Pub Date : 2026-03-12Epub Date: 2025-10-10DOI: 10.1016/j.chempr.2025.102756
Mingpeng Li , Waqar Ali Memon , Zihao Deng , Huan Wang , Shilong Xiong , Heng Li , Top Archie Dela Peña , Cuifen Zhang , Yunpeng Wang , Jiaying Wu , Zaifei Ma , Nan Zheng , Leilei Tian , Feng He
Nitration is rarely employed to optimize non-fullerene acceptors (NFAs) owing to the pronounced steric hindrance and strong electron-withdrawing inductive effects of nitro groups. This study presents a site-specific nitration strategy to systematically modulate NFA properties and photovoltaic performance. A series of nitrated and non-nitrated NFAs were synthesized, exhibiting distinct energy levels, molecular configurations, and packing modes. Notably, the quasi-planar heterojunction (Q-PHJ) device based on NO2Q-2F, which incorporates a central nitration site, achieved a champion efficiency of 19.14% and an extended T80 lifetime of 6,450 h under dark storage conditions, attributed to its tighter three-dimensional network stacking. In contrast, the HQ-NO2-based device, which features terminal nitration, yielded a lower efficiency of 12.45%. This work underscores the critical role of nitration positioning in unlocking the potential of NFAs. It also provides new opportunities to further explore the impact of nitration on photovoltaic performance for developing advanced organic semiconductors.
{"title":"Photovoltaic potential of nitro-functionalized non-fullerene acceptors depends on its bonding site","authors":"Mingpeng Li , Waqar Ali Memon , Zihao Deng , Huan Wang , Shilong Xiong , Heng Li , Top Archie Dela Peña , Cuifen Zhang , Yunpeng Wang , Jiaying Wu , Zaifei Ma , Nan Zheng , Leilei Tian , Feng He","doi":"10.1016/j.chempr.2025.102756","DOIUrl":"10.1016/j.chempr.2025.102756","url":null,"abstract":"<div><div>Nitration is rarely employed to optimize non-fullerene acceptors (NFAs) owing to the pronounced steric hindrance and strong electron-withdrawing inductive effects of nitro groups. This study presents a site-specific nitration strategy to systematically modulate NFA properties and photovoltaic performance. A series of nitrated and non-nitrated NFAs were synthesized, exhibiting distinct energy levels, molecular configurations, and packing modes. Notably, the quasi-planar heterojunction (Q-PHJ) device based on NO<sub>2</sub>Q-2F, which incorporates a central nitration site, achieved a champion efficiency of 19.14% and an extended <em>T</em><sub>80</sub> lifetime of 6,450 h under dark storage conditions, attributed to its tighter three-dimensional network stacking. In contrast, the HQ-NO<sub>2</sub>-based device, which features terminal nitration, yielded a lower efficiency of 12.45%. This work underscores the critical role of nitration positioning in unlocking the potential of NFAs. It also provides new opportunities to further explore the impact of nitration on photovoltaic performance for developing advanced organic semiconductors.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102756"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255473","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 : 2026-03-12Epub Date: 2025-10-10DOI: 10.1016/j.chempr.2025.102759
Yongseok Hong , Ding Xu , Milan Delor
Exciton-polaritons (EPs) are hybrid light-matter quasiparticles that combine exciton-mediated nonlinearities with long-range coherence, ideal for energy harvesting and nonlinear optics. Optimizing EPs is predicated on a still-elusive understanding of how disorder affects their propagation and dephasing times. Here, using cutting-edge femtosecond spatiotemporal microscopy, we image EP propagation in two-dimensional semiconductors, molecular crystals, and amorphous molecular films with systematically varied exciton-phonon coupling, exciton delocalization, and static disorder. Despite possessing similar EP dispersions, we observe dramatically different transport velocities and scattering times across systems. We establish a robust scaling law linking EP scattering to exciton transfer integral, demonstrating that polaritons based on materials with large exciton bandwidths are protected against disorder even for highly excitonic EPs. This observation cannot be deduced from the systems’ linear optical properties. Our work highlights the critical role of the matter component in dictating polariton properties and provides precise guidelines for simultaneously optimizing EP propagation and nonlinearities.
