K. Steinhäuser, Arnim von Gleich, Markus Große Ophoff, W. Körner
Sustainable chemicals and materials management deals with both the risks and the opportunities of chemicals and products. It is not only focused on hazards and risks of chemicals for human health and the environment but also includes the management of material flows from extraction of raw materials up to waste. It becomes apparent meanwhile that the ever-growing material streams endanger the Earth system. According to a recent publication of Persson et al., the planetary boundaries for chemicals and plastics have already been exceeded. Therefore, sustainable chemicals and materials management must become a third pillar of international sustainability policy. For climate change and biodiversity, binding international agreements already exist. Accordingly, a global chemicals and materials framework convention integrating the current fragmented and non-binding approaches is needed. The impacts of chemicals and materials are closely related to climate change. About one third of greenhouse gas (GHG) emissions are linked to the production of chemicals, materials and products and the growing global transport of goods. Most of it is assigned to the energy demand of production and transport. GHG emissions must be reduced by an expansion of the circular economy, i.e., the use of secondary instead of primary raw materials. The chemical industry is obliged to change its feedstock since chemicals based on mineral oil and natural gas are not sustainable. Climate change in turn has consequences for the fate and effects of substances in the environment. Rising temperature implies higher vapor pressure and may enhance the release of toxicants into the atmosphere. Organisms that are already stressed may react more sensitively when exposed to toxic chemicals. The increasing frequency of extreme weather events may re-mobilize contaminants in river sediments. Increasing chemical and material load also threatens biodiversity, e.g., by the release of toxic chemicals into air, water and soil up to high amounts of waste. Fertilizers and pesticides are damaging the biocoenoses in agrarian landscapes. In order to overcome these fatal developments, sustainable management of chemicals and materials is urgently needed. This includes safe and sustainable chemicals, sustainable chemical production and sustainable materials flow management. All these three sustainability strategies are crucial and complement each other: efficiency, consistency and sufficiency. This obligates drastic changes not only of the quantities of material streams but also of the qualities of chemicals and materials in use. A significant reduction in production volumes is necessary, aiming not only to return to a safe operating space with respect to the planetary boundary for chemicals, plastics and waste but also in order to achieve goals regarding climate and biodiversity.
{"title":"The Necessity of a Global Binding Framework for Sustainable Management of Chemicals and Materials—Interactions with Climate and Biodiversity","authors":"K. Steinhäuser, Arnim von Gleich, Markus Große Ophoff, W. Körner","doi":"10.3390/suschem3020014","DOIUrl":"https://doi.org/10.3390/suschem3020014","url":null,"abstract":"Sustainable chemicals and materials management deals with both the risks and the opportunities of chemicals and products. It is not only focused on hazards and risks of chemicals for human health and the environment but also includes the management of material flows from extraction of raw materials up to waste. It becomes apparent meanwhile that the ever-growing material streams endanger the Earth system. According to a recent publication of Persson et al., the planetary boundaries for chemicals and plastics have already been exceeded. Therefore, sustainable chemicals and materials management must become a third pillar of international sustainability policy. For climate change and biodiversity, binding international agreements already exist. Accordingly, a global chemicals and materials framework convention integrating the current fragmented and non-binding approaches is needed. The impacts of chemicals and materials are closely related to climate change. About one third of greenhouse gas (GHG) emissions are linked to the production of chemicals, materials and products and the growing global transport of goods. Most of it is assigned to the energy demand of production and transport. GHG emissions must be reduced by an expansion of the circular economy, i.e., the use of secondary instead of primary raw materials. The chemical industry is obliged to change its feedstock since chemicals based on mineral oil and natural gas are not sustainable. Climate change in turn has consequences for the fate and effects of substances in the environment. Rising temperature implies higher vapor pressure and may enhance the release of toxicants into the atmosphere. Organisms that are already stressed may react more sensitively when exposed to toxic chemicals. The increasing frequency of extreme weather events may re-mobilize