Pub Date : 2025-02-21DOI: 10.1016/j.chempr.2025.102485
Jason S. DesVeaux, Katrina M. Knauer
Plastic pollution is a pressing challenge, such that traditional recycling struggles to handle mixed waste. In the March issue of Chem Catalysis, Li et al. introduce a process that co-upcycles two societally important plastics, polyethylene terephthalate (PET) and polyoxymethylene (POM), offering a solution for more complex waste streams.
{"title":"Harnessing plastic depolymerization products to upcycle mixed waste into high-value chemicals","authors":"Jason S. DesVeaux, Katrina M. Knauer","doi":"10.1016/j.chempr.2025.102485","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102485","url":null,"abstract":"Plastic pollution is a pressing challenge, such that traditional recycling struggles to handle mixed waste. In the March issue of <em>Chem Catalysis</em>, Li et al. introduce a process that co-upcycles two societally important plastics, polyethylene terephthalate (PET) and polyoxymethylene (POM), offering a solution for more complex waste streams.","PeriodicalId":268,"journal":{"name":"Chem","volume":"25 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463072","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-20DOI: 10.1016/j.chempr.2025.102458
Ning Han, Xianqiang Xiong, Mohamed Noufal, Bo Weng, Alain R. Puente-Santiago
Heterogenized molecular electrocatalysts offer the potential to convert waste into valuable products, but the effect of molecular dispersion states on catalytic processes is poorly understood. Reporting recently in Nature Catalysis, Baker and co-workers investigate how molecular solvation structure and cation coordination affect the activity and selectivity of electrocatalytic CO2 reduction.
{"title":"Interfacial solvation-structure effects of molecularly dispersed CoPc catalysts on CO2 electrochemical conversion","authors":"Ning Han, Xianqiang Xiong, Mohamed Noufal, Bo Weng, Alain R. Puente-Santiago","doi":"10.1016/j.chempr.2025.102458","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102458","url":null,"abstract":"Heterogenized molecular electrocatalysts offer the potential to convert waste into valuable products, but the effect of molecular dispersion states on catalytic processes is poorly understood. Reporting recently in <em>Nature Catalysis</em>, Baker and co-workers investigate how molecular solvation structure and cation coordination affect the activity and selectivity of electrocatalytic CO<sub>2</sub> reduction.","PeriodicalId":268,"journal":{"name":"Chem","volume":"7 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-20DOI: 10.1016/j.chempr.2025.102438
Leo Padva, Lukas Zimmer, Jemma Gullick, Yongwei Zhao, Vishnu Mini Sasi, Ralf B. Schittenhelm, Colin J. Jackson, Max J. Cryle, Max Crüsemann
Peptide natural products possess a fascinating array of complex structures and diverse biological activities. Central to this is a repertoire of structurally modified amino acid building blocks, which stem from fundamentally different biosynthetic pathways for peptides of non-ribosomal and ribosomal origins. Given these origins, the integration of non-ribosomal and ribosomal peptide biosynthesis has previously been thought implausible. Now, we report how nature has synergized ribosomal and non-ribosomal peptide pathways in the biosynthesis of the rufomycins, exceptionally potent antitubercular antibiotics. In this pathway, a biarylitide-type ribosomal pentapeptide precursor is nitrated by a modified cytochrome P450 biaryl-crosslinking enzyme. The nitrated residue, key for antibiotic activity, is liberated by a dedicated protease before activation and peptide incorporation by the non-ribosomal rufomycin synthetase assembly line. This resolves the enigmatic origins of 3-nitrotyrosine within rufomycin biosynthesis and unveils a novel function for ribosomally synthesized peptides as templates for biosynthesis of modified non-ribosomal peptide building blocks.
