Pub Date : 2024-02-08DOI: 10.1038/s44286-023-00018-w
Zhengyuan Li, Peng Wang, Xiang Lyu, Vamsi Krishna Reddy Kondapalli, Shuting Xiang, Juan D. Jimenez, Lu Ma, Takeshi Ito, Tianyu Zhang, Jithu Raj, Yanbo Fang, Yaocai Bai, Jianlin Li, Alexey Serov, Vesselin Shanov, Anatoly I. Frenkel, Sanjaya D. Senanayake, Shize Yang, Thomas P. Senftle, Jingjie Wu
Manipulating the selectivity-determining step in post-C–C coupling is crucial for enhancing C2 product specificity during electrocatalytic CO2 reduction, complementing efforts to boost rate-determining step kinetics. Here we highlight the role of single-site noble metal dopants on Cu surfaces in influencing C–O bond dissociation in an oxygen-bound selectivity-determining intermediate, steering post-C–C coupling toward ethylene versus ethanol. Integrating theoretical and experimental analyses, we demonstrate that the oxygen binding strength of the Cu surface controls the favorability of C–O bond scission, thus tuning the selectivity ratio of ethylene-to-ethanol. The Rh-doped Cu catalyst with optimal oxygen binding energy achieves a Faradaic efficiency toward ethylene of 61.2% and an ethylene-to-ethanol Faradaic efficiency ratio of 4.51 at –0.66 V versus RHE (reversible hydrogen electrode). Integrating control of both rate-determining and selectivity-determining steps further raises ethylene Faradaic efficiency to 68.8% at 1.47 A cm−2 in a tandem electrode. Our insights guide the rational design of Cu-based catalysts for selective CO2 electroreduction to a single C2 product. Steering the selectivity-determining steps is as important as the C–C coupling steps in CO2 electroreduction. Here the authors highlight that single-site noble metal dopants on the Cu surface can influence C–O bond dissociation and direct the post-C–C coupling pathways to ethylene versus ethanol.
{"title":"Directing CO2 electroreduction pathways for selective C2 product formation using single-site doped copper catalysts","authors":"Zhengyuan Li, Peng Wang, Xiang Lyu, Vamsi Krishna Reddy Kondapalli, Shuting Xiang, Juan D. Jimenez, Lu Ma, Takeshi Ito, Tianyu Zhang, Jithu Raj, Yanbo Fang, Yaocai Bai, Jianlin Li, Alexey Serov, Vesselin Shanov, Anatoly I. Frenkel, Sanjaya D. Senanayake, Shize Yang, Thomas P. Senftle, Jingjie Wu","doi":"10.1038/s44286-023-00018-w","DOIUrl":"10.1038/s44286-023-00018-w","url":null,"abstract":"Manipulating the selectivity-determining step in post-C–C coupling is crucial for enhancing C2 product specificity during electrocatalytic CO2 reduction, complementing efforts to boost rate-determining step kinetics. Here we highlight the role of single-site noble metal dopants on Cu surfaces in influencing C–O bond dissociation in an oxygen-bound selectivity-determining intermediate, steering post-C–C coupling toward ethylene versus ethanol. Integrating theoretical and experimental analyses, we demonstrate that the oxygen binding strength of the Cu surface controls the favorability of C–O bond scission, thus tuning the selectivity ratio of ethylene-to-ethanol. The Rh-doped Cu catalyst with optimal oxygen binding energy achieves a Faradaic efficiency toward ethylene of 61.2% and an ethylene-to-ethanol Faradaic efficiency ratio of 4.51 at –0.66 V versus RHE (reversible hydrogen electrode). Integrating control of both rate-determining and selectivity-determining steps further raises ethylene Faradaic efficiency to 68.8% at 1.47 A cm−2 in a tandem electrode. Our insights guide the rational design of Cu-based catalysts for selective CO2 electroreduction to a single C2 product. Steering the selectivity-determining steps is as important as the C–C coupling steps in CO2 electroreduction. Here the authors highlight that single-site noble metal dopants on the Cu surface can influence C–O bond dissociation and direct the post-C–C coupling pathways to ethylene versus ethanol.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00018-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710637","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 : 2024-02-08DOI: 10.1038/s44286-023-00028-8
O. K. Matar
Omar Matar explains how changes in surface tension can cause fluid flow, while navigating a sea of related dimensionless numbers.