contaminants in river sediments. Increasing chemical and material load also threatens biodiversity, e.g., by the release of toxic chemicals into air, water and soil up to high amounts of waste. Fertilizers and pesticides are damaging the biocoenoses in agrarian landscapes. In order to overcome these fatal developments, sustainable management of chemicals and materials is urgently needed. This includes safe and sustainable chemicals, sustainable chemical production and sustainable materials flow management. All these three sustainability strategies are crucial and complement each other: efficiency, consistency and sufficiency. This obligates drastic changes not only of the quantities of material streams but also of the qualities of chemicals and materials in use. A significant reduction in production volumes is necessary, aiming not only to return to a safe operating space with respect to the planetary boundary for chemicals, plastics and waste but also in order to achieve goals regarding climate and biodiversity.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89046403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
H. Rathnayake, Sheeba Dawood, G. Pathiraja, Kelvin Adrah, Olubunmi O. Ayodele
Bioinspired porous microstructures of iron-tannate (Fe(III)-TA) coordination polymer framework were synthesized by catenating natural tannic acid with iron(II), using a scalable aqueous synthesis method in ambient conditions. The chemical composition, morphology, physiochemical properties, and colloidal stability of microstructures were elucidated. The surface area (SBET) and the desorption pore volume were measured to be 70.47 m2/g and 0. 44 cm3/g, respectively, and the porous structure was confirmed with an average pore dimension of ~27 nm. Microstructures were thermally stable up to 180 °C, with an initial weight loss of 13.7% at 180 °C. They exhibited high chemical stability with pH-responsive amphoteric properties in aqueous media at pH levels ranging from 2 to 12. Supporting their amphoteric sorption, microstructures exhibited rapid removal of Pb+2 from water, with 99% removal efficiency, yielding a maximum sorption capacity of 166.66 mg/g. Amphoteric microstructures of bioinspired metal–phenolate coordination polymers remain largely unexplored. Additionally, natural polyphenols have seldomly been used as polytopic linkers to construct both porous and pH-responsive amphoteric coordination polymer frameworks with a robust structure in both acidic and basic media. Thus, this de novo porous microstructure of Fe(III)-TA and its physiochemical surface properties have opened new avenues to design thermally and chemically stable, eco-friendly, low-cost amphoteric sorbents with multifunctionality for adsorption, ion exchange, separation, storage, and sensing of both anions and cations present in heterogeneous media.
{"title":"Green Synthesis of De Novo Bioinspired Porous Iron-Tannate Microstructures with Amphoteric Surface Properties","authors":"H. Rathnayake, Sheeba Dawood, G. Pathiraja, Kelvin Adrah, Olubunmi O. Ayodele","doi":"10.3390/suschem3020013","DOIUrl":"https://doi.org/10.3390/suschem3020013","url":null,"abstract":"Bioinspired porous microstructures of iron-tannate (Fe(III)-TA) coordination polymer framework were synthesized by catenating natural tannic acid with iron(II), using a scalable aqueous synthesis method in ambient conditions. The chemical composition, morphology, physiochemical properties, and colloidal stability of microstructures were elucidated. The surface area (SBET) and the desorption pore volume were measured to be 70.47 m2/g and 0. 44 cm3/g, respectively, and the porous structure was confirmed with an average pore dimension of ~27 nm. Microstructures were thermally stable up to 180 °C, with an initial weight loss of 13.7% at 180 °C. They exhibited high chemical stability with pH-responsive amphoteric properties in aqueous media at pH levels ranging from 2 to 12. Supporting their amphoteric sorption, microstructures exhibited rapid removal of Pb+2 from water, with 99% removal efficiency, yielding a maximum sorption capacity of 166.66 mg/g. Amphoteric microstructures of bioinspired metal–phenolate coordination polymers remain largely unexplored. Additionally, natural polyphenols have seldomly been used as polytopic linkers to construct both porous and pH-responsive amphoteric coordination polymer frameworks with a robust structure in both acidic and basic media. Thus, this de novo porous microstructure of Fe(III)-TA and its physiochemical surface properties have opened new avenues to design thermally and chemically stable, eco-friendly, low-cost amphoteric sorbents with multifunctionality for adsorption, ion exchange, separation, storage, and sensing of both anions and cations present in heterogeneous media.