The oxidative coupling of methane (OCM) involves directly converting methane to C2+ hydrocarbons (such as ethylene and ethane) via a reaction with oxygen. This study elucidated the effect of the calcination temperature on the structure and catalytic performance of potassium-doped-cobalt oxide supported on an alumina (K-Co/Al2O3) catalyst for the OCM reaction. The catalyst was highly active at relatively low reactor temperatures (500–640 °C). Four calcination temperatures (400, 500, 600, and 700 °C) were investigated, with the results showing that the calcination temperature strongly affected catalytic properties, such as the crystalline phases, elemental distribution, physical properties, and catalytic basicity, leading to a wide range in catalytic performances. The catalyst calcined at 400 °C was superior among the catalysts, with 8.3 % C2+ yield, 24.8 % C2+ selectivity, and 33.6 % CH4 conversion at 640 °C. Furthermore, the catalyst was robust over 24 h of testing.
{"title":"Effect of calcination temperature on the performance of K-Co/Al2O3 catalyst for oxidative coupling of methane","authors":"Sarannuch Sringam , Thongthai Witoon , Chularat Wattanakit , Waleeporn Donphai , Metta Chareonpanich , Günther Rupprechter , Anusorn Seubsai","doi":"10.1016/j.crcon.2024.100261","DOIUrl":"10.1016/j.crcon.2024.100261","url":null,"abstract":"<div><div>The oxidative coupling of methane (OCM) involves directly converting methane to C<sub>2+</sub> hydrocarbons (such as ethylene and ethane) via a reaction with oxygen. This study elucidated the effect of the calcination temperature on the structure and catalytic performance of potassium-doped-cobalt oxide supported on an alumina (K-Co/Al<sub>2</sub>O<sub>3</sub>) catalyst for the OCM reaction. The catalyst was highly active at relatively low reactor temperatures (500–640 °C). Four calcination temperatures (400, 500, 600, and 700 °C) were investigated, with the results showing that the calcination temperature strongly affected catalytic properties, such as the crystalline phases, elemental distribution, physical properties, and catalytic basicity, leading to a wide range in catalytic performances. The catalyst calcined at 400 °C was superior among the catalysts, with 8.3 % C<sub>2+</sub> yield, 24.8 % C<sub>2+</sub> selectivity, and 33.6 % CH<sub>4</sub> conversion at 640 °C. Furthermore, the catalyst was robust over 24 h of testing.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 2","pages":"Article 100261"},"PeriodicalIF":6.4,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144070457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-05-09DOI: 10.1016/j.crcon.2024.100250
Zixuan Wang , Yuming Zhang , Yanan Wang , Jiazhou Li , Xicheng Jia , Zhijie Wu
The production of biodiesel generates a significant amount of glycerol by-products. One way to utilize glycerol is converting it into lactic acid, which can then be further transformed into pyruvic acid. In this review, we examine existing reaction pathways and propose a new approach for the indirect synthesis of pyruvic acid using glycerol and lactic acid as intermediates. Noble metals and transition metals are suitable for the oxidation of glycerol and lactic acid, and the combination of different metal sites may exhibit synergy effect and promote the process. It should be noted that the dehydration and isomerization of 1,3-dehydroxyacetone to lactic acid can be catalyzed by Lewis acids, which can be utilized in the base-free system that simplifies the postprocess procedure. Excepting noble metals, synergistic effect between iron and molybdenum also shows promising performance in catalyzed oxidation of lactic acid. Furthermore, many research results also suggest that mass transfer plays a critical role in this cascade reaction, which shed light on the catalysts modification for the similar reactions.