{"title":"Ribosomal pentapeptide nitration for non-ribosomal peptide antibiotic precursor biosynthesis","authors":"Leo Padva, Lukas Zimmer, Jemma Gullick, Yongwei Zhao, Vishnu Mini Sasi, Ralf B. Schittenhelm, Colin J. Jackson, Max J. Cryle, Max Crüsemann","doi":"10.1016/j.chempr.2025.102438","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102438","url":null,"abstract":"Peptide natural products possess a fascinating array of complex structures and diverse biological activities. Central to this is a repertoire of structurally modified amino acid building blocks, which stem from fundamentally different biosynthetic pathways for peptides of non-ribosomal and ribosomal origins. Given these origins, the integration of non-ribosomal and ribosomal peptide biosynthesis has previously been thought implausible. Now, we report how nature has synergized ribosomal and non-ribosomal peptide pathways in the biosynthesis of the rufomycins, exceptionally potent antitubercular antibiotics. In this pathway, a biarylitide-type ribosomal pentapeptide precursor is nitrated by a modified cytochrome P450 biaryl-crosslinking enzyme. The nitrated residue, key for antibiotic activity, is liberated by a dedicated protease before activation and peptide incorporation by the non-ribosomal rufomycin synthetase assembly line. This resolves the enigmatic origins of 3-nitrotyrosine within rufomycin biosynthesis and unveils a novel function for ribosomally synthesized peptides as templates for biosynthesis of modified non-ribosomal peptide building blocks.","PeriodicalId":268,"journal":{"name":"Chem","volume":"15 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-18DOI: 10.1016/j.chempr.2025.102433
Zhongtao Feng, Rei Kinjo
In this issue of Chem, Braunschweig et al. report the selective synthesis of an electron-precise tetra(amino)tetraborane featuring a puckered B4 ring. Chemical redox reactions lead to the stable radical anion, dianion, and radical cation. The four charge states of the B4 ring are poised to spark a revolution in boron chemistry.
{"title":"Redox chemistry of cyclotetraborane","authors":"Zhongtao Feng, Rei Kinjo","doi":"10.1016/j.chempr.2025.102433","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102433","url":null,"abstract":"In this issue of <em>Chem</em>, Braunschweig et al. report the selective synthesis of an electron-precise tetra(amino)tetraborane featuring a puckered B<sub>4</sub> ring. Chemical redox reactions lead to the stable radical anion, dianion, and radical cation. The four charge states of the B<sub>4</sub> ring are poised to spark a revolution in boron chemistry.","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435641","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.09.001
Lishan Geng , Jiashen Meng , Xuanpeng Wang , Weidong Wu , Kang Han , Meng Huang , Chunhua Han , Lu Wu , Jinghao Li , Liang Zhou , Liqiang Mai
Conventional hybrid aqueous electrolytes with solvated organic co-solvents encounter sluggish desolvation kinetics, especially under low-temperature conditions, due to the strong binding of organic solvents with Zn2+. Here, we develop a class of hybrid aqueous electrolytes with an organic-solvent-free primary solvation shell, favoring facile desolvation. As demonstrated by 1 M zinc acetate with dimethyl sulfoxide (DMSO) dipolar aprotic solvent, CH3COO− and H2O surround Zn2+, forming Zn2+(CH3COO−)2(H2O)4 clusters. The enhanced hydrogen bonds between solvated CH3COO− and H2O hinder DMSO from replacing solvated H2O. This weak solvation structure facilitates fast charge transfer kinetics and rapid Zn2+ flow through gradient solid electrolyte interphase. At −20°C, stable plating/stripping (5,600 h) and high Zn utilization (51%) are achieved. Furthermore, polyaniline||Zn batteries manifest low polarization (0.05 V), long cycling (8,800 cycles), and high rate. Importantly, this design strategy is generally extended to other hybrid electrolyte systems. This work represents advancements in electrolyte design for aqueous batteries.
