Pub Date : 2017-10-11DOI: 10.15496/PUBLIKATION-29195
L. Angenent
Renewable electrical energy production, such as wind power or photovoltaics, faces temporal fluctuations and spatial separation of source and sink creating the need for suitable storage and conversion technologies. Furthermore, a bio-based economy needs technologies allowing the on-demand and on-site conversion of biomass to platform chemicals and chemical energy carriers. This study combines microbial and electrochemical conversions, allowing production of chemicals from biomass and electricity. Carboxylic acids (CAs) are produced by anaerobic conversion of a renewable feedstock with reactor microbiomes. CAs are subsequently electrochemically upgraded to yield energy-dense alkanes. We present a proof-of-concept based on experimental data for each step in two independent case studies at laboratory scale. During continuous CA fermentation from corn beer, mainly n-caproic and n-caprylic acid were produced yielding in total 0.638 g COD g−1 COD [CA/corn beer]. A batch system fed with corn silage yielded mainly n-butyric acid (0.207 g COD g−1 COD [CA/corn silage]), and some n-caproic acid (0.030 g COD g−1 COD [CA/corn silage]). The CAs were removed from the fermentation broth using a pertraction system. Subsequently, the CAs were electrochemically converted via Kolbe reaction and other reaction pathways. Depending on the carbon chain length of the CAs, liquid alkanes (from medium-chain CAs) or gaseous alkanes and alcohols (from short-chain CAs) were gained. Coulombic efficiencies of up to 80% were achieved despite the alkaline (pH 9) electrolysis conditions that are dictated by the pertraction system. Remarkably, CAs with a carbon chain length of six or more C-atoms were successfully converted to liquid alkanes at a high yield (in total: 0.480 g COD g−1 COD [hydrocarbon/corn beer]). This was achieved at an energy input of only 0.100 kW h per mol of converted CA (considering the electrochemical half cell reaction). Noteworthily, the electrochemical CA conversion is much faster than the CA fermentation, allowing intermittent electrolysis during periods of excess electrical power. We demonstrate that the finally gained product is suitable as a drop-in fuel without any further downstream processing. The future general potential as well as requirements for the concept are discussed.
可再生电力生产,如风力发电或光伏发电,面临着时间波动和源汇空间分离的问题,因此需要适当的储存和转换技术。此外,基于生物的经济需要允许按需和现场将生物质转化为平台化学品和化学能载体的技术。这项研究结合了微生物和电化学转化,允许从生物质和电力中生产化学物质。羧酸(CAs)是由可再生原料与反应器微生物群厌氧转化产生的。CAs随后被电化学升级为能量密集的烷烃。我们在实验室规模的两个独立案例研究中提出了基于每个步骤的实验数据的概念验证。在以玉米啤酒为原料的连续CA发酵过程中,主要产生正己酸和正辛酸,总COD为0.638 g g−1 COD [CA/玉米啤酒]。间歇式玉米青贮饲料体系主要产出正丁酸(0.207 g COD g−1 COD [CA/玉米青贮])和部分正己酸(0.030 g COD g−1 COD [CA/玉米青贮])。使用抽吸系统将CAs从发酵液中去除。随后,通过Kolbe反应和其他反应途径对CAs进行电化学转化。根据CAs的碳链长度,可以得到液态烷烃(由中链CAs生成)或气态烷烃和醇(由短链CAs生成)。在碱性电解条件下(pH值为9),库仑效率高达80%。值得注意的是,碳链长度为6个或更多c原子的CAs以高收率成功转化为液态烷烃(总计:0.480 g COD g−1 COD[烃/玉米啤酒])。这是在每mol转化CA的能量输入仅为0.100 kW h的情况下实现的(考虑到电化学半电池反应)。值得注意的是,电化学CA转化比CA发酵快得多,允许在电力过剩期间间歇性电解。我们证明,最终获得的产品是合适的作为直接燃料,不需要进一步的下游处理。讨论了该概念未来的一般潜力和要求。
{"title":"Production of drop-in fuels from biomass at high selectivity by combined microbial and electrochemical conversion","authors":"L. Angenent","doi":"10.15496/PUBLIKATION-29195","DOIUrl":"https://doi.org/10.15496/PUBLIKATION-29195","url":null,"abstract":"Renewable electrical energy production, such as wind power or photovoltaics, faces temporal fluctuations and spatial separation of source and sink creating the need for suitable storage and conversion technologies. Furthermore, a bio-based economy needs technologies allowing the on-demand and on-site conversion of biomass to platform chemicals and chemical energy carriers. This study combines microbial and electrochemical conversions, allowing production of chemicals from biomass and electricity. Carboxylic acids (CAs) are produced by anaerobic conversion of a renewable feedstock with reactor microbiomes. CAs are subsequently electrochemically upgraded to yield energy-dense alkanes. We present a proof-of-concept based on experimental data for each step in two independent case studies at laboratory scale. During continuous CA fermentation from corn beer, mainly n-caproic and n-caprylic acid were produced yielding in total 0.638 g COD g−1 COD [CA/corn beer]. A batch system fed with corn silage yielded mainly n-butyric acid (0.207 g COD g−1 COD [CA/corn silage]), and some n-caproic acid (0.030 g COD g−1 COD [CA/corn silage]). The CAs were removed from the fermentation broth using a pertraction system. Subsequently, the CAs were electrochemically converted via Kolbe reaction and other reaction pathways. Depending on the carbon chain length of the CAs, liquid alkanes (from medium-chain CAs) or gaseous alkanes and alcohols (from short-chain CAs) were gained. Coulombic efficiencies of up to 80% were achieved despite the alkaline (pH 9) electrolysis conditions that are dictated by the pertraction system. Remarkably, CAs with a carbon chain length of six or more C-atoms were successfully converted to liquid alkanes at a high yield (in total: 0.480 g COD g−1 COD [hydrocarbon/corn beer]). This was achieved at an energy input of only 0.100 kW h per mol of converted CA (considering the electrochemical half cell reaction). Noteworthily, the electrochemical CA conversion is much faster than the CA fermentation, allowing intermittent electrolysis during periods of excess electrical power. We demonstrate that the finally gained product is suitable as a drop-in fuel without any further downstream processing. The future general potential as well as requirements for the concept are discussed.","PeriodicalId":11589,"journal":{"name":"Energy and Environmental Science","volume":"59 1","pages":"2231-2244"},"PeriodicalIF":0.0,"publicationDate":"2017-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79920722","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}
