{"title":"Interface M-O-Fe (M=Ru, Rh, Pd, Ag) Bonding Excitation Stabilized Bifunctional Electrocatalysts for Water Splitting","authors":"Mingjing Ma, Huanhuan Yu, Baolin Zhu, Wenjun Zheng, Shoumin Zhang","doi":"10.1039/d5ta04249f","DOIUrl":"https://doi.org/10.1039/d5ta04249f","url":null,"abstract":"The design of efficient catalysts with atom clusters (ACs) and single atoms (SAs) as active sites for water splitting presents an effective approach for improving bifunctional electrocatalytic performance by synergistically promoting electron transport and proton transfer kinetics. In this work, a series of Fe2O3-supported noble metal catalysts (M = Ru, Rh, Pd, Ag) incorporating both ACs and SAs sites were developed, with detailed characterization identifying Ru ACs as the primary active centers. The designed-interfacial M-O-Fe bonds play a critical role in charge redistribution, subsequently enhancing electron and proton transfer kinetics. The resulting heterostructure optimizes both the electronic environment and active site accessibility, yielding exceptional electrocatalytic performance. Further density functional theory calculations demonstrate that the incorporation of Ru species leads to increased filling of antibonding orbitals and modulation of the d-band center, subsequently reducing the energy barrier of the rate-determining steps to −0.267 eV for HER and 1.522 eV for OER, respectively. Consequently, the representative Ru/Fe2O3 with Ru content of 1.1 wt.% achieves an OER overpotential of 189 mV and a HER overpotential of 21 mV at a current density of 10 mA cm−2. This study highlights a novel approach to the design of advanced bifunctional electrocatalysts by engineering interfacial bridge bonds.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"25 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685124","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}
Anu Renjith, V. Lakshminarayanan, Harish C. Barshilia
{"title":"Repurposing PVA-based slime to address electrolyte challenges in portable electrochemical devices","authors":"Anu Renjith, V. Lakshminarayanan, Harish C. Barshilia","doi":"10.1039/d5ta03449c","DOIUrl":"https://doi.org/10.1039/d5ta03449c","url":null,"abstract":"Application-oriented materials are being developed at a rapid pace, each providing enhanced properties compared to the existing options. While it is evident that these materials are proven to contribute positively to the intended application, they are often not translated to commercial utilization due to multiple reasons. Some of the reasons are the lack of ready availability of raw materials, their high cost or the requirement of multistep procedures of synthesis. In some cases, the reported shelf life of the material was evaluated only for a short span or has been studied under simulated accelerated conditions, which may vary in real-life scenarios. All these factors pose significant hurdles to their commercialization. Under such circumstances, repurposing appropriate commercially available materials, which exhibit enhanced shelf life and cost-effectiveness for novel applications, presents a feasible route to reduce the time required for commercial deployment. This perspective paper focuses on the scope of repurposing poly vinyl alcohol (PVA)-based slime as an electrolyte for portable electrochemical devices. An electrochemical measurement necessitates the presence of adequate salts for ionic conductivity. The conventional liquid electrolytes cause corrosion when spilled or seeped into the underlying surface. A spill-proof electrolyte with adequate flow properties is crucial for the development of <em>in situ</em> electrochemical probes. The gel electrolytes, which are currently being explored widely, have their own challenges. Originally marketed as a sensory toy, due to its low cost, inert, biocompatible nature, strippability, and long shelf life, slime has the potential to be used as an electrolyte because of the fact that borax in it provides sufficient ionic conductivity. Thus, PVA-based slime with its unique combination of characteristics is a potential material to be explored as another alternative to liquid electrolyte and conventional polymeric gels. However, to date, the medium has only been engineered from the perspective of improving mechanical properties to suit applications. This work analyzes the perspective of engineering slime medium for enhanced flow properties to achieve high ionic conductivity and conformability while retaining its strippability and spill-proof nature.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"14 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685119","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}
Shuang Wang, Xiaowa Nie, Chunshan Song, Xinwen Guo