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"84619171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this work, the photocatalytic activity of Hydrated Niobium Pentoxide (synthesized by a simple and inexpensive method) was explored in two unknown reactions reported for this catalyst: the photodegradation of phenol in seawater and the photoreforming of methanol. The Hydrated Niobium Pentoxide (Nb1) was synthesized from the reaction of niobium ammoniacal oxalate NH4[NbO(C2O4)2·H2O]•XH2O with a strong base (NaOH). Further treatment of this catalyst with H2O2 led to a light-sensitive Hydrated Niobium Pentoxide (Nb2). The photocatalysts were characterized by XRD, DRS, SEM Microscopy, FTIR-ATR, EDX, and specific surface area (SBET). The characterization results demonstrate that the treatment of Hydrated Niobium Pentoxide sensitized the material, increased the surface area of the material, diminished the average particle size, and modified its surface charge, and formed peroxo groups on the catalytic surface. Although both photocatalysts (Nb1 and Nb2) were active for both proposed reactions, the sensitization of the photocatalyst was beneficial in distinct situations. In the photocatalytic degradation of phenol in seawater, the sensitization of the photocatalyst did not enhance the photocatalytic activity. In both photoreactions studied, the addition of the Pt° promoter readily increased the photocatalytic performance of both photocatalysts; in this case, the sensitized photocatalyst recorded the best results. The presence of OH• radicals was confirmed, and the great contribution of the Pt° promoter was in the increase in OH• radical generation; this increase was more effective in the sensitized photocatalyst. Our work demonstrated a simple and inexpensive way to synthesize niobium photocatalysts that can effectively be used in the photodegradation of phenol in seawater and in the photoreforming of methanol to produce hydrogen.
{"title":"Photodegradation of Organic Pollutants in Seawater and Hydrogen Production via Methanol Photoreforming with Hydrated Niobium Pentoxide Catalysts","authors":"Y. J. Asencios, V. Machado","doi":"10.3390/suschem3020012","DOIUrl":"https://doi.org/10.3390/suschem3020012","url":null,"abstract":"In this work, the photocatalytic activity of Hydrated Niobium Pentoxide (synthesized by a simple and inexpensive method) was explored in two unknown reactions reported for this catalyst: the photodegradation of phenol in seawater and the photoreforming of methanol. The Hydrated Niobium Pentoxide (Nb1) was synthesized from the reaction of niobium ammoniacal oxalate NH4[NbO(C2O4)2·H2O]•XH2O with a strong base (NaOH). Further treatment of this catalyst with H2O2 led to a light-sensitive Hydrated Niobium Pentoxide (Nb2). The photocatalysts were characterized by XRD, DRS, SEM Microscopy, FTIR-ATR, EDX, and specific surface area (SBET). The characterization results demonstrate that the treatment of Hydrated Niobium Pentoxide sensitized the material, increased the surface area of the material, diminished the average particle size, and modified its surface charge, and formed peroxo groups on the catalytic surface. Although both photocatalysts (Nb1 and Nb2) were active for both proposed reactions, the sensitization of the photocatalyst was beneficial in distinct situations. In the photocatalytic degradation of phenol in seawater, the sensitization of the photocatalyst did not enhance the photocatalytic activity. In both photoreactions studied, the addition of the Pt° promoter readily increased the photocatalytic performance of both photocatalysts; in this case, the sensitized photocatalyst recorded the best results. The presence of OH• radicals was confirmed, and the great contribution of the Pt° promoter was in the increase in OH• radical generation; this increase was more effective in the sensitized photocatalyst. Our work demonstrated a simple and inexpensive way to synthesize niobium photocatalysts that can effectively be used in the photodegradation of phenol in seawater and in the photoreforming of methanol to produce hydrogen.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78179282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Synthetic ammonia, manufactured by the Haber–Bosch process and its variants, is the key to securing global food security. Hydrogen is the most important feedstock for all synthetic ammonia processes. Renewable ammonia production relies on hydrogen generated by water electrolysis using electricity generated from hydropower. This was used commercially as early as 1921. In the present work, we discuss how renewable ammonia production subsequently emerged in those countries endowed with abundant hydropower, and in particular in regions with limited or no oil, gas, and coal deposits. Thus, renewable ammonia played an important role in national food security for countries without fossil fuel resources until after the mid-20th century. For economic reasons, renewable ammonia production declined from the 1960s onward in favor of fossil-based ammonia production. However, renewable ammonia has recently gained traction again as an energy vector. It is an important component of the rapidly emerging hydrogen economy. Renewable ammonia will probably play a significant role in maintaining national and global energy and food security during the 21st century.
