Pub Date : 2026-02-01DOI: 10.1021/acs.chemmater.6c00266
Cristina Thomas, Jennifer L. Schaefer
In the original publication, the caption for Figure 2 indicated that Dr. Lisa Baugh was the 2020 PMSE Chair, whereas in reality Dr. Lisa Baugh was the 2022 PMSE Chair. The corrected caption should read as follows: Figure 2. PMSE desk at the 2023 ACS Fall Meeting with Dr. Lisa Baugh, 2022 PMSE Chair, and Eileen Ernst, PMSE Executive Coordinator. This article has not yet been cited by other publications.
{"title":"Correction to “PMSE in the Next 100 Years: Shaping the Future of Polymers”","authors":"Cristina Thomas, Jennifer L. Schaefer","doi":"10.1021/acs.chemmater.6c00266","DOIUrl":"https://doi.org/10.1021/acs.chemmater.6c00266","url":null,"abstract":"In the original publication, the caption for Figure 2 indicated that Dr. Lisa Baugh was the 2020 PMSE Chair, whereas in reality Dr. Lisa Baugh was the 2022 PMSE Chair. The corrected caption should read as follows: <b>Figure 2.</b> PMSE desk at the 2023 ACS Fall Meeting with Dr. Lisa Baugh, 2022 PMSE Chair, and Eileen Ernst, PMSE Executive Coordinator. This article has not yet been cited by other publications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"82 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-01DOI: 10.1021/acs.chemmater.6c00184
K. M. Srishti Barnwal, Xin Li, Aryan Keshri, Mohit Tanwani, Yongjun Wu, Zijian Hong, Sujit Das
In the original publication, relevant funding from the National Natural Science Foundation of China (Grant No. 12174328) was omitted from the Acknowledgments. The third sentence of the Acknowledgments should be revised as shown below. The financial supports from the National Natural Science Foundation of China (No. 92463306; No. 12174328, Z.H.), the Joint Funds of the National Natural Science Foundation of China (No. U21A2067, Y.W.), and the Natural Science Foundation of Zhejiang Province (No. LR25E020003, Z.H.; No. LD24E020003, Y.W.) are acknowledged. This article has not yet been cited by other publications.
{"title":"Correction to “Mechanical Manipulation of Ferroelectric Domains in Molecular Ferroelectric”","authors":"K. M. Srishti Barnwal, Xin Li, Aryan Keshri, Mohit Tanwani, Yongjun Wu, Zijian Hong, Sujit Das","doi":"10.1021/acs.chemmater.6c00184","DOIUrl":"https://doi.org/10.1021/acs.chemmater.6c00184","url":null,"abstract":"In the original publication, relevant funding from the National Natural Science Foundation of China (Grant No. 12174328) was omitted from the Acknowledgments. The third sentence of the Acknowledgments should be revised as shown below. The financial supports from the National Natural Science Foundation of China (No. 92463306; No. 12174328, Z.H.), the Joint Funds of the National Natural Science Foundation of China (No. U21A2067, Y.W.), and the Natural Science Foundation of Zhejiang Province (No. LR25E020003, Z.H.; No. LD24E020003, Y.W.) are acknowledged. This article has not yet been cited by other publications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"99 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098058","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-01DOI: 10.1021/acs.chemmater.5c02736
Dahye Lee, Seungjun Kim, Jaewon Ha, Hyunseok Choi, Kyuhyun Im, Myungwoong Kim
We report the rational design and synthesis of acid-cleavable 3-arm polymers via core-first approach using a degradable reversible addition–fragmentation chain transfer (RAFT) agent, in which three chain transfer units are attached to the core through acetal bonds that are cleavable under acidic conditions. Its efficacy is confirmed through RAFT polymerization of methyl methacrylate (MMA), resulting in 3-arm PMMA with a molecular weight reduction to ≈30% of its original value after acid treatment. This approach is extended to a 3-arm terpolymer suitable for chemically amplified resists, exhibiting significantly enhanced sensitivity compared to the conventional linear terpolymer: onset energy for development decreases by ≈21% (DUV) and ≈50% (e-beam), while the energy at which development ends decreases by ≈50% for both. With DUV light, pattern formation is achieved at ≈50% lower energy than the linear terpolymer, and with e-beam, sub-100 nm pattern definition is demonstrated, which is not feasible with the linear terpolymer. The enhanced sensitivity and patternability stem from reduced molecular weight and functional group transformation induced by acid released from a photoacid generator. These findings highlight the significance of rationally designing multiarm architectures to tailor the structure and functionality of complex copolymers through an effective synthetic route, offering potential applications in advanced photoimaging materials and broader stimuli-responsive systems.