{"title":"Recent progress in glycerol oxidation to lactic acid and pyruvic acid with heterogeneous metal catalysts","authors":"Zixuan Wang , Yuming Zhang , Yanan Wang , Jiazhou Li , Xicheng Jia , Zhijie Wu","doi":"10.1016/j.crcon.2024.100250","DOIUrl":"10.1016/j.crcon.2024.100250","url":null,"abstract":"<div><div>The production of biodiesel generates a significant amount of glycerol by-products. One way to utilize glycerol is converting it into lactic acid, which can then be further transformed into pyruvic acid. In this review, we examine existing reaction pathways and propose a new approach for the indirect synthesis of pyruvic acid using glycerol and lactic acid as intermediates. Noble metals and transition metals are suitable for the oxidation of glycerol and lactic acid, and the combination of different metal sites may exhibit synergy effect and promote the process. It should be noted that the dehydration and isomerization of 1,3-dehydroxyacetone to lactic acid can be catalyzed by Lewis acids, which can be utilized in the base-free system that simplifies the postprocess procedure. Excepting noble metals, synergistic effect between iron and molybdenum also shows promising performance in catalyzed oxidation of lactic acid. Furthermore, many research results also suggest that mass transfer plays a critical role in this cascade reaction, which shed light on the catalysts modification for the similar reactions.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 2","pages":"Article 100250"},"PeriodicalIF":6.4,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141036121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-27DOI: 10.1016/j.crcon.2024.100249
Emad Al-Shafei , Mohammed Albahar , Reem Albashrayi , Mohammad F. Aljishi , Wala Algozeeb , Ahmed Alasseel , Gazali Tanimu , Abdullah Aitani
Ethane, one of the key components of shale gas, is a valuable feedstock for the production of syngas (CO + H2) via the CC bond cleavage during dry reforming of ethane (DRE) reaction. Selective catalysts are needed to direct this reaction pathway against the competing CH bond cleavage for ethylene formation. In this study, Fe, V and Rh oxides supported on TiO2 catalysts were prepared by impregnation method. The catalysts were tested for DRE with the main target of enhancing selectivity to syngas (CO and H2) and reducing byproducts (methane and ethylene) formation. The catalysts were characterized using X-ray diffraction, scanning electron microscopy, NH3/CO2 temperature programmed desorption and H2-temperature programmed reduction. Temperature programmed oxidation was utilized to characterize the coke contents of the spent catalysts. The catalysts were evaluated for DRE reaction in a fixed-bed reactor at the temperature range from 500 °C to 650 °C and CO2/ethane ratio from 2:1 to 10:1 (mol/mol). It was found that ethane conversion over the three catalysts increased in the order Rh/TiO2 > Fe/TiO2 > V/TiO2. Rh/TiO2 catalyst exhibited > 99 % ethane conversion, 36 % and 61 % yields of H2 and CO, respectively, at 650 °C and CO2/ethane ratio of 5.0. The high conversion of ethane was mainly attributed to the enhanced dispersion of Rh oxides on the TiO2 support coupled with the balanced surface acidic and basic sites. The Rh catalyst facilitated CC bond dissociation of ethane thereby forming methyl intermediates which then reacted with adsorbed CO2, thereby enhancing higher syngas production during DRE reaction.
{"title":"Dry reforming of ethane over titania-based catalysts for higher selectivity and conversion to syngas","authors":"Emad Al-Shafei , Mohammed Albahar , Reem Albashrayi , Mohammad F. Aljishi , Wala Algozeeb , Ahmed Alasseel , Gazali Tanimu , Abdullah Aitani","doi":"10.1016/j.crcon.2024.100249","DOIUrl":"10.1016/j.crcon.2024.100249","url":null,"abstract":"<div><div>Ethane, one of the key components of shale gas, is a valuable feedstock for the production of syngas (CO + H<sub>2</sub>) via the C<img>C bond cleavage during dry reforming of ethane (DRE) reaction. Selective catalysts are needed to direct this reaction pathway against the competing C<img>H bond cleavage for ethylene formation. In this study, Fe, V and Rh oxides supported on TiO<sub>2</sub> catalysts were prepared by impregnation method. The catalysts were tested for DRE with the main target of enhancing selectivity to syngas (CO and H<sub>2</sub>) and reducing byproducts (methane and ethylene) formation. The catalysts were characterized using X-ray diffraction, scanning electron microscopy, NH<sub>3</sub>/CO<sub>2</sub> temperature programmed desorption and H<sub>2</sub>-temperature programmed reduction. Temperature programmed oxidation was