Chimin Song, Soonchul Kwon, Jungmin Lee, Yongmin Cho, Joohyung Lee
Ice accumulation on surfaces in cold environments poses persistent safety and operational challenges across diverse sectors, including transportation, aviation, outdoor equipment, residential buildings, and industrial facilities. In this study, we present a dual-mode de-/anti-icing platform that synergistically integrates the photothermal and electrothermal functionalities of Ga-based liquid metals (LMs). The photothermal component, consisting of micronized LM droplets hybridized with a phase change material (PCM), efficiently converts solar irradiation into heat while self-regulating surface temperature through latent heat absorption under varying seasonal conditions. Separately, the electrothermal component maintains LM continuity and is engineered with Si fillers to enable printable Joule heating with tunable electrical and thermal properties. Both components are formulated as viscoelastic pastes with excellent rheological processability, allowing direct and customizable application to diverse substrates. When sequentially integrated, the system demonstrates reliable and energy-efficient performance, achieving rapid surface heating and effective prevention of ice formation under simulated winter conditions, including overcast and nighttime scenarios. Owing to its ease of application and high performance, the system offers a practical and effective solution for ice management across diverse operational and environmental contexts.
{"title":"Light-On and Power-On: A Dual Mode Active De-/Anti-Icing System Using Liquid Metal-Based Photothermal and Electrothermal Pastes","authors":"Chimin Song, Soonchul Kwon, Jungmin Lee, Yongmin Cho, Joohyung Lee","doi":"10.1039/d5ta10376b","DOIUrl":"https://doi.org/10.1039/d5ta10376b","url":null,"abstract":"Ice accumulation on surfaces in cold environments poses persistent safety and operational challenges across diverse sectors, including transportation, aviation, outdoor equipment, residential buildings, and industrial facilities. In this study, we present a dual-mode de-/anti-icing platform that synergistically integrates the photothermal and electrothermal functionalities of Ga-based liquid metals (LMs). The photothermal component, consisting of micronized LM droplets hybridized with a phase change material (PCM), efficiently converts solar irradiation into heat while self-regulating surface temperature through latent heat absorption under varying seasonal conditions. Separately, the electrothermal component maintains LM continuity and is engineered with Si fillers to enable printable Joule heating with tunable electrical and thermal properties. Both components are formulated as viscoelastic pastes with excellent rheological processability, allowing direct and customizable application to diverse substrates. When sequentially integrated, the system demonstrates reliable and energy-efficient performance, achieving rapid surface heating and effective prevention of ice formation under simulated winter conditions, including overcast and nighttime scenarios. Owing to its ease of application and high performance, the system offers a practical and effective solution for ice management across diverse operational and environmental contexts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"5 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101884","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}
Surface vacancies play an important role in the chemistry of reducible oxides such as TiO2. It has been shown through experiments and quantum chemistry calculations that surface vacancies can trap precious metal atoms more effectively than pristine surfaces. In this study, we perform nanosecond timescale molecular dynamics (MD) and metadynamics simulations at 1000 K to probe the evolution of platinum metal atoms adsorbed at or adjacent to cationic and anionic surface vacancies on rutile titania (110). To this end, we employ machine learned interatomic potentials (MLIPs) that are iteratively trained on density functional theory (DFT) data. MD simulations show that Pt atom motion is subdiffusive across both anionic and cationic vacancies, indicating that these sites are thermally stable. Near-linear O-Pt-O motifs, found in earlier studies to be stable on the pristine surface of TiO2 are no longer stable in the vicinity of a vacancy. We utilize well-tempered, multiple walker metadynamics to map the free energy landscape of Pt migration out of the vacancy sites. The free energy barriers to Pt migration are highest for the cationic vacancy, followed by bridging oxygen and basal oxygen vacancies. The fact that Pt at the cationic vacancy site is most stable is encouraging because it has also been shown to be one of the most active sites for reactions such as CO oxidation.