{"title":"Rational Design of Degradable Multiarm Polymers Applicable for Photoimaging Materials","authors":"Dahye Lee, Seungjun Kim, Jaewon Ha, Hyunseok Choi, Kyuhyun Im, Myungwoong Kim","doi":"10.1021/acs.chemmater.5c02736","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02736","url":null,"abstract":"We report the rational design and synthesis of acid-cleavable 3-arm polymers via core-first approach using a degradable reversible addition–fragmentation chain transfer (RAFT) agent, in which three chain transfer units are attached to the core through acetal bonds that are cleavable under acidic conditions. Its efficacy is confirmed through RAFT polymerization of methyl methacrylate (MMA), resulting in 3-arm PMMA with a molecular weight reduction to ≈30% of its original value after acid treatment. This approach is extended to a 3-arm terpolymer suitable for chemically amplified resists, exhibiting significantly enhanced sensitivity compared to the conventional linear terpolymer: onset energy for development decreases by ≈21% (DUV) and ≈50% (e-beam), while the energy at which development ends decreases by ≈50% for both. With DUV light, pattern formation is achieved at ≈50% lower energy than the linear terpolymer, and with e-beam, sub-100 nm pattern definition is demonstrated, which is not feasible with the linear terpolymer. The enhanced sensitivity and patternability stem from reduced molecular weight and functional group transformation induced by acid released from a photoacid generator. These findings highlight the significance of rationally designing multiarm architectures to tailor the structure and functionality of complex copolymers through an effective synthetic route, offering potential applications in advanced photoimaging materials and broader stimuli-responsive systems.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"292 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-31DOI: 10.1021/acs.chemmater.5c02646
Yanli Du, Lulu Zhou, Jing Hu
Microarchitected materials with programmable topological configurations provide a versatile platform for enhancing functionalities and broadening applications in advanced materials science. Metal-quinone networks (MQNs) uniquely combine the inherent bioactivity of natural quinones with the structural tunability of framework-based materials, conferring integrated advantages, including high drug-loading capacity, bidirectional pH responsiveness, extensive adhesion capability, and ease of modification. However, the achievable dimensional range of MQNs through existing synthetic approaches remains limited, restricting precise control over their structural characteristics. Here, we present a strategy involving prepolymerization of natural quinones, followed by the construction of rodlike micelles and metal-coordination assembly, to achieve precise morphological control of MQNs. By systematically varying parameters including ligand-to-metal ratio, solvent types, surfactant types, and cross-linking agents, a series of MQN architectures such as book-, sheet-, thread-, spindle-, and rodlike structures were obtained. Moreover, the morphology progressively evolves from one-dimensional (1D) rod- and needle-like structures to three-dimensional (3D) rectangular blocklike forms. Notably, the rod-shaped MQNs exhibit tunable aspect ratios ranging from 3.0 to 80.0. Scanning electron microscopy (SEM) characterized solvent-induced facet-selective growth and stoichiometrically dependent anisotropic growth, thereby enabling predictable control over the geometrical shape. The findings of this work provide guiding insights into the rational construction of sophisticated structures of MQNs for potential applications.