utilized to characterize the coke contents of the spent catalysts. The catalysts were evaluated for DRE reaction in a fixed-bed reactor at the temperature range from 500 °C to 650 °C and CO<sub>2</sub>/ethane ratio from 2:1 to 10:1 (mol/mol). It was found that ethane conversion over the three catalysts increased in the order Rh/TiO<sub>2</sub> > Fe/TiO<sub>2</sub> > V/TiO<sub>2</sub>. Rh/TiO<sub>2</sub> catalyst exhibited > 99 % ethane conversion, 36 % and 61 % yields of H<sub>2</sub> and CO, respectively, at 650 °C and CO<sub>2</sub>/ethane ratio of 5.0. The high conversion of ethane was mainly attributed to the enhanced dispersion of Rh oxides on the TiO<sub>2</sub> support coupled with the balanced surface acidic and basic sites. The Rh catalyst facilitated C<img>C bond dissociation of ethane thereby forming methyl intermediates which then reacted with adsorbed CO<sub>2</sub>, thereby enhancing higher syngas production during DRE reaction.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 2","pages":"Article 100249"},"PeriodicalIF":6.4,"publicationDate":"2024-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This study assesses a two-stage anaerobic digestion process designed to efficiently recover energy through hydrogen and methane production by co-digesting filter cake (FC), biogas effluent (BE), and anaerobic sludge (AS) from the sugar and ethanol industry. The optimal proportions of FC, BE, and AS were determined in batch fermentation experiments using Design Expert software, which identified a suitable ratio of 31.05:28.95:0.00 (g VS/L), respectively. The results indicated that hydrogen production in the first stage could occur solely through the hydrogenic bacteria present in the BE and FC mixture, without the need for AS as an inoculum. This optimized FC:BE ratio was then applied in a semi-continuous fermentation system, achieving a hydrogen production rate of 193.6 mL H2/L.d and a hydrogen yield of 9.8 mL H2/g VS at an optimal hydraulic retention time (HRT) of 3 d. In the subsequent second stage, the effluent from the hydrogen reactor was used for methane production. This stage achieved a methane production rate of 422.0 mL CH4/L·d and a methane yield of 140.2 mL CH4/g VS, with an HRT of 20 d. Overall, the two-stage process exhibited an impressive energy output, peaking at 5.17 kJ/g VS. This suggests the potential for an annual electricity generation of 194,655 MWh and an estimated reduction of 85,668 tCO2eq/year in greenhouse gas emissions. This study highlights the efficiency of the two-stage anaerobic digestion process for harnessing energy through the co-digestion of FC and BE, without the need for additional AS inoculum. The findings demonstrate the potential for sustainable energy recovery from industrial waste streams while mitigating environmental impacts.
本研究评估了一种两阶段厌氧消化工艺，该工艺旨在通过共消化来自糖和乙醇工业的滤饼（FC）、沼气排出物（BE）和厌氧污泥（AS），有效地通过产生氢气和甲烷来回收能量。采用Design Expert软件进行分批发酵实验，确定了FC、BE和AS的最佳配比，确定的最佳配比分别为31.05:28.95:0.00 （g VS/L）。结果表明，第一阶段的产氢可以完全通过BE和FC混合物中存在的产氢细菌进行，而不需要AS作为接种物。然后将优化后的FC:BE比例应用于半连续发酵系统，产氢率为193.6 mL H2/L。d，在最佳水力停留时间（HRT）为3 d的情况下，产氢量为9.8 mL H2/g VS。在随后的第二阶段，氢气反应器的出水用于甲烷生产。这一阶段的甲烷产率为422.0 mL CH4/L·d，甲烷产率为140.2 mL CH4/g VS， HRT为20 d。总的来说，这两阶段的过程表现出了令人印象深刻的能量输出，峰值为5.17 kJ/g VS.这表明年发电量可能达到194,655兆瓦时，温室气体排放量估计减少85,668吨二氧化碳当量/年。这项研究强调了两阶段厌氧消化过程的效率，通过FC和BE的共同消化来利用能量，而不需要额外的AS接种。研究结果表明，在减轻环境影响的同时，从工业废物流中可持续回收能源的潜力。
{"title":"Co-digestion of filter cake, biogas effluent, and anaerobic sludge for hydrogen and methane production: Optimizing energy recovery through two-stage anaerobic digestion","authors":"Worapong Wongarmat , Sureewan Sittijunda , Tsuyoshi Imai , Alissara Reungsang","doi":"10.1016/j.crcon.2024.100248","DOIUrl":"10.1016/j.crcon.2024.100248","url":null,"abstract":"<div><div>This study assesses a two-stage anaerobic digestion process designed to efficiently recover energy through hydrogen and methane production by co-digesting filter cake (FC), biogas effluent (BE), and anaerobic sludge (AS) from the sugar and ethanol industry. The optimal proportions of FC, BE, and AS were determined in batch fermentation experiments using Design Expert software, which identified a suitable ratio of 31.05:28.95:0.00 (g VS/L), respectively. The results indicated that hydrogen production in the first stage could occur solely through the hydrogenic bacteria present in the BE and FC mixture, without the need for AS as an inoculum. This optimized FC:BE ratio was then applied in a semi-continuous fermentation system, achieving a hydrogen production rate of 193.6 mL H<sub>2</sub>/L.d and a hydrogen yield of 9.8 mL H<sub>2</sub>/g VS at an optimal hydraulic retention time (HRT) of 3 d. In the subsequent