Pub Date : 2024-02-08DOI: 10.1038/s44286-023-00020-2
Samay Garg, Zhenhua Xie, Jingguang G. Chen
Carbon dioxide (CO2) valorization is a promising pathway for mitigating greenhouse gas emissions from the chemical sector and reducing the reliance of chemical manufacturing on fossil fuel feedstocks. This Perspective discusses tandem catalytic paradigms for sustainable CO2 conversion that have potential advantages over processes using single-functional catalysts. Recent progress is discussed for tandem catalysis using multifunctional catalysts in a single reactor, as well as tandem reactors involving multiple catalysts. Opportunities for further developing these tandem strategies for thermochemical and electrochemical processes in various configurations are presented to encourage research in this burgeoning field. Tandem catalysis and tandem reactors provide unique opportunities for sustainably converting CO2 into valuable products that are not accessible by traditional catalytic processes. This Perspective discusses progress in and opportunities for developing tandem catalytic process that involve various combinations of thermocatalysis, electrocatalysis, photocatalysis, plasma catalysis and biocatalysis.
{"title":"Tandem reactors and reactions for CO2 conversion","authors":"Samay Garg, Zhenhua Xie, Jingguang G. Chen","doi":"10.1038/s44286-023-00020-2","DOIUrl":"10.1038/s44286-023-00020-2","url":null,"abstract":"Carbon dioxide (CO2) valorization is a promising pathway for mitigating greenhouse gas emissions from the chemical sector and reducing the reliance of chemical manufacturing on fossil fuel feedstocks. This Perspective discusses tandem catalytic paradigms for sustainable CO2 conversion that have potential advantages over processes using single-functional catalysts. Recent progress is discussed for tandem catalysis using multifunctional catalysts in a single reactor, as well as tandem reactors involving multiple catalysts. Opportunities for further developing these tandem strategies for thermochemical and electrochemical processes in various configurations are presented to encourage research in this burgeoning field. Tandem catalysis and tandem reactors provide unique opportunities for sustainably converting CO2 into valuable products that are not accessible by traditional catalytic processes. This Perspective discusses progress in and opportunities for developing tandem catalytic process that involve various combinations of thermocatalysis, electrocatalysis, photocatalysis, plasma catalysis and biocatalysis.","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/s44286-023-00020-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710654","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}
The rapid accumulation of end-of-life electronics around the world has a disastrous impact on the environment because much of this otherwise valuable resource goes to landfills. Electronic waste (e-waste) contains significant amounts of precious metals, in the case of gold (Au), far in excess of those found in natural minerals. Recovering these metals from e-waste provides a potential sustainable path, but current recycling routes are not yet up to the task. Here we show a photocatalytic process that allows for selective, efficient and scalable extraction of Au from different forms of e-waste. The dissolution takes no more than 12 h, and further reducing the leachate yields Au metal with purity up to 99.0%. In a large-scale setting, our system can treat 10 kg of e-waste for a single batch and recover 8.82 g of Au. By advancing precious metal recycling to a level closer to practical implementation, this work will contribute to a more sustainable future for electronics. Selective recovery of gold from electronic waste using mild reagents is a challenge. Now a photocatalytic technology is reported to enable highly selective gold dissolution through solvent pH adjustment. This process is scaled up to allow for the efficient handling of a single batch of 10 kg of electronic waste.
