Biogeochemistry of arsenic and lead in sediment and water amended with biochar

Detalhes bibliográficos
Autor(a) principal: Soares, Matheus Bortolanza
Data de Publicação: 2023
Tipo de documento: Tese
Idioma: eng
Título da fonte: Biblioteca Digital de Teses e Dissertações da USP
Texto Completo: https://www.teses.usp.br/teses/disponiveis/11/11140/tde-10022023-100933/
Resumo: Potentially toxic elements (PTEs), such as arsenic (As) and lead (Pb), constantly cause the development of diseases in living beings due to the continuous ingestion of water and food with high levels of these elements. Daily anthropogenic practices, such as domestic, health, industrial, agricultural, and mining activities can contribute to the increase in the concentration of As and Pb in soils and sediments exposed to the Earth\'s surface, and this increases the probability of contact with living beings. Although the occurrence of As and Pb in the environment is not necessarily recent, it has become more relevant in recent decades due to their harmful effects and to the global concern to recover natural resources. To restore the functionality of ecosystems contaminated by As and Pb, the scientific community has sought to use remediation techniques to reduce the bioavailable levels of these elements in soil and water. Among them, the use of biochar has stood out due to its ability to immobilize contaminants, supply nutrients, and store carbon. In situ remediation with biochar is an ecological alternative that can be economically viable when compared to other conventional remediation techniques that generate waste and/or are expensive. Biochar is a product of the pyrolysis of organic compounds, and its effectiveness in immobilizing contaminants depends on the manufacturing conditions, including the pyrolysis temperature. In addition, environmental conditions such as redox fluctuation, other factors as high precipitation, and exposure to weather can alter the potential of biochar to (i)mobilize EPTs in the environment. The following itens were evaluated in this study: (i) the effect of biochar pyrolysis temperature on As and Pb dynamics in sediment exposed to environments with total and partial presence of oxygen; (ii) the biogeochemistry of As and Pb in sediment and water submitted to the application of in natura biochar and modified with ferric chloride; and (iii) effects of dissolved organic carbon (DOC) on the competition for specific sorption sites with As. To evaluate the dynamics of As and Pb, several experiments were carried out with sediment and water contaminated with As and Pb due to mining and ore processing. Samples contaminated with As and Pb were conditioned with biochar from sugarcane straw (Saccharum officinarum) pyrolyzed at 350 (BC350), 550 (BC550), and 750°C (BC750), and the potential competition for sorption sites was evaluated in water samples artificially contaminated with arsenate [As(V)]. Sorption competition was performed in the presence of biogenic iron (Fe) (oxyhydr)oxide (BIOS), which is a Fe(III) biomineral widely known to be a natural sink for As. The pyrolysis temperature played a key role in the physicochemical characteristics of the biochar, and this affected the ability to (i)mobilize As and Pb in sediment and water. The application of biochar reduced the β-glucosidase activity and increased the phosphatase activity, which demonstrates the microbiota\'s difficulty in degrading the carbon in the biochar and, at the same time, its ease in providing hydrolase capable of mineralizing phosphate present in organic forms. The aging time of the biochar caused an increase in the bioavailable and exchangeable contents of As to the same extent that it reduced the bioavailable and exchangeable contents of Pb. The increase in bioavailable and exchangeable As contents were related to changes in carbon pools caused by surface oxidation of biochar and by biodegradation promoted by microorganisms. In environments with high precipitation, biochar application increased As release and mobility without affecting As species distribution. The chemical modification of biochar, as a way to improve a water filter, increased the speed and sorption capacity of As and Pb and made biochar modified with ferric chloride a promising alternative for filtering water contaminated with these elements. The presence of DOC from biochar was able to reduce As(V) sorption in BIOS by up to 30%. However, the presence of DOC did not alter As(V) sorption mechanisms in BIOS, which shows that site blocking the main mechanism responsible for reducing As(V) sorption. The biochar was able to reduce the mobility of As in the sediment under environments with partial presence of oxygen. In addition to the change in the mobility of As and Pb, it was verified that the supply of biochar to the sediment considerably increased the DOC content in the solution, which possibly buffered the assimilative biotic reduction of Fe(III) and As(V) and reduced the As methylation.