second stage, the effluent from the hydrogen reactor was used for methane production. This stage achieved a methane production rate of 422.0 mL CH<sub>4</sub>/L·d and a methane yield of 140.2 mL CH<sub>4</sub>/g VS, with an HRT of 20 d. Overall, the two-stage process exhibited an impressive energy output, peaking at 5.17 kJ/g VS. This suggests the potential for an annual electricity generation of 194,655 MWh and an estimated reduction of 85,668 tCO<sub>2</sub>eq/year in greenhouse gas emissions. This study highlights the efficiency of the two-stage anaerobic digestion process for harnessing energy through the co-digestion of FC and BE, without the need for additional AS inoculum. The findings demonstrate the potential for sustainable energy recovery from industrial waste streams while mitigating environmental impacts.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 2","pages":"Article 100248"},"PeriodicalIF":6.4,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140756574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
By introducing oxalic acid, succinic acid, and tartaric acid into the synthesis process of Mo-V-O composite metal oxides, the structure directing effect of polybasic organic acids on the crystal structure of Mo-V-O compositee metal oxide was studied. Moreover, the prepared Mo-V-O samples with different crystal phase compositions were used to the conversion of glycerol, and the effect of crystal phase structure on its catalytic performance was investigated. Results show that the crystal phase structure of Mo-V-O can be regulated by changing the type and additive amount of polybasic organic acids. The crystal phase of Mo-V-O changed from MoV2O8 to Mo0.97V0.95O5 with the increase of succinic acid and tartaric acid. The change in the Mo-V-O crystal phase is related to the amount of organic acid and the carbon chain length. When the crystal phase is MoV2O8, the selectivity of acrolein and acetone is 25.7 % and 16.2 %. According to the XPS results, Mo6+ in MoV2O8 promoted the formation of acrolein, while Mo5+ in Mo0.97V0.95O5 promoted the formation of acetone. So when the crystal phase is Mo0.97V0.95O5, the selectivity of acrolein and acetone is 11.9 % and 24.6 %. Therefore, the results of catalyzing glycerol can be controlled by selecting different crystal phases.
{"title":"Polybasic organic acids controlled synthesis of Mo-V-O composite metal oxide for the catalytic conversion of glycerol","authors":"Siqi Zhang, Shuangming Li, Tianyue Su, Xiaojun Yu, Jingyi Ai, Yuanzhi Li, Sansan Yu","doi":"10.1016/j.crcon.2024.100247","DOIUrl":"10.1016/j.crcon.2024.100247","url":null,"abstract":"<div><div>By introducing oxalic acid, succinic acid, and tartaric acid into the synthesis process of Mo-V-O composite metal oxides, the structure directing effect of polybasic organic acids on the crystal structure of Mo-V-O compositee metal oxide was studied. Moreover, the prepared Mo-V-O samples with different crystal phase compositions were used to the conversion of glycerol, and the effect of crystal phase structure on its catalytic performance was investigated. Results show that the crystal phase structure of Mo-V-O can be regulated by changing the type and additive amount of polybasic organic acids. The crystal phase of Mo-V-O changed from MoV<sub>2</sub>O<sub>8</sub> to Mo<sub>0.97</sub>V<sub>0.95</sub>O<sub>5</sub> with the increase of succinic acid and tartaric acid. The change in the Mo-V-O crystal phase is related to the amount of organic acid and the carbon chain length. When the crystal phase is MoV<sub>2</sub>O<sub>8</sub>, the selectivity of acrolein and acetone is 25.7 % and 16.2 %. According to the XPS results, Mo<sup>6+</sup> in MoV<sub>2</sub>O<sub>8</sub> promoted the formation of acrolein, while Mo<sup>5+</sup> in Mo<sub>0.97</sub>V<sub>0.95</sub>O<sub>5</sub> promoted the formation of acetone. So when the crystal phase is Mo<sub>0.97</sub>V<sub>0.95</sub>O<sub>5</sub>, the selectivity of acrolein and acetone is 11.9 % and 24.6 %. Therefore, the results of catalyzing glycerol can be controlled by selecting different crystal phases.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 2","pages":"Article 100247"},"PeriodicalIF":6.4,"publicationDate":"2024-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140776848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-15DOI: 10.1016/j.crcon.2024.100246
