Sven Brückner, Quanchen Feng, Wen Ju, Daniela Galliani, Anna Testolin, Malte Klingenhof, Sebastian Ott, Peter Strasser
{"title":"Design and diagnosis of high-performance CO2-to-CO electrolyzer cells","authors":"Sven Brückner, Quanchen Feng, Wen Ju, Daniela Galliani, Anna Testolin, Malte Klingenhof, Sebastian Ott, Peter Strasser","doi":"10.1038/s44286-024-00035-3","DOIUrl":"10.1038/s44286-024-00035-3","url":null,"abstract":"This work reports the design and diagnostic analysis of a pH-neutral CO2-to-CO zero-gap electrolyzer cell incorporating a nickel–nitrogen-doped carbon catalyst. The cell yields ~100% CO faradaic efficiency at applied current densities of up to 250 mA cm−2 at low cell voltage and 40% total energy efficiency. It features a low stoichiometric CO2 excess, λstoich, of 1.2 that yields a molar CO concentration of ~70%vol in the electrolyzer exit stream at 40% single-pass CO2 conversion, with over 100 h stability. Here we introduce the experimental carbon crossover coefficient (CCC) as a tool for electrolyzer cell diagnostics. The CCC describes the ratio between noncatalytic acid–base CO2 consumption and catalytically generated alkalinity, thereby offering insight into the nature of the prevalent ionic transport and transport mechanisms of undesired CO2 losses. We demonstrate the diagnostic value of the CCC in transport-based cell failure during oscillatory cell flooding between salt precipitation and salt redissolution. The present dynamic cell diagnostics provide practical guidelines toward improved CO2 electrolyzer designs. Optimizing CO2-to-CO electrolyzers is important for developing tandem electrolysis processes. Now an efficient precious metal-free CO2-to-CO electrolyzer cathode design allows operation under a low stoichiometric CO2 excess ratio that yields a molar CO concentration of 70% in the exit stream along with a diagnostic approach to its catalytic and mass transport characteristics.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063888","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":"Bringing biomolecular engineering on board","authors":"","doi":"10.1038/s44286-024-00051-3","DOIUrl":"10.1038/s44286-024-00051-3","url":null,"abstract":"Biomolecular engineering enriches the toolkit of chemical engineers, enabling them to tackle diverse challenges in biotechnology and medicine; we welcome submissions in this space.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00051-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063873","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}
Chang-Xin Zhao, Xi-Yao Li, Han Han, Yuanning Feng, Chun Tang, Xuesong Li, Long Zhang, Charlotte L. Stern, Qiang Zhang, J. Fraser Stoddart
{"title":"Analytical noncovalent electrochemistry for battery engineering","authors":"Chang-Xin Zhao, Xi-Yao Li, Han Han, Yuanning Feng, Chun Tang, Xuesong Li, Long Zhang, Charlotte L. Stern, Qiang Zhang, J. Fraser Stoddart","doi":"10.1038/s44286-024-00038-0","DOIUrl":"10.1038/s44286-024-00038-0","url":null,"abstract":"Despite the fact that noncovalent bonding interactions are ubiquitous, it is primarily those interactions, which are amenable to spectroscopic analysis, that have been well investigated and applied in chemical engineering. New principles and techniques for characterizing noncovalent interactions are required to gain insight into their detailed nature and explore their potential applications. Here we introduce the practice of analytical noncovalent electrochemistry for probing such interactions. The strengths of noncovalent interactions can be determined more accurately by electrochemical means than by relying on spectroscopic measurements. Specifically, electrochemical analyses are capable of recording/identifying minor signals, leading to the discovery of an unexpected 2:1 host–guest complex. Moreover, the proposed technique is capable of probing multiple properties and facilitates the design and screening of active complexes as catalysts. We also demonstrate achieving a high energy density of 495 Wh kg−1 in rechargeable batteries. The analytical procedure provides a fresh perspective for supramolecular science and takes noncovalent chemistry closer to practical applications. Quantifying the strength of noncovalent interactions in supramolecular host–guest systems is key to guiding molecular design for a desired application. Now, a quantitative relationship between noncovalent interactions and electrochemistry is established that provides a new dimension for investigations into noncovalent interactions and enables the control of electrochemical properties in battery engineering.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063867","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":"Generative artificial intelligence in chemical engineering","authors":"Artur M. Schweidtmann","doi":"10.1038/s44286-024-00041-5","DOIUrl":"10.1038/s44286-024-00041-5","url":null,"abstract":"Generative artificial intelligence will transform the way we design and operate chemical processes, argues Artur M. Schweidtmann.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063870","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":"Piloting formic acid production from hydrogenated CO2","authors":"Mo Qiao","doi":"10.1038/s44286-024-00044-2","DOIUrl":"10.1038/s44286-024-00044-2","url":null,"abstract":"","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063874","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":"Sustainability research at a national laboratory","authors":"Thomas Dursch","doi":"10.1038/s44286-024-00042-4","DOIUrl":"10.1038/s44286-024-00042-4","url":null,"abstract":"Researchers Katrina Knauer, Taylor Uekert and Alberta Carpenter, each at different stages of their careers, share perspectives on the national laboratory research ecosystem and how it can inspire transformative work in plastics recycling, sustainable manufacturing and beyond.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063879","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":"Supercharged supramolecular binding constants","authors":"Pall Thordarson","doi":"10.1038/s44286-024-00037-1","DOIUrl":"10.1038/s44286-024-00037-1","url":null,"abstract":"Conventional linearly responsive methods for quantifying host–guest complexation in supramolecular chemistry have a fairly narrow dynamic range. Now, a logarithmically responsive electrochemical method promises to facilitate the measurement of complex equilibria over a larger dynamic range in host–guest systems.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063885","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":"Think feedstocks first","authors":"Katarina Babić","doi":"10.1038/s44286-024-00040-6","DOIUrl":"10.1038/s44286-024-00040-6","url":null,"abstract":"Katarina Babić reflects on the need to account for variability in plastic waste feedstocks when designing plastic upcycling and recycling processes.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063890","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":"A self-driving lab for accelerated catalyst development","authors":"","doi":"10.1038/s44286-024-00043-3","DOIUrl":"10.1038/s44286-024-00043-3","url":null,"abstract":"A self-driving lab, called Fast-Cat, is developed for the rapid, autonomous Pareto-front mapping of homogeneous catalysts in high-pressure, high-temperature gas–liquid reactions. The efficacy of Fast-Cat was demonstrated in performing Pareto-front mappings of phosphorus-based ligands for the hydroformylation of olefins.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063881","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":"Self-sufficient metal–air batteries for autonomous systems","authors":"Shuo Jin, Shifeng Hong, Lynden A. Archer","doi":"10.1038/s44286-024-00039-z","DOIUrl":"10.1038/s44286-024-00039-z","url":null,"abstract":"We explore the challenges and opportunities for electrochemical energy storage technologies that harvest active materials from their surroundings. Progress hinges on advances in chemical engineering science related to membrane design; control of mass transport, reaction kinetics and precipitation at electrified interfaces; and regulation of electrocrystallization of metals through substrate design.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00039-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140063887","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}