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spelling Biogeochemistry of arsenic and lead in sediment and water amended with biocharBiogeoquímica de arsênio e chumbo em sedimento e água condicionado com biocarvãoArsenateArsenatoArseniteArsenitoBiogenic iron (oxyhydr)oxidesEspeciaçãoOxihidróxidos de ferro biogênicoPyrolysis temperatureRemediaçãoRemediationSpeciationTemperatura de pirólisePotentially toxic elements (PTEs), such as arsenic (As) and lead (Pb), constantly cause the development of diseases in living beings due to the continuous ingestion of water and food with high levels of these elements. Daily anthropogenic practices, such as domestic, health, industrial, agricultural, and mining activities can contribute to the increase in the concentration of As and Pb in soils and sediments exposed to the Earth\'s surface, and this increases the probability of contact with living beings. Although the occurrence of As and Pb in the environment is not necessarily recent, it has become more relevant in recent decades due to their harmful effects and to the global concern to recover natural resources. To restore the functionality of ecosystems contaminated by As and Pb, the scientific community has sought to use remediation techniques to reduce the bioavailable levels of these elements in soil and water. Among them, the use of biochar has stood out due to its ability to immobilize contaminants, supply nutrients, and store carbon. In situ remediation with biochar is an ecological alternative that can be economically viable when compared to other conventional remediation techniques that generate waste and/or are expensive. Biochar is a product of the pyrolysis of organic compounds, and its effectiveness in immobilizing contaminants depends on the manufacturing conditions, including the pyrolysis temperature. In addition, environmental conditions such as redox fluctuation, other factors as high precipitation, and exposure to weather can alter the potential of biochar to (i)mobilize EPTs in the environment. The following itens were evaluated in this study: (i) the effect of biochar pyrolysis temperature on As and Pb dynamics in sediment exposed to environments with total and partial presence of oxygen; (ii) the biogeochemistry of As and Pb in sediment and water submitted to the application of in natura biochar and modified with ferric chloride; and (iii) effects of dissolved organic carbon (DOC) on the competition for specific sorption sites with As. To evaluate the dynamics of As and Pb, several experiments were carried out with sediment and water contaminated with As and Pb due to mining and ore processing. Samples contaminated with As and Pb were conditioned with biochar from sugarcane straw (Saccharum officinarum) pyrolyzed at 350 (BC350), 550 (BC550), and 750°C (BC750), and the potential competition for sorption sites was evaluated in water samples artificially contaminated with arsenate [As(V)]. Sorption competition was performed in the presence of biogenic iron (Fe) (oxyhydr)oxide (BIOS), which is a Fe(III) biomineral widely known to be a natural sink for As. The pyrolysis temperature played a key role in the physicochemical characteristics of the biochar, and this affected the ability to (i)mobilize As and Pb in sediment and water. The application of biochar reduced the β-glucosidase activity and increased the phosphatase activity, which demonstrates the microbiota\'s difficulty in degrading the carbon in the biochar and, at the same time, its ease in providing hydrolase capable of mineralizing phosphate present in organic forms. The aging time of the biochar caused an increase in the bioavailable and exchangeable contents of As to the same extent that it reduced the bioavailable and exchangeable contents of Pb. The increase in bioavailable and exchangeable As contents were related to changes in carbon pools caused by surface oxidation of biochar and by biodegradation promoted by microorganisms. In environments with high precipitation, biochar application increased As release and mobility without affecting As species distribution. The chemical modification of biochar, as a way to improve a water filter, increased the speed and sorption capacity of As and Pb and made biochar modified with ferric chloride