{"title":"Scalable and selective gold recovery from end-of-life electronics","authors":"Hengjun Shang, Yao Chen, Shuhui Guan, Yue Wang, Jiazhen Cao, Xinru Wang, Hexing Li, Zhenfeng Bian","doi":"10.1038/s44286-023-00026-w","DOIUrl":"10.1038/s44286-023-00026-w","url":null,"abstract":"The rapid accumulation of end-of-life electronics around the world has a disastrous impact on the environment because much of this otherwise valuable resource goes to landfills. Electronic waste (e-waste) contains significant amounts of precious metals, in the case of gold (Au), far in excess of those found in natural minerals. Recovering these metals from e-waste provides a potential sustainable path, but current recycling routes are not yet up to the task. Here we show a photocatalytic process that allows for selective, efficient and scalable extraction of Au from different forms of e-waste. The dissolution takes no more than 12 h, and further reducing the leachate yields Au metal with purity up to 99.0%. In a large-scale setting, our system can treat 10 kg of e-waste for a single batch and recover 8.82 g of Au. By advancing precious metal recycling to a level closer to practical implementation, this work will contribute to a more sustainable future for electronics. Selective recovery of gold from electronic waste using mild reagents is a challenge. Now a photocatalytic technology is reported to enable highly selective gold dissolution through solvent pH adjustment. This process is scaled up to allow for the efficient handling of a single batch of 10 kg of electronic waste.","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":"139710657","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 : 2024-02-05DOI: 10.1038/s44286-023-00023-z
Yi Zeng, Sen Li, Zhejun Chong, Yanfang Niu, Keliang Liu, Jiankang Zhou, Zhenzhu He, Junning Zhang, Jing Zhao, Shuang Ding, Xin Du, Zhongze Gu
Liquids are widely applied in the construction of various functional devices due to their abilities to flow, dissolve, deform and phase separate; however, the fabrication of liquid-based devices can be costly and lack reconfigurability due to the need for predesigned solid enclosing walls. Herein we report a strategy to generate and manipulate functional liquid devices by assembling and disassembling different types of liquid droplets like toy building blocks; we also uncover the underlying mechanisms. Multiphase liquid devices with diverse compositions and geometries can be quickly constructed and reconfigured in a pillared substrate, enabling the ability to freely structure liquids and precisely program liquid–liquid interfaces. The applications in fluidic devices, microreactors and their combinations are demonstrated. Building liquid devices from solid enclosing walls can be costly and lack reconfigurability. Now the rapid construction and reconfiguration of diverse liquid devices is demonstrated through assembly and disassembly of droplet arrays in a pillared substrate.
{"title":"Reconfigurable liquid devices from liquid building blocks","authors":"Yi Zeng, Sen Li, Zhejun Chong, Yanfang Niu, Keliang Liu, Jiankang Zhou, Zhenzhu He, Junning Zhang, Jing Zhao, Shuang Ding, Xin Du, Zhongze Gu","doi":"10.1038/s44286-023-00023-z","DOIUrl":"10.1038/s44286-023-00023-z","url":null,"abstract":"Liquids are widely applied in the construction of various functional devices due to their abilities to flow, dissolve, deform and phase separate; however, the fabrication of liquid-based devices can be costly and lack reconfigurability due to the need for predesigned solid enclosing walls. Herein we report a strategy to generate and manipulate functional liquid devices by assembling and disassembling different types of liquid droplets like toy building blocks; we also uncover the underlying mechanisms. Multiphase liquid devices with diverse compositions and geometries can be quickly constructed and reconfigured in a pillared substrate, enabling the ability to freely structure liquids and precisely program liquid–liquid interfaces. The applications in fluidic devices, microreactors and their combinations are demonstrated. Building liquid devices from solid enclosing walls can be costly and lack reconfigurability. Now the rapid construction and reconfiguration of diverse liquid devices is demonstrated through assembly and disassembly of droplet arrays in a pillared substrate.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00023-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139710650","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 : 2024-01-11DOI: 10.1038/s44286-023-00016-y
Robert Langer, Nicholas A. Peppas
Chemical engineering principles will continue to help scientists design and optimize new medical devices, treatments and modalities. This Comment reflects on historical developments and potential opportunities in medicine for chemical engineering.
