Journal of Materials Chemistry A最新文献_第3页

Flexocatalytic driven Water Splitting: Unprecedented Hydrogen Production by Symmetry invariant ZnIn2S4 Nanosheets 柔催化驱动的水分解：对称不变性ZnIn2S4纳米片史无前例的产氢

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-02 DOI: 10.1039/d5ta05386b

Jatin Mahajan, Shivali Dhingra, Anand Babu, Ajay Partap Singh Rana, Arpna Jaryal, Chandan Bera, Dipankar Mandal, Kamalakannan Kailasam

{"title":"Flexocatalytic driven Water Splitting: Unprecedented Hydrogen Production by Symmetry invariant ZnIn2S4 Nanosheets","authors":"Jatin Mahajan, Shivali Dhingra, Anand Babu, Ajay Partap Singh Rana, Arpna Jaryal, Chandan Bera, Dipankar Mandal, Kamalakannan Kailasam","doi":"10.1039/d5ta05386b","DOIUrl":"https://doi.org/10.1039/d5ta05386b","url":null,"abstract":"Flexocatalytic water splitting offers an intriguing avenue for “sustainable hydrogen” generation and has potential to overcome several inherent limitations of photocatalytic, electrocatalytic, and even piezocatalytic methods. In particular, flexocatalysis does not necessitate a non-centrosymmetric crystal structure, unlike piezocatalysis which allows to choose from a large materials database. In this context, centrosymmetric 2D zinc indium sulfide (ZnIn2S4) nanosheets were utilized as an active material for flexoelectric-driven water-splitting. Notably, utilizing methanol as a sacrificial agent under an ultrasonic frequency of 40 kHz, an unprecedented H2 evolution rate of 60 mmol g-1 h-1 (0.120 mmol h-1) was achieved without using a co-catalyst, demonstrating the practical viability of the ZnIn2S4 (ZIS) nanosheets. FEA (finite element analysis) simulation reveals that induced flexoelectric polarization developed over the ZIS nanosheets due to inhomogeneous stress distribution that facilitates the progressive water-splitting reaction. A series of control experiments with electrochemical impedance spectroscopy, and surface potential studies were conducted to bestow mechanistic insights into the flexocatalytic-driven water splitting over ZIS nanosheets. The density functional theory corroborates the experimental findings, revealing that applying stress on the catalyst lowers the Gibbs free energy, promoting H2 production over ZIS nanosheets. Thus, the present study presents the symmetry invariant pathway for transforming mechanical energy into H2 production, thereby paving the potential way for sustainable and economically feasible H2 production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203600","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}

引用次数: 0

Revisiting the Original 2003 Garnet-like Li-ion Conducting Solid Electrolytes Li5La3M2O12 (M = Nb, Ta, Nb/Ta): A Look into Phase Formation and the Identification of Carbonate and Alumina Contamination 重新审视2003年原始的石榴石状锂离子导电固体电解质Li5La3M2O12 (M = Nb, Ta, Nb/Ta)：碳酸盐和氧化铝污染的相形成和鉴定

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta06905j

Heather A Ritchie, Ioanna Maria Pateli, Oxana V. Magdysyuk, Aaron Naden, Heitor Secco Seleghini, Federico Grillo, Gavin Peters, Sharon Elizabeth Ashbrook, John Irvine, Venkataraman Thangadurai