A series of related experiments were carried out based on prepared hydrocracking catalyst, Catalyst-HC. Ni & W and USY molecular sieve were selected as the hydrogenation active component and the cracking component of Catalyst-HC, respectively. Meanwhile, a kinetic model for paraffin conversion was constructed based on paraffin conversion law. Results obtained through this work indicate that the impact of H2-pressure is relatively complex. As the H2-pressure changes, the degree of hydrocracking reaction may be influenced by both hydrogen supply capacity and hydrogen proton concentration. Obtained conversion priority for three types of hydrocarbons on USY molecular sieve is as follows, aromatic ≫ cycloalkane > paraffin. Aromatic content in SRGO can affect its paraffin-retention in Hydro-D. Compared with the hydrotreating of SRGO with low aromatic content, when SRGO with relatively higher aromatic content is hydrotreated, its paraffin-retention is higher and its paraffin loss is also relatively smaller. Base on constructed model, the calculated values of SRGO-BJ conversion rate and paraffin-retention in Hydro-D are within ±10 % and ±5 % error lines, respectively. Thus, model schematic diagram is reasonable and can provide modeling reference for relevant model research.
{"title":"Hydrocarbon-conversion reaction and new paraffin-kinetic model during straight-run gas oil (SRGO) hydrotreating","authors":"","doi":"10.1016/j.crcon.2024.100246","DOIUrl":"10.1016/j.crcon.2024.100246","url":null,"abstract":"<div><p>A series of related experiments were carried out based on prepared hydrocracking catalyst, Catalyst-HC. Ni & W and USY molecular sieve were selected as the hydrogenation active component and the cracking component of Catalyst-HC, respectively. Meanwhile, a kinetic model for paraffin conversion was constructed based on paraffin conversion law. Results obtained through this work indicate that the impact of H<sub>2</sub>-pressure is relatively complex. As the H<sub>2</sub>-pressure changes, the degree of hydrocracking reaction may be influenced by both hydrogen supply capacity and hydrogen proton concentration. Obtained conversion priority for three types of hydrocarbons on USY molecular sieve is as follows, aromatic ≫ cycloalkane > paraffin. Aromatic content in SRGO can affect its paraffin-retention in Hydro-D. Compared with the hydrotreating of SRGO with low aromatic content, when SRGO with relatively higher aromatic content is hydrotreated, its paraffin-retention is higher and its paraffin loss is also relatively smaller. Base on constructed model, the calculated values of SRGO-BJ conversion rate and paraffin-retention in Hydro-D are within ±10 % and ±5 % error lines, respectively. Thus, model schematic diagram is reasonable and can provide modeling reference for relevant model research.</p></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"7 4","pages":"Article 100246"},"PeriodicalIF":6.4,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2588913324000358/pdfft?md5=18ae1e0eb12d60856eee0981d34f5268&pid=1-s2.0-S2588913324000358-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140780029","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-14DOI: 10.1016/j.crcon.2024.100239
Dewi Sartika , Denny Widhiyanuriyawan , Agung Sugeng Widodo , Purnami , I.N.G Wardana
Fe3O4 is an internal magnet that can work as a medium for the electrolyte solution in electrochemical hydrogen production to facilitate electron movement. When Fe3O4 is combined with activated carbon made from banana leaves (ACBL), electron transfer occurs between the ACBL aromatic ring and Fe3+ ions from solved Fe3O4, which increases the solution’s conductivity and finally produces more hydrogen. ACBL is a biomass catalyst used as a free parameter to increase the Fe3O4 magnetic field in the solution. The Fe3O4 was synthesized using the coprecipitation method, while ACBL was obtained through an activation process to produce graphene oxide. Graphene oxide in ACBL was characterized using Scanning Electron Microscopy (SEM) EDX, Fourier Transform Infra-Red (FTIR), Brunauer, Emmett, and Teller (BET), and TEM (Transmission Electron Microscopy). BET was used to determine the surface area of ACBL. Hydrogen was produced using the electrolysis method. The SEM results showed that the elemental content of graphene oxide in ACBL was 72.47 %. The graphene oxide in ACBL had a positive charge represented by a bright color on the sample surface. The positive charge was due to the FTIR O-H and C-O groups working with Fe3O4. BET analysis showed that the average pore diameter of ACBL was 1.68 nm. The largest hydrogen production results were obtained at ACBL 200 mesh, which was 15.5 ml. ACBL from abundant biomass has magnetic and electrical potential within its aromatic ring. As the aromatic ring interacts with the magnetic field of Fe3O4, the electromagnetic field of the solution is strengthened. As a result, hydrogen production increases.