{"title":"Impact of surface vacancies on the dynamics of metal atoms on reducible oxides: An enhanced sampling study with machine-learned potentials for Pt1/TiO2","authors":"Usama Saleem, Shaama Mallikarjun Sharada","doi":"10.1039/d5ta09561a","DOIUrl":"https://doi.org/10.1039/d5ta09561a","url":null,"abstract":"Surface vacancies play an important role in the chemistry of reducible oxides such as TiO<small><sub>2</sub></small>. It has been shown through experiments and quantum chemistry calculations that surface vacancies can trap precious metal atoms more effectively than pristine surfaces. In this study, we perform nanosecond timescale molecular dynamics (MD) and metadynamics simulations at 1000 K to probe the evolution of platinum metal atoms adsorbed at or adjacent to cationic and anionic surface vacancies on rutile titania (110). To this end, we employ machine learned interatomic potentials (MLIPs) that are iteratively trained on density functional theory (DFT) data. MD simulations show that Pt atom motion is subdiffusive across both anionic and cationic vacancies, indicating that these sites are thermally stable. Near-linear O-Pt-O motifs, found in earlier studies to be stable on the pristine surface of TiO<small><sub>2</sub></small> are no longer stable in the vicinity of a vacancy. We utilize well-tempered, multiple walker metadynamics to map the free energy landscape of Pt migration out of the vacancy sites. The free energy barriers to Pt migration are highest for the cationic vacancy, followed by bridging oxygen and basal oxygen vacancies. The fact that Pt at the cationic vacancy site is most stable is encouraging because it has also been shown to be one of the most active sites for reactions such as CO oxidation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"34 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101886","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}
Taimoor Raza, Sining Yun, Naveed Mushtaq, Muhammad Akbar, Abdullah Nasir, Yanbei Liu, Muhammad Qadeer, Rizwan Raza
High entropy perovskite oxides (HEPOs) possess transformative potential for electrochemical energy devices by facilitating unprecedented tunability in structure and functionality. Herein, we report the development of a conventional La2NiO4+δ (LNO) cathode and a novel A-site high entropy (La0.2Ca0.2Sr0.2Sm0.2Pr0.2)2NiO4+δ (HELNO) cathode as a highly active, bifunctional oxygen electrocatalyst for solid oxide fuel/electrolysis cells (SOFCs/SOECs). Systematic substitution of five equimolar cations at the A-site induces severe lattice distortion, thereby stabilizing and facilitating the mobility of oxygen defects, which synergistically enhance the oxygen reduction and evolution kinetics. In SOFC mode, the HELNO cathode achieves exceptional peak power densities of 1160, 939, 739, 509, and 310 mW cm−2 at temperatures of 650, 600, 550, 500, and 450 °C, respectively. For the OER in electrolysis, HELNO exhibits a low overpotential of 280 mV at 10 mA cm−2 and a reduced Tafel slope (88.4 mV dec−1), significantly outperforming LNO. Combined spectroscopic and electrochemical analyses confirm that entropy-driven lattice strain optimizes Ni valence states (Ni3+/Ni2+), enriches stable surface-active oxygen species, and accelerates ion diffusion. This study establishes high entropy Ruddlesden–Popper perovskites as a paradigm for next-generation bifunctional electrodes, illustrating the significant influence of entropy engineering on electrocatalytic activity and stability.
