Achieving precise fabrication of ordered superstructures with multifunctional catalytic activity is fascinating but elusive due to uncontrollable interfacial energy and growth kinetics at the material surface. Herein, we develop a facile strategy for oriented formation of carbon nanotubes (CNT) anchored on three-dimensionally ordered macro-microporous (3DOM) superstructure derived from a Co-based 3DOM metal-organic framework (3DOM-MOF). Mechanism studies based on density functional theory (DFT) calculations and in situ spectroscopy reveal that the synergistic coupling of curved CNTs supports and Co nanoparticles in the as-prepared Co-based porous superstructures CNTs catalysts (Co-HOPS-CNTs20D) can regulate the electronic structure of the isolated Co-N4 sites, thus optimizing the binding strength of the oxygenated intermediates and facilitating intrinsic catalyst activity. The unique feature of the superstructure is validated using 3D transmission electron microscopy tomography, and the corresponding finite element analysis (FEA) simulations prove enhanced conductivity of Co-HOPS-CNTs20D superstructure, which facilitates transfer efficiency of electrons and improves catalytic activity. As a result, the Co-HOPS-CNTs20D exhibits a low overpotential of 287 mV at 10 mA cm−2 for OER and a high ORR half-wave potential of 0.863 V. The zinc-air battery incorporating Co-HOPS-CNTs20D demonstrates efficient and stable operation over a period of 160 h.
{"title":"Carbon Nanotubes Assembled Ordered Macro-Microporous Superstructure as Bifunctional Oxygen Electrocatalyst for Long-Life Rechargeable Zn–Air Batteries","authors":"Shilong Wen, Ke Ma, Yongfang Zhang, Ying Wang, Wenjie Yu, Liyang Shao, Xue Yang, Yanchao Zhao, Cong Han, Rutao Wang, Jianxing Shen, Enyan Guo, Liting Yan, Lili Han, Xuebo Zhao, Lianzhou Wang","doi":"10.1002/adfm.202531733","DOIUrl":"https://doi.org/10.1002/adfm.202531733","url":null,"abstract":"Achieving precise fabrication of ordered superstructures with multifunctional catalytic activity is fascinating but elusive due to uncontrollable interfacial energy and growth kinetics at the material surface. Herein, we develop a facile strategy for oriented formation of carbon nanotubes (CNT) anchored on three-dimensionally ordered macro-microporous (3DOM) superstructure derived from a Co-based 3DOM metal-organic framework (3DOM-MOF). Mechanism studies based on density functional theory (DFT) calculations and in situ spectroscopy reveal that the synergistic coupling of curved CNTs supports and Co nanoparticles in the as-prepared Co-based porous superstructures CNTs catalysts (Co-HOPS-CNTs<sub>20D</sub>) can regulate the electronic structure of the isolated Co-N<sub>4</sub> sites, thus optimizing the binding strength of the oxygenated intermediates and facilitating intrinsic catalyst activity. The unique feature of the superstructure is validated using 3D transmission electron microscopy tomography, and the corresponding finite element analysis (FEA) simulations prove enhanced conductivity of Co-HOPS-CNTs<sub>20D</sub> superstructure, which facilitates transfer efficiency of electrons and improves catalytic activity. As a result, the Co-HOPS-CNTs<sub>20D</sub> exhibits a low overpotential of 287 mV at 10 mA cm<sup>−2</sup> for OER and a high ORR half-wave potential of 0.863 V. The zinc-air battery incorporating Co-HOPS-CNTs<sub>20D</sub> demonstrates efficient and stable operation over a period of 160 h.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"89 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Phase-change memory (PCM) displays great promise for the storage-class memory (SCM) technology due to its combination of fast speed of dynamic random-access memory and nonvolatility of Flash. Yet, to meet the high industrial requirement of write/erase speed for the SCM application, robust strategies for further accelerating phase transition, particularly from amorphous to crystalline PCM materials, are urgently needed. In this work, we propose a unique strategy of coherent-interface induced ultrafast crystallization in PCM materials. Employing rock-salt YAs/Ge2Sb2Te5 as a prototype, systematic first-principles molecular dynamics demonstrate that rapid nonstochastic crystallization behaviors can be achieved by the rock-salt-lattice-matching and high-temperature-resistant heterogeneous interface attached to the popular PCM material Ge2Sb2Te5 (GST). Further experiment shows that the YAs-incorporated GST device has a faster SET process compared with the pure GST device. Finally, to extend the strategy in the family of inorganic materials, high-throughput screening from over 150 000 structures discovers as many as 71 candidates for coherent interfaces with PCM GST. The present study establishes a promising strategy to overcome the speed bottleneck of PCM through atomic-scale interface design for future storage-class memory implementation.
