钢渣中,气固相反应可分别在高压釜、泥浆反应器和超重力旋转床的水溶液中一步完成,并将其分别定义为T1、T2、T3.通过Umberto软件建立生命周期模型,对3种技术的资源环境影响进行评估.结果表明,T1的环境影响最高,其次为T3,T2的环境影响最小.技术评价显示,T3在技术效率、资源消耗、环境影响方面具有较好的综合效益.敏感性分析表明,加热效率的敏感性系数分别为0.97、0.97和0.46.转换率与温室气体排放的关系分别呈上升、倒U型和下降的变化趋势.提高加热效率、合理利用热源及选择合适的技术效率,将有利于技术优化,减少技术的环境影响,提高固碳效率.     

CO2泡沫混凝土碳封存潜力分析

CO₂捕集、利用与封存是碳中和技术体系的重要组成部分,混凝土在大规模吸收CO₂方面具有巨大的发展潜力.为了掌握CO₂泡沫混凝土的碳封存潜力,分析了CO₂泡沫混凝土的固碳机制,建立了CO₂泡沫混凝土固碳能力的数学模型,估算了CO₂泡沫混凝土的固碳和储碳能力.结果表明,CO₂泡沫混凝土碳封存能力的99%以上是由混凝土骨架的化学碳化方式完成的,而泡孔的储碳能力较弱;按照30%碳化率估算,我国每年生产的混凝土在全生命周期内的碳封存量平均为2.18亿t,超过大兴安岭林区森林1 a的碳汇;近5年,我国CO₂泡沫混凝土的碳封存潜力为5.80亿t ·a^-1,在煤电一体化矿区的固废和废气资源化利用方面具有很好的应用前景.CO₂泡沫混凝土在凝固前的稳定性是下一步要重点解决的技术难题.     

加速碳酸化技术对城市垃圾焚烧飞灰重金属稳定性影响研究

对南方某城市生活垃圾焚烧厂新鲜焚烧飞灰对CO₂的吸收及其碳酸化的过程进行了研究,实验从水分添加量、CO₂的分压等因素,考察了飞灰中重金属Pb的稳定化效果,并利用X射线衍射实验(XRD)、扫描电镜实验(SEM)对反应机理进行了分析.结果表明,不添加水分时,焚烧飞灰对CO₂的吸收效果较差;当水分添加量大于10％时,焚烧飞灰对CO₂的吸收效果较好.焚烧飞灰对纯CO₂的吸收效果较好,空气中的CO₂含量较低,在反应1 d后吸收效果不是十分明显.XRD实验结果表明,CO₂的吸收会使焚烧飞灰中大量的Ca(OH)₂与CO₂反应转化为CaCO₃,从而降低焚烧飞灰的碱性;部分重金属的氧化物会被碳酸化成生相应的碳酸盐.SEM实验结果表明,经过碳酸化处理后的飞灰颗粒表面生成了片状和圆柱状的晶体物质.     

Influence of SO2 in incineration flue gas on the sequestration of CO2 by municipal solid waste incinerator fly ash

The influence of CO2 content and presence of SO2 on the sequestration of CO2 by municipal solid waste incinerator(MSWI) fly ash was studied by investigating the carbonation reaction of MSWI fly ash with different combinations of simulated flue gas.The reaction between fly ash and 100% CO2 was relatively fast;the uptake of CO2 reached 87g CO2/kg ash,and the sequestered CO2 could be entirely released at high temperatures.When CO2 content was reduced to 12%,the reaction rate decreased;the uptake fell to 41g CO2/kg ash,and 70.7% of the sequestered CO2 could be released.With 12% CO2 in the presence of SO2,the reaction rate significantly decreased;the uptake was just 17g CO2/kg ash,and only 52.9% of the sequestered CO2 could be released.SO2 in the simulated gas restricted the ability of fly ash to sequester CO2 because it blocked the pores of the ash.     