高熵钙钛矿氧化物（HEPOs）在结构和功能上具有前所未有的可调性，具有改变电化学能源装置的潜力。本文报道了传统La2NiO4+δ (LNO)阴极和新型a位高熵（La0.2Ca0.2Sr0.2Sm0.2Pr0.2）2NiO4+δ (HELNO)阴极作为固体氧化物燃料/电解电池（SOFCs/SOECs）的高活性双功能氧电催化剂的开发。5个等摩尔阳离子在a位的系统取代引起了严重的晶格畸变，从而稳定并促进了氧缺陷的迁移，从而协同增强了氧还原和进化动力学。在SOFC模式下，HELNO阴极在650、600、550、500和450℃的温度下分别达到了1160、939、739、509和310 mW cm - 2的峰值功率密度。对于电解中的OER， HELNO在10 mA cm−2时表现出280 mV的低过电位和降低的Tafel斜率（88.4 mV dec−1），明显优于LNO。结合光谱和电化学分析证实，熵驱动的晶格应变优化了Ni价态（Ni3+/Ni2+），丰富了稳定的表面活性氧，加速了离子扩散。本研究建立了高熵Ruddlesden-Popper钙钛矿作为下一代双功能电极的范例，说明了熵工程对电催化活性和稳定性的重要影响。
{"title":"Entropy-mediated lattice strain in a Ruddlesden–Popper perovskite oxide for highly active and bifunctional oxygen electrocatalysis","authors":"Taimoor Raza, Sining Yun, Naveed Mushtaq, Muhammad Akbar, Abdullah Nasir, Yanbei Liu, Muhammad Qadeer, Rizwan Raza","doi":"10.1039/d5ta08740f","DOIUrl":"https://doi.org/10.1039/d5ta08740f","url":null,"abstract":"High entropy perovskite oxides (HEPOs) possess transformative potential for electrochemical energy devices by facilitating unprecedented tunability in structure and functionality. Herein, we report the development of a conventional La<small><sub>2</sub></small>NiO<small><sub>4+<em>δ</em></sub></small> (LNO) cathode and a novel A-site high entropy (La<small><sub>0.2</sub></small>Ca<small><sub>0.2</sub></small>Sr<small><sub>0.2</sub></small>Sm<small><sub>0.2</sub></small>Pr<small><sub>0.2</sub></small>)<small><sub>2</sub></small>NiO<small><sub>4+<em>δ</em></sub></small> (HELNO) cathode as a highly active, bifunctional oxygen electrocatalyst for solid oxide fuel/electrolysis cells (SOFCs/SOECs). Systematic substitution of five equimolar cations at the A-site induces severe lattice distortion, thereby stabilizing and facilitating the mobility of oxygen defects, which synergistically enhance the oxygen reduction and evolution kinetics. In SOFC mode, the HELNO cathode achieves exceptional peak power densities of 1160, 939, 739, 509, and 310 mW cm<small><sup>−2</sup></small> at temperatures of 650, 600, 550, 500, and 450 °C, respectively. For the OER in electrolysis, HELNO exhibits a low overpotential of 280 mV at 10 mA cm<small><sup>−2</sup></small> and a reduced Tafel slope (88.4 mV dec<small><sup>−1</sup></small>), significantly outperforming LNO. Combined spectroscopic and electrochemical analyses confirm that entropy-driven lattice strain optimizes Ni valence states (Ni<small><sup>3+</sup></small>/Ni<small><sup>2+</sup></small>), enriches stable surface-active oxygen species, and accelerates ion diffusion. This study establishes high entropy Ruddlesden–Popper perovskites as a paradigm for next-generation bifunctional electrodes, illustrating the significant influence of entropy engineering on electrocatalytic activity and stability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098351","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}
Qing Cheng, Yuqi Zhang, Yingying Cao, Long Liu, Yanqiang Zhang
The novel ionic liquid-H2O2 propellants are urgently to solve the intrinsic ignition problem for achieving the aerospace applications. We addressed this issue by tuning the d-band center to adjust the catalyst's adsorption strength for IL/H2O2 toward the optimal value, thus enhancing catalytic activities for the efficient decomposition of H2O2 to generate reactive oxygen species. Herein, the regulation of the d-band center of Cu(I) in Cu(I)-MOF catalyst by precise ligand engineering design was studied. Remarkably, The Cu-S3 coordination of Cu-SH' shifts its d-band center closer to the Fermi level, promoting the adsorption of [BMIM]N(CN)2 and H2O2. Cu-SH' enables efficient H2O2 activation and robust •OH and 1 O2 generation to trigger the rapid self-ignition of [BMIM]N(CN)2-H2O2 propellant. The resulted tid as low as 18.4 ms is nearly 34% lower than that of homogeneous catalyst [FcCH2N(CH3)3]2[Cu2I4]. This work provides fundamental insights into the design of efficient ligand-based combustion catalysts for the higher performance of rockets and spacecrafts.