a promising alternative for filtering water contaminated with these elements. The presence of DOC from biochar was able to reduce As(V) sorption in BIOS by up to 30%. However, the presence of DOC did not alter As(V) sorption mechanisms in BIOS, which shows that site blocking the main mechanism responsible for reducing As(V) sorption. The biochar was able to reduce the mobility of As in the sediment under environments with partial presence of oxygen. In addition to the change in the mobility of As and Pb, it was verified that the supply of biochar to the sediment considerably increased the DOC content in the solution, which possibly buffered the assimilative biotic reduction of Fe(III) and As(V) and reduced the As methylation.Elementos potencialmente tóxicos (EPTs), como arsênio (As) e chumbo (Pb), constantemente ocasionam o desenvolvimento de doenças em seres vivos devido à ingestão contínua de água e alimentos com teores elevados desses elementos. Práticas antropogênicas diárias, como atividades domésticos, de saúde, industriais, agrícolas e de mineração podem contribuir para aumento da concentração de As e Pb em solos e sedimentos expostos à superfície terrestre, e isso aumenta a probabilidade de contato com os seres vivos. Embora a ocorrência de As e Pb no meio ambiente não seja necessariamente recente, ela se tornou mais relevante nas últimas décadas devido ao seu efeitos nocivo e à preocupação global em recuperar recursos naturais. Como forma de retomar a funcionalidade de ecossistemas contaminados por As e Pb, a comunidade científica tem buscado utilizar técnicas de remediação que visam a reduzir os teores biodisponíveis desses elementos no solo e na água. Dentre elas, tem se destacado o uso de biocarvão devido à sua capacidade de imobilização de contaminantes, fornecimento de nutrientes e estoque de carbono. A remediação in situ com biocarvão é alternativa ecológica e que pode ser economicamente viável quando comparada a outras técnicas convencionais de remediação que geram resíduos e/ou são de alto custo. O biocarvão é um produto da pirólise de compostos orgânicos, e sua efetividade na imobilização de contaminantes está condicionada às condições de fabricação, dentre elas a temperatura de pirólise. Além disso, as condições ambientais como flutuação redox, elevada precipitação e exposição ao tempo são fatores que podem alterar o potencial do biocarvão em (i)mobilizar EPTs como As e Pb no ambiente. Neste trabalho foram avaliados (i) o efeito da temperatura de pirólise do biocarvão na dinâmica de As e Pb em sedimento exposto a ambientes com presença total e parcial de oxigênio; (ii) a biogeoquímica de As e Pb em sedimento e água submetidos a aplicação de biocarvão in natura e modificado com cloreto férrico; e (iii) efeitos do carbono orgânico dissolvido (COD) na competição por sítios específicos de sorção com As. Para avaliar a dinâmica de As e Pb, foram realizados diversos experimentos com sedimento e água contaminada com As e Pb devido à atividade antropogênica associada à mineração e beneficiamento de minério. As amostras contaminadas com As e Pb foram condicionadas com biocarvão de palha de cana-de-açúcar (Saccharum officinarum) pirolisado a 350 (BC350), 550 (BC550) e 750°C (BC750), enquanto a potencial competição por sítios de sorção foi avaliada em amostras de água contaminadas artificialmente com arsenato [As(V)]. A competição por sorção foi realizada na presença de oxihidróxidos de ferro (Fe) biogênico (BIOS), que é um biomineral de Fe(III) amplamente conhecido por ser sumidouro natural de As. A temperatura de pirólise exerceu papel fundamental nas características fisico-químicas do biocarvão, e isso afetou a capacidade de (i)mobilização de As e Pb em sedimento e água. A aplicação de biocarvão reduziu a atividade da β-glicosidase e aumentou a atividade da fosfatase, o que evidencia a dificuldade da microbiota em degradar o carbono do biocarvão, assim como sua facilidade em fornecer hidrolase capaz de mineralizar fosfato presente em formas orgânicas. O tempo de envelhecimento do biocarvão ocasionou aumento nos teores biodisponíveis e trocáveis de As, na mesma medida em que reduziu os teores biodisponíveis e trocáveis de Pb. O aumento dos teores biodisponíveis e trocáveis de As esteve relacionado