Bradie S. Crandall, Byung Hee Ko, Sean Overa, Luke Cherniack, Ahryeon Lee, Izak Minnie, Feng Jiao
{"title":"Kilowatt-scale tandem CO2 electrolysis for enhanced acetate and ethylene production","authors":"Bradie S. Crandall, Byung Hee Ko, Sean Overa, Luke Cherniack, Ahryeon Lee, Izak Minnie, Feng Jiao","doi":"10.1038/s44286-024-00076-8","DOIUrl":"10.1038/s44286-024-00076-8","url":null,"abstract":"The conversion of carbon dioxide (CO2) into valuable chemicals is a key strategy for carbon utilization. Although tandem CO2 electrolysis has shown promise, it has been largely confined to watt-scale studies and larger-scale studies are needed to accelerate commercialization. In this work, we demonstrate a tandem CO2 electrolyzer engineered for the production of multicarbon products, acetate and ethylene, at the kilowatt (kW) scale. Here, from insights gained at the watt scale, we have successfully designed and operated a 1,000 cm2 CO electrolyzer at 0.71 kW and a 500 cm2 CO2 electrolyzer at 0.40 kW. The kW-scale CO electrolyzer stack demonstrated a stable current of 300 A over 125 h, yielding 98 l of 1.2 M acetate at 96% purity. The system exhibited resilience against typical industrial impurities, maintaining high performance. These results mark a crucial advancement in scaling tandem CO2 electrolysis systems toward industrial feasibility. Finally, an experimentally informed techno-economic analysis is offered to provide a pathway for commercially viable tandem CO2 electrolysis at an industrial scale. Tandem CO2 electrolysis has demonstrated strong potential for transforming captured CO2 into multicarbon products, but more effort is needed in scaling these systems to commercial levels. The authors address this crucial need by elevating tandem CO2 electrolysis to the kilowatt scale, marking a significant step toward real-world implementation.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 6","pages":"421-429"},"PeriodicalIF":0.0,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141272153","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}
{"title":"That one time","authors":"Thomas Dursch","doi":"10.1038/s44286-024-00071-z","DOIUrl":"10.1038/s44286-024-00071-z","url":null,"abstract":"Identifying and estimating operative timescales can help win over a skeptical referee, as Tom Dursch recounts.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"385-385"},"PeriodicalIF":0.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907151","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}
{"title":"Closing the thermoset recycling loop","authors":"Mo Qiao","doi":"10.1038/s44286-024-00072-y","DOIUrl":"10.1038/s44286-024-00072-y","url":null,"abstract":"","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"333-333"},"PeriodicalIF":0.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907140","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}
{"title":"Striking a theoretical balance","authors":"","doi":"10.1038/s44286-024-00078-6","DOIUrl":"10.1038/s44286-024-00078-6","url":null,"abstract":"Modeling chemical processes and systems underpins progress in chemical engineering science; we encourage submissions in this domain.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"325-325"},"PeriodicalIF":0.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00078-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Enzymatic method for the conversion of carbon monoxide from industrial off-gases into formate","authors":"","doi":"10.1038/s44286-024-00070-0","DOIUrl":"10.1038/s44286-024-00070-0","url":null,"abstract":"Decarbonizing the steel industry is crucial but challenging. Now, an enzymatic method is introduced for converting carbon monoxide from industrial off-gases into formate, offering a path towards carbon-neutral steel production. The enzymatic process achieves high selectivity, and operation of a 10-liter-scale reactor with real industrial emissions indicates its scalability and practical applicability.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"338-339"},"PeriodicalIF":0.0,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907150","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}
Jinhee Lee, Suk Min Kim, Byoung Wook Jeon, Ho Won Hwang, Eleni G. Poloniataki, Jingu Kang, Sanghyung Lee, Ho Won Ra, Jonggeol Na, Jeong-Geol Na, Jinwon Lee, Yong Hwan Kim