{"title":"Manipulating d-Band Center of Cu(I)-MOFs for Catalytic Ignition of [BMIM]N(CN) 2 IL-H 2 O 2 Propellants","authors":"Qing Cheng, Yuqi Zhang, Yingying Cao, Long Liu, Yanqiang Zhang","doi":"10.1039/d5ta09529h","DOIUrl":"https://doi.org/10.1039/d5ta09529h","url":null,"abstract":"The novel ionic liquid-H2O2 propellants are urgently to solve the intrinsic ignition problem for achieving the aerospace applications. We addressed this issue by tuning the d-band center to adjust the catalyst's adsorption strength for IL/H2O2 toward the optimal value, thus enhancing catalytic activities for the efficient decomposition of H2O2 to generate reactive oxygen species. Herein, the regulation of the d-band center of Cu(I) in Cu(I)-MOF catalyst by precise ligand engineering design was studied. Remarkably, The Cu-S3 coordination of Cu-SH' shifts its d-band center closer to the Fermi level, promoting the adsorption of [BMIM]N(CN)2 and H2O2. Cu-SH' enables efficient H2O2 activation and robust •OH and 1 O2 generation to trigger the rapid self-ignition of [BMIM]N(CN)2-H2O2 propellant. The resulted tid as low as 18.4 ms is nearly 34% lower than that of homogeneous catalyst [FcCH2N(CH3)3]2[Cu2I4]. This work provides fundamental insights into the design of efficient ligand-based combustion catalysts for the higher performance of rockets and spacecrafts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"290 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095957","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}
Photothermal synergistic catalysis, integrating light and heat, is an encouraging green strategy for various catalytic reactions, yet the fundamental role of light in governing activity remains unclear. Herein, using toluene oxidation as a model reaction, we investigated the light contribution at different wavelengths over an atomically dispersed Pd/H-TiO2 catalyst and observed dynamic structural changes on Pd and TiO2 active centers during toluene oxidation. In situ XPS and finite-difference timedomain (FDTD) simulations demonstrated two inverse electron-transfer pathways under UV and visible irradiation. Under visible light at 130 °C, high-energy hot electrons generated from Pd overcame the Schottky barrier and injected into TiO2 via Pd-O-Ti bridges to react with TiO2, inducing abundant oxygen vacancies. This process accelerated O2 activation and photogenerated carrier separation, generating more • O2 -than UV conditions and delivering 91.1% toluene conversion and 93.6% CO2 selectivity, comparable with UV-Vis conditions and far surpassing UV conditions. Conversely, free electrons produced from TiO2 under UV exposure transferred to Pd to increase its electron density, whereas these hardly altered the structure and reactivity of Pd/H-TiO2, leading to approximately 7.0% toluene conversion and CO2 yield. This work revealed the essential role of light at different wavelengths in promoting toluene degradation, guiding the design of efficient photothermal catalysts for VOCs remediation.
光热协同催化，整合光和热，是各种催化反应的一种令人鼓舞的绿色策略，但光在控制活性中的基本作用尚不清楚。本文以甲苯氧化为模型反应，研究了原子分散的Pd/H-TiO2催化剂上不同波长的光贡献，并观察了甲苯氧化过程中Pd和TiO2活性中心的动态结构变化。原位XPS和时域有限差分（FDTD）模拟显示了紫外和可见光照射下的两个逆电子转移路径。在130℃的可见光下，Pd产生的高能热电子克服肖特基势垒，通过Pd- o - ti桥注入到TiO2中，与TiO2发生反应，产生丰富的氧空位。该工艺加速了O2活化和光生载体分离，产生的•O2 -比紫外条件下更多，甲苯转化率为91.1%，CO2选择性为93.6%，与紫外-可见条件相当，远远超过紫外条件。相反，TiO2在紫外线照射下产生的自由电子转移到Pd上，增加了Pd的电子密度，而这些几乎没有改变Pd/H-TiO2的结构和反应性，导致约7.0%的甲苯转化率和CO2产率。本研究揭示了不同波长光在促进甲苯降解中的重要作用，指导了高效VOCs修复光热催化剂的设计。
{"title":"Unveiling Wavelength-Dependent Light Roles on Dynamic Structures for Photothermal Toluene Oxidation over Atomically Dispersed Pd/TiO2","authors":"Xin Wang, Maosen Xu, Jinhua Feng, De-Yun Ma, Weiping Zhang, Meicheng Wen, Hongli Liu","doi":"10.1039/d6ta00011h","DOIUrl":"https://doi.org/10.1039/d6ta00011h","url":null,"abstract":"Photothermal synergistic catalysis, integrating light and heat, is an encouraging green strategy for various catalytic reactions, yet the fundamental role of light in governing activity remains unclear. Herein, using toluene oxidation as a model reaction, we investigated the light contribution at different wavelengths over an atomically dispersed Pd/H-TiO2 catalyst and observed dynamic structural changes on Pd and TiO2 active centers during toluene oxidation. In situ XPS and finite-difference timedomain (FDTD) simulations demonstrated two inverse electron-transfer pathways under UV and visible irradiation. Under visible light at 130 °C, high-energy hot electrons generated from Pd overcame the Schottky barrier and injected into TiO2 via Pd-O-Ti bridges to react with TiO2, inducing abundant oxygen vacancies. This process accelerated O2 activation and photogenerated carrier separation, generating more • O2 -than UV conditions and delivering 91.1% toluene conversion and 93.6% CO2 selectivity, comparable with UV-Vis conditions and far surpassing UV conditions. Conversely, free electrons produced from TiO2 under UV exposure transferred to Pd to increase its electron density, whereas these hardly altered the structure and reactivity of Pd/H-TiO2, leading to approximately 7.0% toluene conversion and CO2 yield. This work revealed the essential role of light at different wavelengths in promoting toluene degradation, guiding the design of efficient photothermal catalysts for VOCs remediation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"14 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089454","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}