{"title":"Heterogeneous Coherent Interface Enabling Nonstochastic Crystallization for Phase-Change Memory","authors":"Tian-Yu Zhao, Jiahao Li, Nian-Ke Chen, Bai-Qian Wang, Xiaomin Cheng, Shun-Yao Qin, Huan-Ran Ding, Shengbai Zhang, Hong-Bo Sun, Xiangshui Miao, Xian-Bin Li","doi":"10.1002/adfm.202523223","DOIUrl":"https://doi.org/10.1002/adfm.202523223","url":null,"abstract":"Phase-change memory (PCM) displays great promise for the storage-class memory (SCM) technology due to its combination of fast speed of dynamic random-access memory and nonvolatility of Flash. Yet, to meet the high industrial requirement of write/erase speed for the SCM application, robust strategies for further accelerating phase transition, particularly from amorphous to crystalline PCM materials, are urgently needed. In this work, we propose a unique strategy of coherent-interface induced ultrafast crystallization in PCM materials. Employing rock-salt YAs/Ge<sub>2</sub>Sb<sub>2</sub>Te<sub>5</sub> as a prototype, systematic first-principles molecular dynamics demonstrate that rapid nonstochastic crystallization behaviors can be achieved by the rock-salt-lattice-matching and high-temperature-resistant heterogeneous interface attached to the popular PCM material Ge<sub>2</sub>Sb<sub>2</sub>Te<sub>5</sub> (GST). Further experiment shows that the YAs-incorporated GST device has a faster SET process compared with the pure GST device. Finally, to extend the strategy in the family of inorganic materials, high-throughput screening from over 150 000 structures discovers as many as 71 candidates for coherent interfaces with PCM GST. The present study establishes a promising strategy to overcome the speed bottleneck of PCM through atomic-scale interface design for future storage-class memory implementation.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"87 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenjie Zhang, Xiaosong Xiong, Run Xu, Guangyao Xiang, Tao Wang, Xu Liu, Yong Wang, Lili Liu, Yuping Wu
With the increasing demand for energy storage devices with higher energy density, lithium metal anode (LMA) has emerged as promising candidate due to ultra-high theoretical specific capacity (3860 mAh g−1) and the lowest reduction potential (-3.04 V vs. S.H.E.). However, the practical application of LMA is still restricted by notorious active lithium loss and lithium dendrite growth, which cause low Coulombic efficiency, poor cycling life, and even potential safety hazards. In this study, a multifunctional diethyl sulfide electrolyte additive is proposed to synergistically construct a stable Li2S-rich solid electrolyte interphase (SEI) and Li2S/Li2SO4/Li2SO3-rich cathode electrolyte interphases (CEI), which could accelerate Li ions (Li+) transport kinetics and enhance the interfacial stability during long-term cycling. Moreover, the sulfur-rich composite in electrolyte interface could reduce the energy barrier for Li+ desolvation and thereby enhance interface dynamics. Based on these merits, the introduction of 2.0 vol.% diethyl sulfide into a carbonate electrolyte (without FEC) enables the lithium anode to achieve a 7-fold enhancement in long-term cycling performance. More impressively, the Li||LiFePO4 (LFP) pouch cell with the modified electrolyte achieves an outstanding capacity retention of 98.75% after 200 cycles at 0.1 C. The multifunctional diethyl sulfide additive paves the way for high-performance LMBs for practical applications.