{"title":"Rational Design of Metal Node-modified Ti-Based MOFs for Selective Photoreduction of Carbon Dioxide to Ethanol by Computational Screening","authors":"Shuang Wang, Xiaowa Nie, Chunshan Song, Xinwen Guo","doi":"10.1039/d5ta03415a","DOIUrl":"https://doi.org/10.1039/d5ta03415a","url":null,"abstract":"In this work, density functional theory (DFT) calculations were conducted to investigate a series of metal node-modied Ti-MOF catalysts using transition metals (Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ru, Rh, Pd, Hf, Ta, W, Os, Ir, Au) introduced into Ti-ATA (ATA = 2-aminoterephthalic acid) for the photocatalytic reduction of CO2 to C2 products. CO2 can be sufficiently activated on Ti(M)-ATA but the adsorption configuration depends on the nature of M. Over Ti(Nb)-ATA, Ti(Ta)-ATA, Ti(Zr)-ATA and Ti(Hf)-ATA, the two *CHO species undergo C-C coupling to form *CHOCHO, the important C2 intermediate. Ti(Nb)-ATA and Ti(Ta)-ATA tend to generate ethanol, while Ti(Zr)-ATA and Ti(Hf)-ATA are more selective to ethylene. Among the Ti(M)-ATA candidates studied, Ti(Nb)-ATA was identified as the most active catalyst for CO2 reduction to ethanol due to its smallest limiting free energy change (1.12 eV), over which the *CH2CH2O reduction to *CH2CH2OH was found to be the rate-determining step. The correlation curve analysis illustrates that the reduction activity of Ti(M)-ATA catalysts is highly dependent on the binding strength of CO2 and key reaction intermediate such as *OCHOH. The analysis of electronic and optical properties indicates that the altered energy band structure and charge transfer behavior around the bimetallic nodes of Ti(Nb)-ATA account for its excellent catalytic activity for CO2 reduction to ethanol.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 7 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685114","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}
Liju Bai, Xiaotong Jiang, Yimin Deng, Shuai Wang, Helei Liu
{"title":"Amine-functionalized CNTs@mSiO2 with short radical mesochannels for fast and efficient CO2 capture","authors":"Liju Bai, Xiaotong Jiang, Yimin Deng, Shuai Wang, Helei Liu","doi":"10.1039/d5ta04410c","DOIUrl":"https://doi.org/10.1039/d5ta04410c","url":null,"abstract":"Amine functionalized adsorbents exhibit significant potential for CO2 capture due to their high efficiency and selectivity. However, their practical application remains constrained by the limited adsorption capacity and slow adsorption kinetics. Herein, we demonstrated an ethylenediamine (ED) functionalized mesoporous silica coated carbon nanotubes (CNTs@mSiO2-ED) composites for fast and efficient CO2 capture. The novel adsorbent was synthesized through a two-step process, consisting of the synthesis of mesoporous silica coated carbon nanotubes (CNTs@mSiO2) as amine carriers via an interfacial self-assembly strategy, followed by amine functionalization using a vapor deposition method. Both the carriers and final adsorbents possess abundant short radical mesochannels, offering direct and ultra-short diffusion paths for amine during functionalism and CO2 for adsorption. As a result, the CNTs@mSiO2-ED adsorbent achieved a maximum CO2 adsorption capacity of 68 mL g-1 (~ 3 mmol g-1, at 298 K, 1 bar) and facile uptake of CO2 reaching a t50 (being the time to achieve 50% of the maximum adsorption capacity) of 1.93 min, 1.70 times higher and 1.32 times faster than for ED-functionalized SBA-15, respectively. This work opens up a new avenue for the design of CO2 adsorption materials to overcome the adsorption and reaction kinetics limitations of other solid porous materials envisaged.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684960","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}
{"title":"Viscoelasticity-Controllable Dynamic Borate Polydimethylsiloxane Network For Enhancing Energy Dissipation of Elastomers","authors":"Fu-Long Gong, Shuang Long, Wenqing Lv, Xiaotong Shu, Bin Huang, ping ping Lou, Huafeng Fei, Zhijie Zhang","doi":"10.1039/d5ta04308e","DOIUrl":"https://doi.org/10.1039/d5ta04308e","url":null,"abstract":"Borosiloxane-based materials, such as polyborosiloxane (PBS) are ideally utilized as impact-protective materials due to the shear-stiffening behaviors, providing effective protection against injury. Current strategies rely on blending them with functional fillers or scaffolds to enhance impact-protective performance or achieve specific functionalities. However, the unclear structure-property relationships of borosiloxane-based materials have hindered their further development. Herein, we utilize a viscoelasticity-controllable dynamic borate PDMS network (PPDBS) for constructing PPDBS/PDMS double-network elastomers (SSEs) that exhibiting excellent