{"title":"Molar-scale formate production via enzymatic hydration of industrial off-gases","authors":"Jinhee Lee, Suk Min Kim, Byoung Wook Jeon, Ho Won Hwang, Eleni G. Poloniataki, Jingu Kang, Sanghyung Lee, Ho Won Ra, Jonggeol Na, Jeong-Geol Na, Jinwon Lee, Yong Hwan Kim","doi":"10.1038/s44286-024-00063-z","DOIUrl":"10.1038/s44286-024-00063-z","url":null,"abstract":"Decarbonizing the steel industry, a major CO2 emitter, is crucial for achieving carbon neutrality. Escaping the grip of CO combustion methods, a key contributor to CO2 discharge, is a seemingly simple yet formidable challenge on the path to industry-wide net-zero carbon emissions. Here we suggest enzymatic CO hydration (enCOH) inspired by the biological Wood‒Ljungdahl pathway, enabling efficient CO2 fixation. By employing the highly efficient, inhibitor-robust CO dehydrogenase (ChCODH2) and formate dehydrogenase (MeFDH1), we achieved spontaneous enCOH to convert industrial off-gases into formate with 100% selectivity. This process operates seamlessly under mild conditions (room temperature, neutral pH), regardless of the CO/CO2 ratio. Notably, the direct utilization of flue gas without pretreatment yielded various formate salts, including ammonium formate, at concentrations nearing two molar. Operating a 10-liter-scale immobilized enzyme reactor feeding live off-gas at a steel mill resulted in the production of high-purity formate powder after facile purification, thus demonstrating the potential for decarbonizing the steel industry. With the global climate crisis, approaches to capture emissions are critical, with the heavy industry sector being particularly challenging to decarbonize. The authors describe a new enzyme cascade for converting industrial emissions into formate salts as a hydrogen carrier or building block for chemicals.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"354-364"},"PeriodicalIF":0.0,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00063-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"The core of particle technology","authors":"Alessio Lavino","doi":"10.1038/s44286-024-00069-7","DOIUrl":"10.1038/s44286-024-00069-7","url":null,"abstract":"Jennifer Curtis from the University of California Davis talks to Nature Chemical Engineering about her path into particle technology, work in computational simulations of multiphase particle flows and the importance of industrial collaborations in advancing the field.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"330-331"},"PeriodicalIF":0.0,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907164","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}
{"title":"Solvent reorganization model takes the lead","authors":"Ahmad Elgazzar, Haotian Wang","doi":"10.1038/s44286-024-00065-x","DOIUrl":"10.1038/s44286-024-00065-x","url":null,"abstract":"Accurately modeling CO2 electroreduction is key to advancing the technology and understanding its productivity and CO2 utilization trends. Now, Marcus–Hush–Chidsey theory offers accurate predictions of experimental results, leading to further insights beyond reaction kinetics.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"334-335"},"PeriodicalIF":0.0,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907155","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}
Eric W. Lees, Justin C. Bui, Oyinkansola Romiluyi, Alexis T. Bell, Adam Z. Weber
{"title":"Exploring CO2 reduction and crossover in membrane electrode assemblies","authors":"Eric W. Lees, Justin C. Bui, Oyinkansola Romiluyi, Alexis T. Bell, Adam Z. Weber","doi":"10.1038/s44286-024-00062-0","DOIUrl":"10.1038/s44286-024-00062-0","url":null,"abstract":"Electrochemical CO2 reduction (CO2R) using renewable electricity is a key pathway toward synthesizing fuels and chemicals. In this study, multi-physics modeling is used to interpret experimental data obtained for CO2R to CO using Ag catalysts in a membrane electrode assembly. The one-dimensional model is validated using measured CO2 crossover and product formation rates. The kinetics of CO formation are described by Marcus–Hush–Chidsey kinetics, which enables accurate prediction of the experimental data by accounting for the reorganization of the solvent during CO2R. The results show how the performance is dictated by competing phenomena including ion formation and transport, CO2 solubility, and water management. The model shows that increasing the ion-exchange capacity of the membrane and surface area of the catalyst increases CO formation rates by >100 mA cm–2 without negatively impacting CO2 utilization. Here we provide insights into how to manage the trade-off between productivity and CO2 utilization in CO2 electrolyzers. The design of CO2 electrolyzers is complicated by coupled transport and reaction phenomena. Here the authors develop a continuum model incorporating physical phenomena across multiple scales to predict the activity and selectivity of CO2 electrolysis, along with the loss of CO2 due to crossover in membrane electrode assemblies.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":"1 5","pages":"340-353"},"PeriodicalIF":0.0,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00062-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140907148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}