Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101814
This study presents the synthesis of a series of FeOx-NbOx mixed oxide catalysts for the selective catalytic reduction (SCR) of NO by NH3. By meticulously controlling the Fe/Nb molar ratio, we have rationally tailored the proceeding of the main reaction of NO reduction and the side reaction of NH3 oxidation to NOx. The incorporation of NbOx introduced a significant number of acid sites, which enhanced the adsorption of NH3 on the catalyst surface, particularly at elevated temperatures. Additionally, the oxidative capacity of the catalyst was moderated by the addition of NbOx, hindering the over-oxidation of NH3 to NO or NO2, thus preserving more NH3 to act as a reductant for NO reduction. Consequently, the NbOx-enriched samples exhibited improved deNOx performance. However, an excessive amount of NbOx led to a notably weakened oxidative ability, which negatively impacted the activation of reactants and resulted in decreased NO conversion at lower temperatures. The optimized catalyst presented >80 % NO conversion and >95 % N2 selectivity within a temperature range of 250–400 °C. These findings offer valuable insights for the development of new catalysts with an extended operational temperature window.
本研究介绍了一系列用于 NH3 对 NO 的选择性催化还原 (SCR) 的 FeOx-NbOx 混合氧化物催化剂的合成。通过精心控制铁/铌摩尔比,我们合理地调整了氮氧化物还原主反应和 NH3 氧化为氮氧化物副反应的进行。NbOx 的加入引入了大量酸性位点,从而增强了催化剂表面对 NH3 的吸附,尤其是在高温条件下。此外,NbOx 的加入还缓和了催化剂的氧化能力,阻碍了 NH3 过度氧化为 NO 或 NO2,从而保留了更多的 NH3 作为还原剂用于还原 NO。因此,富含氧化铌的样品具有更好的脱硝性能。然而,过量的氧化铌会导致氧化能力明显减弱,从而对反应物的活化产生负面影响,并导致在较低温度下氮氧化物的转化率降低。优化后的催化剂在 250-400 °C 的温度范围内具有 80% 的 NO 转化率和 95% 的 N2 选择性。这些发现为开发具有更宽工作温度窗口的新型催化剂提供了宝贵的启示。
{"title":"Tailoring the proceeding of the NH3-SCO and NH3-SCR reactions over FeOx catalysts by modifying with NbOx","authors":"","doi":"10.1016/j.joei.2024.101814","DOIUrl":"10.1016/j.joei.2024.101814","url":null,"abstract":"<div><p>This study presents the synthesis of a series of FeO<sub><em>x</em></sub>-NbO<sub><em>x</em></sub> mixed oxide catalysts for the selective catalytic reduction (SCR) of NO by NH<sub>3</sub>. By meticulously controlling the Fe/Nb molar ratio, we have rationally tailored the proceeding of the main reaction of NO reduction and the side reaction of NH<sub>3</sub> oxidation to NO<sub><em>x</em></sub>. The incorporation of NbO<sub><em>x</em></sub> introduced a significant number of acid sites, which enhanced the adsorption of NH<sub>3</sub> on the catalyst surface, particularly at elevated temperatures. Additionally, the oxidative capacity of the catalyst was moderated by the addition of NbO<sub><em>x</em></sub>, hindering the over-oxidation of NH<sub>3</sub> to NO or NO<sub>2</sub>, thus preserving more NH<sub>3</sub> to act as a reductant for NO reduction. Consequently, the NbO<sub><em>x</em></sub>-enriched samples exhibited improved deNO<sub><em>x</em></sub> performance. However, an excessive amount of NbO<sub><em>x</em></sub> led to a notably weakened oxidative ability, which negatively impacted the activation of reactants and resulted in decreased NO conversion at lower temperatures. The optimized catalyst presented >80 % NO conversion and >95 % N<sub>2</sub> selectivity within a temperature range of 250–400 °C. These findings offer valuable insights for the development of new catalysts with an extended operational temperature window.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101813
In the present work, co-pyrolysis experiments of walnut shell (WS), polyethylene (PE) and their blends were performed in the thermogravimetric analyzer and lab-scale bubbling fluidized bed reactor, to clarify co-pyrolysis behaviors, synergy interactions and pyrolysis oil properties. Besides, the HZSM-5 zeolite was used as the catalyst and its catalytic characteristics were studied. Results indicated that as PE mass ratio rose from 0 to 100 %, the initial temperature monotonically increased from 265.4 to 417.3 °C, while its terminal temperature progressively decreased from 668.3 to 527.5 °C, suggesting that the addition of PE was able to accelerate the pyrolysis of samples. The co-pyrolysis of blends was distinguished into three stages, with a negative interaction observed in the first stage and positive interactions found in second and third stages. Besides, in the bubbling fluidized bed experiments, the liquid phase product yield first elevated and then reduced with rising temperature, and a high temperature promoted the degradation of oxygen-containing compounds and enhanced aromatics generation. The synergistic interaction in the co-pyrolysis of WS and PE declined the liquid phase product yield while elevating the gas phase product yield. On the other hand, blending with PE facilitated the generation of alkanes and olefins, while inhibiting the contents of oxygen-containing components and aromatics, and simultaneously, the heavy oil fraction was increased. Finally, the carbon deposited on the surface of catalysts was amorphous carbons, and could be removed by oxidation process, whereas its catalytic properties progressively declined with rising cycle number, leading to a downtrend of aromatics and olefins and an opposite trend for oxygen-containing components.