随着对高能量密度储能器件的需求不断增加，锂金属阳极（LMA）因其超高的理论比容量（3860 mAh g - 1）和最低的还原电位（-3.04 V vs. S.H.E.）而成为有希望的候选材料。然而，LMA的实际应用仍然受到活性锂损失和锂枝晶生长严重的制约，导致库仑效率低，循环寿命差，甚至存在安全隐患。本研究提出了一种多功能二乙基硫化物电解质添加剂，协同构建稳定的富Li2S固体电解质界面（SEI）和富Li2S/Li2SO4/ li2so3阴极电解质界面（CEI），加速Li离子（Li+）传输动力学，增强界面在长期循环过程中的稳定性。此外，电解质界面中的富硫复合材料可以降低Li+脱溶的能垒，从而增强界面动力学。基于这些优点，在碳酸电解质（不含FEC）中引入2.0 vol.%的二乙基硫化物，使锂阳极的长期循环性能提高了7倍。更令人印象深刻的是，在0.1℃下，经过200次循环后，Li||LiFePO4 （LFP）袋状电池的容量保持率达到98.75%。多功能二乙基硫化物添加剂为高性能LFP的实际应用铺平了道路。
{"title":"Diethyl Sulfide as a Multifunctional Electrolyte Additive for Enhancing Electrochemical Performance of Lithium Metal Batteries","authors":"Wenjie Zhang, Xiaosong Xiong, Run Xu, Guangyao Xiang, Tao Wang, Xu Liu, Yong Wang, Lili Liu, Yuping Wu","doi":"10.1002/adfm.202529688","DOIUrl":"https://doi.org/10.1002/adfm.202529688","url":null,"abstract":"With the increasing demand for energy storage devices with higher energy density, lithium metal anode (LMA) has emerged as promising candidate due to ultra-high theoretical specific capacity (3860 mAh g<sup>−1</sup>) and the lowest reduction potential (-3.04 V vs. S.H.E.). However, the practical application of LMA is still restricted by notorious active lithium loss and lithium dendrite growth, which cause low Coulombic efficiency, poor cycling life, and even potential safety hazards. In this study, a multifunctional diethyl sulfide electrolyte additive is proposed to synergistically construct a stable Li<sub>2</sub>S-rich solid electrolyte interphase (SEI) and Li<sub>2</sub>S/Li<sub>2</sub>SO<sub>4</sub>/Li<sub>2</sub>SO<sub>3</sub>-rich cathode electrolyte interphases (CEI), which could accelerate Li ions (Li<sup>+</sup>) transport kinetics and enhance the interfacial stability during long-term cycling. Moreover, the sulfur-rich composite in electrolyte interface could reduce the energy barrier for Li<sup>+</sup> desolvation and thereby enhance interface dynamics. Based on these merits, the introduction of 2.0 vol.% diethyl sulfide into a carbonate electrolyte (without FEC) enables the lithium anode to achieve a 7-fold enhancement in long-term cycling performance. More impressively, the Li||LiFePO<sub>4</sub> (LFP) pouch cell with the modified electrolyte achieves an outstanding capacity retention of 98.75% after 200 cycles at 0.1 C. The multifunctional diethyl sulfide additive paves the way for high-performance LMBs for practical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"88 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yi Yuan, Qiufeng Song, Linwen Lan, Xuefen Chen, Jiangchuan Du, Linjun Zhang, Nan Chen, Zhifa Shen, Chang Xue
Chemotherapy remains the cornerstone of malignant tumor treatment; however, off-target effects and severe systemic toxicity limit its efficacy. Here, we developed a programmable theranostic platform based on an all-in-one smart DNA nanodevice (SND) that integrates a programmable cancer-cell classifier (PCC) with a responsive delivery system (RDS). By employing a modular design that permits the customization of aptamer combinations for specific cancer cell types, the platform achieves accurate tumor recognition and spatially controlled drug release. Functioning as a dual-aptamer molecular guide, the PCC utilizes an interlocked configuration to identify cell-surface biomarkers in a stepwise manner, thereby ensuring highly specific target cell recognition. The RDS is constructed from a 1D central trunk flanked by double-stranded drug-loading units, a structure that confers high payload capacity and nuclease-enhanced resistance. These peripheral units also function as recognition elements for endogenous stimuli; upon activation, they trigger conformational changes that facilitate efficient intracellular drug release. In vivo studies in tumor-bearing mice demonstrate that this programmable theranostic platform selectively accumulates in tumor tissues, leading to marked inhibition of tumor growth and a substantial reduction in systemic toxicity. By integrating programmable molecular recognition with stimulus-responsive drug delivery, our theranostic platform offers a promising strategy for advancing targeted cancer therapy.