奥马尔-马塔尔解释了表面张力的变化如何导致流体流动，同时在相关无量纲数字的海洋中遨游。
{"title":"A soap boat trip on ‘Lake Marangoni’","authors":"O. K. Matar","doi":"10.1038/s44286-023-00028-8","DOIUrl":"10.1038/s44286-023-00028-8","url":null,"abstract":"Omar Matar explains how changes in surface tension can cause fluid flow, while navigating a sea of related dimensionless numbers.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710640","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 : 2024-02-08DOI: 10.1038/s44286-023-00027-9
Ting Wang, Zuankai Wang
Designing liquid devices with liquid pathways that can be reconfigured on-demand is important to many chemical and biological applications. Now, a facile approach enables reconfigurable liquid devices through precisely arranged connected liquid droplets that can be rapidly assembled and disassembled.
{"title":"Reconfiguring liquid devices","authors":"Ting Wang, Zuankai Wang","doi":"10.1038/s44286-023-00027-9","DOIUrl":"10.1038/s44286-023-00027-9","url":null,"abstract":"Designing liquid devices with liquid pathways that can be reconfigured on-demand is important to many chemical and biological applications. Now, a facile approach enables reconfigurable liquid devices through precisely arranged connected liquid droplets that can be rapidly assembled and disassembled.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710632","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 : 2024-02-08DOI: 10.1038/s44286-024-00031-7
Alessio Lavino
{"title":"Cool down and power up","authors":"Alessio Lavino","doi":"10.1038/s44286-024-00031-7","DOIUrl":"10.1038/s44286-024-00031-7","url":null,"abstract":"","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710636","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 : 2024-02-08DOI: 10.1038/s44286-024-00034-4
Systems-level thinking is an important practice, but accounting for system boundary expansion is a complex and timely challenge.
系统层面的思考是一项重要的实践，但对系统边界扩展进行核算是一项复杂而及时的挑战。
{"title":"Drawing the line for process design","authors":"","doi":"10.1038/s44286-024-00034-4","DOIUrl":"10.1038/s44286-024-00034-4","url":null,"abstract":"Systems-level thinking is an important practice, but accounting for system boundary expansion is a complex and timely challenge.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00034-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710646","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 : 2024-02-08DOI: 10.1038/s44286-023-00024-y
Nicola L. Bell, Florian Boser, Andrius Bubliauskas, Dominic R. Willcox, Victor Sandoval Luna, Leroy Cronin
We design a modular programmable inert-atmosphere Schlenkputer (Schlenk-line computer) for the synthesis and manipulation of highly reactive compounds, including those that are air and moisture sensitive or pyrophoric. Here, to do this, we constructed a programmable Schlenk line using the Chemputer architecture for the inertization of glassware that can achieve a vacuum line pressure of 1.5 × 10−3 mbar, and integrated a range of automated Schlenk glassware for the handling, storage and isolation of reactive compounds at sub-ppm levels of O2 and H2O. This has enabled automation of a range of common organometallic reaction types for the synthesis of four highly reactive compounds: [Cp2TiIII(MeCN)2]+, CeIII{N(SiMe3)2}3, B(C6F5)3 and {DippNacNacMgI}2, which are variously sensitive to temperature, pressure, water and oxygen. Automated crystallization, filtration and sublimation are demonstrated, along with analysis using inline nuclear magnetic resonance or reaction sampling for ultraviolet–visible spectroscopy. Finally, we demonstrate low-temperature reactivity down to −90 °C as well as safe handling and quenching of alkali metal reagents using dynamic feedback from an in situ temperature probe. The automated synthesis of highly reactive compounds is challenging. Now a digital automated platform is developed for safer, inert-atmosphere synthesis of air-, moisture-, pressure- and temperature-sensitive compounds from across the periodic table.