{"title":"1921–2021: A Century of Renewable Ammonia Synthesis","authors":"Kevin H. R. Rouwenhorst, A. Travis, L. Lefferts","doi":"10.3390/suschem3020011","DOIUrl":"https://doi.org/10.3390/suschem3020011","url":null,"abstract":"Synthetic ammonia, manufactured by the Haber–Bosch process and its variants, is the key to securing global food security. Hydrogen is the most important feedstock for all synthetic ammonia processes. Renewable ammonia production relies on hydrogen generated by water electrolysis using electricity generated from hydropower. This was used commercially as early as 1921. In the present work, we discuss how renewable ammonia production subsequently emerged in those countries endowed with abundant hydropower, and in particular in regions with limited or no oil, gas, and coal deposits. Thus, renewable ammonia played an important role in national food security for countries without fossil fuel resources until after the mid-20th century. For economic reasons, renewable ammonia production declined from the 1960s onward in favor of fossil-based ammonia production. However, renewable ammonia has recently gained traction again as an energy vector. It is an important component of the rapidly emerging hydrogen economy. Renewable ammonia will probably play a significant role in maintaining national and global energy and food security during the 21st century.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74752748","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A. Hashem, A. Abdel-Ghany, R. El-Tawil, A. Mauger, C. Julien
This study aims to investigate the effect of Na doping on the structure, electrical, and electrochemical properties of lithium-rich cathode material. Pristine Li1.2Ni0.13Mn0.54Co0.13O2 (LNMC) and Na-doped Li1.17Na0.03Ni0.13Mn0.54Co0.13O2 (Na-LNMC) layered lithium-rich/manganese-rich compounds are prepared by the sol-gel method. The structural and morphological characterization reveals that the Na doping leads to an ordered structure with regular cubic morphology and enlarged Li layer spacing. This enlargement facilitates the diffusion of lithium ion inside the bulk lattice. Electrochemical impedance spectroscopy (EIS) shows that doping by a small amount of Na (3 mol%) decreases the impedance by more than three orders of magnitude and enhances the diffusion of lithium ions in the same proportion. This remarkable improvement in the conductivity and diffusion coefficient of lithium ions of Na-LNMC improves its capacity retention. In addition, this structure and mode of preparation results in “U-shaped” capacity vs. cycle curves, similar to the curves observed for transition metal oxide electrodes, resulting in an exceptional cycle life, tested for up to 400 cycles at 2C.
{"title":"Effect of Na Doping on the Electrochemical Performance of Li1.2Ni0.13Co0.13Mn0.54O2 Cathode for Lithium-Ion Batteries","authors":"A. Hashem, A. Abdel-Ghany, R. El-Tawil, A. Mauger, C. Julien","doi":"10.3390/suschem3020010","DOIUrl":"https://doi.org/10.3390/suschem3020010","url":null,"abstract":"This study aims to investigate the effect of Na doping on the structure, electrical, and electrochemical properties of lithium-rich cathode material. Pristine Li1.2Ni0.13Mn0.54Co0.13O2 (LNMC) and Na-doped Li1.17Na0.03Ni0.13Mn0.54Co0.13O2 (Na-LNMC) layered lithium-rich/manganese-rich compounds are prepared by the sol-gel method. The structural and morphological characterization reveals that the Na doping leads to an ordered structure with regular cubic morphology and enlarged Li layer spacing. This enlargement facilitates the diffusion of lithium ion inside the bulk lattice. Electrochemical impedance spectroscopy (EIS) shows that doping by a small amount of Na (3 mol%) decreases the impedance by more than three orders of magnitude and enhances the diffusion of lithium ions in the same proportion. This remarkable improvement in the conductivity and diffusion coefficient of lithium ions of Na-LNMC improves its capacity retention. In addition, this structure and mode of preparation results in “U-shaped” capacity vs. cycle curves, similar to the curves observed for transition metal oxide electrodes, resulting in an exceptional cycle life, tested for up to 400 cycles at 2C.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"76295973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
F. Lamberti, Chiara Mazzariol, F. Spolaore, R. Ceccato, L. Salmaso, Silvia Gross
This review was devoted to outlining the use and potential increasing application of the Design of Experiment (DoE) approach to the rational and planned synthesis of inorganic nanomaterials, with a particular focus on polycrystalline nanostructures (metal and alloys, oxides, chalcogenides, halogenides, etc.) produced by sustainable wet chemistry routes based on a multi-parameter experimental landscape. After having contextualised the stringent need for a rational approach to inorganic materials’ synthesis, a concise theoretical background on DoE is provided, focusing on its statistical basis, shortly describing the different sub-methodologies, and outlining the pros and cons of each. In the second part of the review, a wider section is dedicated to the application of DoE to the rational synthesis of different kinds of chemical systems, with a specific focus on inorganic materials.