{"title":"Organic-solvent-free primary solvation shell for low-temperature aqueous zinc batteries","authors":"Lishan Geng , Jiashen Meng , Xuanpeng Wang , Weidong Wu , Kang Han , Meng Huang , Chunhua Han , Lu Wu , Jinghao Li , Liang Zhou , Liqiang Mai","doi":"10.1016/j.chempr.2024.09.001","DOIUrl":"10.1016/j.chempr.2024.09.001","url":null,"abstract":"<div><div>Conventional hybrid aqueous electrolytes with solvated organic co-solvents encounter sluggish desolvation kinetics, especially under low-temperature conditions, due to the strong binding of organic solvents with Zn<sup>2+</sup>. Here, we develop a class of hybrid aqueous electrolytes with an organic-solvent-free primary solvation shell, favoring facile desolvation. As demonstrated by 1 M zinc acetate with dimethyl sulfoxide (DMSO) dipolar aprotic solvent, CH<sub>3</sub>COO<sup>−</sup> and H<sub>2</sub>O surround Zn<sup>2+</sup>, forming Zn<sup>2+</sup>(CH<sub>3</sub>COO<sup>−</sup>)<sub>2</sub>(H<sub>2</sub>O)<sub>4</sub> clusters. The enhanced hydrogen bonds between solvated CH<sub>3</sub>COO<sup>−</sup> and H<sub>2</sub>O hinder DMSO from replacing solvated H<sub>2</sub>O. This weak solvation structure facilitates fast charge transfer kinetics and rapid Zn<sup>2+</sup> flow through gradient solid electrolyte interphase. At −20°C, stable plating/stripping (5,600 h) and high Zn utilization (51%) are achieved. Furthermore, polyaniline||Zn batteries manifest low polarization (0.05 V), long cycling (8,800 cycles), and high rate. Importantly, this design strategy is generally extended to other hybrid electrolyte systems. This work represents advancements in electrolyte design for aqueous batteries.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102302"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142363118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.10.018
Wentao Song , Xinyue Zhang , Wanrong Li , Bowen Li , Bin Liu
Constructing biotic-abiotic hybrid systems for solar energy conversion receives growing interest owing to their sustainable and eco-friendly approach to producing chemicals. The integration of intracellular biochemical pathways with semiconductor materials offers superior product selectivity and efficient light utilization in solar-driven biocatalysis. However, the complicated multidisciplinary features and limited understanding of extracellular electron transfer at the biological-material interfaces hinder the practical application of biotic-abiotic hybrid systems for converting solar energy. In this perspective, we summarize the fundamental mechanisms of biohybrid systems for solar-to-chemical conversion and highlight ongoing challenges and promising directions for future development. First, a comprehensive overview of biotic-abiotic hybrid systems is introduced together with the mechanism of extracellular electron transfer for chemical production. Then, recent achievements of biohybrid systems for H2 production, CO2 reduction, N2 fixation, and chemical synthesis are discussed in detail. Finally, the current challenges in biotic-abiotic hybrid systems and prospective research directions are explored.
{"title":"Engineering biotic-abiotic hybrid systems for solar-to-chemical conversion","authors":"Wentao Song , Xinyue Zhang , Wanrong Li , Bowen Li , Bin Liu","doi":"10.1016/j.chempr.2024.10.018","DOIUrl":"10.1016/j.chempr.2024.10.018","url":null,"abstract":"<div><div>Constructing biotic-abiotic hybrid systems for solar energy conversion receives growing interest owing to their sustainable and eco-friendly approach to producing chemicals. The integration of intracellular biochemical pathways with semiconductor materials offers superior product selectivity and efficient light utilization in solar-driven biocatalysis. However, the complicated multidisciplinary features and limited understanding of extracellular electron transfer at the biological-material interfaces hinder the practical application of biotic-abiotic hybrid systems for converting solar energy. In this perspective, we summarize the fundamental mechanisms of biohybrid systems for solar-to-chemical conversion and highlight ongoing challenges and promising directions for future development. First, a comprehensive overview of biotic-abiotic hybrid systems is introduced together with the mechanism of extracellular electron transfer for chemical production. Then, recent achievements of biohybrid systems for H<sub>2</sub> production, CO<sub>2</sub> reduction, N<sub>2</sub> fixation, and chemical synthesis are discussed in detail. Finally, the current challenges in biotic-abiotic hybrid systems and prospective research directions are explored.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102351"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2025.102451
Seungheon Lee , Devleena Samanta
Enhancing enzyme functionality while retaining stability has been a long-standing challenge in chemistry. In this issue of Chem, Tan and co-workers present a strategy for encasing enzymes within DNA nanostructures, effectively addressing this limitation. They demonstrate the broad utility of this approach in catalysis, chemical sensing, and tumor therapy.