本研究在热重分析仪和实验室规模的鼓泡流化床反应器中进行了核桃壳(WS)、聚乙烯(PE)及其混合物的共热解实验,以阐明共热解行为、协同作用和热解油特性。此外,还使用 HZSM-5 沸石作为催化剂,研究了其催化特性。结果表明,随着聚乙烯质量比从 0% 上升到 100%,初始温度从 265.4 ℃单调上升到 417.3 ℃,而最终温度则从 668.3 ℃逐渐下降到 527.5 ℃,这表明聚乙烯的加入能够加速样品的热解。混合物的共热解分为三个阶段,第一阶段为负作用,第二和第三阶段为正作用。此外,在鼓泡流化床实验中,随着温度的升高,液相产物产率先升高后降低,高温促进了含氧化合物的降解,并增强了芳烃的生成。WS 和 PE 共热解过程中的协同作用降低了液相产物产率,同时提高了气相产物产率。另一方面,与 PE 的混合促进了烷烃和烯烃的生成,同时抑制了含氧成分和芳烃的含量,重油馏分也随之增加。最后,沉积在催化剂表面的碳为无定形碳,可通过氧化过程去除,但其催化性能随着循环次数的增加而逐渐下降,导致芳烃和烯烃含量呈下降趋势,而含氧组分则呈相反趋势。
{"title":"Study of the co-pyrolysis behavior and bio-oil characterization of walnut shell and polyethylene by thermogravimetric analyzer and bubbling fluidized bed","authors":"","doi":"10.1016/j.joei.2024.101813","DOIUrl":"10.1016/j.joei.2024.101813","url":null,"abstract":"<div><p>In the present work, co-pyrolysis experiments of walnut shell (WS), polyethylene (PE) and their blends were performed in the thermogravimetric analyzer and lab-scale bubbling fluidized bed reactor, to clarify co-pyrolysis behaviors, synergy interactions and pyrolysis oil properties. Besides, the HZSM-5 zeolite was used as the catalyst and its catalytic characteristics were studied. Results indicated that as PE mass ratio rose from 0 to 100 %, the initial temperature monotonically increased from 265.4 to 417.3 °C, while its terminal temperature progressively decreased from 668.3 to 527.5 °C, suggesting that the addition of PE was able to accelerate the pyrolysis of samples. The co-pyrolysis of blends was distinguished into three stages, with a negative interaction observed in the first stage and positive interactions found in second and third stages. Besides, in the bubbling fluidized bed experiments, the liquid phase product yield first elevated and then reduced with rising temperature, and a high temperature promoted the degradation of oxygen-containing compounds and enhanced aromatics generation. The synergistic interaction in the co-pyrolysis of WS and PE declined the liquid phase product yield while elevating the gas phase product yield. On the other hand, blending with PE facilitated the generation of alkanes and olefins, while inhibiting the contents of oxygen-containing components and aromatics, and simultaneously, the heavy oil fraction was increased. Finally, the carbon deposited on the surface of catalysts was amorphous carbons, and could be removed by oxidation process, whereas its catalytic properties progressively declined with rising cycle number, leading to a downtrend of aromatics and olefins and an opposite trend for oxygen-containing components.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122930","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101807
Converting hydrocarbons can make the fossil fuel industry more flexible in responding to market changes by producing various products to meet market demands. Efficient, clean, and flexible plasma processes are a highly promising technology for hydrocarbon processing and conversion. In this study, the conversion of n-hexadecane was investigated using ethanol solution-assisted pulsed liquid-phase discharge plasma. The effects of recycle and batch devices and discharge frequency on feedstocks conversions and product yields were examined. The use of a recycle device facilitated the conversion of n-hexadecane. Adjusting the frequency enabled the regulation of products concentration. High discharge frequency increased the cracking of n-hexadecane and promoted further cracking of reactants into smaller molecular products, boosting the proportion of H2 and C2 hydrocarbons, and enhancing the yield of gases and light hydrocarbons. Reducing the frequency favored polymerization reactions, resulting in the formation of heavy hydrocarbons. At a frequency of 10.2 kHz, the recycle device achieved a gas production rate of 112.1 mL/min and a gas production efficiency of 87.5 mL/kJ. With an SEI of 3202 kJ/L, the conversion of n-hexadecane was 15.5 %, the yield of light hydrocarbons was 717.0 mg, and the light product selectivity was 97.1 %. This study offers an efficient approach for the processing and conversion of hydrocarbons in the fossil fuel industry.