{"title":"A bright future in medicine for chemical engineering","authors":"Robert Langer, Nicholas A. Peppas","doi":"10.1038/s44286-023-00016-y","DOIUrl":"10.1038/s44286-023-00016-y","url":null,"abstract":"Chemical engineering principles will continue to help scientists design and optimize new medical devices, treatments and modalities. This Comment reflects on historical developments and potential opportunities in medicine for chemical engineering.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00016-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431094","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 : 2024-01-11DOI: 10.1038/s44286-023-00004-2
Heng Zeng, Xiao-Jing Xie, Ting Wang, Mo Xie, Ying Wang, Rong-Jia Wei, Weigang Lu, Dan Li
Molecular sieving adsorbents can offer maximum adsorption selectivity with respect to molecular sizes, yet it is still challenging to discriminate middle-sized molecules from a mixture of three or more components. Here we report a metal–organic framework (JNU-3a) with dynamic molecular pockets along one-dimensional channels, enabling the one-step removal of ethylene (C2H4) from mixtures with C2–C4 alkynes in a single adsorption step regardless of their molecular sizes. Laboratory-scale column breakthrough experiments on 1.4 g of JNU-3a reveal that the three alkynes break through the column at almost the same but a later time, resulting in the high-purity separation of C2H4 (≥99.9995%) from a mixture with C2–C4 alkynes in a single adsorption operation. We further demonstrate pilot-scale column breakthrough on 107 g of JNU-3a and the collection of C2H4 in a gas cylinder. In particular, 30 continuous runs for a C2H2/C3H4/1-C4H6/C2H4 mixture (1:1:1:97) afford an average of 76.1 g per cycle of high-purity C2H4. Overall, JNU-3a may have great potential for industrial C2H4 purification via the concurrent removal of C2–C4 alkynes. It is challenging to separate middle-sized molecules from complex mixtures using traditional molecular sieves. Here a metal–organic framework has been developed with dynamic molecular pockets that can adjust and accommodate alkynes preferentially, realizing efficient production of high-purity ethylene from its mixtures with alkynes regardless of their molecular sizes.
{"title":"Dynamic molecular pockets on one-dimensional channels for splitting ethylene from C2–C4 alkynes","authors":"Heng Zeng, Xiao-Jing Xie, Ting Wang, Mo Xie, Ying Wang, Rong-Jia Wei, Weigang Lu, Dan Li","doi":"10.1038/s44286-023-00004-2","DOIUrl":"10.1038/s44286-023-00004-2","url":null,"abstract":"Molecular sieving adsorbents can offer maximum adsorption selectivity with respect to molecular sizes, yet it is still challenging to discriminate middle-sized molecules from a mixture of three or more components. Here we report a metal–organic framework (JNU-3a) with dynamic molecular pockets along one-dimensional channels, enabling the one-step removal of ethylene (C2H4) from mixtures with C2–C4 alkynes in a single adsorption step regardless of their molecular sizes. Laboratory-scale column breakthrough experiments on 1.4 g of JNU-3a reveal that the three alkynes break through the column at almost the same but a later time, resulting in the high-purity separation of C2H4 (≥99.9995%) from a mixture with C2–C4 alkynes in a single adsorption operation. We further demonstrate pilot-scale column breakthrough on 107 g of JNU-3a and the collection of C2H4 in a gas cylinder. In particular, 30 continuous runs for a C2H2/C3H4/1-C4H6/C2H4 mixture (1:1:1:97) afford an average of 76.1 g per cycle of high-purity C2H4. Overall, JNU-3a may have great potential for industrial C2H4 purification via the concurrent removal of C2–C4 alkynes. It is challenging to separate middle-sized molecules from complex mixtures using traditional molecular sieves. Here a metal–organic framework has been developed with dynamic molecular pockets that can adjust and accommodate alkynes preferentially, realizing efficient production of high-purity ethylene from its mixtures with alkynes regardless of their molecular sizes.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00004-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431080","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 : 2024-01-11DOI: 10.1038/s44286-023-00012-2
Elena Subbotina, Joseph S. M. Samec
Lignin contains both C–O and C–C bonds, where C–C bonds are highly resistant to cleavage. Now, a bifunctional catalyst enables the cleavage of the challenging C–C bonds in lignin to produce biofuels.