{"title":"DNA-enzyme nanostructures enhance enzyme stability and functionality","authors":"Seungheon Lee , Devleena Samanta","doi":"10.1016/j.chempr.2025.102451","DOIUrl":"10.1016/j.chempr.2025.102451","url":null,"abstract":"<div><div>Enhancing enzyme functionality while retaining stability has been a long-standing challenge in chemistry. In this issue of <em>Chem</em>, Tan and co-workers present a strategy for encasing enzymes within DNA nanostructures, effectively addressing this limitation. They demonstrate the broad utility of this approach in catalysis, chemical sensing, and tumor therapy.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102451"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077417","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2025.102449
Honghao Cao , Hanyang Shen , Zhijie Chen
Stoddart and co-workers have synthesized two chiral Archimedean polyhedra assembled from small organic molecules via non-covalent interactions. This recent Nature paper has garnered considerable attention from structural chemists and materials scientists.
{"title":"Non-covalent assembly of chiral Archimedean polyhedra","authors":"Honghao Cao , Hanyang Shen , Zhijie Chen","doi":"10.1016/j.chempr.2025.102449","DOIUrl":"10.1016/j.chempr.2025.102449","url":null,"abstract":"<div><div>Stoddart and co-workers have synthesized two chiral Archimedean polyhedra assembled from small organic molecules via non-covalent interactions. This recent <em>Nature</em> paper has garnered considerable attention from structural chemists and materials scientists.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102449"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077418","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.09.017
Jose M. Carceller , Bhumika Jayee , Claire G. Page , Daniel G. Oblinsky , Gustavo Mondragón-Solórzano , Nithin Chintala , Jingzhe Cao , Zayed Alassad , Zheyu Zhang , Nathaniel White , Danny J. Diaz , Andrew D. Ellington , Gregory D. Scholes , Sijia S. Dong , Todd K. Hyster
Photoenzymatic reactions involving flavin-dependent “ene”-reductases (EREDs) rely on protein-templated charge transfer (CT) complexes between the cofactor and substrate for radical initiation. These complexes typically absorb in the blue region of the electromagnetic spectrum. Here, we engineered an ERED to form CT complexes that absorb red light. Mechanistic studies indicate that red-light activity is due to the growth of a red-absorbing shoulder off the previously identified cyan absorption feature. Molecular dynamics simulations, docking, and excited-state calculations suggest that the cyan feature involves a π→π∗ transition on flavin, whereas the red-light absorption is a π→π∗ transition between flavin and the substrate. Differences in the electronic transition are due to changes in the substrate-binding conformation and allosteric tuning of the electronic structure of the cofactor-substrate complex. Microenvironment tuning of the CT complex for red-light activity is observed with other engineered photoenzymatic reactions, highlighting this effect’s generality.