Negative emissions of carbon dioxide through chemical-looping combustion (CLC) and gasification (CLG) using oxygen carriers based on manganese and iron

Carbon capture and storage (CCS) is an economically attractive strategy for avoiding carbon dioxide (CO₂) emissions from, e.g., power plants to the atmosphere. The combination of CCS and biomass combustion would result in a reduction of atmospheric CO₂, or net negative emissions, as plant growth is a form of sequestration of atmospheric carbon. Carbon capture can be achieved in a variety of ways, one of which is chemical looping. Chemical-looping combustion (CLC) and chemical looping gasification (CLG) are two promising technologies for conversion of biomass to heat and power or syngas/methane with carbon capture. There have been significant advances made with respect to CLC in the last two decades for all types of fuel, with much less research on the gasification technology. CLG offers some interesting opportunities for production of biofuels together with carbon capture and may have several advantages with respect to the bench mark indirect gasification process or dual-bed fluidized bed (DFBG) in this respect. In CLG, an oxygen carrier is used as a bed material instead of sand, which is common in indirect gasification, and this could have several advantages: (i) all generated CO₂ is present together with the syngas or methane in the fuel reactor outlet stream, thus in a concentrated stream, viable for separation and capture; (ii) the air reactor (or combustion chamber) should largely be free from trace impurities, thus preventing corrosion and fouling in this reactor; and (iii) the highly oxidizing conditions in the fuel reactor together with solid oxide surfaces should be advantageous with respect to limiting formation of tar species. In this study, two manganese ores and an iron-based waste material, LD slag, were investigated with respect to performance in these chemical-looping technologies. The materials were also impregnated with alkali (K) in order to gauge possible catalytic effects and also to establish a better understanding of the general behavior of oxygen carriers with alkali, an important component in biomass and biomass waste streams and often a precursor for high-temperature corrosion. The viability of the oxygen carriers was investigated using a synthetic biogas in a batch fluidized bed reactor. The conversion of CO, H₂, CH₄, and C₂H₄ was investigated in the temperature interval 800–950 °C. The reactivity, or oxygen transfer rate, was highest for the manganese ores, followed by the LD slag. The conversion of C₂H₄ was generally high but could largely be attributed to thermal decomposition. The K-impregnated samples showed enhanced reactivity during combustion conditions, and the Mangagran-K sample was able to achieve full conversion of benzene. The interaction of the solid material with alkali showed widely different behavior. The two manganese ores retained almost all alkali after redox testing, albeit exhibiting different migration patterns inside the particles. LD slag lost most alkali to the gas phase during testing, although some remained, possibly explaining a small difference in reactivity. In summary, the CLC and CLG processes could clearly be interesting for production of heat, power, or biofuel with negative CO₂ emissions. Manganese ores are most promising from this study, as they could absorb alkali, giving a better conversion and perhaps also inhibiting or limiting corrosion mechanisms in a combustor or gasifier.

     

Comparison of two reactor concepts for anoxygenic H2 production by Rhodobacter capsulatus

In the contribution at hand two main concepts of photobioreactors are considered: the flat-panel reactor and the tubular reactor. Both reactors are investigated under outdoor conditions in Germany in the summer time for their applicability for H₂ production by means of purple non-sulphur bacteria Rhodobacter capsulatus. The experiments are performed as fed batch. The performance of a photobioreactor is evaluated in terms of H₂ productivity per IRS (illuminated reactor surface). It is demonstrated that both reactors could be operated stable for several weeks with comparable H₂ productivities. The mean hydrogen productivity for the panel and the tubular reactor is 3690 ml H₂/(m_IRS² d) and 3350 ml H₂/(m_IRS² d) respectively. While approximately 8 m² of the illuminated reactor surface of the panel reactor can be installed on 1 m² of ground space, the relation of the illuminated reactor surface to the ground area for the tubular reactor is approximately 1–1.     

