Pub Date : 2025-04-23DOI: 10.1016/j.chempr.2025.102553
Scot M. Sutton, Sunil Pulletikurti, Huacan Lin, Ramanarayanan Krishnamurthy, Charles L. Liotta
The aldol reactions of formaldehyde is the essence of the formose reaction, considered the leading prebiotic pathway for accessing sugars on the early Earth. However, the formose reaction produces an intractable mixture, and efforts to tame the reaction to selectively and efficiently form aldose sugars have been unsuccessful. We have undertaken an NMR-mechanistic study of the aldol reactions of excess formaldehyde with glycolaldehyde, dihydroxyacetone, erythrulose, and erythrose under mild conditions and show that the reaction pathway is dominated by the formation linear ketoses and eventual accumulation of branched ketoses. Formation of C4 and higher aldo-sugars were not observed, implying that neither carbonyl migrations nor retroaldol reactions are occurring. Our results suggest that (1) controlling the aldol reaction of formaldehyde to selectively produce linear aldoses appears unfeasible; and (2) the concept of the formose reaction as a prebiotic source of ribose on early Earth needs serious reconsideration, and other models/options should be explored.
{"title":"Abiotic aldol reactions of formaldehyde with ketoses and aldoses—Implications for the prebiotic synthesis of sugars by the formose reaction","authors":"Scot M. Sutton, Sunil Pulletikurti, Huacan Lin, Ramanarayanan Krishnamurthy, Charles L. Liotta","doi":"10.1016/j.chempr.2025.102553","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102553","url":null,"abstract":"The aldol reactions of formaldehyde is the essence of the formose reaction, considered the leading prebiotic pathway for accessing sugars on the early Earth. However, the formose reaction produces an intractable mixture, and efforts to tame the reaction to selectively and efficiently form aldose sugars have been unsuccessful. We have undertaken an NMR-mechanistic study of the aldol reactions of excess formaldehyde with glycolaldehyde, dihydroxyacetone, erythrulose, and erythrose under mild conditions and show that the reaction pathway is dominated by the formation linear ketoses and eventual accumulation of branched ketoses. Formation of C4 and higher aldo-sugars were not observed, implying that neither carbonyl migrations nor retroaldol reactions are occurring. Our results suggest that (1) controlling the aldol reaction of formaldehyde to selectively produce linear aldoses appears unfeasible; and (2) the concept of the formose reaction as a prebiotic source of ribose on early Earth needs serious reconsideration, and other models/options should be explored.","PeriodicalId":268,"journal":{"name":"Chem","volume":"51 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862586","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 : 2025-04-21DOI: 10.1016/j.chempr.2025.102550
Ke Liu, David Egea-Arrebola, Ruchuta Ardkhean, Laura Cunningham, Kirsten E. Christensen, Robert S. Paton, Stephen P. Fletcher
Chiral non-racemic allylic species are key building blocks for many carbon-containing molecules, including pharmaceuticals and polymers. Metal-catalyzed asymmetric additions of nucleophiles to allylic species undergo different pathways depending on the metal and nucleophile combination, hindering the development of useful addition reactions with aromatic nucleophiles. We report an asymmetric cross-coupling method between aryl boronic acids and linear allylic phosphates to give branched allylic products. This Suzuki-type reaction overcomes the “memory effect” in Rh catalysis, enabling an overall SN2′ transformation by rate-determining reductive elimination and forming a new stereogenic center adjacent to a terminal vinyl moiety. The method tolerates preexisting stereogenic centers, allowing for synthetic strategies where drugs and natural products are elaborated via diastereoselective allylic arylations. The method is used, as the catalyst-controlled stereochemistry-setting step, in an iterative strategy to give arrays of aryl-substituted contiguous stereogenic centers. This approach will complement existing catalyst-controlled stereoselective methods for forming C–C bonds.