{"title":"Engineering a photoenzyme to use red light","authors":"Jose M. Carceller , Bhumika Jayee , Claire G. Page , Daniel G. Oblinsky , Gustavo Mondragón-Solórzano , Nithin Chintala , Jingzhe Cao , Zayed Alassad , Zheyu Zhang , Nathaniel White , Danny J. Diaz , Andrew D. Ellington , Gregory D. Scholes , Sijia S. Dong , Todd K. Hyster","doi":"10.1016/j.chempr.2024.09.017","DOIUrl":"10.1016/j.chempr.2024.09.017","url":null,"abstract":"<div><div>Photoenzymatic reactions involving flavin-dependent “ene”-reductases (EREDs) rely on protein-templated charge transfer (CT) complexes between the cofactor and substrate for radical initiation. These complexes typically absorb in the blue region of the electromagnetic spectrum. Here, we engineered an ERED to form CT complexes that absorb red light. Mechanistic studies indicate that red-light activity is due to the growth of a red-absorbing shoulder off the previously identified cyan absorption feature. Molecular dynamics simulations, docking, and excited-state calculations suggest that the cyan feature involves a π→π∗ transition on flavin, whereas the red-light absorption is a π→π∗ transition between flavin and the substrate. Differences in the electronic transition are due to changes in the substrate-binding conformation and allosteric tuning of the electronic structure of the cofactor-substrate complex. Microenvironment tuning of the CT complex for red-light activity is observed with other engineered photoenzymatic reactions, highlighting this effect’s generality.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102318"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-13DOI: 10.1016/j.chempr.2024.10.019
Wenhao Ren , Huanlei Zhang , Miyeon Chang , Nanjun Chen , Wenchao Ma , Jun Gu , Meng Lin , Xile Hu
Zero-gap membrane electrode assembly (MEA) CO electrolyzer stands as a promising technology for circular carbon economy. However, current CO electrolyzers are energetically inefficient when operating at ampere-level current densities. Here, by analyzing the performance discrepancies between MEA and flow cells, we identify the depletion of K+ and water at the cathode as the main contributor to the low performance of MEA CO electrolyzers. This is attributed to the unique cathodic interface in catholyte-free MEA, where there is no aqueous electrolyte to maintain the three-phase interface. Through the development of needle-array catalysts with intensified electric fields (EFs) at their tips, we are able to concentrate the limited K+ cations onto the tips of the cathode, while simultaneously facilitating water uptake via electro-osmosis. We construct an MEA CO electrolyzer that achieves a large current density of 2,500 mA cm−2 at a voltage of only 2.7 V.
零间隙膜电极组件（MEA）一氧化碳电解槽是一种很有前途的循环碳经济技术。然而，目前的二氧化碳电解槽在安培级电流密度下运行时能量效率较低。在这里，通过分析 MEA 和流动电池之间的性能差异，我们发现阴极的 K+ 和水耗尽是导致 MEA CO 电解槽性能低下的主要原因。这归因于无阴极电解质 MEA 中独特的阴极界面，即没有水电解质来维持三相界面。通过开发针状阵列催化剂，并在其顶端加强电场 (EF)，我们能够将有限的 K+ 阳离子集中到阴极顶端，同时通过电渗透促进水的吸收。我们构建的 MEA CO 电解槽在电压仅为 2.7 V 的情况下可达到 2,500 mA cm-2 的大电流密度。
{"title":"Field-enhanced CO electroreduction in membrane electrolyzers at a dehydrated interface","authors":"Wenhao Ren , Huanlei Zhang , Miyeon Chang , Nanjun Chen , Wenchao Ma , Jun Gu , Meng Lin , Xile Hu","doi":"10.1016/j.chempr.2024.10.019","DOIUrl":"10.1016/j.chempr.2024.10.019","url":null,"abstract":"<div><div>Zero-gap membrane electrode assembly (MEA) CO electrolyzer stands as a promising technology for circular carbon economy. However, current CO electrolyzers are energetically inefficient when operating at ampere-level current densities. Here, by analyzing the performance discrepancies between MEA and flow cells, we identify the depletion of K<sup>+</sup> and water at the cathode as the main contributor to the low performance of MEA CO electrolyzers. This is attributed to the unique cathodic interface in catholyte-free MEA, where there is no aqueous electrolyte to maintain the three-phase interface. Through the development of needle-array catalysts with intensified electric fields (EFs) at their tips, we are able to concentrate the limited K<sup>+</sup> cations onto the tips of the cathode, while simultaneously facilitating water uptake via electro-osmosis. We construct an MEA CO electrolyzer that achieves a large current density of 2,500 mA cm<sup>−2</sup> at a voltage of only 2.7 V.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102352"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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