{"title":"Cleavage of challenging chemical bonds in lignin enables biofuels","authors":"Elena Subbotina, Joseph S. M. Samec","doi":"10.1038/s44286-023-00012-2","DOIUrl":"10.1038/s44286-023-00012-2","url":null,"abstract":"Lignin contains both C–O and C–C bonds, where C–C bonds are highly resistant to cleavage. Now, a bifunctional catalyst enables the cleavage of the challenging C–C bonds in lignin to produce biofuels.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00012-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431086","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 : 2024-01-11DOI: 10.1038/s44286-023-00001-5
Chaoyu Yang, Yunru Yu, Luoran Shang, Yuanjin Zhao
Directional liquid transport is important in both fundamental studies and industrial applications. Most existing strategies rely on the use of predesigned surfaces with sophisticated microstructures that limit the versatility and universality of the liquid transport. Here we present a platform for liquid transport based on flexible microfluidic-derived fibers with hemline-shaped cross-sections. These microfibers have periodic parallel microcavities along the axial direction, with sharp edges and wedge corners that enable unilateral pinning and capillary rise of liquids. This structure enables directional liquid transport along hydrophilic substrates with the use of a single fiber. Alternatively, a pair of fibers enables directional liquid transport along hydrophobic substrates or even without any additional substrate; the directional transport behavior applies to a wide range of liquids. We demonstrate the use of these fibers in open microfluidics, water extraction and liquid transport along arbitrary three-dimensional paths. Our platform provides a facile and universal solution for directional liquid transport in a range of different scenarios. A flexible hemline-shaped microfiber featuring periodic parallel microcavities with sharp edges and wedges was developed using microfluidics to achieve unidirectional liquid transport along arbitrary pathways.
{"title":"Flexible hemline-shaped microfibers for liquid transport","authors":"Chaoyu Yang, Yunru Yu, Luoran Shang, Yuanjin Zhao","doi":"10.1038/s44286-023-00001-5","DOIUrl":"10.1038/s44286-023-00001-5","url":null,"abstract":"Directional liquid transport is important in both fundamental studies and industrial applications. Most existing strategies rely on the use of predesigned surfaces with sophisticated microstructures that limit the versatility and universality of the liquid transport. Here we present a platform for liquid transport based on flexible microfluidic-derived fibers with hemline-shaped cross-sections. These microfibers have periodic parallel microcavities along the axial direction, with sharp edges and wedge corners that enable unilateral pinning and capillary rise of liquids. This structure enables directional liquid transport along hydrophilic substrates with the use of a single fiber. Alternatively, a pair of fibers enables directional liquid transport along hydrophobic substrates or even without any additional substrate; the directional transport behavior applies to a wide range of liquids. We demonstrate the use of these fibers in open microfluidics, water extraction and liquid transport along arbitrary three-dimensional paths. Our platform provides a facile and universal solution for directional liquid transport in a range of different scenarios. A flexible hemline-shaped microfiber featuring periodic parallel microcavities with sharp edges and wedges was developed using microfluidics to achieve unidirectional liquid transport along arbitrary pathways.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00001-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431107","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 : 2024-01-11DOI: 10.1038/s44286-023-00003-3
Michael Massen-Hane, Kyle M. Diederichsen, T. Alan Hatton
With ever-increasing atmospheric carbon dioxide concentrations and commitments to limit global temperatures to less than 1.5 °C above pre-industrial levels, the need for versatile, low-cost carbon dioxide capture technologies is paramount. Electrochemically mediated carbon dioxide separation systems promise low energetics, modular scalability and ease of implementation, with direct integration to renewable energy for net-negative carbon dioxide operations. For these systems to be cost-competitive, key factors around their operation, stability and scaling need to be addressed. Energy penalties associated with redox-active species transport, gas transport and bubble formation limit the volumetric productivity and scaling potential due to their cost and footprint. Here we highlight the importance of engineering approaches towards enhancing the performance of redox-active electrochemically mediated carbon dioxide capture systems to enable their widespread implementation. This Perspective discusses electrochemically mediated carbon dioxide capture systems, which can offer lower energetics than standard thermal methods, with modular scalability. New integrated configurations can further reduce costs and improve unit productivity, while further engineering of existing cell designs will enable more rapid implementation.