às mudanças nos reservatórios de carbono ocasionados pela oxidação de superfície do biocarvão e pela biodegradação promovida pelos microorganismos. Em ambientes com elevada precipitação, a aplicação de biocarvão aumentou a liberação e a mobilidade de As sem afetar a distribuição das espécies de As. A modificação química do biocarvão, como forma de aperfeiçoar um filtro de água, aumentou a velocidade e capacidade de sorção de As e Pb e tornou o biocarvão modificado com cloreto férrico uma alternativa promissora para filtro de água contaminada com esses elementos. A presença do DOC do biocarvão foi capaz de reduzir em até 30% a sorção de As(V) em BIOS. No entanto, a presença de DOC não alterou os mecanismos de sorção de As(V) em BIOS, o que mostra que o principal meio responsável pela redução da sorção de As(V) é o bloqueio de sítio. Já no sedimento em ambientes com presença parcial de oxigênio, o biocarvão foi capaz de reduzir a mobilidade de As. Além da mudança na mobilidade de As e Pb, verificou-se que o fornecimento de biocarvão ao sedimento aumentou consideravelmente o teor de DOC em solução, o que possivelmente tamponou a redução biótica assimilativa de Fe(III) e As(V) e reduziu a metilação de As.Biblioteca Digitais de Teses e Dissertações da USPAlleoni, Luis Reynaldo FerracciúSoares, Matheus Bortolanza2023-01-27info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisapplication/pdfhttps://www.teses.usp.br/teses/disponiveis/11/11140/tde-10022023-100933/reponame:Biblioteca Digital de Teses e Dissertações da USPinstname:Universidade de São Paulo (USP)instacron:USPReter o conteúdo por motivos de patente, publicação e/ou direitos autoriais.info:eu-repo/semantics/openAccesseng2023-02-10T20:52:01Zoai:teses.usp.br:tde-10022023-100933Biblioteca Digital de Teses e Dissertaçõeshttp://www.teses.usp.br/PUBhttp://www.teses.usp.br/cgi-bin/mtd2br.plvirginia@if.usp.br|| atendimento@aguia.usp.br||virginia@if.usp.bropendoar:27212023-02-10T20:52:01Biblioteca Digital de Teses e Dissertações da USP - Universidade de São Paulo (USP)false
dc.title.none.fl_str_mv Biogeochemistry of arsenic and lead in sediment and water amended with biochar
Biogeoquímica de arsênio e chumbo em sedimento e água condicionado com biocarvão
title Biogeochemistry of arsenic and lead in sediment and water amended with biochar
spellingShingle Biogeochemistry of arsenic and lead in sediment and water amended with biochar
Soares, Matheus Bortolanza
Arsenate
Arsenato
Arsenite
Arsenito
Biogenic iron (oxyhydr)oxides
Especiação
Oxihidróxidos de ferro biogênico
Pyrolysis temperature
Remediação
Remediation
Speciation
Temperatura de pirólise
title_short Biogeochemistry of arsenic and lead in sediment and water amended with biochar
title_full Biogeochemistry of arsenic and lead in sediment and water amended with biochar
title_fullStr Biogeochemistry of arsenic and lead in sediment and water amended with biochar
title_full_unstemmed Biogeochemistry of arsenic and lead in sediment and water amended with biochar
title_sort Biogeochemistry of arsenic and lead in sediment and water amended with biochar
author Soares, Matheus Bortolanza
author_facet Soares, Matheus Bortolanza
author_role author
dc.contributor.none.fl_str_mv Alleoni, Luis Reynaldo Ferracciú
dc.contributor.author.fl_str_mv Soares, Matheus Bortolanza
dc.subject.por.fl_str_mv Arsenate
Arsenato
Arsenite
Arsenito
Biogenic iron (oxyhydr)oxides
Especiação
Oxihidróxidos de ferro biogênico
Pyrolysis temperature
Remediação
Remediation
Speciation
Temperatura de pirólise
topic Arsenate
Arsenato
Arsenite
Arsenito
Biogenic iron (oxyhydr)oxides
Especiação
Oxihidróxidos de ferro biogênico
Pyrolysis temperature
Remediação
Remediation
Speciation
Temperatura de pirólise