{"title":"The role of graphene Oxide’s aromatic rings in activated carbon made from banana leaves (ACBL) and Fe3O4 in hydrogen production","authors":"Dewi Sartika , Denny Widhiyanuriyawan , Agung Sugeng Widodo , Purnami , I.N.G Wardana","doi":"10.1016/j.crcon.2024.100239","DOIUrl":"10.1016/j.crcon.2024.100239","url":null,"abstract":"<div><div>Fe<sub>3</sub>O<sub>4</sub> is an internal magnet that can work as a medium for the electrolyte solution in electrochemical hydrogen production to facilitate electron movement. When Fe<sub>3</sub>O<sub>4</sub> is combined with activated carbon made from banana leaves (ACBL), electron transfer occurs between the ACBL aromatic ring and Fe<sup>3+</sup> ions from solved Fe<sub>3</sub>O<sub>4</sub>, which increases the solution’s conductivity and finally produces more hydrogen. ACBL is a biomass catalyst used as a free parameter to increase the Fe<sub>3</sub>O<sub>4</sub> magnetic field in the solution. The Fe<sub>3</sub>O<sub>4</sub> was synthesized using the coprecipitation method, while ACBL was obtained through an activation process to produce graphene oxide. Graphene oxide in ACBL was characterized using Scanning Electron Microscopy (SEM) EDX, Fourier Transform Infra-Red (FTIR), Brunauer, Emmett, and Teller (BET), and TEM (Transmission Electron Microscopy). BET was used to determine the surface area of ACBL. Hydrogen was produced using the electrolysis method. The SEM results showed that the elemental content of graphene oxide in ACBL was 72.47 %. The graphene oxide in ACBL had a positive charge represented by a bright color on the sample surface. The positive charge was due to the FTIR O-H and C-O groups working with Fe<sub>3</sub>O<sub>4</sub>. BET analysis showed that the average pore diameter of ACBL was 1.68 nm. The largest hydrogen production results were obtained at ACBL 200 mesh, which was 15.5 ml. ACBL from abundant biomass has magnetic and electrical potential within its aromatic ring. As the aromatic ring interacts with the magnetic field of Fe<sub>3</sub>O<sub>4</sub>, the electromagnetic field of the solution is strengthened. As a result, hydrogen production increases.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 1","pages":"Article 100239"},"PeriodicalIF":6.4,"publicationDate":"2024-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140759698","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-04-13DOI: 10.1016/j.crcon.2024.100242
Dimitris Karayannis , Nikos Angelou , Gabriel Vasilakis , Ioannis Charisteidis , Alexandros Litinas , Seraphim Papanikolaou
The production and recovery of 2,3-butanediol (BDO) through biodiesel derived glycerol valorization by Klebsiella oxytoca ACA-DC 1581 was holistically optimized with regard to the efficiency and cost of the bioprocess. The absence of thermal treatment of the substrate had no negative effect upon the growth of microorganism and the bioconversion of crude glycerol into BDO, enabling the development of a non-aseptic and lower-cost bioprocess. Both digestate and corn steep liquor (CSL), the main by-products of the biogas and corn industries respectively, successfully served as the sole source of nitrogen, contributing to the complete replacement of more expensive sources (e.g., yeast extract). The biochemical pathway of glycerol catabolism was examined under varying concentrations of dissolved oxygen and BDO production was optimized in a fully aerobic environment (volumetric mass transfer coefficient; kLa = 70.5 1/h.) The glycerol consumption rate was 2.80 g/L/h, the BDO productivity reached 1.12 g/L/h and the yield of BDO produced per unit of glycerol consumed was 0.46 g/g, with these values being among the highest ones reported in the literature for wild-type strains cultivated on crude glycerol. In all fed-batch fermentations, final BDO and acetoin concentration reached ∼80 g/L, while a plateau was observed at ∼68 g/L of BDO. Finally, the culture was carried out efficiently in the pilot-scale reactor (250 L). The salting-out extraction (SOE), consisting of ethanol (24 %) and K2HPO4 (25 %), recovered 91.7 % of BDO from the fermentation medium and was studied for the first time in a glycerol-based medium. The study suggests the potential industrialization of the bioprocess through sustainable, pilot-scale and low-cost bioconversion of biodiesel-derived crude glycerol and CSL or digestate into BDO.