{"title":"Exciton delocalization suppresses polariton scattering","authors":"Yongseok Hong , Ding Xu , Milan Delor","doi":"10.1016/j.chempr.2025.102759","DOIUrl":"10.1016/j.chempr.2025.102759","url":null,"abstract":"<div><div>Exciton-polaritons (EPs) are hybrid light-matter quasiparticles that combine exciton-mediated nonlinearities with long-range coherence, ideal for energy harvesting and nonlinear optics. Optimizing EPs is predicated on a still-elusive understanding of how disorder affects their propagation and dephasing times. Here, using cutting-edge femtosecond spatiotemporal microscopy, we image EP propagation in two-dimensional semiconductors, molecular crystals, and amorphous molecular films with systematically varied exciton-phonon coupling, exciton delocalization, and static disorder. Despite possessing similar EP dispersions, we observe dramatically different transport velocities and scattering times across systems. We establish a robust scaling law linking EP scattering to exciton transfer integral, demonstrating that polaritons based on materials with large exciton bandwidths are protected against disorder even for highly excitonic EPs. This observation cannot be deduced from the systems’ linear optical properties. Our work highlights the critical role of the matter component in dictating polariton properties and provides precise guidelines for simultaneously optimizing EP propagation and nonlinearities.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102759"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255471","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 : 2026-03-12Epub Date: 2025-10-15DOI: 10.1016/j.chempr.2025.102785
David Panáček , Renata Večeřová , Zdeněk Baďura , Vítězslav Hrubý , Lukáš Zdražil , Milan Kolář , Thamraa Alshahrani , Aleš Panáček , Aristides Bakandritsos , Radek Zbořil
Access to clean water remains a major global challenge, especially in remote and disaster-affected areas, where centralized water treatment is often unavailable. This study introduces a single-atom engineering approach to designing a filtration system capable of simultaneously purifying water from bacteria and heavy metals on site, thus providing a sustainable and user-friendly method for water purification. The system demonstrates exceptional efficiency in removing bacterial and heavy metal contaminants from various water sources. Our findings show remarkable filtration efficiency (>99.999%) against a broad spectrum of microorganisms in distilled, tap, and river water. Moreover, the membrane demonstrates a high adsorption capacity for heavy metals, specifically 661 and 248 mg g−1 for Pb2+ and Cd2+, respectively. The simple operation and high membrane permeability, requiring only a hand-powered vacuum, ensure applicability in off-grid settings. In addition, the membrane material maintains more than 90% efficiency after 20 regeneration cycles, addressing both cost and sustainability issues.
{"title":"Single-atom-enhanced membrane for simultaneous bacteria and heavy metal on-site water treatment","authors":"David Panáček , Renata Večeřová , Zdeněk Baďura , Vítězslav Hrubý , Lukáš Zdražil , Milan Kolář , Thamraa Alshahrani , Aleš Panáček , Aristides Bakandritsos , Radek Zbořil","doi":"10.1016/j.chempr.2025.102785","DOIUrl":"10.1016/j.chempr.2025.102785","url":null,"abstract":"<div><div>Access to clean water remains a major global challenge, especially in remote and disaster-affected areas, where centralized water treatment is often unavailable. This study introduces a single-atom engineering approach to designing a filtration system capable of simultaneously purifying water from bacteria and heavy metals on site, thus providing a sustainable and user-friendly method for water purification. The system demonstrates exceptional efficiency in removing bacterial and heavy metal contaminants from various water sources. Our findings show remarkable filtration efficiency (>99.999%) against a broad spectrum of microorganisms in distilled, tap, and river water. Moreover, the membrane demonstrates a high adsorption capacity for heavy metals, specifically 661 and 248 mg g<sup>−1</sup> for Pb<sup>2+</sup> and Cd<sup>2+</sup>, respectively. The simple operation and high membrane permeability, requiring only a hand-powered vacuum, ensure applicability in off-grid settings. In addition, the membrane material maintains more than 90% efficiency after 20 regeneration cycles, addressing both cost and sustainability issues.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102785"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289238","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 : 2026-03-12Epub Date: 2026-02-06DOI: 10.1016/j.chempr.2025.102881