{"title":"Effects of discharge frequency on the conversion of n-hexadecane by pulsed liquid-phase discharge in recycle and batch devices","authors":"","doi":"10.1016/j.joei.2024.101807","DOIUrl":"10.1016/j.joei.2024.101807","url":null,"abstract":"<div><p>Converting hydrocarbons can make the fossil fuel industry more flexible in responding to market changes by producing various products to meet market demands. Efficient, clean, and flexible plasma processes are a highly promising technology for hydrocarbon processing and conversion. In this study, the conversion of n-hexadecane was investigated using ethanol solution-assisted pulsed liquid-phase discharge plasma. The effects of recycle and batch devices and discharge frequency on feedstocks conversions and product yields were examined. The use of a recycle device facilitated the conversion of n-hexadecane. Adjusting the frequency enabled the regulation of products concentration. High discharge frequency increased the cracking of n-hexadecane and promoted further cracking of reactants into smaller molecular products, boosting the proportion of H<sub>2</sub> and C<sub>2</sub> hydrocarbons, and enhancing the yield of gases and light hydrocarbons. Reducing the frequency favored polymerization reactions, resulting in the formation of heavy hydrocarbons. At a frequency of 10.2 kHz, the recycle device achieved a gas production rate of 112.1 mL/min and a gas production efficiency of 87.5 mL/kJ. With an SEI of 3202 kJ/L, the conversion of n-hexadecane was 15.5 %, the yield of light hydrocarbons was 717.0 mg, and the light product selectivity was 97.1 %. This study offers an efficient approach for the processing and conversion of hydrocarbons in the fossil fuel industry.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142098660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101810
A process of producing hydrogen-rich syngas by chemical looping steam gasification is proposed, using pickling sludge (PS) as the oxygen carrier and paper-making sludge(PMS) along with municipal sludge(MS) as the fuel. The reaction characteristics of producing hydrogen-rich syngas through the gasification of PMS and MS were studied. The effects of temperature, steam flow rate and the blended ratio of PS on carbon conversion rate and gasification reaction efficiency were discussed, and the migration mechanisms of the main elements were explained. The results show that FeF3 in PS exhibits stronger activity than conventional Fe2O3 in catalyzing the gasification of PMS and MS at high temperature. With the blended mass ratio of 1:1 of PS, the carbon conversion rate of PMS and MS was increased by 11.8 % and 42.5 %, and the gasification efficiency was increased by 11.1 % and 25.85 %. The Fe3+ in PS catalyzed the cleavage of C-H bonds in biomass sludge, and Fe3+ was reduced to form the intermediate product FeCr2O4 with tar cracking function. After the gasification reaction, the Fe in PS was completely converted to Fe3O4 under the action of MS, while the CaO in PMS promoted the valence cycle of Fe to some extent, resulting in partial Fe being fully cycled to Fe3+ to form γFe2O3. In addition, the CaO can fix the F element in PS to form CaF2, thus reducing the environmental hazard.