{"title":"Revisiting the Original 2003 Garnet-like Li-ion Conducting Solid Electrolytes Li5La3M2O12 (M = Nb, Ta, Nb/Ta): A Look into Phase Formation and the Identification of Carbonate and Alumina Contamination","authors":"Heather A Ritchie, Ioanna Maria Pateli, Oxana V. Magdysyuk, Aaron Naden, Heitor Secco Seleghini, Federico Grillo, Gavin Peters, Sharon Elizabeth Ashbrook, John Irvine, Venkataraman Thangadurai","doi":"10.1039/d5ta06905j","DOIUrl":"https://doi.org/10.1039/d5ta06905j","url":null,"abstract":"Garnet-type electrolytes are a promising class of solid-state oxide materials for next-generation lithium batteries. In this study, parent-phase garnets, Li5La3M2O12 (M = Nb, Ta, Nb/Ta), were synthesised via solid-state reaction at 900 °C and 1100 °C, enabling comprehensive structural and chemical stability characterisation. Powder X-ray diffraction (PXRD) and Raman spectroscopy confirmed single-phase garnets with Ia¯3 d symmetry, while scanning electron microscopy (SEM) imaging revealed improved densification at 1100 °C. Electrochemical impedance spectroscopy showed the high ionic conductivities of 4.8 × 10⁻⁵ S cm⁻¹ at 55 °C for Nb and Ta co-substituted Li5La3NbTaO12 prepared at 1100 °C. X-ray photoelectron spectroscopy and thermogravimetric analysis identified a surface lithium carbonate layer formed under ambient conditions, which was not discussed in the original garnet reported in 2003. Solid-state nuclear magnetic resonance spectroscopy provided an insight into the lithium environment in the surface and bulk of the samples and confirmed aluminium contamination in samples sintered at the base of alumina crucibles at 1100 °C, with LaAlO3 identified as the dominant secondary phase, corroborated by PXRD, SEM, and energy dispersive X-ray spectroscopy analysis. Nb-doped garnet showed the most severe reaction with the alumina crucible. The use of a sacrificial mother powder of targeted garnet oxides, an approach commonly used for the preparation of Li-garnets, or sintering at 900 °C effectively reduced Al contamination. This work delivers a detailed evaluation of the parent-phase garnet, offering renewed insights into phase and structure two decades on from its initial development in 2003.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203541","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}

引用次数: 0

Bifunctional Electrocatalyst Engineered via Polyanionic Synergy and Heterointerface Modulation for Robust Seawater Electrolysis 通过聚阴离子协同作用和异质界面调制设计的双功能电催化剂用于稳健的海水电解

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta05443e

Fang Zheng, Zhenhua Fang, Mayur Anandrao Gaikwad, Suyoung Jang, Seyeon Cho, Jongsung Park, Jin Hyeok Kim

{"title":"Bifunctional Electrocatalyst Engineered via Polyanionic Synergy and Heterointerface Modulation for Robust Seawater Electrolysis","authors":"Fang Zheng, Zhenhua Fang, Mayur Anandrao Gaikwad, Suyoung Jang, Seyeon Cho, Jongsung Park, Jin Hyeok Kim","doi":"10.1039/d5ta05443e","DOIUrl":"https://doi.org/10.1039/d5ta05443e","url":null,"abstract":"The sustainable production of hydrogen (H2) through water electrolysis is a promising solution for renewable energy storage, yet its scalability is restricted by the scarcity of freshwater resources. Seawater electrolysis offers an alternative, but chloride-induced corrosion and chlorine evolution reactions hinder practical use. Here, we report an Fe-Ni layered double hydroxide/Co-doped nickel sulfide (LDH/Co-Ni3S2) hybrid electrocatalyst, engineered with a multi-anion synergistic interface. The electrocatalyst utilizes an interlayer carbonate (CO32⁻) in the LDH and in-situ generated sulfate (SO42⁻) from Co-Ni3S2 to form a double electric layer shielding effect, preventing Cl- penetration. In-situ Raman spectroscopy shows that FeNi-LDH partially converts to iron-nickel oxyhydroxide (FeNiOOH) during operation, which, with strong Lewis acidity, reduces hydroxide adsorption energy. The hybrid structure provides abundant active sites and efficient mass transport, achieving an OER overpotential of 451 mV at 500 mA cm⁻2 in alkaline seawater. The electrocatalyst demonstrated remarkable stability for 500 h at 500 mA cm⁻2 in 1 M KOH seawater, while also exhibiting 120 h of durability in the 6 M KOH seawater at the same current density. As a bifunctional electrocatalyst, it enables methanol-assisted seawater splitting at 1.68 V for 100 mA cm⁻2 with near-unity Faradaic efficiency, effectively suppressing chloride oxidation. This dual engineering strategy offers new insights for robust seawater-based H2 production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"82 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195490","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}