{"title":"Ligand-enabled override of the memory effect in Rh-catalyzed asymmetric Suzuki reactions","authors":"Ke Liu, David Egea-Arrebola, Ruchuta Ardkhean, Laura Cunningham, Kirsten E. Christensen, Robert S. Paton, Stephen P. Fletcher","doi":"10.1016/j.chempr.2025.102550","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102550","url":null,"abstract":"Chiral non-racemic allylic species are key building blocks for many carbon-containing molecules, including pharmaceuticals and polymers. Metal-catalyzed asymmetric additions of nucleophiles to allylic species undergo different pathways depending on the metal and nucleophile combination, hindering the development of useful addition reactions with aromatic nucleophiles. We report an asymmetric cross-coupling method between aryl boronic acids and linear allylic phosphates to give branched allylic products. This Suzuki-type reaction overcomes the “memory effect” in Rh catalysis, enabling an overall SN2′ transformation by rate-determining reductive elimination and forming a new stereogenic center adjacent to a terminal vinyl moiety. The method tolerates preexisting stereogenic centers, allowing for synthetic strategies where drugs and natural products are elaborated via diastereoselective allylic arylations. The method is used, as the catalyst-controlled stereochemistry-setting step, in an iterative strategy to give arrays of aryl-substituted contiguous stereogenic centers. This approach will complement existing catalyst-controlled stereoselective methods for forming C–C bonds.","PeriodicalId":268,"journal":{"name":"Chem","volume":"6 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853600","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 : 2025-04-18DOI: 10.1016/j.chempr.2025.102546
Jorge D. Martín-Bernardos, Katrin Golob, Wei W. Chen, Orsola A. Luongo, Inés Sedó, Ana B. Cuenca, Alexandr Shafir
We introduce a C–H coupling process in which an aromatic C–I position serves as trampoline for targeting various aromatic C–H positions. The reaction is set in motion by an interaction between the λ3-iodane ArI(OAc)2 and the π system of polyunsaturated organosilanes. In particular, the silyl-terminated enynes engage in fully regioselective ortho and para C–H functionalization, with selectivity switch achieved by reversing the order of the substrate’s ene and yne fragments. Density functional theory (DFT) calculations show that the ortho selectivity is governed by a [3,3] sigmatropic rearrangement, while the para coupling occurs through a directional three-point π interaction of the enyne-derived cationic π system, giving rise to an essentially barrierless [5,5] sigmatropic rearrangement. Furthermore, iodane-guided C–H functionalization of 2-iodonaphthalene could be directed to the ultra-remote C6 position through further π extension of the organosilanes partner. The latter reaction represents a nearly unprecedented example of a formal [7,7] sigmatropic rearrangement.
{"title":"Polar π stacking for metal-free near, remote, and ultra-remote C–H coupling with aryliodanes","authors":"Jorge D. Martín-Bernardos, Katrin Golob, Wei W. Chen, Orsola A. Luongo, Inés Sedó, Ana B. Cuenca, Alexandr Shafir","doi":"10.1016/j.chempr.2025.102546","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102546","url":null,"abstract":"We introduce a C–H coupling process in which an aromatic C–I position serves as trampoline for targeting various aromatic C–H positions. The reaction is set in motion by an interaction between the λ<sup>3</sup>-iodane ArI(OAc)<sub>2</sub> and the π system of polyunsaturated organosilanes. In particular, the silyl-terminated enynes engage in fully regioselective <em>ortho</em> and <em>para</em> C–H functionalization, with selectivity switch achieved by reversing the order of the substrate’s ene and yne fragments. Density functional theory (DFT) calculations show that the <em>ortho</em> selectivity is governed by a [3,3] sigmatropic rearrangement, while the <em>para</em> coupling occurs through a directional three-point π interaction of the enyne-derived cationic π system, giving rise to an essentially barrierless [5,5] sigmatropic rearrangement. Furthermore, iodane-guided C–H functionalization of 2-iodonaphthalene could be directed to the ultra-remote C6 position through further π extension of the organosilanes partner. The latter reaction represents a nearly unprecedented example of a formal [7,7] sigmatropic rearrangement.","PeriodicalId":268,"journal":{"name":"Chem","volume":"30 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846495","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 : 2025-04-18DOI: 10.1016/j.chempr.2025.102534
Sheng-Yi Yang, Liang Zhang, Fan-Cheng Kong, Yingying Chen, Wei-Jian Li, Fei Wang, Cheng Liu, Xuan He, Xuedong Xiao, Jin Wang, Jianwei Sun, Philip C.Y. Chow, Ryan T.K. Kwok, Jacky W.Y. Lam, Ben Zhong Tang
Scintillators are vital components in high-energy radiation detectors and are used in fields like high-energy physics, non-destructive testing, radiochemistry, and medical diagnostics. Scintillators with aggregation-induced emission (AIE), through rational molecular design and preparation techniques, can be endowed with such properties that effectively overcome the inherent defects of existing inorganic and/or organic scintillators, such as high costs and poor mechanical properties in inorganic types and low light yield and aggregation-caused quenching for organic kinds, thus affording novel optoelectronic properties, superior performance, and broader applications. This review classifies AIE scintillators from a molecular perspective, based on their luminescence mechanisms and construction strategies, into fluorescent scintillators, thermally activated delayed fluorescence scintillators, metal cluster scintillators, organic-inorganic hybrid scintillators, and metal-organic framework scintillators. This review starts with analyses of these building strategies and the structure-performance relationships and then describes the applications of AIE scintillators based on their molecular structures and optoelectronic properties.