以酸洗污泥(PS)为氧载体,造纸污泥(PMS)和市政污泥(MS)为燃料,提出了一种通过化学循环蒸汽气化生产富氢合成气的工艺。研究了通过气化 PMS 和 MS 产生富氢合成气的反应特性。讨论了温度、蒸汽流速和 PS 混合比例对碳转化率和气化反应效率的影响,并解释了主要元素的迁移机制。结果表明,与传统的 Fe2O3 相比,PS 中的 FeF3 在高温下催化 PMS 和 MS 的气化过程中表现出更强的活性。当 PS 的混合质量比为 1:1 时,PMS 和 MS 的碳转化率分别提高了 11.8 % 和 42.5 %,气化效率分别提高了 11.1 % 和 25.85 %。PS 中的 Fe3+ 催化了生物质污泥中 C-H 键的裂解,Fe3+ 被还原形成具有焦油裂解功能的中间产物 FeCr2O4。气化反应后,PS 中的 Fe 在 MS 的作用下完全转化为 Fe3O4,而 PMS 中的 CaO 则在一定程度上促进了 Fe 的价态循环,使部分 Fe 完全循环为 Fe3+,形成γFe2O3。此外,氧化钙还能固定 PS 中的 F 元素,形成 CaF2,从而减少对环境的危害。
{"title":"Study on interaction mechanism of steam coupling biomass sludge gasification to syngas with pickling sludge as oxygen carrier","authors":"","doi":"10.1016/j.joei.2024.101810","DOIUrl":"10.1016/j.joei.2024.101810","url":null,"abstract":"<div><p>A process of producing hydrogen-rich syngas by chemical looping steam gasification is proposed, using pickling sludge (PS) as the oxygen carrier and paper-making sludge(PMS) along with municipal sludge(MS) as the fuel. The reaction characteristics of producing hydrogen-rich syngas through the gasification of PMS and MS were studied. The effects of temperature, steam flow rate and the blended ratio of PS on carbon conversion rate and gasification reaction efficiency were discussed, and the migration mechanisms of the main elements were explained. The results show that FeF<sub>3</sub> in PS exhibits stronger activity than conventional Fe<sub>2</sub>O<sub>3</sub> in catalyzing the gasification of PMS and MS at high temperature. With the blended mass ratio of 1:1 of PS, the carbon conversion rate of PMS and MS was increased by 11.8 % and 42.5 %, and the gasification efficiency was increased by 11.1 % and 25.85 %. The Fe<sup>3+</sup> in PS catalyzed the cleavage of C-H bonds in biomass sludge, and Fe<sup>3+</sup> was reduced to form the intermediate product FeCr<sub>2</sub>O<sub>4</sub> with tar cracking function. After the gasification reaction, the Fe in PS was completely converted to Fe<sub>3</sub>O<sub>4</sub> under the action of MS, while the CaO in PMS promoted the valence cycle of Fe to some extent, resulting in partial Fe being fully cycled to Fe<sup>3+</sup> to form γFe<sub>2</sub>O<sub>3</sub>. In addition, the CaO can fix the F element in PS to form CaF<sub>2</sub>, thus reducing the environmental hazard.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142098656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101808
The impacts of climate change and the issue of greenhouse gas emissions have sparked research into renewable energy alternatives to fossil fuels. Hydrogen has gained attention as a clean, renewable and environmentally friendly energy source. Enhanced-ethanol steam reforming has been proposed as a promising method for blue hydrogen production, addressing greenhouse gas emission issues. The use of catalysts enhances the adsorption of ethanol and water molecules on the surface, promoting the reaction rate. This study systematically explored the effects of different Fe loading and CaO addition ratios on the ethanol steam reforming and CO2 conversion processes to optimize catalyst performance. The experimental results showed that Fe/SiC catalysts effectively promoted the conversion of ethanol and generated high-purity hydrogen, exhibiting excellent catalytic activity. Specifically, a catalyst with 10 % Fe loading and mixed with 0.3g CaO significantly increased the hydrogen yield to 64.4 mmol/g, which was 2.88 times higher than that without the catalyst.
气候变化的影响和温室气体排放问题引发了对化石燃料的可再生能源替代品的研究。氢气作为一种清洁、可再生和环保的能源受到了关注。有人提出,强化乙醇蒸汽转化是一种很有前途的蓝色制氢方法,可以解决温室气体排放问题。催化剂的使用可增强乙醇和水分子在催化剂表面的吸附,从而提高反应速率。本研究系统地探讨了不同 Fe 负载和 CaO 添加比对乙醇蒸汽转化和 CO2 转化过程的影响,以优化催化剂性能。实验结果表明,Fe/SiC 催化剂能有效促进乙醇转化并产生高纯度氢气,表现出优异的催化活性。具体而言,铁含量为 10% 并与 0.3g CaO 混合的催化剂可显著提高氢气产量,使其达到 64.4 mmol/g,是未添加催化剂时的 2.88 倍。
{"title":"Sorption-enhanced ethanol steam reforming coupled with in-situ CO2 capture and conversion","authors":"","doi":"10.1016/j.joei.2024.101808","DOIUrl":"10.1016/j.joei.2024.101808","url":null,"abstract":"<div><p>The impacts of climate change and the issue of greenhouse gas emissions have sparked research into renewable energy alternatives to fossil fuels. Hydrogen has gained attention as a clean, renewable and environmentally friendly energy source. Enhanced-ethanol steam reforming has been proposed as a promising method for blue hydrogen production, addressing greenhouse gas emission issues. The use of catalysts enhances the adsorption of ethanol and water molecules on the surface, promoting the reaction rate. This study systematically explored the effects of different Fe loading and CaO addition ratios on the ethanol steam reforming and CO<sub>2</sub> conversion processes to optimize catalyst performance. The experimental results showed that Fe/SiC catalysts effectively promoted the conversion of ethanol and generated high-purity hydrogen, exhibiting excellent catalytic activity. Specifically, a catalyst with 10 % Fe loading and mixed with 0.3g CaO significantly increased the hydrogen yield to 64.4 mmol/g, which was 2.88 times higher than that without the catalyst.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142149445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101805