Tian Jin , Meng Zhao , Xi-Yao Li , Zi-Xian Chen , Bo-Quan Li , Jia-Qi Huang , Qiang Zhang
Lithium–sulfur (Li–S) batteries are promising in realizing high energy density. Employing weakly solvating electrolytes (WSEs) further improves the anode stability. However, the lithium polysulfide (LiPS) redox kinetics is hindered in WSEs, and the underlying mechanism remains unclear. Herein, the LiPS kinetics in WSEs is quantitatively deciphered using rotating disk electrode analysis. The electron transfer number during oxidation is reduced in WSEs, evidencing intrinsically suppressed oxidation extent. Meanwhile, the diffusion coefficient and the electrolyte viscosity concurrently increase, implying a reduced LiPS hydrodynamic radius in WSEs based on the Stokes–Einstein relation and corresponding to inhibited LiPS molecular aggregation. Attributed to the reduced aggregation, WSE-based Li–S batteries exhibit record-low-temperature performances, delivering 8.0 mAh cm−2 and 303 Wh kg−1 at 0°C in 6 Ah-level pouch cells. This work establishes a new kinetic analysis methodology to guide rational electrolyte design and highlights the promise of WSEs to enable low-temperature Li–S batteries.
锂硫电池是实现高能量密度的理想电池。采用弱溶剂化电解质（wse）进一步提高了阳极的稳定性。然而，锂多硫化物（LiPS）在wse中的氧化还原动力学受到阻碍，其潜在机制尚不清楚。在这里，利用旋转圆盘电极分析定量地破译了WSEs中的LiPS动力学。氧化过程中的电子转移数在wse中减少，表明氧化程度受到内在抑制。同时，扩散系数和电解质粘度同时增加，表明基于Stokes-Einstein关系的wse中LiPS流体动力半径减小，对应于LiPS分子聚集受到抑制。由于减少了聚集，基于wse的Li-S电池表现出创纪录的低温性能，在6 ah级别的袋状电池中，在0°C下提供8.0 mAh cm - 2和303 Wh kg - 1。这项工作建立了一种新的动力学分析方法来指导合理的电解质设计，并突出了wse在低温锂硫电池中的应用前景。
{"title":"Reducing polysulfide hydrodynamic radius toward low-temperature lithium–sulfur batteries","authors":"Tian Jin , Meng Zhao , Xi-Yao Li , Zi-Xian Chen , Bo-Quan Li , Jia-Qi Huang , Qiang Zhang","doi":"10.1016/j.chempr.2025.102881","DOIUrl":"10.1016/j.chempr.2025.102881","url":null,"abstract":"<div><div>Lithium–sulfur (Li–S) batteries are promising in realizing high energy density. Employing weakly solvating electrolytes (WSEs) further improves the anode stability. However, the lithium polysulfide (LiPS) redox kinetics is hindered in WSEs, and the underlying mechanism remains unclear. Herein, the LiPS kinetics in WSEs is quantitatively deciphered using rotating disk electrode analysis. The electron transfer number during oxidation is reduced in WSEs, evidencing intrinsically suppressed oxidation extent. Meanwhile, the diffusion coefficient and the electrolyte viscosity concurrently increase, implying a reduced LiPS hydrodynamic radius in WSEs based on the Stokes–Einstein relation and corresponding to inhibited LiPS molecular aggregation. Attributed to the reduced aggregation, WSE-based Li–S batteries exhibit record-low-temperature performances, delivering 8.0 mAh cm<sup>−2</sup> and 303 Wh kg<sup>−1</sup> at 0°C in 6 Ah-level pouch cells. This work establishes a new kinetic analysis methodology to guide rational electrolyte design and highlights the promise of WSEs to enable low-temperature Li–S batteries.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102881"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146209","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}