Bang Yuan, Min He, Qing Zhou, Ying Wang, Renheng Tang, Liming Zeng
Nickel-rich ternary layered oxides are mainstream cathode materials for highperformance lithium-ion batteries, but they face critical challenges (lattice oxygen release, Li⁺/Ni²⁺ cation mixing, microcrack propagation, and transition metal (TM) dissolution) during repeated charge-discharge cycles. Herein, we report a synergistic modification strategy for high-nickel oxides via spray-drying coupled with hightemperature solid-state reaction, enabling simultaneous Sm-containing oxide coating and Sm³⁺ lattice doping. Structural characterizations confirm uniform encapsulation by a thin Sm-based oxide layer, which suppresses TM dissolution and mitigates electrodeelectrolyte side reactions. DFT calculations and experimental analyses verify that Sm³⁺ substitutes partial Ni²⁺ sites in the lattice. This dual modification enhances structural integrity and enlarges interlayer spacing via a "pillaring effect," reducing the Li⁺ diffusion barrier. Electrochemically, the optimized Sm-modified cathode retains 94.5% of its initial capacity after 150 cycles at 1.0C (41.5% improvement over the unmodified sample) and exhibits excellent rate capability (153.49 mAh•g⁻¹ at 10C). This work provides a promising avenue for the rational design of high-stability, high-rate nickelrich cathodes for advanced lithium-ion batteries.
{"title":"Rare earth-Mediated Synergistic Lattice Stabilization and Interface Protection for Suppressed Phase Transition and Superior Electrochemical Performance in Ni-Rich Cathodes","authors":"Bang Yuan, Min He, Qing Zhou, Ying Wang, Renheng Tang, Liming Zeng","doi":"10.1039/d5ta09882c","DOIUrl":"https://doi.org/10.1039/d5ta09882c","url":null,"abstract":"Nickel-rich ternary layered oxides are mainstream cathode materials for highperformance lithium-ion batteries, but they face critical challenges (lattice oxygen release, Li⁺/Ni²⁺ cation mixing, microcrack propagation, and transition metal (TM) dissolution) during repeated charge-discharge cycles. Herein, we report a synergistic modification strategy for high-nickel oxides via spray-drying coupled with hightemperature solid-state reaction, enabling simultaneous Sm-containing oxide coating and Sm³⁺ lattice doping. Structural characterizations confirm uniform encapsulation by a thin Sm-based oxide layer, which suppresses TM dissolution and mitigates electrodeelectrolyte side reactions. DFT calculations and experimental analyses verify that Sm³⁺ substitutes partial Ni²⁺ sites in the lattice. This dual modification enhances structural integrity and enlarges interlayer spacing via a \"pillaring effect,\" reducing the Li⁺ diffusion barrier. Electrochemically, the optimized Sm-modified cathode retains 94.5% of its initial capacity after 150 cycles at 1.0C (41.5% improvement over the unmodified sample) and exhibits excellent rate capability (153.49 mAh•g⁻¹ at 10C). This work provides a promising avenue for the rational design of high-stability, high-rate nickelrich cathodes for advanced lithium-ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"26 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089455","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}
FeCoCrMnZn) 3 O 4 high entropy oxide samples were prepared through solid state synthesis route involving two major steps viz., ball milling and annealing. One sample (HEO1) was prepared via 12 hours of ball milling and 5 hours of air annealing at 1000°C, while the other sample (HEO2) was prepared via 3 hours of ball milling and 12 hours of air annealing at 1000°C. Structural, morphological and compositional analysis of both the samples were done by XRD, FTIR, HRTEM, SAED FESEM and EDS measurements. XANES and EXAFAS measurements and detail analysis have been done to establish the possible compositions of both the samples and their relative stability has been estimated by theoretical calculations, both empirically and by using DFT. Lithium-ion half cells were prepared using both the samples as anodes and battery performances were tested by galvanostatic charge-discharge (GCD) measurements. It has been found that the HEO sample prepared with shorter ball milling and longer annealing (HEO2) shows better cycle performance as anode of Li ion battery at high current than that prepared with longer ball milling and shorter annealing (HEO1). Finally, operando XANES measurements have been carried out during discharging of HEO anodes to obtain insight into the role of various cations during the lithiation process of the HEO. The detail structural, morphological and electrochemical insight into (FeCoCrMnZn)₃O₄ HEO material prepared by solid state synthesis route, while applied as high capacity anodes in Li ion batteries, as presented in this manuscript, will be very useful in the pursuit for new and novel electrode materials for Li ion batteries.