{"title":"An All-in-One DNA Nanodevice as a Programmed Theranostic Platform for Intelligent Cancer Cell Identification and On-Site Drug Release","authors":"Yi Yuan, Qiufeng Song, Linwen Lan, Xuefen Chen, Jiangchuan Du, Linjun Zhang, Nan Chen, Zhifa Shen, Chang Xue","doi":"10.1002/adfm.202531762","DOIUrl":"https://doi.org/10.1002/adfm.202531762","url":null,"abstract":"Chemotherapy remains the cornerstone of malignant tumor treatment; however, off-target effects and severe systemic toxicity limit its efficacy. Here, we developed a programmable theranostic platform based on an all-in-one smart DNA nanodevice (SND) that integrates a programmable cancer-cell classifier (PCC) with a responsive delivery system (RDS). By employing a modular design that permits the customization of aptamer combinations for specific cancer cell types, the platform achieves accurate tumor recognition and spatially controlled drug release. Functioning as a dual-aptamer molecular guide, the PCC utilizes an interlocked configuration to identify cell-surface biomarkers in a stepwise manner, thereby ensuring highly specific target cell recognition. The RDS is constructed from a 1D central trunk flanked by double-stranded drug-loading units, a structure that confers high payload capacity and nuclease-enhanced resistance. These peripheral units also function as recognition elements for endogenous stimuli; upon activation, they trigger conformational changes that facilitate efficient intracellular drug release. In vivo studies in tumor-bearing mice demonstrate that this programmable theranostic platform selectively accumulates in tumor tissues, leading to marked inhibition of tumor growth and a substantial reduction in systemic toxicity. By integrating programmable molecular recognition with stimulus-responsive drug delivery, our theranostic platform offers a promising strategy for advancing targeted cancer therapy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"38 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Julia S. Babkova, Ivan V. Zelepukin, Lyubov V. Gorelik, Anton L. Popov, Andrei I. Pastukhov, Gleb V. Tikhonowski, Maxim S. Savinov, Danil D. Kolmanovich, Nikita A. Pivovarov, Alina Yu. Kapitannikova, Anton A. Popov, Anna S. Sogomonyan, Vsevolod A. Skribitsky, Aziz B. Mirkasymov, Andrei V. Kabashin, Sergey M. Deyev
Transition metal nitrides are robust alternatives to noble metals in plasmonics, offering strong NIR absorption, high melting points, and chemical stability. Hafnium nitride (HfN) nanoparticles are especially promising owing to the high atomic number of hafnium, which could provide X-ray-based theranostic functionalities in addition to the prominent plasmonic properties. However, their biomedical potential has remained unexplored due to difficulties in synthesis of pure water-dispersible nanostructures. Here, we use femtosecond laser ablation in acetone to produce HfN-based nanoparticles exhibiting a red-shifted plasmon resonance spanning both the NIR-I and NIR-II windows. We then present the first in vivo assessment of the biocompatibility, photothermal performance, and radiosensitizing capacity of HfN-based nanomaterials. We show that PEGylated HfN nanoparticles exhibit negligible cytotoxicity across three cancer cell lines in vitro and no significant long-term adverse effects in healthy mice following intravenous administration. NIR-I photothermal therapy of 4T1 tumor-bearing mice after systemic nanoparticle administration leads to a 2.4-fold suppression of tumor growth and a significant extension of survival. The multimodal therapeutic potential of HfN is demonstrated by the enhanced efficacy of X-ray radiotherapy after local administration of nanoparticles. Laser ablated engineering of hafnium nitrides establishes this nanomaterial as a promising candidate for multimodal optical and radiosensitizing theranostics.