Introducing low-carbon oxygenated fuels into the current transport sector provides an effective pathway for mitigating the emissions of greenhouse gases and harmful pollutants such as soot. Previous studies have revealed that oxygenated fuels can reduce soot formation, but the soot-reduction potential is closely related to the chemical interaction between the oxygenates and the baseline hydrocarbons. This work is devoted to study the effects of blending dimethoxymethane (DMM) and isopropanol (IPA) on soot formation in ethylene-based and propane-based counterflow diffusion flames. Soot formation in the target flames was experimentally characterized using a planar light extinction technique, accompanied by numerical analysis to provide complementary insights. The results confirmed that the effects of blending oxygenates on soot formation are sensitive to the fuel-specific molecular structure of the oxygenates and hydrocarbons. For the C2H4-based flames, blending DMM and IPA could lead to a synergistic effect on soot formation due to chemical fuel interaction, with stronger synergy observed with IPA blending. In contrast, no evident synergistic effects on soot formation were observed in the C3H8-based flames, for which a notable soot reduction was observed with DMM blending. Reaction pathway analysis suggested that the occurrence of soot synergy in the C2H4-based flames is mainly due to the chemical interaction between the methyl radicals generated from DMM/IPA and the C2 species from C2H4. This study is expected to deepen our understanding of the soot formation behavior of DMM- and IPA-blended flames, thus contributing to their successful usage as clean alternative fuels.
{"title":"Effects of dimethoxymethane and isopropanol blending on soot formation in ethylene and propane counterflow diffusion flames","authors":"","doi":"10.1016/j.joei.2024.101805","DOIUrl":"10.1016/j.joei.2024.101805","url":null,"abstract":"<div><p>Introducing low-carbon oxygenated fuels into the current transport sector provides an effective pathway for mitigating the emissions of greenhouse gases and harmful pollutants such as soot. Previous studies have revealed that oxygenated fuels can reduce soot formation, but the soot-reduction potential is closely related to the chemical interaction between the oxygenates and the baseline hydrocarbons. This work is devoted to study the effects of blending dimethoxymethane (DMM) and isopropanol (IPA) on soot formation in ethylene-based and propane-based counterflow diffusion flames. Soot formation in the target flames was experimentally characterized using a planar light extinction technique, accompanied by numerical analysis to provide complementary insights. The results confirmed that the effects of blending oxygenates on soot formation are sensitive to the fuel-specific molecular structure of the oxygenates and hydrocarbons. For the C<sub>2</sub>H<sub>4</sub>-based flames, blending DMM and IPA could lead to a synergistic effect on soot formation due to chemical fuel interaction, with stronger synergy observed with IPA blending. In contrast, no evident synergistic effects on soot formation were observed in the C<sub>3</sub>H<sub>8</sub>-based flames, for which a notable soot reduction was observed with DMM blending. Reaction pathway analysis suggested that the occurrence of soot synergy in the C<sub>2</sub>H<sub>4</sub>-based flames is mainly due to the chemical interaction between the methyl radicals generated from DMM/IPA and the C<sub>2</sub> species from C<sub>2</sub>H<sub>4</sub>. This study is expected to deepen our understanding of the soot formation behavior of DMM- and IPA-blended flames, thus contributing to their successful usage as clean alternative fuels.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101812
Co-pyrolysis technology offers a viable solution for utilizing biomass and waste plastics as a valuable energy resource, to support waste management, energy supply and environmental protection. In this paper, co-pyrolysis of poplar tree (PT) and polystyrene (PS) at mixture ratios of 0:1, 3:1, 2:1, 1:1, 1:2, 1:3 and 1:0 under different pyrolysis temperatures (450, 550, 650, and 700 °C), using different catalysts (HZSM-5, MCM-41, Fe/HZSM-5, and Cu/HZSM-5) were investigated using gas chromatography/mass spectrometry (Py-GC/MS) diagnostics for determining products distribution and synergistic effects. The results showed that PT performed best at a pyrolysis temperature of 650 °C, whereas PS performed best at 550 °C. The relative amount of aromatics in the co-pyrolysis products of PT and PS was highest at 550 °C that showed positive synergistic effects. The synergistic effects from the co-pyrolysis of PT and PS were significantly different at different mixture ratios of the PT and PS feedstocks. At mixture ratios of 1:1 and 1:2, the relative amounts of polycyclic aromatic hydrocarbons (PAHs) and monocyclic aromatic hydrocarbons (MAH) were higher and showed positive synergistic effects. The catalysts promoted the generation of MAH and inhibited the PAHs formation in the co-pyrolysis. The Fe/HZSM-5 catalyst provided the most significant effect on MAH showing the highest relative amounts. The results showed that highest yield of monocyclic aromatic hydrocarbons can be achieved from the pyrolysis of PT and PS materials at 1:1 mixture ratio using Fe/HZSM-5 catalyst, at a reaction temperature of 550 °C.