{"title":"Ex-situ and operando investigations on (FeCoCrMnZn) 3 O 4 High Entropy Oxide as Anode for Li ion battery","authors":"Sidhartha Sankar Sahoo, Chandrani Nayak, Ravi Kumar, Ankita Pathak, Seemita Banerjee, Jitendra Bahadur, Himanshu Srivastava, Dibyendu Bhattacharyya","doi":"10.1039/d5ta08614k","DOIUrl":"https://doi.org/10.1039/d5ta08614k","url":null,"abstract":"FeCoCrMnZn) 3 O 4 high entropy oxide samples were prepared through solid state synthesis route involving two major steps viz., ball milling and annealing. One sample (HEO1) was prepared via 12 hours of ball milling and 5 hours of air annealing at 1000°C, while the other sample (HEO2) was prepared via 3 hours of ball milling and 12 hours of air annealing at 1000°C. Structural, morphological and compositional analysis of both the samples were done by XRD, FTIR, HRTEM, SAED FESEM and EDS measurements. XANES and EXAFAS measurements and detail analysis have been done to establish the possible compositions of both the samples and their relative stability has been estimated by theoretical calculations, both empirically and by using DFT. Lithium-ion half cells were prepared using both the samples as anodes and battery performances were tested by galvanostatic charge-discharge (GCD) measurements. It has been found that the HEO sample prepared with shorter ball milling and longer annealing (HEO2) shows better cycle performance as anode of Li ion battery at high current than that prepared with longer ball milling and shorter annealing (HEO1). Finally, operando XANES measurements have been carried out during discharging of HEO anodes to obtain insight into the role of various cations during the lithiation process of the HEO. The detail structural, morphological and electrochemical insight into (FeCoCrMnZn)₃O₄ HEO material prepared by solid state synthesis route, while applied as high capacity anodes in Li ion batteries, as presented in this manuscript, will be very useful in the pursuit for new and novel electrode materials for Li ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"81 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089458","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}
Thermal and strain recognition is a promising modality for wearable electronics and human-machine interfaces, taking advantage of its natural, efficient, and userdistinctive characteristic. However, current sensing materials are typically limited by structural rigidity, functional constraints, and significant external power dependency, hindering their practical applications. This work proposes a unique strain-thermal sensing mechanism based on a planar interdigitated thermogalvanic hydrogel (PITH), integrating MXene interdigitated electrodes with a polyacrylamide (PAAm)-Fe(CN)₆³⁻/⁴⁻ hydrogel. Operating under a temperature gradient, this self-powered device responds to hand-writing motions, thereby enabling real-time capture of subtle writing dynamics. Distinct from resistive strain-based designs, the PITH employs a strain-thermal coupling mechanism, where mechanical strain modulates the hydrogel's redox kinetics, thereby influencing thermoelectric voltage output and establishing a direct strain-voltage correlation. Through random forest algorithm processing dynamic 2 voltage signals, discriminative feature is extracted, achieving high recognition accuracy (99.09% for letters, 97.85% for digits) under entirely passive operation. This study presents a structurally integrated, fully self-powered, and signal-programmable flexible handwriting recognition device, which is important for developing next-generation low-power wearable HMI systems.