{"title":"Scintillators with aggregation-induced emission","authors":"Sheng-Yi Yang, Liang Zhang, Fan-Cheng Kong, Yingying Chen, Wei-Jian Li, Fei Wang, Cheng Liu, Xuan He, Xuedong Xiao, Jin Wang, Jianwei Sun, Philip C.Y. Chow, Ryan T.K. Kwok, Jacky W.Y. Lam, Ben Zhong Tang","doi":"10.1016/j.chempr.2025.102534","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102534","url":null,"abstract":"Scintillators are vital components in high-energy radiation detectors and are used in fields like high-energy physics, non-destructive testing, radiochemistry, and medical diagnostics. Scintillators with aggregation-induced emission (AIE), through rational molecular design and preparation techniques, can be endowed with such properties that effectively overcome the inherent defects of existing inorganic and/or organic scintillators, such as high costs and poor mechanical properties in inorganic types and low light yield and aggregation-caused quenching for organic kinds, thus affording novel optoelectronic properties, superior performance, and broader applications. This review classifies AIE scintillators from a molecular perspective, based on their luminescence mechanisms and construction strategies, into fluorescent scintillators, thermally activated delayed fluorescence scintillators, metal cluster scintillators, organic-inorganic hybrid scintillators, and metal-organic framework scintillators. This review starts with analyses of these building strategies and the structure-performance relationships and then describes the applications of AIE scintillators based on their molecular structures and optoelectronic properties.","PeriodicalId":268,"journal":{"name":"Chem","volume":"75 5 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846761","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 : 2025-04-18DOI: 10.1016/j.chempr.2025.102547
Rohan Bhimpuria, Rima Charaf, Ke Ye, Anders Thapper, Harsha Sathyan, Mårten Ahlquist, Leif Hammarström, K. Eszter Borbas
Industrial dinitrogen (N2) reduction to ammonia in the Haber-Bosch synthesis is essential for producing fertilizers and, consequently, food. Methods wherein the energy for nitrogen activation is supplied by light could provide more sustainable alternatives to existing ones. The combination of a photosensitizer and a lanthanide catalyst is reported for an effective >2e− reduction of N2 in what is the first transition-metal-free molecular photocatalyst for ammonia synthesis. The lanthanide is Earth-abundant Sm. The reaction proceeds at ambient pressure and temperature, with high turnover numbers (up to 98), with visible light irradiation in aqueous solvent mixtures and even pure water, and it uses an environmentally benign non-metallic sacrificial reductant. Nitrite and nitrate were also efficiently reduced to ammonia. Thus, the first photocatalytic co-reduction of nitrite and bicarbonate to urea using an Sm-based photocatalyst was achieved.
{"title":"A Sm(II)-based catalyst for the reduction of dinitrogen, nitrite, and nitrate to ammonia or urea","authors":"Rohan Bhimpuria, Rima Charaf, Ke Ye, Anders Thapper, Harsha Sathyan, Mårten Ahlquist, Leif Hammarström, K. Eszter Borbas","doi":"10.1016/j.chempr.2025.102547","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102547","url":null,"abstract":"Industrial dinitrogen (N<sub>2</sub>) reduction to ammonia in the Haber-Bosch synthesis is essential for producing fertilizers and, consequently, food. Methods wherein the energy for nitrogen activation is supplied by light could provide more sustainable alternatives to existing ones. The combination of a photosensitizer and a lanthanide catalyst is reported for an effective >2e<sup>−</sup> reduction of N<sub>2</sub> in what is the first transition-metal-free molecular photocatalyst for ammonia synthesis. The lanthanide is Earth-abundant Sm. The reaction proceeds at ambient pressure and temperature, with high turnover numbers (up to 98), with visible light irradiation in aqueous solvent mixtures and even pure water, and it uses an environmentally benign non-metallic sacrificial reductant. Nitrite and nitrate were also efficiently reduced to ammonia. Thus, the first photocatalytic co-reduction of nitrite and bicarbonate to urea using an Sm-based photocatalyst was achieved.","PeriodicalId":268,"journal":{"name":"Chem","volume":"67 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846763","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 : 2025-04-17DOI: 10.1016/j.chempr.2025.102554
Ying Sun, Chang Yu, Jieshan Qiu
In Science, Ma and co-workers report a zero-CO2-emission reaction strategy involving the thermal catalytic ethanol reforming over a 3Pt3Ir/α-MoC catalyst to realize an unprecedented hydrogen production rate of 331.3 mmol H2 gcat−1 h−1 with 84.5% selectivity for value-added acetic acid at a low temperature of 270°C. This breakthrough could become a milestone in sustainable energy technologies and beyond.