{"title":"Design of Experiment: A Rational and Still Unexplored Approach to Inorganic Materials’ Synthesis","authors":"F. Lamberti, Chiara Mazzariol, F. Spolaore, R. Ceccato, L. Salmaso, Silvia Gross","doi":"10.3390/suschem3010009","DOIUrl":"https://doi.org/10.3390/suschem3010009","url":null,"abstract":"This review was devoted to outlining the use and potential increasing application of the Design of Experiment (DoE) approach to the rational and planned synthesis of inorganic nanomaterials, with a particular focus on polycrystalline nanostructures (metal and alloys, oxides, chalcogenides, halogenides, etc.) produced by sustainable wet chemistry routes based on a multi-parameter experimental landscape. After having contextualised the stringent need for a rational approach to inorganic materials’ synthesis, a concise theoretical background on DoE is provided, focusing on its statistical basis, shortly describing the different sub-methodologies, and outlining the pros and cons of each. In the second part of the review, a wider section is dedicated to the application of DoE to the rational synthesis of different kinds of chemical systems, with a specific focus on inorganic materials.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78464436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This Special Issue is focused on the chemical aspects of sustainable energy engineering and the clean production of materials [...]
本期特刊聚焦于可持续能源工程的化学方面和材料的清洁生产[…]
{"title":"Innovations in Energy Engineering and Cleaner Production: A Sustainable Chemistry Perspective","authors":"F. Deganello, J. Bos","doi":"10.3390/suschem3010008","DOIUrl":"https://doi.org/10.3390/suschem3010008","url":null,"abstract":"This Special Issue is focused on the chemical aspects of sustainable energy engineering and the clean production of materials [...]","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73860780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kyriazis Rekos, I. Charisteidis, E. Tzamos, G. Palantzas, A. Zouboulis, K. Triantafyllidis
The management of municipal and industrial organic solid wastes has become one of the most critical environmental problems in modern societies. Nowadays, commonly used management techniques are incineration, composting, and landfilling, with the former one being the most common for hazardous organic wastes. An alternative eco-friendly method that offers a sustainable and economically viable solution for hazardous wastes management is fast pyrolysis, being one of the most important thermochemical processes in the petrochemical and biomass valorization industry. The objective of this work was to study the application of fast pyrolysis for the valorization of three types of wastes, i.e., petroleum-based sludges and sediments, residual paints left on used/scrap metal packaging, and creosote-treated wood waste, towards high-added-value fuels, chemicals, and (bio)char. Fast pyrolysis experiments were performed on a lab-scale fixed-bed reactor for the determination of product yields, i.e., pyrolysis (bio)oil, gases, and solids (char). In addition, the composition of (bio)oil was also determined by Py/GC-MS tests. The thermal pyrolysis oil from the petroleum sludge was only 15.8 wt.% due to the remarkably high content of ash (74 wt.%) of this type of waste, in contrast to the treated wood and the residual paints (also containing 30 wt.% inorganics), which provided 46.9 wt.% and 35 wt.% pyrolysis oil, respectively. The gaseous products ranged from ~7.9 wt.% (sludge) to 14.7 (wood) and 19.2 wt.% (paints), while the respective solids (ash, char, reaction coke) values were 75.1, 35, and 36.9 wt.%. The thermal (non-catalytic) pyrolysis of residual paint contained relatively high concentrations of short acrylic aliphatic ester (i.e., n-butyl methacrylate), being valuable monomers in the polymer industry. The use of an acidic zeolitic catalyst (ZSM-5) for the in situ upgrading of the pyrolysis vapors induced changes on the product yields (decreased oil due to cracking reactions and increased gases and char/coke), but mostly on the pyrolysis oil composition. The main effect of the ZSM-5 zeolite catalyst was that, for all three organic wastes, the catalytic pyrolysis oils were enriched in the value-added mono-aromatics (BTX), especially in the case of the treated wood waste and residual paints. The non-condensable gases were mostly consisting of CO, CO2, and different amounts of C1–C4 hydrocarbons, depending on initial feed and use or not of the catalyst that increased the production of ethylene and propylene.