Electrochemical synthesis offers a sustainable and atom-economical alternative to conventional methods. Although recent advances have enabled electrochemical discovery, the integration of real-time control with analysis promises to allow electrochemical “fly by wire.” Herein, we present the ElectroChemputer, a programmable, modular standard platform enabling fully automated execution of electrochemical workflows. It integrates nuclear magnetic resonance (NMR) spectroscopy and electroanalytical reaction monitoring to provide structural and quantitative insight into reaction progression. Across 170 h of runtime, the system accumulated >1,500 coordinated unit operations and acquired >600 cyclic voltammograms. The ElectroChemputer enabled real-time stopped-flow NMR monitoring and data analysis of complex processes, such as decarboxylation via alternating polarity. Furthermore, we explored its flexibility for diverse transformations, including nucleophilic substitutions, oxidative couplings, and electrodepositions. By using queues and blueprints, it could run multiple protocols in parallel, demonstrating its adaptability across reaction classes, electrode materials, and configurations. Through its modular architecture, the ElectroChemputer sets the stage for programmable, autonomous, and democratized electrochemical synthesis.
{"title":"ElectroChemputer with integrated monitoring for programmable electrochemistry","authors":"Melanie Guillén Soler , Robert Rauschen , Kristine Laws , Abhishek Sharma , Niclas Grocholski , Mark McNulty , Leroy Cronin","doi":"10.1016/j.chempr.2025.102907","DOIUrl":"10.1016/j.chempr.2025.102907","url":null,"abstract":"<div><div>Electrochemical synthesis offers a sustainable and atom-economical alternative to conventional methods. Although recent advances have enabled electrochemical discovery, the integration of real-time control with analysis promises to allow electrochemical “fly by wire.” Herein, we present the ElectroChemputer, a programmable, modular standard platform enabling fully automated execution of electrochemical workflows. It integrates nuclear magnetic resonance (NMR) spectroscopy and electroanalytical reaction monitoring to provide structural and quantitative insight into reaction progression. Across 170 h of runtime, the system accumulated >1,500 coordinated unit operations and acquired >600 cyclic voltammograms. The ElectroChemputer enabled real-time stopped-flow NMR monitoring and data analysis of complex processes, such as decarboxylation via alternating polarity. Furthermore, we explored its flexibility for diverse transformations, including nucleophilic substitutions, oxidative couplings, and electrodepositions. By using queues and blueprints, it could run multiple protocols in parallel, demonstrating its adaptability across reaction classes, electrode materials, and configurations. Through its modular architecture, the ElectroChemputer sets the stage for programmable, autonomous, and democratized electrochemical synthesis.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102907"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147319830","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 : 2026-03-12Epub Date: 2025-11-07DOI: 10.1016/j.chempr.2025.102817
Marco Pierau , Mathis J. Karrasch , Paulina Hartmann , Constantin G. Daniliuc , Andrea Hamza , Frank Glorius
Nitrogen-enriched (partially) saturated fused heterocycles have emerged as highly relevant scaffolds for improved pharmaceuticals. Increased solubility, along with fine-tuneable target affinity and specificity, differentiate them from their nitrogen-poor aromatic counterparts. Contrary to their growing demand, applications are severely limited by arduous bottom-up synthesis routes and the lack of a general solution for facile access. Herein, we report an efficient method for the synthesis of chiral (semi-)saturated pyridine-fused heterocycles and their respective N-permutations by enantioselective arene hydrogenation with a newly developed ruthenium catalyst. We obtained versatile and highly valuable product motifs, including pyridine- and piperidine-fused scaffolds with up to four newly formed stereocenters, of which several have not been previously reported. We conducted extensive in silico studies to elucidate a rare inverse-pressure-dependent enantioselectivity and to develop a rational model for predicting the stereochemical outcome. This contribution is expected to accelerate the exploration of new frameworks in drug discovery.
