Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00035-3
Sven Brückner, Quanchen Feng, Wen Ju, Daniela Galliani, Anna Testolin, Malte Klingenhof, Sebastian Ott, Peter Strasser
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.
本研究报告介绍了一种 pH 值中性 CO2 到 CO 零间隙电解槽的设计和诊断分析，该电解槽采用了掺杂镍氮的碳催化剂。该电池在低电压和高达 250 mA cm-2 的应用电流密度下可产生约 100% 的 CO 远电解效率和 40% 的总能效。它的特点是二氧化碳的低化学计量过量（λstoich）为 1.2，在单程二氧化碳转化率为 40% 时，电解槽出口流中的二氧化碳摩尔浓度约为 70%vol，稳定性超过 100 小时。在此，我们介绍实验性碳交叉系数（CCC），作为电解槽诊断的工具。CCC 描述了非催化酸碱 CO2 消耗量与催化产生的碱度之间的比率，从而提供了对普遍存在的离子传输性质和不希望的 CO2 损失的传输机制的深入了解。在盐沉淀和盐再溶解之间的振荡细胞淹没过程中，我们展示了 CCC 在基于传输的细胞失效方面的诊断价值。目前的电池动态诊断为改进二氧化碳电解槽设计提供了实用指南。优化 CO2 到 CO 电解槽对于开发串联电解工艺非常重要。现在，一种高效的无贵金属 CO2 转 CO 电解槽阴极设计可在低化学计量 CO2 过剩率下运行，出口流中的 CO 摩尔浓度为 70%，同时还可对其催化和质量传输特性进行诊断。
{"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":"1 3","pages":"229-239"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00051-3
Biomolecular engineering enriches the toolkit of chemical engineers, enabling them to tackle diverse challenges in biotechnology and medicine; we welcome submissions in this space.
{"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":"1 3","pages":"191-192"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00038-0
Chang-Xin Zhao, Xi-Yao Li, Han Han, Yuanning Feng, Chun Tang, Xuesong Li, Long Zhang, Charlotte L. Stern, Qiang Zhang, J. Fraser Stoddart
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.
{"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":"1 3","pages":"251-260"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00041-5
Artur M. Schweidtmann
Generative artificial intelligence will transform the way we design and operate chemical processes, argues Artur M. Schweidtmann.
阿图尔-M.-施魏德曼（Artur M. Schweidtmann）认为，生成式人工智能将改变我们设计和操作化学过程的方式。
{"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":"1 3","pages":"193-193"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00044-2
Mo Qiao
{"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":"1 3","pages":"205-205"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00042-4
Thomas Dursch
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.
{"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":"1 3","pages":"198-200"},"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}
Pub Date : 2024-03-08DOI: 10.1038/s44286-024-00037-1
Pall Thordarson
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.
{"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":"1 3","pages":"203-204"},"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":"1 3","pages":"261-261"},"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}
Pub Date : 2024-03-06DOI: 10.1038/s44286-024-00043-3
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.
{"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":"1 3","pages":"206-207"},"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}
Pub Date : 2024-03-06DOI: 10.1038/s44286-024-00039-z
Shuo Jin, Shifeng Hong, Lynden A. Archer
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.
{"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":"1 3","pages":"194-197"},"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}
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