{"title":"Engineering redox-active electrochemically mediated carbon dioxide capture systems","authors":"Michael Massen-Hane, Kyle M. Diederichsen, T. Alan Hatton","doi":"10.1038/s44286-023-00003-3","DOIUrl":"10.1038/s44286-023-00003-3","url":null,"abstract":"With ever-increasing atmospheric carbon dioxide concentrations and commitments to limit global temperatures to less than 1.5 °C above pre-industrial levels, the need for versatile, low-cost carbon dioxide capture technologies is paramount. Electrochemically mediated carbon dioxide separation systems promise low energetics, modular scalability and ease of implementation, with direct integration to renewable energy for net-negative carbon dioxide operations. For these systems to be cost-competitive, key factors around their operation, stability and scaling need to be addressed. Energy penalties associated with redox-active species transport, gas transport and bubble formation limit the volumetric productivity and scaling potential due to their cost and footprint. Here we highlight the importance of engineering approaches towards enhancing the performance of redox-active electrochemically mediated carbon dioxide capture systems to enable their widespread implementation. This Perspective discusses electrochemically mediated carbon dioxide capture systems, which can offer lower energetics than standard thermal methods, with modular scalability. New integrated configurations can further reduce costs and improve unit productivity, while further engineering of existing cell designs will enable more rapid implementation.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00003-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431131","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 : 2024-01-11DOI: 10.1038/s44286-023-00006-0
Zhicheng Luo, Chong Liu, Alexandra Radu, Davey F. de Waard, Yun Wang, Jean T. Behaghel de Bueren, Panos D. Kouris, Michael D. Boot, Jun Xiao, Huiyan Zhang, Rui Xiao, Jeremy S. Luterbacher, Emiel J. M. Hensen
Carbon–carbon bonds, ubiquitous in lignin, limit monomer yields from current depolymerization strategies, which mainly target C–O bonds. Selective cleavage of the inherently inert σ-type C–C bonds without pre-functionalization remains challenging. Here we report the breaking of C–C bonds in lignin obtained upon initial disruption of labile C–O bonds, achieving monocyclic hydrocarbon yields up to an order of magnitude higher than previously reported. The use of a Pt (de)hydrogenation function leads to olefinic groups close to recalcitrant C–C bonds, which can undergo β-scission over zeolitic Brønsted acid sites. After confirming that this approach can selectively cleave common C–C linkages (5–5′, β–1′, β–5′ and β–β′) in lignin skeletons, we demonstrate its utility in the valorization of various representative lignins. A techno-economic analysis shows the promise of our method for producing gasoline- and jet-range cycloalkanes and aromatics, while a life-cycle assessment confirms its potential for CO2-neutral fuel production. Carbon–carbon bonds are ubiquitous in lignin, limiting monomer yields from current depolymerization strategies mainly targeting C–O bonds. Now, a bifunctional hydrocracking approach uses a Pt/zeolite catalyst to break C–C bonds in lignin waste, achieving monocyclic hydrocarbon yields up to 54 C%.