引用次数: 0

Leveraging the Ingenuity of Carbon Nanomaterials towards Water Quality Amelioration 利用碳纳米材料的独创性改善水质

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta05332c

Malini S S Bapat, Hema Singh, Shankar Bhausaheb Chaudhari, Suresh Shendage, Raj Kumar, Arun Karnwal, Deepak Kumar

{"title":"Leveraging the Ingenuity of Carbon Nanomaterials towards Water Quality Amelioration","authors":"Malini S S Bapat, Hema Singh, Shankar Bhausaheb Chaudhari, Suresh Shendage, Raj Kumar, Arun Karnwal, Deepak Kumar","doi":"10.1039/d5ta05332c","DOIUrl":"https://doi.org/10.1039/d5ta05332c","url":null,"abstract":"In this review, we explore carbon nanomaterial properties, synthesis pathways and their action in pristine/composite form(s) for the cause of water remediation. Water being the essence of life, upkeep of its quality is imperative for the health and development of all beings. With rapid urbanization, climate change, population growth and unsustainable practices, the availability and quality of water has been largely compromised. Carbonaceous nanomaterials are fascinating and possess exceptional properties with great potential for use in water quality amelioration. As per the UN Sustainable Development Goals (SDG 6), there is a need to design the right strategies for managing current water resources and making globally available safe and affordable drinking water. For recycling as well as treating wastewater for reuse we need technological developments which are balanced and consider the environmental, social, financial and health aspects of the society. Therefore, discussed in this review article is the structural features, preparation schemes along with the properties of the carbon materials and the mechanism of removal of impurities such as heavy metals, VOCs, oils, dyes, alkyl halides and common organic contaminants present in wastewater.The detrimental effect of these contaminants when present in water on humans too has been highlighted. This study presents a comprehensive overview of the carbon materials and their composites in various dimensions befitting the cause of water redressal.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"7 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203542","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}

引用次数: 0

Thermally-Driven Conformational Twist in Organic Azobenzene Linker Activates Molecular Doping Effect in Thin Films of Lanthanide MOFs 有机偶氮苯连接体中的热驱动构象扭曲激活镧系mof薄膜中的分子掺杂效应

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta05740j

Umashis Bhoi, Mini Kalyani, K. S. Ananthram, Sauvik Saha, Aradhana Acharya, Nahid Hassan, Minnu Raj, Kartick Tarafder, Nirmalya Ballav

{"title":"Thermally-Driven Conformational Twist in Organic Azobenzene Linker Activates Molecular Doping Effect in Thin Films of Lanthanide MOFs","authors":"Umashis Bhoi, Mini Kalyani, K. S. Ananthram, Sauvik Saha, Aradhana Acharya, Nahid Hassan, Minnu Raj, Kartick Tarafder, Nirmalya Ballav","doi":"10.1039/d5ta05740j","DOIUrl":"https://doi.org/10.1039/d5ta05740j","url":null,"abstract":"Azobenzene-based photo-switchable molecules have shown significant potential in stimuli-responsive systems, especially when incorporated into metal-organic frameworks (MOFs). This study reports thin films of lanthanide-based metal-organic frameworks (Ln-MOFs) with 4,4′-azobenzene dicarboxylic acid (H2ADA) as the organic linker – Tb-ADA, Eu-ADA, and Gd-ADA – using an electrodeposition method. Upon heating to 400 K, a reversible structural transition was observed via variable temperature grazing-incidence X-ray diffraction (GIXRD) and Raman spectroscopy, not due to trans-cis isomerization but rather a thermally-induced conformational twist of the ADA linker. Density functional theory (DFT) combined with molecular dynamics (MD) simulations supports this interpretation, revealing high-energy atropisomeric states stabilized by MOF confinement. Molecular doping of these films with 7,7,8,8-tetracyanoquinodimethane (TCNQ) significantly enhanced their electrical conductivity, increasing by two orders of magnitude at 400 K. This enhancement is attributed to improved π-π stacking and charge-transfer interactions facilitated by the conformational twist. Temperature-dependent X-ray photoelectron spectroscopy (XPS) confirmed redox activity in TCNQ@Tb-ADA films, showing reversible conversion between Tb(III) and Tb(IV), with back electron transfer at 400 K restoring Tb(III). These findings introduce a new mechanism of thermally-driven conformational switching in MOFs and open avenues for developing responsive electronic materials based on azobenzene linkers.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195158","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}