{"title":"Precisely Tailoring the Architecture of Metal-Quinone Networks via a Template-Directed Coordination Assembly","authors":"Yanli Du, Lulu Zhou, Jing Hu","doi":"10.1021/acs.chemmater.5c02646","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02646","url":null,"abstract":"Microarchitected materials with programmable topological configurations provide a versatile platform for enhancing functionalities and broadening applications in advanced materials science. Metal-quinone networks (MQNs) uniquely combine the inherent bioactivity of natural quinones with the structural tunability of framework-based materials, conferring integrated advantages, including high drug-loading capacity, bidirectional pH responsiveness, extensive adhesion capability, and ease of modification. However, the achievable dimensional range of MQNs through existing synthetic approaches remains limited, restricting precise control over their structural characteristics. Here, we present a strategy involving prepolymerization of natural quinones, followed by the construction of rodlike micelles and metal-coordination assembly, to achieve precise morphological control of MQNs. By systematically varying parameters including ligand-to-metal ratio, solvent types, surfactant types, and cross-linking agents, a series of MQN architectures such as book-, sheet-, thread-, spindle-, and rodlike structures were obtained. Moreover, the morphology progressively evolves from one-dimensional (1D) rod- and needle-like structures to three-dimensional (3D) rectangular blocklike forms. Notably, the rod-shaped MQNs exhibit tunable aspect ratios ranging from 3.0 to 80.0. Scanning electron microscopy (SEM) characterized solvent-induced facet-selective growth and stoichiometrically dependent anisotropic growth, thereby enabling predictable control over the geometrical shape. The findings of this work provide guiding insights into the rational construction of sophisticated structures of MQNs for potential applications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"143 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089450","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-30DOI: 10.1021/acs.chemmater.5c02578
Aurland K. Watkins, Anthony K. Cheetham, Ram Seshadri
Oxides exhibiting metallic conduction are crucial for various applications, including fuel cells, battery electrodes, resistive and magnetoresistive materials, electrocatalysts, transparent conductors, and high-temperature superconductors. Oxides that approach metallicity also play significant roles in switching applications, where the metal–insulator transition phenomenon is utilized across a range of technologies. This perspective, motivated by the question of when oxides are metallic, employs electronic structure calculations on metallic oxides to identify typical features in the electronic structure that promote metallic behavior. The critical factor of the bandwidth of the electronic energy bands near the Fermi energy is emphasized since it has been somewhat overlooked in the literature. For example, bandwidth considerations would suggest that the recently proposed phosphate “LK-99” would never be a suitable target for superconductivity. By relating the crystal structure and electronic band features obtained through density functional theory calculations, we present the general heuristic that crystals with conduction bands narrower than 1 eV (as obtained from routine electronic structure methods) are unlikely to be metallic. We further examine the origins of narrow or flat bands to distinguish between structural properties that are conducive or detrimental to physical behavior like superconductivity. This survey of representative oxide metals highlights the essential chemical and structural ingredients that contribute to extended covalent interactions and ultimately wide electronic bands. A key takeaway is that oxyanion compounds such as borates, carbonates, silicates, sulfates, nitrates, and phosphates are unlikely to exhibit metallic conduction at ambient pressure. While the focus here is on oxides, the general findings should apply across various material families, extending to conducting organic crystals, conducting polymers, and hybrid and framework materials.
{"title":"Metallic Oxides and the Overlooked Role of Bandwidth","authors":"Aurland K. Watkins, Anthony K. Cheetham, Ram Seshadri","doi":"10.1021/acs.chemmater.5c02578","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02578","url":null,"abstract":"Oxides exhibiting metallic conduction are crucial for various applications, including fuel cells, battery electrodes, resistive and magnetoresistive materials, electrocatalysts, transparent conductors, and high-temperature superconductors. Oxides that approach metallicity also play significant roles in switching applications, where the metal–insulator transition phenomenon is utilized across a range of technologies. This perspective, motivated by the question of when oxides are metallic, employs electronic structure calculations on metallic oxides to identify typical features in the electronic structure that promote metallic behavior. The critical factor of the bandwidth of the electronic energy bands near the Fermi energy is emphasized since it has been somewhat overlooked in the literature. For example, bandwidth considerations would suggest that the recently proposed phosphate “LK-99” would never be a suitable target for superconductivity. By relating the crystal structure and electronic band features obtained through density functional theory calculations, we present the general heuristic that crystals with conduction bands narrower than 1 eV (as obtained from routine electronic structure methods) are unlikely to be metallic. We further examine the origins of narrow or flat bands to distinguish between structural properties that are conducive or detrimental to physical behavior like superconductivity. This survey of representative oxide metals highlights the essential chemical and structural ingredients that contribute to extended covalent interactions and ultimately wide electronic bands. A key takeaway is that oxyanion compounds such as borates, carbonates, silicates, sulfates, nitrates, and phosphates are unlikely to exhibit metallic conduction at ambient pressure. While the focus here is on oxides, the general findings should apply across various material families, extending to conducting organic crystals, conducting polymers, and hybrid and framework materials.