{"title":"Direct access to chiral nitrogen-rich (semi-)saturated heterocycles","authors":"Marco Pierau , Mathis J. Karrasch , Paulina Hartmann , Constantin G. Daniliuc , Andrea Hamza , Frank Glorius","doi":"10.1016/j.chempr.2025.102817","DOIUrl":"10.1016/j.chempr.2025.102817","url":null,"abstract":"<div><div>Nitrogen-enriched (partially) saturated fused heterocycles have emerged as highly relevant scaffolds for improved pharmaceuticals. Increased solubility, along with fine-tuneable target affinity and specificity, differentiate them from their nitrogen-poor aromatic counterparts. Contrary to their growing demand, applications are severely limited by arduous bottom-up synthesis routes and the lack of a general solution for facile access. Herein, we report an efficient method for the synthesis of chiral (semi-)saturated pyridine-fused heterocycles and their respective N-permutations by enantioselective arene hydrogenation with a newly developed ruthenium catalyst. We obtained versatile and highly valuable product motifs, including pyridine- and piperidine-fused scaffolds with up to four newly formed stereocenters, of which several have not been previously reported. We conducted extensive <em>in silico</em> studies to elucidate a rare inverse-pressure-dependent enantioselectivity and to develop a rational model for predicting the stereochemical outcome. This contribution is expected to accelerate the exploration of new frameworks in drug discovery.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102817"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455209","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 : 2026-03-12Epub Date: 2026-02-26DOI: 10.1016/j.chempr.2026.102996
Felipe Jiménez-Ángeles , Monica Olvera de la Cruz
Random copolymers containing charged, polar, and hydrophobic monomers protect enzymes so they can function in non-biological environments. These heteropolymers imitate unstructured proteins in coacervates that mimic membraneless organelles. Reporting in a recent issue of Nature, a team led by Xu and Alexander-Katz has designed heteropolymers with enzymatic activity by selecting monomers that modulate their chemical microenvironment to replicate enzymatic functionalities.
{"title":"Unstructured protein mimics have enzymatic activity","authors":"Felipe Jiménez-Ángeles , Monica Olvera de la Cruz","doi":"10.1016/j.chempr.2026.102996","DOIUrl":"10.1016/j.chempr.2026.102996","url":null,"abstract":"<div><div>Random copolymers containing charged, polar, and hydrophobic monomers protect enzymes so they can function in non-biological environments. These heteropolymers imitate unstructured proteins in coacervates that mimic membraneless organelles. Reporting in a recent issue of <em>Nature</em>, a team led by Xu and Alexander-Katz has designed heteropolymers with enzymatic activity by selecting monomers that modulate their chemical microenvironment to replicate enzymatic functionalities.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102996"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147319827","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 : 2026-03-12Epub Date: 2026-02-25DOI: 10.1016/j.chempr.2026.102994
Francesco Mascia , Magdalena Abramiuk , Aneta Swárovská , Wolfgang Kroutil
Amide formation represents a key reaction in pharmaceutical synthesis, for which more environmentally friendly methods are sought. In Science, Gao et al. report a biocatalytic oxidative strategy exploiting a redesigned aldehyde dehydrogenase that allows the coupling of aldehydes with amines at the expense of an oxidant [NAD(P)+, molecular oxygen].