{"title":"Machine Learning-Enabled Planar Interdigitated Thermogalvanic Hydrogel for Synergistic Thermal and Strain Sensing","authors":"Qi Hu, Hao Wu, Chunxuan Yu, Hao Xiao, Chen Shen, Zhaoquan Zhao, Yuan Yao, Xuelin Yong, Xing Liang, Hongwei Wu, Xiaoze Du, CHENG CHI","doi":"10.1039/d5ta08892e","DOIUrl":"https://doi.org/10.1039/d5ta08892e","url":null,"abstract":"Thermal and strain recognition is a promising modality for wearable electronics and human-machine interfaces, taking advantage of its natural, efficient, and userdistinctive characteristic. However, current sensing materials are typically limited by structural rigidity, functional constraints, and significant external power dependency, hindering their practical applications. This work proposes a unique strain-thermal sensing mechanism based on a planar interdigitated thermogalvanic hydrogel (PITH), integrating MXene interdigitated electrodes with a polyacrylamide (PAAm)-Fe(CN)₆³⁻/⁴⁻ hydrogel. Operating under a temperature gradient, this self-powered device responds to hand-writing motions, thereby enabling real-time capture of subtle writing dynamics. Distinct from resistive strain-based designs, the PITH employs a strain-thermal coupling mechanism, where mechanical strain modulates the hydrogel's redox kinetics, thereby influencing thermoelectric voltage output and establishing a direct strain-voltage correlation. Through random forest algorithm processing dynamic 2 voltage signals, discriminative feature is extracted, achieving high recognition accuracy (99.09% for letters, 97.85% for digits) under entirely passive operation. This study presents a structurally integrated, fully self-powered, and signal-programmable flexible handwriting recognition device, which is important for developing next-generation low-power wearable HMI systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"5 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089457","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}
The effective monitoring and selective removal of hexavalent chromium (Cr(VI)) are critical for aquatic environmental remediation and human health protection. Herein, a series of binary and ternary covalent organic frameworks (COFs) containing donor–acceptor linkages or hydroxyl nanotraps were synthesized via a molecular engineering strategy for simultaneous detection, selective adsorption, and photocatalytic reduction of Cr(VI). The optimized ternary COF (BTD-OH-COF) outperformed binary COFs containing only adsorptive or photocatalytic groups, exhibiting enhanced fluorescence properties, a rapid response to Cr(VI), and a limit of detection of 68 nmol L−1. Moreover, with its dual adsorption and photocatalytic functionalities, the BTD-OH-COF achieves a Cr(VI) removal efficiency of 99.9% under simulated sunlight irradiation without the use of sacrificial agents. Its removal efficiency was approximately 1.50 times higher than those of binary COFs, respectively. Theoretical and experimental results confirm that constructing hydroxyl adsorption sites with donor–acceptor photoactive units synergistically enhances adsorption capacity while significantly reducing the energy gaps, thereby facilitating electron–hole separation and boosting photocatalytic activity. This study provides novel design principles for bifunctional monitoring/photocatalytic materials and offers an innovative approach for remediating heavy metal pollution in water.