Pub Date : 2015-01-01DOI: 10.1533/9780857098764.3.473
Markus Hösel, Dechan Angmo, F. Krebs
Organic-based photoconverters are subject to a considerable interest due to their promising functionalities and their potential use as alternatives to the more expensive inorganic analogues. We introduce the basic operational mechanisms, limitations and some ideas towards improving the efficiency of organic solar cells by focusing on probing the morphological/structural, dynamical, and electronic aspects of a model organic material consisting of charge-transfer discotic liquid-crystal system hexakis(n-hexyloxy)triphenylene/2,4,7 trinitro-9-fluorenone (HAT6/TNF). For the electronic ground-state investigations, neutron-scattering techniques play a key role in gaining deeper insight into structure and dynamics. These measurements are complemented by Raman and nuclear magnetic resonance probes, as well as resonant Raman and UV-vis spectroscopies that are used to explore the low-lying excited states, at the vibronic level. Synergistically, numerical simulations, either classical via empirical force fields, or first-principles via density functional theory, are used for the analysis, interpretation and predictions.
{"title":"Organic Solar Cells","authors":"Markus Hösel, Dechan Angmo, F. Krebs","doi":"10.1533/9780857098764.3.473","DOIUrl":"https://doi.org/10.1533/9780857098764.3.473","url":null,"abstract":"Organic-based photoconverters are subject to a considerable interest due to their promising functionalities and their potential use as alternatives to the more expensive inorganic analogues. We introduce the basic operational mechanisms, limitations and some ideas towards improving the efficiency of organic solar cells by focusing on probing the morphological/structural, dynamical, and electronic aspects of a model organic material consisting of charge-transfer discotic liquid-crystal system hexakis(n-hexyloxy)triphenylene/2,4,7 trinitro-9-fluorenone (HAT6/TNF). For the electronic ground-state investigations, neutron-scattering techniques play a key role in gaining deeper insight into structure and dynamics. These measurements are complemented by Raman and nuclear magnetic resonance probes, as well as resonant Raman and UV-vis spectroscopies that are used to explore the low-lying excited states, at the vibronic level. Synergistically, numerical simulations, either classical via empirical force fields, or first-principles via density functional theory, are used for the analysis, interpretation and predictions.","PeriodicalId":11589,"journal":{"name":"Energy and Environmental Science","volume":"167 1","pages":"109-135"},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"76000057","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. Borole, G. Reguera, B. Ringeisen, Zhi-wu Wang, Yujie Feng, Byung Hong Kim
Erratum : Strong and binder free structured zeolite sorbents with very high CO2-over-N-2 selectivities and high capacities to adsorb CO2 rapidly (vol 5, pg 7664, 2012)
{"title":"Erratum: Electroactive biofilms: Current status and future research needs (Energy & Environmental Science (2011) 4 (4813-4834) DOI: 10.1039/C1EE02511B)","authors":"A. Borole, G. Reguera, B. Ringeisen, Zhi-wu Wang, Yujie Feng, Byung Hong Kim","doi":"10.1039/C2EE90051C","DOIUrl":"https://doi.org/10.1039/C2EE90051C","url":null,"abstract":"Erratum : Strong and binder free structured zeolite sorbents with very high CO2-over-N-2 selectivities and high capacities to adsorb CO2 rapidly (vol 5, pg 7664, 2012)","PeriodicalId":11589,"journal":{"name":"Energy and Environmental Science","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2012-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"77878513","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 Energy @ Environmental Science Accepted Manuscript was published in error and has been retracted by the publisher, the Royal Society of Chemistry. The publisher regrets that an administrative error led to a duplicate version of the manuscript being published. The correct manuscript can be accessed at http://pubs.rsc.org/en/content/articlelanding/2012/ee/c2ee22777k. The publishers apologise for any inconvenience caused by this error. Retraction published December 2013.
{"title":"Retracted article: Towards Polymer-based Organic Thermoelectric Generators","authors":"Docent Xavier Crispin","doi":"10.1039/C2EE23401G","DOIUrl":"https://doi.org/10.1039/C2EE23401G","url":null,"abstract":"This Energy @ Environmental Science Accepted Manuscript was published in error and has been retracted by the publisher, the Royal Society of Chemistry. The publisher regrets that an administrative error led to a duplicate version of the manuscript being published. The correct manuscript can be accessed at http://pubs.rsc.org/en/content/articlelanding/2012/ee/c2ee22777k. The publishers apologise for any inconvenience caused by this error. Retraction published December 2013.","PeriodicalId":11589,"journal":{"name":"Energy and Environmental Science","volume":"18 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2012-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78458403","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}