{"title":"A non-aseptic bioprocess for production and recovery of 2,3-butanediol via conversion of crude glycerol and corn steep liquor at pilot-scale","authors":"Dimitris Karayannis , Nikos Angelou , Gabriel Vasilakis , Ioannis Charisteidis , Alexandros Litinas , Seraphim Papanikolaou","doi":"10.1016/j.crcon.2024.100242","DOIUrl":"10.1016/j.crcon.2024.100242","url":null,"abstract":"<div><div>The production and recovery of 2,3-butanediol (BDO) through biodiesel derived glycerol valorization by <em>Klebsiella oxytoca</em> ACA-DC 1581 was holistically optimized with regard to the efficiency and cost of the bioprocess. The absence of thermal treatment of the substrate had no negative effect upon the growth of microorganism and the bioconversion of crude glycerol into BDO, enabling the development of a non-aseptic and lower-cost bioprocess. Both digestate and corn steep liquor (CSL), the main by-products of the biogas and corn industries respectively, successfully served as the sole source of nitrogen, contributing to the complete replacement of more expensive sources (e.g., yeast extract). The biochemical pathway of glycerol catabolism was examined under varying concentrations of dissolved oxygen and BDO production was optimized in a fully aerobic environment (volumetric mass transfer coefficient; k<sub>L</sub>a = 70.5 1/h.) The glycerol consumption rate was 2.80 g/L/h, the BDO productivity reached 1.12 g/L/h and the yield of BDO produced per unit of glycerol consumed was 0.46 g/g, with these values being among the highest ones reported in the literature for wild-type strains cultivated on crude glycerol. In all fed-batch fermentations, final BDO and acetoin concentration reached ∼80 g/L, while a plateau was observed at ∼68 g/L of BDO. Finally, the culture was carried out efficiently in the pilot-scale reactor (250 L). The salting-out extraction (SOE), consisting of ethanol (24 %) and K<sub>2</sub>HPO<sub>4</sub> (25 %), recovered 91.7 % of BDO from the fermentation medium and was studied for the first time in a glycerol-based medium. The study suggests the potential industrialization of the bioprocess through sustainable, pilot-scale and low-cost bioconversion of biodiesel-derived crude glycerol and CSL or digestate into BDO.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 1","pages":"Article 100242"},"PeriodicalIF":6.4,"publicationDate":"2024-04-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140792551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The concentration of the major greenhouse gas CO2 is rapidly increasing in the atmosphere, leading to global warming and a range of environmental issues. An efficient circulation and utilization of CO2 is critical in the current environmental context. Methanation, an exothermic process, emerges as a critical strategy for effective CO2 utilization. On this front, there is a significant demand for rational design of catalysts that maintain high activity and methane selectivity over a wide temperature range (250–550 °C). The catalyst that can promise a consistent reaction even at 500 °C under an atmospheric pressure is thus obliged. The present study investigated bimetallic catalysts with SiC, which is known for its exceptional thermal conductivity, and CeO2, which is characterized by its CO₂ affinity, as base materials. We incorporated Ni-M and Ru-M (M = Co and Mn) as the active metals, each loaded at 2 %. Impressively, with merely 20 mg, the Ni-Co/SiC catalyst achieved a CO2 conversion rate of 77 % and CH₄ selectivity of 88 % at 500 °C, in a fixed-bed tubular reactor system with conditions of H2/CO2 = 4, a total flow rate of 70 ml min−1, and a steady GHSV of 12,000 h−1. Moreover, 2Ni-2Co/CeO2 catalyst demonstrated exceptional performance with a 76 % conversion of CO2 and a 83 % selectivity for CH4, all under identical conditions. The catalyst's durability was confirmed by a subsequent 40-hour stability test, which showed only a 3–5 % degradation. The developed catalysts were comprehensively characterized by BET/BJH, CO pulse chemisorption, H2-TPR, HAADF-STEM-EDS, SEM-EDS and XRD etc. to unveil their physicochemical and surface traits. It was found that Co and Mn, when integrated, effectively restrained the agglomeration of Ni and Ru particles, ensuring optimal metal dispersion on the support. In conclusion, our synthesized bimetallic catalysts shown a sustained catalytic capability, even in the high-temperature environment.