引用次数: 0

Significantly enhanced thermoelectric performance of a solution-processable organic polymer and carbon nanotube composite via molecular packing engineering 通过分子包装工程，显著提高了溶液可加工有机聚合物和碳纳米管复合材料的热电性能

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta05302a

Hongbin Chen, Jianrong Guo, Siqi Liu, Yijie Liu, Binting Huang, Yunxin Zhang, Yu Zhu, Xiangjian Cao, Guankui Long, Chaobin He

{"title":"Significantly enhanced thermoelectric performance of a solution-processable organic polymer and carbon nanotube composite via molecular packing engineering","authors":"Hongbin Chen, Jianrong Guo, Siqi Liu, Yijie Liu, Binting Huang, Yunxin Zhang, Yu Zhu, Xiangjian Cao, Guankui Long, Chaobin He","doi":"10.1039/d5ta05302a","DOIUrl":"https://doi.org/10.1039/d5ta05302a","url":null,"abstract":"Combining solution-processable organic polymers and carbon nanotubes (CNTs) with excellent electrical conductivity has been demonstrated to be an effective strategy to elevate thermoelectric performance. Nevertheless, the seriously inadequate attention given to constructing superior polymers and the ambiguous correlation between polymeric architectures and the thermoelectric properties of polymer/CNT composites largely impede the further improvement of thermoelectric parameters. Herein, three one-step synthetic organic polymers named BTC8, BTSC8 and BTSC12 are constructed with the same main building units but different alkyl side chains and molecular rigidity/planarity to reveal the significant structure–property relationship. The condensed alkyl chains and simultaneously enhanced rigidity/planarity could reduce electron reorganization energy, facilitate effective molecular packing and thus provide excellent charge transport channels in BTSC8/SWCNT based blend films, affording a superior power factor of 241.4 μW m−1 K−2 with satisfactory air stability compared to 188.8 and 159.7 μW m−1 K−2 for BTSC12 and BTC8 based blend films, respectively. Our work demonstrated that conjugated polymer/CNT based thermoelectric performance could be dramatically increased by balancing the trade-off between the Seebeck coefficient and electrical conductivity via molecular packing engineering such as improving molecular rigidity/planarity, reducing reorganization energy and strengthening molecular packing.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195196","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}

引用次数: 0

Phenanthro[9,10-d]imidazole-Based Hole Transport Materials for Perovskite Solar Cells: Influence of π-Bridge Units 钙钛矿太阳能电池用菲菲[9,10-d]咪唑基空穴传输材料：π桥单元的影响

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-10-01 DOI: 10.1039/d5ta05524e

BHIM RAJU TELUGU, Motonori Watanabe, Dai Senba, Chathuranganie A. M. Senevirathne, Yuki Fujita, Toshinori Matsushima