共热解技术为利用生物质和废塑料作为宝贵的能源资源提供了可行的解决方案,有助于废物管理、能源供应和环境保护。在不同的热解温度(450、550、650 和 700 °C)下,使用不同的催化剂(HZSM-5、MCM-41、Fe/HZSM-5 和 Cu/HZSM-5),采用气相色谱/质谱分析法(Py-GC/MS)对聚苯乙烯和聚苯乙烯(PS)进行了研究,以确定产物分布和协同效应。结果表明,PT 在高温分解温度为 650 °C 时性能最佳,而 PS 在高温分解温度为 550 °C 时性能最佳。在 550 °C 时,PT 和 PS 共同热解产物中芳烃的相对含量最高,显示出积极的协同效应。在 PT 和 PS 原料的不同混合比例下,PT 和 PS 共热解的协同效应有显著差异。当混合比为 1:1 和 1:2 时,多环芳烃(PAHs)和单环芳烃(MAH)的相对含量较高,显示出积极的协同效应。催化剂在共热解过程中促进了 MAH 的生成,抑制了 PAHs 的形成。其中,Fe/HZSM-5 催化剂对 MAH 的影响最为显著,相对含量最高。结果表明,使用 Fe/HZSM-5 催化剂以 1:1 的混合比例热解 PT 和 PS 材料,在 550 °C 的反应温度下可获得最高产量的单环芳烃。
{"title":"Towards enhanced monocyclic aromatic hydrocarbons production from Co-pyrolysis of biomass and waste polystyrene plastic","authors":"","doi":"10.1016/j.joei.2024.101812","DOIUrl":"10.1016/j.joei.2024.101812","url":null,"abstract":"<div><p>Co-pyrolysis technology offers a viable solution for utilizing biomass and waste plastics as a valuable energy resource, to support waste management, energy supply and environmental protection. In this paper, co-pyrolysis of poplar tree (PT) and polystyrene (PS) at mixture ratios of 0:1, 3:1, 2:1, 1:1, 1:2, 1:3 and 1:0 under different pyrolysis temperatures (450, 550, 650, and 700 °C), using different catalysts (HZSM-5, MCM-41, Fe/HZSM-5, and Cu/HZSM-5) were investigated using gas chromatography/mass spectrometry (Py-GC/MS) diagnostics for determining products distribution and synergistic effects. The results showed that PT performed best at a pyrolysis temperature of 650 °C, whereas PS performed best at 550 °C. The relative amount of aromatics in the co-pyrolysis products of PT and PS was highest at 550 °C that showed positive synergistic effects. The synergistic effects from the co-pyrolysis of PT and PS were significantly different at different mixture ratios of the PT and PS feedstocks. At mixture ratios of 1:1 and 1:2, the relative amounts of polycyclic aromatic hydrocarbons (PAHs) and monocyclic aromatic hydrocarbons (MAH) were higher and showed positive synergistic effects. The catalysts promoted the generation of MAH and inhibited the PAHs formation in the co-pyrolysis. The Fe/HZSM-5 catalyst provided the most significant effect on MAH showing the highest relative amounts. The results showed that highest yield of monocyclic aromatic hydrocarbons can be achieved from the pyrolysis of PT and PS materials at 1:1 mixture ratio using Fe/HZSM-5 catalyst, at a reaction temperature of 550 °C.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142149444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101802
DIB (Diisobutylene, JC8H16) strongly correlates with real gasoline and significantly impacts the combustion behavior of alternative fuels designed as gasoline substitutes. However, accuracy concerns persist in laminar burning velocity data reported in literature. In this paper, the laminar burning velocities of DIB + air, DIB + PRF + air, and DIB + TRF + air mixtures were measured by the heat flux method at 1 atm. (PRF, Primary Reference Fuel; TRF, Toluene Reference Fuel) The equivalence ratio was controlled within 0.6–1.3, and the initial temperatures were set at 298K, 318K, and 338K. Additionally, by employing the mechanism proposed by Ren et al., the simulated values align with the experimental data, thus prompting the conduction of a reaction kinetic analysis. The analysis of chemical reaction kinetics reveals the reaction pathways of DIB, with a notable observation that an increase in temperature or a decrease in equivalence ratio can both lead to an elevation in the degree of unsaturation in the bonds of intermediate species. During laminar flame combustion, PRF and TRF compete with DIB for oxygen, with PRF appearing to have a stronger ability to capture oxygen. In addition, the laminar burning velocity temperature dependence coefficient α decreases first and then increases with the increase of the equivalence ratio, where the minimum α is obtained at equivalence ratio = 1.1. Additionally, the laminar burning velocity at higher initial temperatures is estimated by the extrapolation method and compared with the experimental data reported in literature.