大气中主要温室气体二氧化碳的浓度正在迅速增加，导致全球变暖和一系列环境问题。在当前的环境背景下，二氧化碳的有效循环和利用是至关重要的。甲烷化是一种放热过程，是有效利用二氧化碳的关键策略。在这方面，迫切需要合理设计催化剂，在较宽的温度范围（250-550°C）内保持高活性和甲烷选择性。因此，即使在500°C的大气压力下也能保证持续反应的催化剂是必要的。本研究研究了以具有优异导热性的SiC和以CO 2亲和力为特征的CeO2为基础材料的双金属催化剂。我们加入Ni-M和Ru-M （M = Co和Mn）作为活性金属，各加载2%。令人印象深刻的是，在固定床管式反应器系统中，在H2/CO2 = 4，总流量为70 ml min - 1，稳定GHSV为12,000 h - 1的条件下，仅20 mg的Ni-Co/SiC催化剂在500°C下实现了77%的CO2转化率和88%的CH 4选择性。此外，在相同的条件下，2Ni-2Co/CeO2催化剂表现出优异的性能，CO2转化率为76%，CH4选择性为83%。催化剂的耐久性在随后的40小时稳定性测试中得到了证实，测试结果显示，催化剂的降解率仅为3 - 5%。采用BET/BJH、CO脉冲化学吸附、H2-TPR、HAADF-STEM-EDS、SEM-EDS、XRD等手段对所制备的催化剂进行了综合表征，揭示了催化剂的理化和表面特性。结果表明，Co和Mn相结合可有效抑制Ni和Ru颗粒的团聚，确保金属在载体上的最佳分散。综上所述，我们合成的双金属催化剂即使在高温环境下也表现出持续的催化能力。
{"title":"CO2 methanation over low-loaded Ni-M, Ru-M (M = Co, Mn) catalysts supported on CeO2 and SiC","authors":"Chopendra G. Wasnik, Maki Nakamura, Taiki Shimada, Hiroshi Machida, Koyo Norinaga","doi":"10.1016/j.crcon.2024.100241","DOIUrl":"10.1016/j.crcon.2024.100241","url":null,"abstract":"<div><div>The concentration of the major greenhouse gas CO<sub>2</sub> is rapidly increasing in the atmosphere, leading to global warming and a range of environmental issues. An efficient circulation and utilization of CO<sub>2</sub> is critical in the current environmental context. Methanation, an exothermic process, emerges as a critical strategy for effective CO<sub>2</sub> utilization. On this front, there is a significant demand for rational design of catalysts that maintain high activity and methane selectivity over a wide temperature range (250–550 °C). The catalyst that can promise a consistent reaction even at 500 °C under an atmospheric pressure is thus obliged. The present study investigated bimetallic catalysts with SiC, which is known for its exceptional thermal conductivity, and CeO<sub>2</sub>, which is characterized by its CO₂ affinity, as base materials. We incorporated Ni-M and Ru-M (M = Co and Mn) as the active metals, each loaded at 2 %. Impressively, with merely 20 mg, the Ni-Co/SiC catalyst achieved a CO<sub>2</sub> conversion rate of 77 % and CH₄ selectivity of 88 % at 500 °C, in a fixed-bed tubular reactor system with conditions of H<sub>2</sub>/CO<sub>2</sub> = 4, a total flow rate of 70 ml min<sup>−1</sup>, and a steady GHSV of 12,000 h<sup>−1</sup>. Moreover, 2Ni-2Co/CeO<sub>2</sub> catalyst demonstrated exceptional performance with a 76 % conversion of CO<sub>2</sub> and a 83 % selectivity for CH<sub>4</sub>, all under identical conditions. The catalyst's durability was confirmed by a subsequent 40-hour stability test, which showed only a 3–5 % degradation. The developed catalysts were comprehensively characterized by BET/BJH, CO pulse chemisorption, H<sub>2</sub>-TPR, HAADF-STEM-EDS, SEM-EDS and XRD etc. to unveil their physicochemical and surface traits. It was found that Co and Mn, when integrated, effectively restrained the agglomeration of Ni and Ru particles, ensuring optimal metal dispersion on the support. In conclusion, our synthesized bimetallic catalysts shown a sustained catalytic capability, even in the high-temperature environment.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 1","pages":"Article 100241"},"PeriodicalIF":6.4,"publicationDate":"2024-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140758443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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