{"title":"A redesigned aldehyde dehydrogenase enables intermolecular biocatalytic amide formation from aldehydes and amines","authors":"Francesco Mascia , Magdalena Abramiuk , Aneta Swárovská , Wolfgang Kroutil","doi":"10.1016/j.chempr.2026.102994","DOIUrl":"10.1016/j.chempr.2026.102994","url":null,"abstract":"<div><div>Amide formation represents a key reaction in pharmaceutical synthesis, for which more environmentally friendly methods are sought. In <em>Science</em>, Gao et al. report a biocatalytic oxidative strategy exploiting a redesigned aldehyde dehydrogenase that allows the coupling of aldehydes with amines at the expense of an oxidant [NAD(P)<sup>+</sup>, molecular oxygen].</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102994"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147330076","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}
Vacancy-interface coupling has emerged as a powerful strategy for boosting photocatalytic performance through the synergistic regulation of charge dynamics, interfacial structure, and surface pathways. Engineering vacancies at interfaces allow photogenerated carriers to be trapped, separated, and directed to reactive sites, enhancing activity and selectivity. This perspective highlights recent advances in vacancy-mediated interfacial engineering for solar-driven transformations through representative cases in plastics and biomass photoreforming, H2O2 evolution, water splitting, and CO2 reduction. Particular emphasis is placed on in situ spectroscopic evidence for the dynamic evolution of vacancies and their real-time interactions with reactive sites. By integrating experimental insights with theoretical modeling, we demonstrate how vacancy-interface coupling results in robust, tunable, and efficient photocatalysts. Finally, we outline key challenges and opportunities for developing robust and application-oriented systems that fully exploit defect-interface synergy for sustainable energy and environmental applications.
{"title":"Vacancy-interface coupling in nanomaterials for photocatalytic energy and environmental applications","authors":"Meijun Guo , Shuai Zhang , Jingrun Ran , Shi-Zhang Qiao","doi":"10.1016/j.chempr.2025.102913","DOIUrl":"10.1016/j.chempr.2025.102913","url":null,"abstract":"<div><div>Vacancy-interface coupling has emerged as a powerful strategy for boosting photocatalytic performance through the synergistic regulation of charge dynamics, interfacial structure, and surface pathways. Engineering vacancies at interfaces allow photogenerated carriers to be trapped, separated, and directed to reactive sites, enhancing activity and selectivity. This perspective highlights recent advances in vacancy-mediated interfacial engineering for solar-driven transformations through representative cases in plastics and biomass photoreforming, H<sub>2</sub>O<sub>2</sub> evolution, water splitting, and CO<sub>2</sub> reduction. Particular emphasis is placed on <em>in situ</em> spectroscopic evidence for the dynamic evolution of vacancies and their real-time interactions with reactive sites. By integrating experimental insights with theoretical modeling, we demonstrate how vacancy-interface coupling results in robust, tunable, and efficient photocatalysts. Finally, we outline key challenges and opportunities for developing robust and application-oriented systems that fully exploit defect-interface synergy for sustainable energy and environmental applications.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102913"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147428672","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 : 2026-03-12Epub Date: 2026-02-26DOI: 10.1016/j.chempr.2026.102958
Anthony J. Varni , Wade A. Braunecker , Marcos F. Calegari Andrade , G. Michael Carroll , Yoseph A. Guta , Elwin Hunter-Sellars , Christopher W. Jones , Noemi Leick , Sichi Li , Amitesh Maiti , Maxwell A.T. Marple , Hyun June Moon , Miles A. Sakwa-Novak , Carsten Sievers , Nicholas A. Strange , Simon H. Pang
The success of direct air capture (DAC) of CO2 depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents—including solid-supported aminopolymers, grafted amines, and amine-functionalized resins—remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.
{"title":"Understanding and mitigating degradation in amine-based sorbents for CO2 direct air capture","authors":"Anthony J. Varni , Wade A. Braunecker , Marcos F. Calegari Andrade , G. Michael Carroll , Yoseph A. Guta , Elwin Hunter-Sellars , Christopher W. Jones , Noemi Leick , Sichi Li , Amitesh Maiti , Maxwell A.T. Marple , Hyun June Moon , Miles A. Sakwa-Novak , Carsten Sievers , Nicholas A. Strange , Simon H. Pang","doi":"10.1016/j.chempr.2026.102958","DOIUrl":"10.1016/j.chempr.2026.102958","url":null,"abstract":"<div><div>The success of direct air capture (DAC) of CO<sub>2</sub> depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents—including solid-supported aminopolymers, grafted amines, and amine-functionalized resins—remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102958"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147428673","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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