description Potentially toxic elements (PTEs), such as arsenic (As) and lead (Pb), constantly cause the development of diseases in living beings due to the continuous ingestion of water and food with high levels of these elements. Daily anthropogenic practices, such as domestic, health, industrial, agricultural, and mining activities can contribute to the increase in the concentration of As and Pb in soils and sediments exposed to the Earth\'s surface, and this increases the probability of contact with living beings. Although the occurrence of As and Pb in the environment is not necessarily recent, it has become more relevant in recent decades due to their harmful effects and to the global concern to recover natural resources. To restore the functionality of ecosystems contaminated by As and Pb, the scientific community has sought to use remediation techniques to reduce the bioavailable levels of these elements in soil and water. Among them, the use of biochar has stood out due to its ability to immobilize contaminants, supply nutrients, and store carbon. In situ remediation with biochar is an ecological alternative that can be economically viable when compared to other conventional remediation techniques that generate waste and/or are expensive. Biochar is a product of the pyrolysis of organic compounds, and its effectiveness in immobilizing contaminants depends on the manufacturing conditions, including the pyrolysis temperature. In addition, environmental conditions such as redox fluctuation, other factors as high precipitation, and exposure to weather can alter the potential of biochar to (i)mobilize EPTs in the environment. The following itens were evaluated in this study: (i) the effect of biochar pyrolysis temperature on As and Pb dynamics in sediment exposed to environments with total and partial presence of oxygen; (ii) the biogeochemistry of As and Pb in sediment and water submitted to the application of in natura biochar and modified with ferric chloride; and (iii) effects of dissolved organic carbon (DOC) on the competition for specific sorption sites with As. To evaluate the dynamics of As and Pb, several experiments were carried out with sediment and water contaminated with As and Pb due to mining and ore processing. Samples contaminated with As and Pb were conditioned with biochar from sugarcane straw (Saccharum officinarum) pyrolyzed at 350 (BC350), 550 (BC550), and 750°C (BC750), and the potential competition for sorption sites was evaluated in water samples artificially contaminated with arsenate [As(V)]. Sorption competition was performed in the presence of biogenic iron (Fe) (oxyhydr)oxide (BIOS), which is a Fe(III) biomineral widely known to be a natural sink for As. The pyrolysis temperature played a key role in the physicochemical characteristics of the biochar, and this affected the ability to (i)mobilize As and Pb in sediment and water. The application of biochar reduced the β-glucosidase activity and increased the phosphatase activity, which demonstrates the microbiota\'s difficulty in degrading the carbon in the biochar and, at the same time, its ease in providing hydrolase capable of mineralizing phosphate present in organic forms. The aging time of the biochar caused an increase in the bioavailable and exchangeable contents of As to the same extent that it reduced the bioavailable and exchangeable contents of Pb. The increase in bioavailable and exchangeable As contents were related to changes in carbon pools caused by surface oxidation of biochar and by biodegradation promoted by microorganisms. In environments with high precipitation, biochar application increased As release and mobility without affecting As species distribution. The chemical modification of biochar, as a way to improve a water filter, increased the speed and sorption capacity of As and Pb and made biochar modified with ferric chloride a promising alternative for filtering water contaminated with these elements. The presence of DOC from biochar was able to reduce As(V) sorption in BIOS by up to 30%. However, the presence of DOC did not alter As(V) sorption mechanisms in BIOS, which shows that site blocking the main mechanism responsible for reducing As(V) sorption. The biochar was able to reduce the mobility of As in the sediment under environments with partial presence of oxygen. In addition to the change in the mobility of As and Pb, it was verified that the supply of biochar to the sediment considerably increased the DOC content in the solution, which possibly buffered the assimilative biotic reduction of Fe(III) and As(V) and reduced the As methylation.
publishDate 2023
dc.date.none.fl_str_mv 2023-01-27
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instname:Universidade de São Paulo (USP)
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