{"title":"Autonomous execution of highly reactive chemical transformations in the Schlenkputer","authors":"Nicola L. Bell, Florian Boser, Andrius Bubliauskas, Dominic R. Willcox, Victor Sandoval Luna, Leroy Cronin","doi":"10.1038/s44286-023-00024-y","DOIUrl":"10.1038/s44286-023-00024-y","url":null,"abstract":"We design a modular programmable inert-atmosphere Schlenkputer (Schlenk-line computer) for the synthesis and manipulation of highly reactive compounds, including those that are air and moisture sensitive or pyrophoric. Here, to do this, we constructed a programmable Schlenk line using the Chemputer architecture for the inertization of glassware that can achieve a vacuum line pressure of 1.5 × 10−3 mbar, and integrated a range of automated Schlenk glassware for the handling, storage and isolation of reactive compounds at sub-ppm levels of O2 and H2O. This has enabled automation of a range of common organometallic reaction types for the synthesis of four highly reactive compounds: [Cp2TiIII(MeCN)2]+, CeIII{N(SiMe3)2}3, B(C6F5)3 and {DippNacNacMgI}2, which are variously sensitive to temperature, pressure, water and oxygen. Automated crystallization, filtration and sublimation are demonstrated, along with analysis using inline nuclear magnetic resonance or reaction sampling for ultraviolet–visible spectroscopy. Finally, we demonstrate low-temperature reactivity down to −90 °C as well as safe handling and quenching of alkali metal reagents using dynamic feedback from an in situ temperature probe. The automated synthesis of highly reactive compounds is challenging. Now a digital automated platform is developed for safer, inert-atmosphere synthesis of air-, moisture-, pressure- and temperature-sensitive compounds from across the periodic table.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00024-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710635","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 : 2024-02-08DOI: 10.1038/s44286-023-00019-9
Yuting Xu, Fanglin Che
Directing CO2 electroreduction toward a single C2 product poses challenges because the reaction mechanism is unclear. Now, oxygen affinity is identified as a potential key descriptor to manipulate the selectivity of ethylene versus ethanol.
{"title":"Beyond C–C coupling in CO2 reduction","authors":"Yuting Xu, Fanglin Che","doi":"10.1038/s44286-023-00019-9","DOIUrl":"10.1038/s44286-023-00019-9","url":null,"abstract":"Directing CO2 electroreduction toward a single C2 product poses challenges because the reaction mechanism is unclear. Now, oxygen affinity is identified as a potential key descriptor to manipulate the selectivity of ethylene versus ethanol.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710643","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 : 2024-02-08DOI: 10.1038/s44286-024-00030-8
Mo Qiao
Kai Qiao, a senior engineer at SINOPEC Dalian Research Institute of Petroleum and Petrochemicals Co., Ltd, and a visiting professor in the Department of Chemical Engineering at Dalian University of Technology, talks to Nature Chemical Engineering about his career as a chemical engineer working on biomass-derived chemical production.
{"title":"From laboratory research to industrial engineering","authors":"Mo Qiao","doi":"10.1038/s44286-024-00030-8","DOIUrl":"10.1038/s44286-024-00030-8","url":null,"abstract":"Kai Qiao, a senior engineer at SINOPEC Dalian Research Institute of Petroleum and Petrochemicals Co., Ltd, and a visiting professor in the Department of Chemical Engineering at Dalian University of Technology, talks to Nature Chemical Engineering about his career as a chemical engineer working on biomass-derived chemical production.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710655","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 : 2024-02-08DOI: 10.1038/s44286-023-00021-1
Zhongyun Liu, Yuhe Cao, William J. Koros
Polyimide-derived carbon molecular sieve (CMS) membranes mark an important step for various current, key energy-intensive separations. The excellent separation performance combined with economical scalability make CMS membranes ready to enable energy-transition-focused gas separations.
{"title":"Polyimide-derived carbon molecule sieve membranes for gas separations","authors":"Zhongyun Liu, Yuhe Cao, William J. Koros","doi":"10.1038/s44286-023-00021-1","DOIUrl":"10.1038/s44286-023-00021-1","url":null,"abstract":"Polyimide-derived carbon molecular sieve (CMS) membranes mark an important step for various current, key energy-intensive separations. The excellent separation performance combined with economical scalability make CMS membranes ready to enable energy-transition-focused gas separations.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00021-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710634","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 : 2024-02-08DOI: 10.1038/s44286-024-00029-1
Jinlong Gong, David C. Shallcross, Yan Jiao, Venkat Venkatasubramanian, Richard Davis, Christopher G. Arges
We asked a group of chemical engineering educators with a broad set of research interests to reimagine the undergraduate curriculum, highlighting both current strengths and areas of needed development.
{"title":"Rethinking chemical engineering education","authors":"Jinlong Gong, David C. Shallcross, Yan Jiao, Venkat Venkatasubramanian, Richard Davis, Christopher G. Arges","doi":"10.1038/s44286-024-00029-1","DOIUrl":"10.1038/s44286-024-00029-1","url":null,"abstract":"We asked a group of chemical engineering educators with a broad set of research interests to reimagine the undergraduate curriculum, highlighting both current strengths and areas of needed development.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-024-00029-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710644","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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