新安江水库二氧化碳排放的时空变化特征

新安江水库是我国华东地区最大的水库,面积580 km2,平均深度30 m,水库水体处于中贫营养状态.为了研究新安江水库中CO_2排放的时空变化特征,2014年12月至2015年12月采用静态浮箱法收集水库表面以分子扩散方式排放的CO_2,使用气相色谱仪分析CO_2浓度.结果表明,新安江水库CO_2排放通量从上游入库河流[(120.39±135.41)mg·(m~2·h)~(-1)]至库区主体[(36.65~61.94)mg·(m~2·h)~(-1)]呈下降趋势,而大坝下游河流中CO_2排放通量[(1 535.00±1 447.46)mg·(m~2·h)~(-1)]显著增加,约分别是上游入库河流和库区主体的13倍和25~42倍.但随着与大坝距离增加,大坝下游河流中CO_2排放通量显著下降,如7 km处的CO_2排放通量仅为出库水体处的20%.在库区主体中,CO_2排放通量具有明显的季节变化:CO_2排放通量在秋、冬季时为正值,最大值出现在冬季(12月或1月),说明此时库区表层水体是CO_2排放源;而CO_2排放通量在春、夏季为负值,最小值出现在春季(3、4或5月),说明此时库区表层水体是CO_2吸收汇,这可能与春、夏季时水体中藻类繁殖有关.所以,在调查水库表面CO_2排放时,应对水库的上游入库河流、库区主体和坝下河流进行全面长期的观测,才能避免低估水库中CO_2排放总量.     

太湖水-气界面CO2交换通量观测研究

基于2003-01～2005-06利用静态箱法对太湖水-气界面CO₂交换通量的观测,对太湖水-气界面交换通量的变化特征进行了分析研究.结果表明:太湖水-气界面CO₂交换通量存在明显的日变化,春、夏、秋、冬4季日平均通量分别为-0.79mg/(m²·h)、-4.89 mg/(m²·h)、-4.06 mg/(m²·h)和-2.56 mg/(m²·h),太湖均是CO₂的汇.一般污染越重的区域,CO₂通量值越大.藻型湖区水-气界面CO₂交换通量季节变化不明显,草型湖区水-气界面CO₂交换通量季节变化很明显,夏秋季高,冬春季低.CO₂通量变化的可能相关因子还有天气情况、太阳辐射、风速及水温、pH、TA、Chla、TC、TN和TP等.     

太湖水-气界面CO2交换通量观测研究

基于2003-01～2005-06利用静态箱法对太湖水-气界面CO2交换通量的观测,对太湖水-气界面交换通量的变化特征进行了分析研究.结果表明:太湖水-气界面CO2交换通量存在明显的日变化,春、夏、秋、冬4季日平均通量分别为-0.79 mg/(m2·h)、-4.89 mg/(m2·h)、-4.06 mg/(m2·h)和-2.56 mg/(m2·h),太湖均是CO2的汇.一般污染越重的区域,CO2通量值越大.藻型湖区水-气界面CO2交换通量季节变化不明显,草型湖区水-气界面CO2交换通量季节变化很明显,夏秋季高,冬春季低.CO2通量变化的可能相关因子还有天气情况、太阳辐射、风速及水温、pH、TA、Chla、TC、TN和TP等.     

Identification of main influencing factors of life cycle CO2 emissions from the integrated steelworks using sensitivity analysis

The amount of CO₂ emissions from steelworks accounts for a great share of the total CO₂ emissions from industry in China. Thus, reducing CO₂ emissions from steelworks is urgent for China's environmental protection and sustainable development. This study aims at identifying factors that influence CO₂ emissions from steelworks and proposing measures to reduce CO₂ emissions. The life cycle inventory (LCI) of iron and steel products implies the relationship between the CO₂ emissions of the steelworks and the input variables of the LCI. The Tornado Chart Tool is utilized to calculate the variation of CO₂ emissions caused by the change of each input variables of LCI. Then, mean sensitivity of each input variable is calculated and the ranking criterion developed is used to identify the main factors influencing the integrated steelworks. Subsequently, measures for reducing CO₂ emissions are proposed. The results indicate that the very important influencing factors of CO₂ emissions in steelworks are the CO₂ emission factor of Blast Furnace Gas (BFG), liquid steel unit consumption of continuous casting, continuous casting slab unit consumption of hot rolling and hot metal ratio of steel making. Consequently, many efficient measures for reducing CO₂ emissions have been proposed, such as removing CO₂ contained in BFG, decreasing the hot metal ratio of Basic Oxygen Furnace (BOF), recycling BFG, optimizing the products' structure, etc.     