{"title":"Phenanthro[9,10-d]imidazole-Based Hole Transport Materials for Perovskite Solar Cells: Influence of π-Bridge Units","authors":"BHIM RAJU TELUGU, Motonori Watanabe, Dai Senba, Chathuranganie A. M. Senevirathne, Yuki Fujita, Toshinori Matsushima","doi":"10.1039/d5ta05524e","DOIUrl":"https://doi.org/10.1039/d5ta05524e","url":null,"abstract":"Hole transport materials (HTMs) play a critical role in achieving high efficiency and stability in perovskite solar cells (PSCs). In this study, we developed a series of easy-to-synthesize and cost-effective HTMs that exhibit excellent performance. These HTMs contain triphenylamine units substituted at the C6 and C9 positions of the phenanthro[9,10-d]imidazole (PTI-imidazole) core, which serves as the donor unit. Various π-conjugated units were introduced at the C2 position, including benzene (FDIMD-Ph and O-FDIMD-Ph), pyridine (O-FDIMD-Py), 2,2'-bithiophene (O-FDIMD-Th-Th), thieno[3,2-b]thiophene (O-FDIMD-TT), and dithieno[3,2-b:2',3'-d]thiophene (O-FDIMD-TTT). By modifying the π-linker, we tuned the optoelectronic properties of the materials. These materials have fused, planar and symmetrical structures have good solublity and promoted uniform film morphology. As a result, O-FDIMD-Ph achieved an average champion power conversion efficiency (PCE) of over 20.7%, outperforming spiro-OMeTAD (20.3%) based devices. Most HTMs retained ~95% of initial PCE after 500 hours of light exposure at 25 °C, except O-FDIMD-Py. Furthermore, thiophene-based π-linkers, including O-FDIMD-Th-Th, O-FDIMD-TT, and O-FDIMD-TTT, promote pronounced intermolecular interactions and strong π–π stacking, which contribute to the significantly enhanced thermal stability observed at 85 °C under continuous illumination. These results demonstrate that π-extension in PTI-imidazole-based HTMs is a promising strategy for developing efficient and stable PSCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195489","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}

引用次数: 0

Tuning the N-Intermediate Adsorption of Cu Catalyst for Efficient Electroreduction of Nitrate to Ammonia 调整Cu催化剂对n中间体的吸附以实现硝酸盐高效电还原制氨

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-09-30 DOI: 10.1039/d5ta06775h

Ruifang He, Lu Sun, Ke Ren, Xiaona Li, Peng Tian, Junwei Ye

{"title":"Tuning the N-Intermediate Adsorption of Cu Catalyst for Efficient Electroreduction of Nitrate to Ammonia","authors":"Ruifang He, Lu Sun, Ke Ren, Xiaona Li, Peng Tian, Junwei Ye","doi":"10.1039/d5ta06775h","DOIUrl":"https://doi.org/10.1039/d5ta06775h","url":null,"abstract":"Electrocatalytic nitrate reduction reaction (NO3RR) is a promising technique for both harmful nitrate removal and sustainable NH3 production. As yet, developing an electrocatalyst with high activity and stability remains a significant challenge. Herein, a novel electrocatalyst consisting of Cu nanoparticles dispersed on boron (B) and nitrogen (N) co-doped hollow carbon fibers (Cu/BNHCFs) was successfully fabricated. This was achieved through the stereoselective assembly of a Cu-containing zeolitic imidazolate framework onto electrospun fiber films, followed by pyrolysis. The optimized Cu/BNHCFs catalyst achieves a remarkable Faradaic efficiency of 94.2% for NH3 with a yield rate of 32.35 mg h-1 mgcat-1. Electrochemical in situ characterizations reveal that the reaction pathway on Cu/BNHCFs proceeds from *NO to *NH2OH. Theoretical calculations further indicate that B, N co-doped carbon support modulates the d-band center of Cu, effectively optimizing the adsorption/desorption processes of key nitrogen-containing intermediates to lead to the excellent catalytic performance. This work provides a design strategy for modifying the electronic structure of transition metal catalysts to achieve efficient nitrate reduction to ammonia.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"45 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189211","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}

引用次数: 0

Roles of Ru on PtRu Surface in Electrocatalytic Ammonia Oxidation Ru在PtRu表面电催化氨氧化中的作用

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-09-30 DOI: 10.1039/d5ta06040k