energy dissipation property. The ultrahigh energy dissipation characteristic of SSEs are attributed to the rapid characteristic relaxation and high internal friction inherent to the network. We found that SSEs not only exhibit excellent damping property (tan δ>0.3) over a broad frequency (0.01 Hz-50 Hz) and temperature range (-20 °C-140 °C), but also demonstrate superior impact-protective performance compared with most commercial materials, including PBS. This work opens up a new avenue for the design of high-performance impact-protective and damping materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"108 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685122","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}
Akash Gupta, Young Jun Rho, Wei-Chen Lin, Dinesh K. Patel, Chi-Te Liang, Mukesh Kumar Thakur, Ilka Kriegel, Francesco Di Stasio, Sang Hyun Lee, Yong Il Park
{"title":"Graphene-Templated Hybrid Prussian Blue-MXene Nanocomposites for Broadband Photodetection with Ultra-High Carrier Generation","authors":"Akash Gupta, Young Jun Rho, Wei-Chen Lin, Dinesh K. Patel, Chi-Te Liang, Mukesh Kumar Thakur, Ilka Kriegel, Francesco Di Stasio, Sang Hyun Lee, Yong Il Park","doi":"10.1039/d5ta04050g","DOIUrl":"https://doi.org/10.1039/d5ta04050g","url":null,"abstract":"A graphene template provides a unique opportunity to combine nanomaterial building blocks on its surface for versatile optoelectronic applications. Herein, a low-cost, facile, and non-toxic nanocomposite of 2D metallic MXene (MX) and Prussian blue (PB) on a graphene template is reported. The MX nanosheets are exfoliated from the MAX phase via HF etching and are decorated with semiconducting PB by using a novel one-step in-situ method. This conjugation effectively anchors PB to MX, thereby enhancing the light absorption and providing a significant 19-fold increase in fluorescence quenching due to direct charge transfer. The PB@MX nanocomposite is then coated onto the graphene template to fabricate a heterostructured photodetector (PD) that exhibits enhanced photocurrent and highly sensitive broadband photodetection across the 325−808 nm range. The nanocomposite-based PD exhibits a remarkable photocurrent of 47.97 µA, a high photoresponsivity of 14,880 A W<small><sup>−1</sup></small>, a detectivity of 3.72 × 10<small><sup>12</sup></small> cm Hz<small><sup>–1/2</sup></small> W<small><sup>–1</sup></small>, and a normalized gain of 4.15 × 10<small><sup>−4</sup></small> m<small><sup>2</sup></small> V<small><sup>−1</sup></small> under 450 nm illumination at 31.84 µW cm<small><sup>−2</sup></small> and 1 V. These values represent the best performance reported to date for this class of nanohybrids, thus highlighting the potential of this PD for real-world electronic applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685116","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}
{"title":"In-situ borate generation by amorphous Ni-Fe-B nanosheets: a highly active electrocatalyst for oxygen generation in alkaline seawater","authors":"Li He, Zhengwei Cai, Chaolin Wang","doi":"10.1039/d5ta04010h","DOIUrl":"https://doi.org/10.1039/d5ta04010h","url":null,"abstract":"Seawater electrolysis is a highly attractive route for sustainable hydrogen production, yet it demands oxygen evolution reaction (OER) catalysts with exceptional activity and long-term stability. Herein, we report an in-situ fabricated amorphous NiFeB nanoshee-modified nickel foam (NiFeB/NF) as an efficient and durable OER catalyst. Experimental and theoretical results confirm the excellent catalytic performance of NiFeB. In alkaline seawater, NiFeB/NF achieves current densities of 100 and 1000 mA cm-2 at low overpotential of 280 and 350 mV, respectively, and maintains stable performance over 300 h. Notably, the catalyst also exhibits excellent OER activity across a range of operational conditions.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685117","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}
{"title":"A facile strategy to design shape memory rubber composites with tunable mechanical properties and photothermal performance","authors":"Xiao Wang, Jiahui Zhang, Xiaoting Li, Huiwen Yu, Lingcao Tan, Qiongyao Wang, Wenhua Xu, Baiping Xu, Shuping Xiao, Jiarong Huang","doi":"10.1039/d5ta03812j","DOIUrl":"https://doi.org/10.1039/d5ta03812j","url":null,"abstract":"Shape memory polymers (SMPs) represent a prominent category of smart polymers that show attractive prospects in emerging fields of soft robots and biomedical devices. However, most of the existing SMPs show limitations in single-stimulus responsiveness and an imbalance between mechanical and shape memory properties. Herein, biological phytic acid served as a natural curing agent to vulcanize