三峡库区万州段河流水-气界面CO2通量支干流对比及影响机制初探

以三峡库区万州段干流及典型支流澎溪河为研究对象,监测2019年4～9月水华期间水体中CO₂浓度以及12个环境指标,估算水-气界面CO₂通量并进行支干流对比.将12个环境指标分为气候因子、水环境因子、碳源因子、营养因子和沉积物因子,探讨5类因子对CO₂通量的影响途径和贡献率,进一步为控制水库温室气体排放提供数据积累和理论支持.结果表明,监测期间内高阳、黄石和万州平均CO₂通量分别为（1.445±1.739）、（3.118±2.963）和（2.899±1.144）mmol·（m²·h）^-1,表现为:澎溪河支流高阳<干流万州<澎溪河支流黄石.从变化幅度来看,支流水体CO₂通量变幅较大,干流水体变化幅度则相对较小,是较稳定的CO₂"源".长江干流作为陆地向海洋的生源物质运输枢纽,相比其支流碳含量和流速更高,这使得通常情况下干流CO₂通量大于支流.但水文情势的不同使得同一支流不同点位CO<...     

Carbon dioxide emissions from spring ploughing of grassland in Ireland

Grassland re-seeding or land-use change requires ploughing, which may enhance carbon dioxide (CO₂) emissions from soil. This study observed the short to intermediate-term (37 days) effects of ploughing on CO₂ emissions from poorly drained grassland using automated soil respiration chambers. Immediately after ploughing, a brief peak in CO₂ emissions from soil occurred with a maximum observed flux of 6.91 g CO₂ m⁻² h⁻¹. Contradictory to other reported results, ecosystem respiration after ploughing was lower on the ploughed than on the grass site. After including estimates of photosynthesis in the analysis, ploughing led to significantly higher net CO₂ emissions than from grassland. The main mechanism of C loss during ploughing was most likely due to a reduction in gross primary production rather than enhanced soil respiration.     

利用硅灰石原位改善厌氧消化微生物电解池的产气特性

厌氧消化-微生物电解池(Anaerobic digestion-Microbial electrolysis cell,AD-MEC)具有有机物降解速度快、降解率高的优点,但其所产沼气中依然存在CO_2含量较高的问题.为降低AD-MEC所产沼气中CO_2的含量,本研究将矿物碳酸化耦合入AD-MEC中,研究添加硅灰石对AD-MEC中CO_2的固定效果.实验结果表明,添加硅灰石可使AD-MEC中CO_2产生量减少40.0%,沼气中CO_2含量从10.0%±1.3%减少到4.5%±1.1%;X射线衍射(XRD)及扫描电镜-能谱(SEM-EDS)分析表明了CaCO_3沉淀的生成,证明硅灰石介导矿物碳酸化固定了AD-MEC中的CO_2.此外,添加硅灰石使Ca~(2+)溶出,缓冲了pH,减轻了厌氧消化产酸阶段对产甲烷菌的抑制,促进了有机物的降解,可溶性化学需氧量(SCOD)去除率提高了11.2%,并使CH_4产量提高18.0%,CH_4产率达到305 mL·g~(-1),沼气中CH_4含量达到95.5%±1.2%.硅灰石的添加实现了AD-MEC中CO_2的原位捕获,同时增益了厌氧消化效果,提高了甲烷产量.     

炉渣与生物炭施加对稻田温室气体排放及其相关微生物影响

为了减少稻田温室气体排放通量,本研究对稻田土壤进行炉渣和生物炭单一施加和混合施加处理,并测定了早、晚稻拔节期和乳熟期CO_2、CH_4和N_2O排放通量及相关微生物(细菌、真菌、硝化细菌、反硝化细菌)的数量.结果表明,稻田施加废弃物可以减少温室气体的排放通量.在早、晚稻的拔节期,施加生物炭显著降低了CO_2和N_2O的排放通量(p0.05),混合施加显著降低了CO_2和CH_4的排放通量(p0.05),施加炉渣条件下3种温室气体的排放通量与对照组相比没有差异.施加炉渣或生物炭都显著降低硝化细菌的数量(p0.05),混施处理显著降低细菌、硝化细菌、反硝化细菌数量(p0.05),但显著提高了稻田土壤真菌/细菌比值(p0.05).在早、晚稻的乳熟期,炉渣、生物炭、混施处理能显著降低CH_4排放通量(p0.05),而生物炭处理显著降低N_2O排放通量(p0.05).炉渣处理显著降低细菌、硝化细菌、反硝化细菌数量(p0.05),生物炭处理显著降低细菌、反硝化细菌数量(p0.05),混施处理显著降低细菌、硝化细菌数量,并显著提高真菌/细菌比值(p0.05).温室气体排放与微生物数量之间的相关性分析结果表明,CO_2、CH_4排放通量与细菌数量呈显著正相关,与真菌/细菌比值呈显著负相关;而N_2O排放通量则与硝化细菌、反硝化细菌数量呈显著正相关.     