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"389 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acs.chemmater.5c02293
Jaeho Lee, Wengang Huang, Xiangyi Zha, Xuemei Li, Zixi Xie, Peng Chen, Chenghan Sun, Muhammad Yazid Bin Zulkifli, Sang T. Pham, Bun Chan, Marija Švegovec, Atul Shukla, Junyong Zhu, Rijia Lin, Nicholas M. Bedford, Vicki Chen, Sean Collins, Andraž Krajnc, Anthony K. Cheetham, Lianzhou Wang, Jingwei Hou
Developing quantum dots (QDs) with robust and stable photoluminescence are critical for the advancement of optical nanomaterials. However, QD synthesis still usually involves complex nucleation, growth, surface capping, and separation procedures. Herein, we present an approach to generating embedded PbI2 QDs in situ within the matrix of a metal–organic framework (MOF) glass. This is achieved by controllable decomposition of an optoelectronically inactive δ-phase organic lead halide perovskite (OLHP) within the MOF glass, where the high-temperature MOF melt alters the degradation pathway through interfacial bonding and dissolution effects, effectively preventing PbI2 aggregation and passivating the resulting QDs. The resulting composite exhibits high-quality, narrow line width photoluminescence at room temperature, alongside remarkable stability under ambient conditions. This innovative approach offers a sustainable and efficient route for QD generation, underscoring the potential of MOF glass-based composites in optoelectronic applications.
{"title":"Quantum Dot Formation through Controlled Hybrid Perovskite Decomposition within Metal Organic Framework Glass","authors":"Jaeho Lee, Wengang Huang, Xiangyi Zha, Xuemei Li, Zixi Xie, Peng Chen, Chenghan Sun, Muhammad Yazid Bin Zulkifli, Sang T. Pham, Bun Chan, Marija Švegovec, Atul Shukla, Junyong Zhu, Rijia Lin, Nicholas M. Bedford, Vicki Chen, Sean Collins, Andraž Krajnc, Anthony K. Cheetham, Lianzhou Wang, Jingwei Hou","doi":"10.1021/acs.chemmater.5c02293","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02293","url":null,"abstract":"Developing quantum dots (QDs) with robust and stable photoluminescence are critical for the advancement of optical nanomaterials. However, QD synthesis still usually involves complex nucleation, growth, surface capping, and separation procedures. Herein, we present an approach to generating embedded PbI<sub>2</sub> QDs <i>in situ</i> within the matrix of a metal–organic framework (MOF) glass. This is achieved by controllable decomposition of an optoelectronically inactive δ-phase organic lead halide perovskite (OLHP) within the MOF glass, where the high-temperature MOF melt alters the degradation pathway through interfacial bonding and dissolution effects, effectively preventing PbI<sub>2</sub> aggregation and passivating the resulting QDs. The resulting composite exhibits high-quality, narrow line width photoluminescence at room temperature, alongside remarkable stability under ambient conditions. This innovative approach offers a sustainable and efficient route for QD generation, underscoring the potential of MOF glass-based composites in optoelectronic applications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"210 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089865","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acs.chemmater.5c02442
Saeed Borhani, Le Thi Thao, Gregor A. Zickler, Antje Quade, Michael S. Elsaesser, Volker Presser, Stefanie Arnold
The increasing demand for sustainable energy storage drives the development of advanced lithium-ion battery (LIB) materials that combine high performance, cost efficiency, and environmental sustainability. Carbon spherogels, characterized by high surface area, interconnected porosity, and high conductivity, are promising electrode candidates; however, they suffer from low specific capacities when used alone. This study presents iron-loaded carbon spherogels as next-generation LIB electrodes, leveraging iron’s high theoretical capacity, abundance, and eco-friendliness. A scalable and tailorable synthesis method enabled the integration of tunable iron contents (15–40 mass %) into the carbon framework, forming robust porous networks with uniformly distributed iron nanoparticles. Electrochemical characterization revealed high specific capacities (up to 1190 mAh g–1) and high cycling stability (>99% Coulombic efficiency over 300 cycles). Post-mortem analysis highlighted the synergistic interaction between iron redox activity and carbon matrix stability. The medium (27 mass %) iron-loaded carbon spherogel sample achieved the best balance between capacity and durability. These findings position iron-loaded carbon spherogels as sustainable, high-performance LIB electrodes, offering a cobalt-free and nickel-free alternative that addresses key challenges of conversion-type materials, such as volume expansion and capacity fading.