{"title":"Experimental and numerical study of laminar burning velocity for Diisobutylene+ PRF/TRF mixtures","authors":"","doi":"10.1016/j.joei.2024.101802","DOIUrl":"10.1016/j.joei.2024.101802","url":null,"abstract":"<div><p>DIB (Diisobutylene, JC<sub>8</sub>H<sub>16</sub>) strongly correlates with real gasoline and significantly impacts the combustion behavior of alternative fuels designed as gasoline substitutes. However, accuracy concerns persist in laminar burning velocity data reported in literature. In this paper, the laminar burning velocities of DIB + air, DIB + PRF + air, and DIB + TRF + air mixtures were measured by the heat flux method at 1 atm. (PRF, Primary Reference Fuel; TRF, Toluene Reference Fuel) The equivalence ratio was controlled within 0.6–1.3, and the initial temperatures were set at 298K, 318K, and 338K. Additionally, by employing the mechanism proposed by Ren et al., the simulated values align with the experimental data, thus prompting the conduction of a reaction kinetic analysis. The analysis of chemical reaction kinetics reveals the reaction pathways of DIB, with a notable observation that an increase in temperature or a decrease in equivalence ratio can both lead to an elevation in the degree of unsaturation in the bonds of intermediate species. During laminar flame combustion, PRF and TRF compete with DIB for oxygen, with PRF appearing to have a stronger ability to capture oxygen. In addition, the laminar burning velocity temperature dependence coefficient α decreases first and then increases with the increase of the equivalence ratio, where the minimum α is obtained at equivalence ratio = 1.1. Additionally, the laminar burning velocity at higher initial temperatures is estimated by the extrapolation method and compared with the experimental data reported in literature.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142098659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101804
High entropy oxides (HEOs) show great prospects in catalysis owing to their widely tunable component structures and ease of combination with active metals. However, the development of HEO catalysts is limited by the lack of efficient synthesis methods due to the difficulty of homogeneously mixing at least five elements. In this work, flame spray pyrolysis (FSP) is successfully employed to synthesize (CrMnFeCoNi)3O4 HEO with a single phase spinel structure in one step, which is verified by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), and energy-dispersive X-ray spectroscopy (EDS). Taking CO catalytic oxidation as a probe reaction, the Pt@(CrMnFeCoNi)3O4 HEO catalyst synthesized by FSP in one step is compared with the catalyst whose Pt is impregnated on (CrMnFeCoNi)3O4 HEO support. The FSP-made catalysts have a higher catalytic reaction rate and better redox ability, which lowers the temperature of complete CO conversion by nearly 100 °C. Furthermore, it can be observed that the flame parameters can be optimized to modify the particle size and oxygen vacancies of the HEO nanoparticles, thus enhancing the catalytic performances. This work demonstrates that FSP is an effective method for the one-step synthesis of HEO catalysts with excellent catalytic performance, providing a new perspective for the synthesis of HEO-based materials.