{"title":"Valorization of Hazardous Organic Solid Wastes towards Fuels and Chemicals via Fast (Catalytic) Pyrolysis","authors":"Kyriazis Rekos, I. Charisteidis, E. Tzamos, G. Palantzas, A. Zouboulis, K. Triantafyllidis","doi":"10.3390/suschem3010007","DOIUrl":"https://doi.org/10.3390/suschem3010007","url":null,"abstract":"The management of municipal and industrial organic solid wastes has become one of the most critical environmental problems in modern societies. Nowadays, commonly used management techniques are incineration, composting, and landfilling, with the former one being the most common for hazardous organic wastes. An alternative eco-friendly method that offers a sustainable and economically viable solution for hazardous wastes management is fast pyrolysis, being one of the most important thermochemical processes in the petrochemical and biomass valorization industry. The objective of this work was to study the application of fast pyrolysis for the valorization of three types of wastes, i.e., petroleum-based sludges and sediments, residual paints left on used/scrap metal packaging, and creosote-treated wood waste, towards high-added-value fuels, chemicals, and (bio)char. Fast pyrolysis experiments were performed on a lab-scale fixed-bed reactor for the determination of product yields, i.e., pyrolysis (bio)oil, gases, and solids (char). In addition, the composition of (bio)oil was also determined by Py/GC-MS tests. The thermal pyrolysis oil from the petroleum sludge was only 15.8 wt.% due to the remarkably high content of ash (74 wt.%) of this type of waste, in contrast to the treated wood and the residual paints (also containing 30 wt.% inorganics), which provided 46.9 wt.% and 35 wt.% pyrolysis oil, respectively. The gaseous products ranged from ~7.9 wt.% (sludge) to 14.7 (wood) and 19.2 wt.% (paints), while the respective solids (ash, char, reaction coke) values were 75.1, 35, and 36.9 wt.%. The thermal (non-catalytic) pyrolysis of residual paint contained relatively high concentrations of short acrylic aliphatic ester (i.e., n-butyl methacrylate), being valuable monomers in the polymer industry. The use of an acidic zeolitic catalyst (ZSM-5) for the in situ upgrading of the pyrolysis vapors induced changes on the product yields (decreased oil due to cracking reactions and increased gases and char/coke), but mostly on the pyrolysis oil composition. The main effect of the ZSM-5 zeolite catalyst was that, for all three organic wastes, the catalytic pyrolysis oils were enriched in the value-added mono-aromatics (BTX), especially in the case of the treated wood waste and residual paints. The non-condensable gases were mostly consisting of CO, CO2, and different amounts of C1–C4 hydrocarbons, depending on initial feed and use or not of the catalyst that increased the production of ethylene and propylene.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"90312510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jacopo De Maron, L. Bellotti, Alessio Baldelli, A. Fasolini, N. Schiaroli, C. Lucarelli, F. Cavani, T. Tabanelli
In recent years, the upgrading of lignocellulose bio-oils from fast-pyrolysis by means of ketonization has emerged as a frontier research domain to produce a new generation of biofuels. Propionic acid (PA) ketonization is extensively investigated as a model reaction over metal oxides, but the activity of other materials, such as metal phosphates, is mostly unknown. Therefore, PA ketonization was preliminarily investigated in the gas phase over both phosphates and oxides of Al, Zr, and La. Their catalytic activity was correlated to the physicochemical properties of the materials characterized by means of XRD, XRF, BET N2 porosimetry, and CO2- and NH3-TPD. Noteworthy, monoclinic ZrO2 proved to be the most promising candidate for the target reaction, leading to a 3-pentanone productivity as high as 5.6 h−1 in the optimized conditions. This value is higher than most of those reported for the same reaction in both the academic and patent literature.