对可持续能源存储日益增长的需求推动了先进锂离子电池（LIB）材料的发展，这些材料结合了高性能、成本效益和环境可持续性。碳球凝胶具有高表面积、多孔性和高导电性等特点，是很有前途的电极候选物；然而，单独使用时，它们的比容量较低。这项研究提出了铁负载碳球凝胶作为下一代锂离子电池电极，利用铁的高理论容量、丰度和生态友好性。一种可扩展且可定制的合成方法能够将可调节的铁含量（15-40质量%）整合到碳框架中，形成均匀分布的铁纳米颗粒坚固的多孔网络。电化学表征显示了高比容量（高达1190 mAh g-1）和高循环稳定性（超过300次循环的库仑效率>；99%）。事后分析强调了铁氧化还原活性和碳基质稳定性之间的协同相互作用。介质（27质量%）铁负载碳球凝胶样品在容量和耐久性之间达到了最佳平衡。这些发现将铁负载碳球凝胶定位为可持续的高性能LIB电极，提供了一种无钴和无镍的替代方案，解决了转换型材料的关键挑战，如体积膨胀和容量衰退。
{"title":"Iron-Loaded Carbon Spherogels as Sustainable Electrode Materials for High-Performance Lithium-Ion Batteries","authors":"Saeed Borhani, Le Thi Thao, Gregor A. Zickler, Antje Quade, Michael S. Elsaesser, Volker Presser, Stefanie Arnold","doi":"10.1021/acs.chemmater.5c02442","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02442","url":null,"abstract":"The increasing demand for sustainable energy storage drives the development of advanced lithium-ion battery (LIB) materials that combine high performance, cost efficiency, and environmental sustainability. Carbon spherogels, characterized by high surface area, interconnected porosity, and high conductivity, are promising electrode candidates; however, they suffer from low specific capacities when used alone. This study presents iron-loaded carbon spherogels as next-generation LIB electrodes, leveraging iron’s high theoretical capacity, abundance, and eco-friendliness. A scalable and tailorable synthesis method enabled the integration of tunable iron contents (15–40 mass %) into the carbon framework, forming robust porous networks with uniformly distributed iron nanoparticles. Electrochemical characterization revealed high specific capacities (up to 1190 mAh g<sup>–1</sup>) and high cycling stability (>99% Coulombic efficiency over 300 cycles). Post-mortem analysis highlighted the synergistic interaction between iron redox activity and carbon matrix stability. The medium (27 mass %) iron-loaded carbon spherogel sample achieved the best balance between capacity and durability. These findings position iron-loaded carbon spherogels as sustainable, high-performance LIB electrodes, offering a cobalt-free and nickel-free alternative that addresses key challenges of conversion-type materials, such as volume expansion and capacity fading.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"4 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acs.chemmater.5c02657
Yuhong Li, Muhan Tang, Feng Luo
As an extreme field environment, pressure effectively regulates the lattice structures, electron correlations, and coupled order parameters of phase-change materials (PCMs), thus inducing abundant structural, electronic, topological, and dynamic phase transitions. These pressure-induced ground (off-) or excited (on-) states enable PCMs to generate diverse magnetoelectric responses. This review systematically summarizes the underlying mechanisms behind these phase transitions in PCMs under pressure, as well as the resulting cross-scale magnetoelectric responses. These responses can be manipulated by leveraging these phase transitions via multigrade empowered deconstruction, multidimension coupled characterization, multiphysics integrated collaboration, and multivariate combined competition. Moreover, the review discusses major challenges while offering distinct opportunities in translating a fundamental mechanism into a practical application. Finally, we propose a paradigm supported by theoretical prediction, experimental characterization, and computational simulation for the design of magnetoelectric responses, thereby paving the way for next-generation phase-change magnetoelectric devices modulated by pressure.