高熵氧化物(HEOs)由于其组分结构可广泛调整,且易于与活性金属结合,因此在催化领域具有广阔的前景。然而,由于很难将至少五种元素均匀混合,缺乏高效的合成方法限制了高熵氧化物催化剂的发展。本研究采用火焰喷射热解(FSP)技术,成功地一步合成了具有单相尖晶石结构的(CrMnFeCoNi)3O4 HEO,并通过 X 射线衍射(XRD)、高分辨率透射电子显微镜(HRTEM)、选区电子衍射(SAED)和能量色散 X 射线光谱(EDS)进行了验证。以一氧化碳催化氧化反应为研究对象,比较了通过 FSP 一步合成的 Pt@(CrMnFeCoNi)3O4 HEO 催化剂和在(CrMnFeCoNi)3O4 HEO 载体上浸渍 Pt 的催化剂。FSP 制成的催化剂具有更高的催化反应速率和更好的氧化还原能力,可将 CO 完全转化的温度降低近 100 °C。此外,还可以通过优化火焰参数来改变 HEO 纳米颗粒的粒度和氧空位,从而提高催化性能。这项工作表明,FSP 是一步合成具有优异催化性能的 HEO 催化剂的有效方法,为 HEO 基材料的合成提供了一个新的视角。
{"title":"One-step synthesis of Pt@(CrMnFeCoNi)3O4 high entropy oxide catalysts through flame spray pyrolysis","authors":"","doi":"10.1016/j.joei.2024.101804","DOIUrl":"10.1016/j.joei.2024.101804","url":null,"abstract":"<div><p>High entropy oxides (HEOs) show great prospects in catalysis owing to their widely tunable component structures and ease of combination with active metals. However, the development of HEO catalysts is limited by the lack of efficient synthesis methods due to the difficulty of homogeneously mixing at least five elements. In this work, flame spray pyrolysis (FSP) is successfully employed to synthesize (CrMnFeCoNi)<sub>3</sub>O<sub>4</sub> HEO with a single phase spinel structure in one step, which is verified by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), and energy-dispersive X-ray spectroscopy (EDS). Taking CO catalytic oxidation as a probe reaction, the Pt@(CrMnFeCoNi)<sub>3</sub>O<sub>4</sub> HEO catalyst synthesized by FSP in one step is compared with the catalyst whose Pt is impregnated on (CrMnFeCoNi)<sub>3</sub>O<sub>4</sub> HEO support. The FSP-made catalysts have a higher catalytic reaction rate and better redox ability, which lowers the temperature of complete CO conversion by nearly 100 °C. Furthermore, it can be observed that the flame parameters can be optimized to modify the particle size and oxygen vacancies of the HEO nanoparticles, thus enhancing the catalytic performances. This work demonstrates that FSP is an effective method for the one-step synthesis of HEO catalysts with excellent catalytic performance, providing a new perspective for the synthesis of HEO-based materials.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142098657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1016/j.joei.2024.101801
Disposable masks, predominantly made of polypropylene melt-blown fabric, present a significant environmental challenge due to their large volume and resistance to natural degradation. This study explores the co-gasification of forestry waste, specifically pine wood, and waste masks to enhance biomass gasification efficiency while enabling the high-value utilization of waste materials. The Fe/Dol catalyst, prepared by loading transition metal Fe onto calcined dolomite using the impregnation method, was tested in a two-stage fixed-bed gasification system. Steam was employed as the gasifying agent. The study systematically examines the effects of steam flow rate, gasification reforming temperature, the mixing ratio of pine wood to masks, and Fe loading on the catalyst's performance in gas-phase and liquid-phase product formation.Characterization analyses revealed that Fe oxides facilitate the cleavage of aromatic rings in aromatic compounds, leading to the formation of two-carbon chain segments and promoting the production of ethylene and propylene from aliphatic hydrocarbons. Additionally, the catalyst enhanced tar cracking, generating free radicals and ring bonds. Experimental results indicate that at a steam flow rate of 3 mg/min, a gasification temperature of 850 °C, a pine wood to mask mixing ratio of 1:2, and an Fe loading of 8 %, the hydrogen (H2) volume fraction reached 52.48 %, with a gas yield of 1.67 m³/kg and a hydrogen production rate of 78.25 g/kg.
{"title":"Mechanistic analysis of hydrogen-rich Co-gasification of pine wood and polypropylene-based waste masks using Fe/Dol catalyst","authors":"","doi":"10.1016/j.joei.2024.101801","DOIUrl":"10.1016/j.joei.2024.101801","url":null,"abstract":"<div><p>Disposable masks, predominantly made of polypropylene melt-blown fabric, present a significant environmental challenge due to their large volume and resistance to natural degradation. This study explores the co-gasification of forestry waste, specifically pine wood, and waste masks to enhance biomass gasification efficiency while enabling the high-value utilization of waste materials. The Fe/Dol catalyst, prepared by loading transition metal Fe onto calcined dolomite using the impregnation method, was tested in a two-stage fixed-bed gasification system. Steam was employed as the gasifying agent. The study systematically examines the effects of steam flow rate, gasification reforming temperature, the mixing ratio of pine wood to masks, and Fe loading on the catalyst's performance in gas-phase and liquid-phase product formation.Characterization analyses revealed that Fe oxides facilitate the cleavage of aromatic rings in aromatic compounds, leading to the formation of two-carbon chain segments and promoting the production of ethylene and propylene from aliphatic hydrocarbons. Additionally, the catalyst enhanced tar cracking, generating free radicals and ring bonds. Experimental results indicate that at a steam flow rate of 3 mg/min, a gasification temperature of 850 °C, a pine wood to mask mixing ratio of 1:2, and an Fe loading of 8 %, the hydrogen (H<sub>2</sub>) volume fraction reached 52.48 %, with a gas yield of 1.67 m³/kg and a hydrogen production rate of 78.25 g/kg.</p></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142098658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}