{"title":"A new breakthrough in ethanol reforming for zero-carbon hydrogen production","authors":"Ying Sun, Chang Yu, Jieshan Qiu","doi":"10.1016/j.chempr.2025.102554","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102554","url":null,"abstract":"In <em>Science</em>, Ma and co-workers report a zero-CO<sub>2</sub>-emission reaction strategy involving the thermal catalytic ethanol reforming over a 3Pt3Ir/α-MoC catalyst to realize an unprecedented hydrogen production rate of 331.3 mmol H<sub>2</sub> g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> with 84.5% selectivity for value-added acetic acid at a low temperature of 270°C. This breakthrough could become a milestone in sustainable energy technologies and beyond.","PeriodicalId":268,"journal":{"name":"Chem","volume":"6 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841943","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 : 2025-04-17DOI: 10.1016/j.chempr.2025.102533
Yanmei Huang, Ying Gao, Bin Zhang
Electrocatalytic hydrogenation of abundant feedstocks to value-added products using water as the hydrogen source offers promising alternatives to traditional methods. At the electrode-electrolyte interface, water molecules not only act as active hydrogen sources but also facilitate mass transport via hydrogen-bond networks. The configuration, orientation, and distribution of interfacial water molecules are directly related to the connectivity of the hydrogen-bond network, thereby directly determining the hydrogenation efficiency. A fundamental understanding of interfacial water dynamics and the development of precise modulation strategies are key to advancing electrochemical hydrogenation. This perspective systematically discusses three dominant strategies—namely, manipulating the local electric field, engineering surface modifications/electrolyte additives, and tuning solvated-cation interactions—to regulate the properties of interfacial water and enhance the corresponding hydrogenation performance. Finally, we highlight critical issues for future research aimed at better controlling interfacial water dynamics to enhance the performance of electrocatalytic hydrogenation and other water-participating reactions.
{"title":"Interfacial water regulation for water-participating electrocatalytic hydrogenation reactions","authors":"Yanmei Huang, Ying Gao, Bin Zhang","doi":"10.1016/j.chempr.2025.102533","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102533","url":null,"abstract":"Electrocatalytic hydrogenation of abundant feedstocks to value-added products using water as the hydrogen source offers promising alternatives to traditional methods. At the electrode-electrolyte interface, water molecules not only act as active hydrogen sources but also facilitate mass transport via hydrogen-bond networks. The configuration, orientation, and distribution of interfacial water molecules are directly related to the connectivity of the hydrogen-bond network, thereby directly determining the hydrogenation efficiency. A fundamental understanding of interfacial water dynamics and the development of precise modulation strategies are key to advancing electrochemical hydrogenation. This perspective systematically discusses three dominant strategies—namely, manipulating the local electric field, engineering surface modifications/electrolyte additives, and tuning solvated-cation interactions—to regulate the properties of interfacial water and enhance the corresponding hydrogenation performance. Finally, we highlight critical issues for future research aimed at better controlling interfacial water dynamics to enhance the performance of electrocatalytic hydrogenation and other water-participating reactions.","PeriodicalId":268,"journal":{"name":"Chem","volume":"22 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841944","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 : 2025-04-17DOI: 10.1016/j.chempr.2025.102573
Yu Hu, Mengxi Zhang, Han Xiao
The biosynthesis of bioorthogonal chemical handles for precise protein labeling remains a significant challenge. In this issue of Chem, Thomas Huber and colleagues report the successful biosynthesis of nitrile-containing amino acids and their site-specific incorporation into proteins, enabling efficient protein conjugation and fluorogenic labeling.