{"title":"Pressure-Modulated Phase-Change Magnetoelectric Materials and Devices","authors":"Yuhong Li, Muhan Tang, Feng Luo","doi":"10.1021/acs.chemmater.5c02657","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02657","url":null,"abstract":"As an extreme field environment, pressure effectively regulates the lattice structures, electron correlations, and coupled order parameters of phase-change materials (PCMs), thus inducing abundant structural, electronic, topological, and dynamic phase transitions. These pressure-induced ground (off-) or excited (on-) states enable PCMs to generate diverse magnetoelectric responses. This review systematically summarizes the underlying mechanisms behind these phase transitions in PCMs under pressure, as well as the resulting cross-scale magnetoelectric responses. These responses can be manipulated by leveraging these phase transitions via multigrade empowered deconstruction, multidimension coupled characterization, multiphysics integrated collaboration, and multivariate combined competition. Moreover, the review discusses major challenges while offering distinct opportunities in translating a fundamental mechanism into a practical application. Finally, we propose a paradigm supported by theoretical prediction, experimental characterization, and computational simulation for the design of magnetoelectric responses, thereby paving the way for next-generation phase-change magnetoelectric devices modulated by pressure.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"23 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089452","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acs.chemmater.5c02665
Sungwoo Jung, Liang Yan, Anthony Megret-Bonilla, Wei You
While p-type doping of conjugated polymers has been extensively studied, the development of efficient and stable n-type doping remains a significant challenge. Although the importance of the LUMO (lowest unoccupied molecular orbital) energy level of conjugated polymers on effective n-type doping has been widely recognized, there are few systematic studies to quantify the influence of the LUMO level on n-type doping of conjugated polymers. In this work, we synthesized a series of BDOPV-based conjugated polymers with tunable LUMO energy levels (− 4.05 to −4.37 eV) by incorporating fluorine atoms and cyano (−CN) groups onto an otherwise identical conjugated backbone. Our results revealed that a deeper LUMO level facilitates more efficient electron transfer and charge carrier generation, corresponding to the observed higher doping efficiency and conductivity. Our data suggest that polymers with LUMO levels below −4.3 eV exhibit substantially enhanced resistance to oxidative degradation by air. These results highlight the pivotal role of the LUMO energy level in determining the doping characteristics of n-type conjugated polymers and offer insights to further the development of high-performance, air-stable n-doped conjugated polymers.
{"title":"Impact of LUMO Energy Level on n-Type Doping Efficiency and Air Stability of Conjugated Polymers","authors":"Sungwoo Jung, Liang Yan, Anthony Megret-Bonilla, Wei You","doi":"10.1021/acs.chemmater.5c02665","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c02665","url":null,"abstract":"While p-type doping of conjugated polymers has been extensively studied, the development of efficient and stable n-type doping remains a significant challenge. Although the importance of the LUMO (lowest unoccupied molecular orbital) energy level of conjugated polymers on effective n-type doping has been widely recognized, there are few systematic studies to quantify the influence of the LUMO level on n-type doping of conjugated polymers. In this work, we synthesized a series of BDOPV-based conjugated polymers with tunable LUMO energy levels (− 4.05 to −4.37 eV) by incorporating fluorine atoms and cyano (−CN) groups onto an otherwise identical conjugated backbone. Our results revealed that a deeper LUMO level facilitates more efficient electron transfer and charge carrier generation, corresponding to the observed higher doping efficiency and conductivity. Our data suggest that polymers with LUMO levels below −4.3 eV exhibit substantially enhanced resistance to oxidative degradation by air. These results highlight the pivotal role of the LUMO energy level in determining the doping characteristics of n-type conjugated polymers and offer insights to further the development of high-performance, air-stable n-doped conjugated polymers.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"23 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070673","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Defect-rich RuO2 catalysts, although possessing high electrocatalytic activity, are inherently unstable for the anode oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE) due to rapid lattice oxygen depletion. Here we report an atomically Ir-doped, grain-boundary-rich RuO2 catalyst (Ir-GB-RuO2) that suppresses overactivation of lattice oxygen by forming robust Ru–O–Ir bridging motifs at grain boundaries, achieving high-performance acidic OER electrocatalysis and ampere-level stable PEMWE. The induced electronic modulation shifts the catalytic mechanism from a pure lattice oxygen mechanism (LOM) to a balanced coexistence of LOM and the adsorbate evolution mechanism (AEM), thereby achieving robust stability while preserving high intrinsic activity. The primary Ir-GB-RuO2 catalyst requires only 191 mV overpotential to achieve 10 mA cm–2 and exhibits a prolonged durability exceeding 1000 h at 100 mA cm–2. In a PEM electrolyzer, it attains the current density of 1.0 A cm–2 at a notably low cell voltage (1.67 V) and exhibits a minimal potential decay rate of only 55.3 μV h–1 over 1500 h of continuous operation. This work overcomes the intrinsic activity–stability trade-off in defect-rich Ru-based catalysts for industrial PEMWE.