the biobased epoxidized natural rubber (ENR), while Fe3+ was introduced to construct a second cross-linked network based on coordination interaction. Polycaprolactone (PCL) was introduced and acted as net points to regulate the shape fixing behavior, while the dual cross-linked network provided strong resilience to achieve the shape recovery performance. Meanwhile, the Fe3+-based coordination complex not only served as sacrificial elements to realize tunable mechanical properties by effectively dissipating energy, but also acted as a photothermal agent to realize the light-induced shape memory behavior and thermoelectric power generation. The fabricated composites process multi-stimuli-responsive shape memory properties, photothermal capabilities, and tunable mechanical properties, exhibiting outstanding potential in harvesting sunlight for outdoor portable power generation and stimuli-responsive sensors.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"31 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684958","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}
Mahla Sarfaraz Khabbaz, Anupma Thakur, Dipak Maity, Sepideh Biabanialitappeh, Bhargava Mortha, Joshua P. McKay, Gerardo Parada, Mangilal Agarwal, Honghu Zhang, Xin Zhang, Jonathan David Bazak, Xiaoliang Wei
{"title":"A Polysulfide/Ferricyanide Redox Flow Battery with Extended Cycling","authors":"Mahla Sarfaraz Khabbaz, Anupma Thakur, Dipak Maity, Sepideh Biabanialitappeh, Bhargava Mortha, Joshua P. McKay, Gerardo Parada, Mangilal Agarwal, Honghu Zhang, Xin Zhang, Jonathan David Bazak, Xiaoliang Wei","doi":"10.1039/d5ta05404d","DOIUrl":"https://doi.org/10.1039/d5ta05404d","url":null,"abstract":"The inexpensive sulfur raw material is promising to enable cost-effective redox flow batteries for long duration energy storage. But the catastrophic through-membrane crossover of polysulfides remains a severe challenge resulting in irreversible performance degradation and short cycle life. In this work, we demonstrate that use of a permselective cation exchange membrane yields two orders of magnitude enhancement in polysulfide retention compared to the benchmark Nafion membrane. Combined physico-chemical, spectroscopic, and microscopic analyses unravel smaller ion transport channel sizes in the microstructure of this membrane that contribute to the effective mitigation of polysulfide crossover. As a result, the cycle life of polysulfide/ferricyanide flow cells is boosted over a substantially extended test time. This finding sheds light on the fundamental membrane factors that cause polysulfide permeation and can suggest feasible directions in the development of permselective membranes for polysulfide flow batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"108 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685115","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}
{"title":"Nano-Molybdenum Oxide Modified Expanded Graphite for High performance Lithium-ion Batteries","authors":"Changzhun Huang, Zhendong Liu, Fei Wang, Anbang Lu, Dai Dang, Quanbing Liu, Chengzhi Zhang","doi":"10.1039/d5ta04651c","DOIUrl":"https://doi.org/10.1039/d5ta04651c","url":null,"abstract":"Graphite anodes for lithium-ion batteries still faces practical challenges, including the limitation of theoretical specific capacity and sluggish lithium-ion storage kinetics, which correspond to low-energy-density and unsatisfactory fast-charging performance. Nano-molybdenum oxide (nano-MoO3), exhibiting high theoretical specific capacity, work function and excellent stability, represents a promising modification agent for graphite anode to enhanced electrochemical performance. Herein, this study developed the nano-MoO3 decorated within the bulk and surfaces of expanded graphite anode material (nMO-EG). The reversible conversion reactions between nano-MoO3 and lithium enhances the specific capacity of nMO-EG, achieving a high capacity of 701.9 mAh g−1. A stable solid electrolyte interphase film, enriched with inorganic Li2O and LiF, was formed on the surface of the nMO-EG anode, attributing to a reversible capacity of 613.8 mAh g−1 and superior cycling stability over 600 cycles. The expanded layer of nMO-EG anode exhibits a low lithium-ion diffusion energy barrier of 0.15 eV, which enhances its fast-charging capability that delivers a reversible specific capacity of 236.3 mAh g−1 at 5 A g−1. This study provides new insights into the stability of the graphite modification and provides a promising alternative for high-energy-density and fast-charging graphite anode materials in lithium-ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"278 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685121","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}