{"title":"Biosynthesis of nitrile-containing amino acids for rapid protein conjugation and fluorogenic labeling","authors":"Yu Hu, Mengxi Zhang, Han Xiao","doi":"10.1016/j.chempr.2025.102573","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102573","url":null,"abstract":"The biosynthesis of bioorthogonal chemical handles for precise protein labeling remains a significant challenge. In this issue of <em>Chem</em>, Thomas Huber and colleagues report the successful biosynthesis of nitrile-containing amino acids and their site-specific incorporation into proteins, enabling efficient protein conjugation and fluorogenic labeling.","PeriodicalId":268,"journal":{"name":"Chem","volume":"108 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841942","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 : 2025-04-16DOI: 10.1016/j.chempr.2025.102542
Runda Li, Libing Yao, Jingyi Sun, Zengyi Sun, Kai Zhang, Jingjing Xue, Rui Wang
With rapid technological advancements, perovskite photovoltaics are approaching the final stage of commercialization. However, challenges arise due to differences between the fabrication processes for large-scale perovskite solar modules (PSMs) and laboratory-scale perovskite solar cells (PSCs). In this perspective, we highlight key obstacles in the transition from PSCs to PSMs across three main fabrication stages: precursor solution preparation, large-scale perovskite deposition, and post-treatment procedures for modules. Beyond addressing long-term stability, we emphasize critical yet often overlooked factors: reproducibility, cost, quality control, and sustainability in PSM manufacture. Finally, we provide our outlook by posing three controversial questions: which type of PSMs will be finally commercialized, how to balance the device area and lateral resistance, and how to realize a stable supply of raw materials. We hope that this effort may provide insights into targeted scientific strategies that can bridge these gaps and facilitate the commercialization of perovskite photovoltaics.
{"title":"Challenges and perspectives for the perovskite module research","authors":"Runda Li, Libing Yao, Jingyi Sun, Zengyi Sun, Kai Zhang, Jingjing Xue, Rui Wang","doi":"10.1016/j.chempr.2025.102542","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102542","url":null,"abstract":"With rapid technological advancements, perovskite photovoltaics are approaching the final stage of commercialization. However, challenges arise due to differences between the fabrication processes for large-scale perovskite solar modules (PSMs) and laboratory-scale perovskite solar cells (PSCs). In this perspective, we highlight key obstacles in the transition from PSCs to PSMs across three main fabrication stages: precursor solution preparation, large-scale perovskite deposition, and post-treatment procedures for modules. Beyond addressing long-term stability, we emphasize critical yet often overlooked factors: reproducibility, cost, quality control, and sustainability in PSM manufacture. Finally, we provide our outlook by posing three controversial questions: which type of PSMs will be finally commercialized, how to balance the device area and lateral resistance, and how to realize a stable supply of raw materials. We hope that this effort may provide insights into targeted scientific strategies that can bridge these gaps and facilitate the commercialization of perovskite photovoltaics.","PeriodicalId":268,"journal":{"name":"Chem","volume":"3 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837101","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 : 2025-04-16DOI: 10.1016/j.chempr.2025.102543
Mark E. Carrington, Loh Min Yi, Erlendur Jónsson, Clare P. Grey
Aqueous organic flow batteries are a promising technology class for long-duration energy storage. However, the poor stability of redox-active components under the conditions frequently used in these batteries, coupled with the inherently high degree of active material chemical complexity, frequently gives rise to intricate degradation pathways that both limit attainable cycle life and are challenging to probe experimentally. Here, we utilize solution pH and bulk magnetic susceptibility to monitor the native minor equilibrium side reaction between water and the one-electron oxidized state of 2,2,6,6-tetramethyl-4-hydroxy-piperidin-1-oxyl (4-hydroxy-TEMPO)—an archetypical flow battery catholyte. This side reaction readily reports on both the main redox reaction of 4-hydroxy-TEMPO, which itself is not proton coupled, as well as on its principal self-discharge pathway. In so doing, it provides accurate, low-cost, and sensitive experimental insights into battery state of charge, state of health, and operating conditions for both flow and hybrid flow configurations.
{"title":"Practical flow battery diagnostics enabled by chemically mediated monitoring","authors":"Mark E. Carrington, Loh Min Yi, Erlendur Jónsson, Clare P. Grey","doi":"10.1016/j.chempr.2025.102543","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102543","url":null,"abstract":"Aqueous organic flow batteries are a promising technology class for long-duration energy storage. However, the poor stability of redox-active components under the conditions frequently used in these batteries, coupled with the inherently high degree of active material chemical complexity, frequently gives rise to intricate degradation pathways that both limit attainable cycle life and are challenging to probe experimentally. Here, we utilize solution pH and bulk magnetic susceptibility to monitor the native minor equilibrium side reaction between water and the one-electron oxidized state of 2,2,6,6-tetramethyl-4-hydroxy-piperidin-1-oxyl (4-hydroxy-TEMPO)—an archetypical flow battery catholyte. This side reaction readily reports on both the main redox reaction of 4-hydroxy-TEMPO, which itself is not proton coupled, as well as on its principal self-discharge pathway. In so doing, it provides accurate, low-cost, and sensitive experimental insights into battery state of charge, state of health, and operating conditions for both flow and hybrid flow configurations.","PeriodicalId":268,"journal":{"name":"Chem","volume":"55 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837102","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}
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