富缺陷RuO2催化剂虽然具有较高的电催化活性，但由于晶格氧的快速耗竭，在质子交换膜电解（PEMWE）中阳极析氧反应（OER）中具有固有的不稳定性。在这里，我们报道了一种原子掺杂的、富含晶界的RuO2催化剂（Ir-GB-RuO2），它通过在晶界形成鲁棒的Ru-O-Ir桥接基序来抑制晶格氧的过度活化，实现了高性能的酸性OER电催化和安培级稳定的PEMWE。诱导电子调制将催化机制从纯晶格氧机制（LOM）转变为LOM和吸附质演化机制（AEM）的平衡共存，从而在保持高内在活性的同时实现了强大的稳定性。初级Ir-GB-RuO2催化剂只需要191 mV过电位就可以达到10 mA cm-2，并且在100 mA cm-2下表现出超过1000小时的延长耐久性。在PEM电解槽中，在极低的电池电压（1.67 V）下，它的电流密度可达1.0 a cm-2，在连续工作1500小时内，其电位衰减率仅为55.3 μV h - 1。这项工作克服了工业PEMWE中富含缺陷的钌基催化剂的固有活性与稳定性之间的权衡。
{"title":"Stabilizing Grain-Boundary-Rich RuO2 by Atomic Iridium-Doping To Achieve High-Performance Oxygen Evolution for Ampere-Level PEM Water Electrolysis","authors":"Junlin Cai, Pengfei Li, Hongpu Huang, Shupeng Wang, Yu Peng, Yuhang Peng, Qiuxiang Wang, Xiaohong Wang, Zhaoxiong Xie, Shuifen Xie","doi":"10.1021/acs.chemmater.5c03326","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c03326","url":null,"abstract":"Defect-rich RuO<sub>2</sub> catalysts, although possessing high electrocatalytic activity, are inherently unstable for the anode oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE) due to rapid lattice oxygen depletion. Here we report an atomically Ir-doped, grain-boundary-rich RuO<sub>2</sub> catalyst (Ir-GB-RuO<sub>2</sub>) that suppresses overactivation of lattice oxygen by forming robust Ru–O–Ir bridging motifs at grain boundaries, achieving high-performance acidic OER electrocatalysis and ampere-level stable PEMWE. The induced electronic modulation shifts the catalytic mechanism from a pure lattice oxygen mechanism (LOM) to a balanced coexistence of LOM and the adsorbate evolution mechanism (AEM), thereby achieving robust stability while preserving high intrinsic activity. The primary Ir-GB-RuO<sub>2</sub> catalyst requires only 191 mV overpotential to achieve 10 mA cm<sup>–2</sup> and exhibits a prolonged durability exceeding 1000 h at 100 mA cm<sup>–2</sup>. In a PEM electrolyzer, it attains the current density of 1.0 A cm<sup>–2</sup> at a notably low cell voltage (1.67 V) and exhibits a minimal potential decay rate of only 55.3 μV h<sup>–1</sup> over 1500 h of continuous operation. This work overcomes the intrinsic activity–stability trade-off in defect-rich Ru-based catalysts for industrial PEMWE.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"25 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146090124","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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