{"title":"Rational design of multivariate covalent organic frameworks with enhanced light-harvesting for selective detection and photocatalytic reduction of Cr(VI)","authors":"Zhenyu Lu, Xue Liu, Xiaohui Zhu, Li Yang, Hao Lu, Binbin Zhang, Xing Kang, Mingrong Yue, Yunjiang Yu","doi":"10.1039/d5ta09339b","DOIUrl":"https://doi.org/10.1039/d5ta09339b","url":null,"abstract":"The effective monitoring and selective removal of hexavalent chromium (Cr(<small>VI</small>)) are critical for aquatic environmental remediation and human health protection. Herein, a series of binary and ternary covalent organic frameworks (COFs) containing donor–acceptor linkages or hydroxyl nanotraps were synthesized <em>via</em> a molecular engineering strategy for simultaneous detection, selective adsorption, and photocatalytic reduction of Cr(<small>VI</small>). The optimized ternary COF (BTD-OH-COF) outperformed binary COFs containing only adsorptive or photocatalytic groups, exhibiting enhanced fluorescence properties, a rapid response to Cr(<small>VI</small>), and a limit of detection of 68 nmol L<small><sup>−1</sup></small>. Moreover, with its dual adsorption and photocatalytic functionalities, the BTD-OH-COF achieves a Cr(<small>VI</small>) removal efficiency of 99.9% under simulated sunlight irradiation without the use of sacrificial agents. Its removal efficiency was approximately 1.50 times higher than those of binary COFs, respectively. Theoretical and experimental results confirm that constructing hydroxyl adsorption sites with donor–acceptor photoactive units synergistically enhances adsorption capacity while significantly reducing the energy gaps, thereby facilitating electron–hole separation and boosting photocatalytic activity. This study provides novel design principles for bifunctional monitoring/photocatalytic materials and offers an innovative approach for remediating heavy metal pollution in water.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"43 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089456","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}
Carlota Auria-Soro, Nuria Cruz-Navarro, César Luis Folcia, Isabel Sobrados, Alfonso Martinez-Felipe, M. Blanca Ros, Amin Sharifi Haddad
Two new tetraethylene glycol (TEG)-containing bent-core molecules reveal as suitable versatile supramolecular building blocks to form liquid crystalline phases and organogels in novel structured soft-electrolytes. New amphiphilic bent-core molecules [TEG-Bx-10-14], composed of a short polar TEG-segment capping well-defined bent-core mesogenic-like structures, and a set of their [1/1] complexes with TfO - and Tf2N -/ lithium and sodium salts, [MA-TEG-Bx-10-14], have been investigated for the first time. FT-IR, 13 C CP-MAS-NMR and 1 H MAS-NMR studies at variable temperature indicate the selective complexation of the cations in the TEG-regions. Whilst the new four-block bent-core designs [TEG-10-Bx-14] do not exhibit liquid crystal order, most of their complexes with lithium salts [MA-TEG-10-Bx-14] stabilize an attractive number of bent-core lamellar mesophases (SmCP, HNF-like, USmCP and Colob). Diffusion coefficients D of lithium, favoured with the liquid crystal phase transition, have been estimated by solid state NMR spectroscopy. Direct current values of sdc~ 10 -4 S•cm -1 in the mid-high frequency range were found using dielectric spectroscopy, highlighting the potential of bent-core building blocks as organic and nanostructured soft-electrolytes containing both lithium and sodium cations, whose ionic conductivities can be optimised through composition and annealing.
{"title":"New nanostructured ion-conductive bent-core liquid crystals containing lithium and sodium salts as soft electrolyte candidates","authors":"Carlota Auria-Soro, Nuria Cruz-Navarro, César Luis Folcia, Isabel Sobrados, Alfonso Martinez-Felipe, M. Blanca Ros, Amin Sharifi Haddad","doi":"10.1039/d5ta09556e","DOIUrl":"https://doi.org/10.1039/d5ta09556e","url":null,"abstract":"Two new tetraethylene glycol (TEG)-containing bent-core molecules reveal as suitable versatile supramolecular building blocks to form liquid crystalline phases and organogels in novel structured soft-electrolytes. New amphiphilic bent-core molecules [TEG-Bx-10-14], composed of a short polar TEG-segment capping well-defined bent-core mesogenic-like structures, and a set of their [1/1] complexes with TfO - and Tf2N -/ lithium and sodium salts, [MA-TEG-Bx-10-14], have been investigated for the first time. FT-IR, 13 C CP-MAS-NMR and 1 H MAS-NMR studies at variable temperature indicate the selective complexation of the cations in the TEG-regions. Whilst the new four-block bent-core designs [TEG-10-Bx-14] do not exhibit liquid crystal order, most of their complexes with lithium salts [MA-TEG-10-Bx-14] stabilize an attractive number of bent-core lamellar mesophases (SmCP, HNF-like, USmCP and Colob). Diffusion coefficients D of lithium, favoured with the liquid crystal phase transition, have been estimated by solid state NMR spectroscopy. Direct current values of sdc~ 10 -4 S•cm -1 in the mid-high frequency range were found using dielectric spectroscopy, highlighting the potential of bent-core building blocks as organic and nanostructured soft-electrolytes containing both lithium and sodium cations, whose ionic conductivities can be optimised through composition and annealing.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"42 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089812","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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