{"title":"Laser Engineering of HfN-Based Nanoparticles for Safe NIR-I Photothermal and X-ray Enhancing Cancer Therapies","authors":"Julia S. Babkova, Ivan V. Zelepukin, Lyubov V. Gorelik, Anton L. Popov, Andrei I. Pastukhov, Gleb V. Tikhonowski, Maxim S. Savinov, Danil D. Kolmanovich, Nikita A. Pivovarov, Alina Yu. Kapitannikova, Anton A. Popov, Anna S. Sogomonyan, Vsevolod A. Skribitsky, Aziz B. Mirkasymov, Andrei V. Kabashin, Sergey M. Deyev","doi":"10.1002/adfm.202529532","DOIUrl":"https://doi.org/10.1002/adfm.202529532","url":null,"abstract":"Transition metal nitrides are robust alternatives to noble metals in plasmonics, offering strong NIR absorption, high melting points, and chemical stability. Hafnium nitride (HfN) nanoparticles are especially promising owing to the high atomic number of hafnium, which could provide X-ray-based theranostic functionalities in addition to the prominent plasmonic properties. However, their biomedical potential has remained unexplored due to difficulties in synthesis of pure water-dispersible nanostructures. Here, we use femtosecond laser ablation in acetone to produce HfN-based nanoparticles exhibiting a red-shifted plasmon resonance spanning both the NIR-I and NIR-II windows. We then present the first in vivo assessment of the biocompatibility, photothermal performance, and radiosensitizing capacity of HfN-based nanomaterials. We show that PEGylated HfN nanoparticles exhibit negligible cytotoxicity across three cancer cell lines in vitro and no significant long-term adverse effects in healthy mice following intravenous administration. NIR-I photothermal therapy of 4T1 tumor-bearing mice after systemic nanoparticle administration leads to a 2.4-fold suppression of tumor growth and a significant extension of survival. The multimodal therapeutic potential of HfN is demonstrated by the enhanced efficacy of X-ray radiotherapy after local administration of nanoparticles. Laser ablated engineering of hafnium nitrides establishes this nanomaterial as a promising candidate for multimodal optical and radiosensitizing theranostics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"288 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Namuersaihan Namuersaihan, Zhiqiang Zhao, Oliver J. Conquest, Ying Shu, Haoyue Sun, Chunjing Su, Qi Cheng, Aloysius Soon, Catherine Stampfl, Jun Huang
The hydrogen evolution reaction (HER) in alkaline media is a promising strategy for sustainable hydrogen production, but the exploration of efficient and durable HER electrocatalysts is often hindered by the empirical and time-consuming nature of traditional synthesis. Herein, a machine learning (ML)–driven strategy combining Bayesian optimization is introduced to achieve the rational design of Ni3S4/Ni3Mo heterostructures for alkaline HER. By coupling predictive modeling with experimental feedback, this approach efficiently navigated a complex synthesis space and identified conditions yielding a structurally and electronically optimized catalyst. The optimized Ni3S4/Ni3Mo exhibits a vibrant morphological evolution—from compact buds to blooming petal-like structures—enabling enriched active sites and accelerated mass transport. Guided by Bayesian optimization, the optimized Ni3S4/Ni3Mo achieves a 10.5-fold enhancement in Cdl and delivers an exceptionally low overpotential of 18.2 mV at 100 mA cm−2, outperforming most reported transition-metal catalysts and even surpassing commercial Pt/C. Mechanistic insights from in situ Raman and DFT reveal that interfacial charge redistribution between Ni3S4 and Ni3Mo optimizes H* adsorption (ΔGH* ≈ 0.04 eV) and significantly reduces the water-dissociation barrier (0.08 eV), thereby accelerating reaction kinetics. This work demonstrates how the ML-guided optimization can synergistically couple morphology control, interfacial engineering with electronic tuning, offering a generalizable framework for intelligent catalyst discovery and mechanistic understanding in electrochemical energy conversion.