贵州喀斯特水库红枫湖、百花湖P(CO2)季节变化研究

针对贵州喀斯特地区富营养水库（红枫湖、百花湖）表层水中的CO₂分压P(CO₂)进行为期1 a的监测,分析了影响两湖P(CO₂)季节变化的因素并阐明了两湖P(CO₂)季节变化的机理.不同于北部温带地区水库,两湖出现明显的季节变化特征：夏季表层水中CO₂欠饱和,其他季节CO₂过饱和.通过对物理、化学及生物因素与P(CO₂)之间的相关性分析. 结果表明,两湖P(CO₂)与Chla之间存在的显著负相关,是由于浮游植物光合作用与细菌呼吸作用共同影响的结果,也是两湖P(CO₂)出现季节变化的主要原因.水温与P(CO₂)之间的显著负相关,主要是由于水温影响浮游植物生长引起的.降雨量与P(CO₂)之间的显著负相关,主要是由于降雨量影响水库中营养盐的输入和浮游植物生长引起的.NO^-₃、NO^-₂与P(CO₂)之间的显著正相关,是藻类吸收与有机质降解、硝化反应等共同作用的结果.SiO^{2-₃与P(CO₂)之间的显著负相关,是SiO2-₃受降雨输入及藻类吸收共同影响的结果.而两湖DOC与P(CO₂)相关性的差异可能与两湖DOC来源不同有关.}     

Low-carbon transition of iron and steel industry in China: Carbon intensity, economic growth and policy intervention

As the biggest iron and steel producer in the world and one of the highest CO₂ emission sectors, China's iron and steel industry is undergoing a low-carbon transition accompanied by remarkable technological progress and investment adjustment, in response to the macroeconomic climate and policy intervention. Many drivers of the CO₂ emissions of the iron and steel industry have been explored, but the relationships between CO₂ abatement, investment and technological expenditure, and their connections with the economic growth and governmental policies in China, have not been conjointly and empirically examined. We proposed a concise conceptual model and an econometric model to investigate this crucial question. The results of regression, Granger causality test and impulse response analysis indicated that technological expenditure can significantly reduce CO₂ emissions, and that investment expansion showed a negative impact on CO₂ emission reduction. It was also argued with empirical evidence that a good economic situation favored CO₂ abatement in China's iron and steel industry, while achieving CO₂ emission reduction in this industrial sector did not necessarily threaten economic growth. This shed light on the dispute over balancing emission cutting and economic growth. Regarding the policy aspects, the year 2000 was found to be an important turning point for policy evolution and the development of the iron and steel industry in China. The subsequent command and control policies had a significant, positive effect on CO₂ abatement.     

Efficient degradation of chlorobenzene in a non-thermal plasma catalytic reactor supported on CeO2/HZSM-5 catalysts

Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO₂/HZSM-5 catalysts. The performance of catalysts was evaluated in terms of removal and energy efficiency. The decomposition products of chlorobenzene were analyzed. The results show that CeO₂/HZSM-5 exhibited a good catalytic activity, which resulted in enhancements of chlorobenzene removal, energy efficiency, and the formation of lower amounts of by-products. With regards to CO₂ selectivity, the presence of catalysts favors the oxidation of by-products, leading to a higher CO₂ selectivity. With respect to ozone, which is considered as an unavoidable by-product in air plasma reactors, a noticeable decrease in its concentration was observed in the presence of catalysts. Furthermore, the stability of the catalyst was investigated by analyzing the evolution of conversion in time. The experiment results indicated that CeO₂/HZSM-5 catalysts have excellent stability: chlorobenzene conversion only decreased from 78% to 60% after 75 hr, which means that the CeO₂/HZSM-5 suffered a slight deactivation. Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared (FT-IR) spectroscopy, scanning electron microscope (SEM) and energy dispersive X-ray spectroscopy (EDS) analyses of the catalyst before and after the reaction, revealing the cause of catalyst deactivation.