{"title":"Evaluation of the Catalytic Activity of Metal Phosphates and Related Oxides in the Ketonization of Propionic Acid","authors":"Jacopo De Maron, L. Bellotti, Alessio Baldelli, A. Fasolini, N. Schiaroli, C. Lucarelli, F. Cavani, T. Tabanelli","doi":"10.3390/suschem3010005","DOIUrl":"https://doi.org/10.3390/suschem3010005","url":null,"abstract":"In recent years, the upgrading of lignocellulose bio-oils from fast-pyrolysis by means of ketonization has emerged as a frontier research domain to produce a new generation of biofuels. Propionic acid (PA) ketonization is extensively investigated as a model reaction over metal oxides, but the activity of other materials, such as metal phosphates, is mostly unknown. Therefore, PA ketonization was preliminarily investigated in the gas phase over both phosphates and oxides of Al, Zr, and La. Their catalytic activity was correlated to the physicochemical properties of the materials characterized by means of XRD, XRF, BET N2 porosimetry, and CO2- and NH3-TPD. Noteworthy, monoclinic ZrO2 proved to be the most promising candidate for the target reaction, leading to a 3-pentanone productivity as high as 5.6 h−1 in the optimized conditions. This value is higher than most of those reported for the same reaction in both the academic and patent literature.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79886673","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Al Mon E. Dahan, R. Alorro, Mona Lisa C. Pacaña, Ronben M. Baute, Leaniel C. Silva, C. Tabelin, V. Resabal
Coal Fly Ash (CFA) is a hazardous waste from coal-fired power plants, but has increasingly become a popular supplementary cementitious material for cement in the construction industry. As a secondary resource of REE, its main advantage lies in its fine particle size that eliminates the need for costly and energy-intensive comminution. In this study, the potential of CFA from the Philippines as a secondary REE resource was investigated by direct leaching of REEs with hydrochloric acid (HCl). The CFA sample came from a coal-fired power plant with a circulating fluidized bed combustion (CFBC) technology. For the leaching tests, the effects of HCl concentration, leaching time and leaching temperature on REE extractions were elucidate optimized via Response Surface Methodology (RSM). The RSM results showed that the optimum leaching occurred at 3M HCl, 65 °C and 270 min with extractions of Nd, Er, Eu, Tb and Dy at 70.8%, 76.34%, 88.02%, 90.01% and 73.38%, respectively. According to these results, the CFA from the Philippines is a promising secondary resource of REE and the extraction method employed was effective in achieving a relatively high REE dissolution. Moreover, the empirical model that was established accurately predicted the dissolution of REE with an accuracy of 98.20%, 96.66%, 97.09%, 98.17% and 97.78% for Nd, Er, Eu, Tb and Dy, respectively.
{"title":"Hydrochloric Acid Leaching of Philippine Coal Fly Ash: Investigation and Optimisation of Leaching Parameters by Response Surface Methodology (RSM)","authors":"Al Mon E. Dahan, R. Alorro, Mona Lisa C. Pacaña, Ronben M. Baute, Leaniel C. Silva, C. Tabelin, V. Resabal","doi":"10.3390/suschem3010006","DOIUrl":"https://doi.org/10.3390/suschem3010006","url":null,"abstract":"Coal Fly Ash (CFA) is a hazardous waste from coal-fired power plants, but has increasingly become a popular supplementary cementitious material for cement in the construction industry. As a secondary resource of REE, its main advantage lies in its fine particle size that eliminates the need for costly and energy-intensive comminution. In this study, the potential of CFA from the Philippines as a secondary REE resource was investigated by direct leaching of REEs with hydrochloric acid (HCl). The CFA sample came from a coal-fired power plant with a circulating fluidized bed combustion (CFBC) technology. For the leaching tests, the effects of HCl concentration, leaching time and leaching temperature on REE extractions were elucidate optimized via Response Surface Methodology (RSM). The RSM results showed that the optimum leaching occurred at 3M HCl, 65 °C and 270 min with extractions of Nd, Er, Eu, Tb and Dy at 70.8%, 76.34%, 88.02%, 90.01% and 73.38%, respectively. According to these results, the CFA from the Philippines is a promising secondary resource of REE and the extraction method employed was effective in achieving a relatively high REE dissolution. Moreover, the empirical model that was established accurately predicted the dissolution of REE with an accuracy of 98.20%, 96.66%, 97.09%, 98.17% and 97.78% for Nd, Er, Eu, Tb and Dy, respectively.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2022-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"80053715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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