{"title":"Accelerated Discovery of High Performance Ni3S4/Ni3Mo HER Catalysts via Bayesian Optimization","authors":"Namuersaihan Namuersaihan, Zhiqiang Zhao, Oliver J. Conquest, Ying Shu, Haoyue Sun, Chunjing Su, Qi Cheng, Aloysius Soon, Catherine Stampfl, Jun Huang","doi":"10.1002/adfm.202528363","DOIUrl":"https://doi.org/10.1002/adfm.202528363","url":null,"abstract":"The hydrogen evolution reaction (HER) in alkaline media is a promising strategy for sustainable hydrogen production, but the exploration of efficient and durable HER electrocatalysts is often hindered by the empirical and time-consuming nature of traditional synthesis. Herein, a machine learning (ML)–driven strategy combining Bayesian optimization is introduced to achieve the rational design of Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo heterostructures for alkaline HER. By coupling predictive modeling with experimental feedback, this approach efficiently navigated a complex synthesis space and identified conditions yielding a structurally and electronically optimized catalyst. The optimized Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo exhibits a vibrant morphological evolution—from compact buds to blooming petal-like structures—enabling enriched active sites and accelerated mass transport. Guided by Bayesian optimization, the optimized Ni<sub>3</sub>S<sub>4</sub>/Ni<sub>3</sub>Mo achieves a 10.5-fold enhancement in <i>C</i><sub>dl</sub> and delivers an exceptionally low overpotential of 18.2 mV at 100 mA cm<sup>−2</sup>, outperforming most reported transition-metal catalysts and even surpassing commercial Pt/C. Mechanistic insights from in situ Raman and DFT reveal that interfacial charge redistribution between Ni<sub>3</sub>S<sub>4</sub> and Ni<sub>3</sub>Mo optimizes H* adsorption (Δ<i>G</i><sub>H*</sub> ≈ 0.04 eV) and significantly reduces the water-dissociation barrier (0.08 eV), thereby accelerating reaction kinetics. This work demonstrates how the ML-guided optimization can synergistically couple morphology control, interfacial engineering with electronic tuning, offering a generalizable framework for intelligent catalyst discovery and mechanistic understanding in electrochemical energy conversion.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"47 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sebastian Anhäuser, Ana M. Valencia, Sergei I. Ivlev, Marc Zeplichal, Andreas Terfort, Caterina Cocchi, Gregor Witte
Charge-transfer excitons (CTXs) at organic donor/acceptor interfaces are crucial intermediates for charge separation in photovoltaic devices. While blends used in real-world devices hamper detailed characterization of CTXs, atomistic models of cocrystals offer powerful alternatives for gaining microscopic insights. In this work, we investigate electronic and optical properties of acene-perfluoroacene cocrystals (anthracene, tetracene, and pentacene), combining experimental synthesis and characterization with first-principles calculations based on many-body theory. We prepare ultrathin cocrystals for polarization-resolved transmission-absorption spectroscopy, linking exciton polarization with molecular packing. Complementing this analysis, density-functional and many-body perturbation theory reveal complex excitonic landscapes that challenge several common assumptions about CTXs in weakly interacting donor-acceptor systems. For the studied cocrystals, we demonstrate that such CTXs are not limited to the absorption onset, but also occur at higher energy and produce sharp, intense absorption features. Adopting the intrinsic molecular coordinate system, we categorize the various excitons according to their polarization and show that the transition dipole moment of the lowest energy CTX is not necessarily aligned with the donor-acceptor stacking axis. We further characterize triplet excitons from first principles, which are only indirectly accessible experimentally. This work provides a deep understanding of CTXs in organic cocrystals, developing a refined conceptual framework that is crucial for future design of environmentally sustainable photoactive materials.