{"title":"Carbon–carbon bond cleavage for a lignin refinery","authors":"Zhicheng Luo, Chong Liu, Alexandra Radu, Davey F. de Waard, Yun Wang, Jean T. Behaghel de Bueren, Panos D. Kouris, Michael D. Boot, Jun Xiao, Huiyan Zhang, Rui Xiao, Jeremy S. Luterbacher, Emiel J. M. Hensen","doi":"10.1038/s44286-023-00006-0","DOIUrl":"10.1038/s44286-023-00006-0","url":null,"abstract":"Carbon–carbon bonds, ubiquitous in lignin, limit monomer yields from current depolymerization strategies, which mainly target C–O bonds. Selective cleavage of the inherently inert σ-type C–C bonds without pre-functionalization remains challenging. Here we report the breaking of C–C bonds in lignin obtained upon initial disruption of labile C–O bonds, achieving monocyclic hydrocarbon yields up to an order of magnitude higher than previously reported. The use of a Pt (de)hydrogenation function leads to olefinic groups close to recalcitrant C–C bonds, which can undergo β-scission over zeolitic Brønsted acid sites. After confirming that this approach can selectively cleave common C–C linkages (5–5′, β–1′, β–5′ and β–β′) in lignin skeletons, we demonstrate its utility in the valorization of various representative lignins. A techno-economic analysis shows the promise of our method for producing gasoline- and jet-range cycloalkanes and aromatics, while a life-cycle assessment confirms its potential for CO2-neutral fuel production. Carbon–carbon bonds are ubiquitous in lignin, limiting monomer yields from current depolymerization strategies mainly targeting C–O bonds. Now, a bifunctional hydrocracking approach uses a Pt/zeolite catalyst to break C–C bonds in lignin waste, achieving monocyclic hydrocarbon yields up to 54 C%.","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00006-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431087","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 : 2024-01-11DOI: 10.1038/s44286-023-00009-x
Justin C. Bui, Eric W. Lees, Daniela H. Marin, T. Nathan Stovall, Lihaokun Chen, Ahmet Kusoglu, Adam C. Nielander, Thomas F. Jaramillo, Shannon W. Boettcher, Alexis T. Bell, Adam Z. Weber
Bipolar membranes (BPMs) enable control of ion concentrations and fluxes in electrochemical cells suitable for a wide range of applications. Here we present the multi-scale physics of BPMs in an electrochemical engineering context and articulate design principles to drive the development of advanced BPMs. The chemistry, structure, and physics of BPMs are illustrated and related to the thermodynamics, transport phenomena, and chemical kinetics that dictate ion and species fluxes and selectivity. These interactions give rise to emergent structure–property–performance relationships that yield design criteria for BPMs that achieve high permselectivity, durability, and voltaic efficiency. The resulting performance trade-offs for BPMs are presented in the context of emerging applications in energy conversion or storage, and environmental remediation. By connecting the fundamental physical phenomena in BPMs to device-level performance and engineering, we aim to facilitate the development of next-generation BPMs for sustainable electrochemical processes. Bipolar ion-exchange membranes are a class of charged polymers that enable precise control of ionic fluxes and local pH, making them potentially valuable for many energy and environmental applications. This Review focuses on the fundamental physics underpinning their operation across multiple scales, from nanomorphology to integration within devices such as in bipolar-membrane electrodialysis (BPM-ED).
{"title":"Multi-scale physics of bipolar membranes in electrochemical processes","authors":"Justin C. Bui, Eric W. Lees, Daniela H. Marin, T. Nathan Stovall, Lihaokun Chen, Ahmet Kusoglu, Adam C. Nielander, Thomas F. Jaramillo, Shannon W. Boettcher, Alexis T. Bell, Adam Z. Weber","doi":"10.1038/s44286-023-00009-x","DOIUrl":"10.1038/s44286-023-00009-x","url":null,"abstract":"Bipolar membranes (BPMs) enable control of ion concentrations and fluxes in electrochemical cells suitable for a wide range of applications. Here we present the multi-scale physics of BPMs in an electrochemical engineering context and articulate design principles to drive the development of advanced BPMs. The chemistry, structure, and physics of BPMs are illustrated and related to the thermodynamics, transport phenomena, and chemical kinetics that dictate ion and species fluxes and selectivity. These interactions give rise to emergent structure–property–performance relationships that yield design criteria for BPMs that achieve high permselectivity, durability, and voltaic efficiency. The resulting performance trade-offs for BPMs are presented in the context of emerging applications in energy conversion or storage, and environmental remediation. By connecting the fundamental physical phenomena in BPMs to device-level performance and engineering, we aim to facilitate the development of next-generation BPMs for sustainable electrochemical processes. Bipolar ion-exchange membranes are a class of charged polymers that enable precise control of ionic fluxes and local pH, making them potentially valuable for many energy and environmental applications. This Review focuses on the fundamental physics underpinning their operation across multiple scales, from nanomorphology to integration within devices such as in bipolar-membrane electrodialysis (BPM-ED).","PeriodicalId":501699,"journal":{"name":"Nature Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44286-023-00009-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139431133","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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