Geraldo Novaes Tessaro, Joelma Perez

{"title":"Roles of Ru on PtRu Surface in Electrocatalytic Ammonia Oxidation","authors":"Geraldo Novaes Tessaro, Joelma Perez","doi":"10.1039/d5ta06040k","DOIUrl":"https://doi.org/10.1039/d5ta06040k","url":null,"abstract":"Ammonia is both an efficient hydrogen carrier and a carbon-free fuel for direct use in fuel cells. Nevertheless, a poor understanding of the ammonia oxidation reaction (AOR) limits the development of efficient catalysts. Considering the scarcity of studies on Ru surfaces, this work compared AOR over PtRu/C, Pt/C, Ru/C, and RuO₂/C catalysts using high-surface area electrodes, together with online electrochemical mass spectrometry (OLEMS) and ion chromatography (IC) for detecting the gaseous and solution products, respectively. This approach allowed us to determine the reaction potentials of seven gaseous products over PtRu/C and Pt/C: N2, NO, N2H4, NH2OH, HN3, N2O, and NO2. The onset potential of N2 over PtRu/C was 100 mV lower than that over Pt/C. Although Ru/C and RuO2/C showed low AOR catalytic activity, small amounts of N2, NO, HN3, and N2O were still detected, with AOR onset at 0.30 V and 0.95 V for Ru/C and RuO2/C, respectively. These results suggest that the shift in AOR onset for PtRu/C is due to the presence of metallic Ru. The role of RuO2 was revealed at high potentials on Ru-based surfaces, with enhanced generation of oxygenated products in solution (NO2– and NO3–). Moreover, N₃⁻ was detected and quantified for the first time, suggesting a new approach for azide generation. The study's findings provide important mechanistic insights into the electrochemical behavior of Ru-based catalysts during ammonia oxidation, advancing the fundamental understanding of AOR and guiding the design of more efficient catalysts for ammonia fuel cells and the production of high-value-added products.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189153","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}

引用次数: 0

Interfacial Bond Engineering in Antimony Selenosulfide Solar Cells via Methylammonium Lead Bromide Perovskite Particles as Hole Transport Layer 以甲基铵-溴化铅-钙钛矿颗粒为空穴传输层的硒化锑太阳能电池界面键工程

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2025-09-30 DOI: 10.1039/d5ta05744b

Zequan Jiang, Xiaoqi Peng, Shuwei Sheng, Yawu He, Yuchen Li, Junjie Yang, Jianyu Li, Yue Hu, Changfei Zhu, Tao Chen, Hong Wang

{"title":"Interfacial Bond Engineering in Antimony Selenosulfide Solar Cells via Methylammonium Lead Bromide Perovskite Particles as Hole Transport Layer","authors":"Zequan Jiang, Xiaoqi Peng, Shuwei Sheng, Yawu He, Yuchen Li, Junjie Yang, Jianyu Li, Yue Hu, Changfei Zhu, Tao Chen, Hong Wang","doi":"10.1039/d5ta05744b","DOIUrl":"https://doi.org/10.1039/d5ta05744b","url":null,"abstract":"Antimony selenosulfide, Sb2(S,Se)3, materials have emerged as a prominent research hotspot in energy and optoelectronics fields, owing to their tunable band gap, excellent stability and one-dimensional crystal structures. Sb2(S,Se)3 solar cell devices usually adopt layered device structure where the hole transport layers (HTLs) play critical roles in affecting the device efficiency, operational stability, and charge carrier transport capabilities. Despite considerable advances in Sb2(S,Se)3 photovoltaics, their development remains constrained by an efficiency-stability trade-off primarily stemming from interfacial defects and thermal degradation of conventional HTLs such as Spiro-OMeTAD, which exhibit rapid performance decay under ambient conditions. Herein, methylammonium lead bromide (MAPbBr3) films are strategically designed as HTLs, leveraging their covalent Pb-S(Se) and Sb-Br interfacial bonds with Sb2(S,Se)3 to enhance charge extraction efficiency and passivate interfacial defects. Ultraviolet photoelectron spectroscopy (UPS) analysis reveals a cliff-like band alignment at the Sb2(S,Se)3/MAPbBr3 heterojunction interface, which effectively suppresses interfacial electron recombination. Furthermore, we demonstrate a record power conversion efficiency (PCE) of 9.37% in optimized solar cells, which represents the highest reported value for antimony chalcogenides/perovskite heterojunction solar cells. This study proposes a class of perovskite based HTLs that enables efficient interfacial band alignment, establishing a new paradigm for interface engineering in high-performance photovoltaic devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"94 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189159","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}

引用次数: 0