{"title":"Beyond the Edge: Charge-Transfer Excitons in Organic Donor-Acceptor Cocrystals","authors":"Sebastian Anhäuser, Ana M. Valencia, Sergei I. Ivlev, Marc Zeplichal, Andreas Terfort, Caterina Cocchi, Gregor Witte","doi":"10.1002/adfm.202530499","DOIUrl":"https://doi.org/10.1002/adfm.202530499","url":null,"abstract":"Charge-transfer excitons (CTXs) at organic donor/acceptor interfaces are crucial intermediates for charge separation in photovoltaic devices. While blends used in real-world devices hamper detailed characterization of CTXs, atomistic models of cocrystals offer powerful alternatives for gaining microscopic insights. In this work, we investigate electronic and optical properties of acene-perfluoroacene cocrystals (anthracene, tetracene, and pentacene), combining experimental synthesis and characterization with first-principles calculations based on many-body theory. We prepare ultrathin cocrystals for polarization-resolved transmission-absorption spectroscopy, linking exciton polarization with molecular packing. Complementing this analysis, density-functional and many-body perturbation theory reveal complex excitonic landscapes that challenge several common assumptions about CTXs in weakly interacting donor-acceptor systems. For the studied cocrystals, we demonstrate that such CTXs are not limited to the absorption onset, but also occur at higher energy and produce sharp, intense absorption features. Adopting the intrinsic molecular coordinate system, we categorize the various excitons according to their polarization and show that the transition dipole moment of the lowest energy CTX is not necessarily aligned with the donor-acceptor stacking axis. We further characterize triplet excitons from first principles, which are only indirectly accessible experimentally. This work provides a deep understanding of CTXs in organic cocrystals, developing a refined conceptual framework that is crucial for future design of environmentally sustainable photoactive materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenhui Cui, Shuaitong Liang, Junping Miao, Wenli Li, Hanwen An, Rongrong Yu, Juan Zhou, Ruiqi Shao, Zhiwei Xu
Molecular engineering of cellulose is essential for improving ionic conductivity and mechanical stability in solid polymer electrolytes. This work presents the first utilization of apocynum venetum, a drought-resistant biomass, as a sustainable source of cellulose nanofibers (CNFs) to investigate lithium-ion (Li+) transport mechanisms in composite polymer electrolytes for lithium metal batteries (LMBs). The reconstructed type II cellulose disrupts the polymer chain order by reorganizing hydrogen bonds and expanding amorphous regions, leading to a high Li+ transference number of 0.67 and an extended electrochemical window of 5.5 V. Operando synchrotron SAXS/WAXS reveals that CNFs modulate the structural evolution of the electrolyte and facilitate the formation of continuous Li+ conduction pathways within the amorphous phase. Through ion–dipole interactions among CNFs hydroxyl groups, PEO ether oxygens, and Li+, dynamic Li+─O coordination structures are formed, enhancing Li+ mobility. This work demonstrates the critical role of apocynum venetum-derived nanocellulose in enhancing the performance of bio-based polymer electrolytes.
{"title":"Operando SAXS/WAXS Reveals the Formation of Li+ Conduction Pathways Enabled by Apocynum Venetum-Derived Nanocellulose","authors":"Wenhui Cui, Shuaitong Liang, Junping Miao, Wenli Li, Hanwen An, Rongrong Yu, Juan Zhou, Ruiqi Shao, Zhiwei Xu","doi":"10.1002/adfm.202523000","DOIUrl":"https://doi.org/10.1002/adfm.202523000","url":null,"abstract":"Molecular engineering of cellulose is essential for improving ionic conductivity and mechanical stability in solid polymer electrolytes. This work presents the first utilization of apocynum venetum, a drought-resistant biomass, as a sustainable source of cellulose nanofibers (CNFs) to investigate lithium-ion (Li<sup>+</sup>) transport mechanisms in composite polymer electrolytes for lithium metal batteries (LMBs). The reconstructed type II cellulose disrupts the polymer chain order by reorganizing hydrogen bonds and expanding amorphous regions, leading to a high Li<sup>+</sup> transference number of 0.67 and an extended electrochemical window of 5.5 V. Operando synchrotron SAXS/WAXS reveals that CNFs modulate the structural evolution of the electrolyte and facilitate the formation of continuous Li<sup>+</sup> conduction pathways within the amorphous phase. Through ion–dipole interactions among CNFs hydroxyl groups, PEO ether oxygens, and Li<sup>+</sup>, dynamic Li<sup>+</sup>─O coordination structures are formed, enhancing Li<sup>+</sup> mobility. This work demonstrates the critical role of apocynum venetum-derived nanocellulose in enhancing the performance of bio-based polymer electrolytes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"23 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gout is a type of inflammatory arthritis resulting from abnormal uric acid (UA) metabolism. The core issue is elevated UA levels in the body, which cause the formation and accumulation of insoluble crystals in the joints or surrounding tissues, leading to a severe inflammatory response. Due to its complex causes, gout treatment faces challenges such as difficulty in achieving a complete cure and a high recurrence rate, which increases the risk of other systemic diseases. Functionalized biomaterials have been widely applied in the biomedical field and have demonstrated remarkable therapeutic potential, particularly for treating inflammatory diseases. Owing to their excellent biocompatibility and multiple bioactivities, these materials can effectively address multiple challenges faced in gout treatment. In this review, we categorize gout treatment into three aspects: UA degradation, inflammation reduction, and pain relief, and provide a systematic overview of the mechanisms and recent advancements in multifunctional biomaterials for managing gout from these three angles, emphasizing the importance of addressing gout-related pain and highlighting the current scarcity of research in this area. This review offers a novel perspective for optimizing the design and application of functionalized biomaterials, facilitating the development of more effective gout treatment strategies.
{"title":"Advanced Biomaterials Revolutionize Gout Therapy: From Uric Acid Degradation to Pain Alleviation","authors":"Jie Cao, Fei Gong, Zhihui Han, Xinyi Qiao, Xiang Cui, Liang Cheng","doi":"10.1002/adfm.202530174","DOIUrl":"https://doi.org/10.1002/adfm.202530174","url":null,"abstract":"Gout is a type of inflammatory arthritis resulting from abnormal uric acid (UA) metabolism. The core issue is elevated UA levels in the body, which cause the formation and accumulation of insoluble crystals in the joints or surrounding tissues, leading to a severe inflammatory response. Due to its complex causes, gout treatment faces challenges such as difficulty in achieving a complete cure and a high recurrence rate, which increases the risk of other systemic diseases. Functionalized biomaterials have been widely applied in the biomedical field and have demonstrated remarkable therapeutic potential, particularly for treating inflammatory diseases. Owing to their excellent biocompatibility and multiple bioactivities, these materials can effectively address multiple challenges faced in gout treatment. In this review, we categorize gout treatment into three aspects: UA degradation, inflammation reduction, and pain relief, and provide a systematic overview of the mechanisms and recent advancements in multifunctional biomaterials for managing gout from these three angles, emphasizing the importance of addressing gout-related pain and highlighting the current scarcity of research in this area. This review offers a novel perspective for optimizing the design and application of functionalized biomaterials, facilitating the development of more effective gout treatment strategies.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"32 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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