Journal of Materials Chemistry A最新文献

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Efficient synthesis of electroactive CoSe from a deep eutectic solvent 用深共晶溶剂高效合成电活性CoSe
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta05472b
Mikołaj Kozak,Oleg Tkachenko,Marta Gajewska,Mateusz M. Marzec,Łukasz Pięta,Krystian Sokołowski,Grzegorz D. Sulka,Agnieszka Brzózka
{"title":"Efficient synthesis of electroactive CoSe from a deep eutectic solvent","authors":"Mikołaj Kozak,Oleg Tkachenko,Marta Gajewska,Mateusz M. Marzec,Łukasz Pięta,Krystian Sokołowski,Grzegorz D. Sulka,Agnieszka Brzózka","doi":"10.1039/d6ta05472b","DOIUrl":"https://doi.org/10.1039/d6ta05472b","url":null,"abstract":"Transition metal selenides have been intensively investigated due to their promising applications in energy conversion and storage technologies. In line with this interest, the development of simple and cost-effective methods for synthesizing these materials directly on conductive substrates is highly desirable. Here, we report the preparation of CoSe2 films by pulse electrodeposition from a solution based on a Deep Eutectic Solvent (DES). The resulting material consists of a rough, grainy, amorphous cobalt diselenide layer deposited directly onto graphite foil without the need for binders or additional conductive additives. The electrochemical performance of the prepared CoSe2 films was examined in 5 M LiNO3 within the three different potential ranges. A mixed charge storage mechanism was evidenced, whereby the faradaic contribution remarkably decreased with narrowing of the potential window. Those findings were in full agreement with the material's post-mortem analysis, which indicated smaller degradation in a narrow potential range. The abovementioned measurements proved the suitability of the deposited CoSe2 as an electrode material for supercapacitors. The specific capacity, determined in 5 M LiNO3 in three-electrode configuration at 1 mV s−1 was 13.5 F g−1.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173194","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
Nitrogen-engineered covalent synergy in dual-layer encapsulated silicon anodes for superior initial coulombic efficiency 氮工程共价协同作用在双层封装硅阳极优越的初始库仑效率
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta06320a
Hong Liu,Xinhao Zhao,Xin Kong,Zhenhua Ge,Rui Bao,Junpeng Li
{"title":"Nitrogen-engineered covalent synergy in dual-layer encapsulated silicon anodes for superior initial coulombic efficiency","authors":"Hong Liu,Xinhao Zhao,Xin Kong,Zhenhua Ge,Rui Bao,Junpeng Li","doi":"10.1039/d6ta06320a","DOIUrl":"https://doi.org/10.1039/d6ta06320a","url":null,"abstract":"Commercialization of high-capacity silicon (Si) anodes is hampered by fragile physical contacts with the conductive matrix, which inevitably induce irreversible lithium consumption and low initial coulombic efficiency (ICE). To overcome this bottleneck, we first perform density functional theory (DFT) calculations, which predict that constructing nitrogen-induced Si–N–C covalent bridges at the Si/carbon interface dramatically enhances the Li+ adsorption energy (−5.28 eV) and redistributes the interfacial charge density, while synergistically lowering the diffusion barrier (0.9799 eV). Guided by these insights, we design an in situ chemical welding strategy using melamine as the nitrogen source to synthesize a dual-layer Si@SiOx/N-rGO composite. The optimized anode delivers an outstanding ICE of 93.01%, with a high initial discharge capacity of 2244.70 mAh g−1 at 0.1 A g−1 and retains 735.48 mAh g−1 after 500 cycles at 1.0 A g−1, significantly outperforming the undoped control. Multi-scale characterization (EIS-DRT and AFM) studies jointly demonstrate that the interfacial Si–N–C covalent bond acts as a mechanical anchor to suppress volume strain and SEI reconstruction, fundamentally reducing irreversible lithium loss and enhancing kinetics. This work provides atomic-scale insights into covalent interface design and gives a universally applicable, theory-guided strategy for high-energy-density lithium-ion batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"53 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152797","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
Beyond static energy-level alignment: multidentate molecular engineering of imidazophenanthroline scaffolds regulates charge separation at CsPbBr interfaces for selective photocatalysis 超越静态能级对准:咪唑菲罗啉支架的多齿分子工程调节CsPbBr界面的电荷分离,用于选择性光催化
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta05677f
Shivani Gupta,Megha,Himanshu Sonker,Ritika Gautam Singh,Vishal Govind Rao
{"title":"Beyond static energy-level alignment: multidentate molecular engineering of imidazophenanthroline scaffolds regulates charge separation at CsPbBr interfaces for selective photocatalysis","authors":"Shivani Gupta,Megha,Himanshu Sonker,Ritika Gautam Singh,Vishal Govind Rao","doi":"10.1039/d6ta05677f","DOIUrl":"https://doi.org/10.1039/d6ta05677f","url":null,"abstract":"Charge transfer at perovskite–molecule interfaces is commonly interpreted using static frontier energy-level alignment. However, this framework often fails to explain experimentally observed interfacial charge-transfer behaviour because it overlooks the decisive roles of molecular binding geometry, adsorption-induced electronic redistribution, and interfacial electronic coupling. Developing molecular design principles that can simultaneously control these factors remains a fundamental challenge for perovskite photocatalysis. Here, we demonstrate that multidentate imidazophenanthroline (ImPheZ) scaffolds regulate charge separation at CsPbBr3 perovskite interfaces through cooperative control of molecular anchoring, substituent electronics, and metal coordination. A library of electron-donating and electron-withdrawing ImPheZ ligands and their Ru(ii) and Ir(iii) complexes was rationally designed to establish structure–interfacial property relationships. Our spectroscopic, electrochemical, and theoretical studies reveal that efficient interfacial hole extraction is governed not simply by energetic driving forces. Instead, it arises from the synergistic interplay of multidentate binding, interfacial electronic coupling, and metal-induced charge redistribution. Electron-rich ligands, particularly L1, exhibit the most efficient charge separation, while metal coordination further reprograms binding modes and electronic communication, leading to enhanced interfacial charge transfer. These molecularly engineered interfaces translate directly into improved photocatalytic benzylamine oxidation, with the CsPbBr3-RuL1 hybrid achieving the highest conversion (38%) together with enhanced E/Z selectivity. Beyond demonstrating a new ligand platform for the CsPbBr3 system, this work establishes multidentate molecular engineering of ImPheZ scaffolds as an effective strategy for regulating charge separation at CsPbBr3 perovskite interfaces beyond conventional energy-level design. The principles developed here may be explored for other perovskite–molecule interfaces, providing a blueprint for the design of highly efficient and selective hybrid photocatalysts for solar-driven organic transformations.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"43 1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152798","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
Ultra-efficient rechargeable liquid and flexible zinc-air batteries enabled by cooperative functions of NiFe-MOF and single FeN4 sites 通过nfe - mof和单一FeN4位点的协同功能,实现了超高效的可充电液体和柔性锌空气电池
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta06861h
Yuqi Zhang,Jie Yang,Xuqian Zhao,Yinuo Su,Jianghao Kang,Xiaoya Qiao,Yu Chen,Xingming Ning,Ruibin Jiang
{"title":"Ultra-efficient rechargeable liquid and flexible zinc-air batteries enabled by cooperative functions of NiFe-MOF and single FeN4 sites","authors":"Yuqi Zhang,Jie Yang,Xuqian Zhao,Yinuo Su,Jianghao Kang,Xiaoya Qiao,Yu Chen,Xingming Ning,Ruibin Jiang","doi":"10.1039/d6ta06861h","DOIUrl":"https://doi.org/10.1039/d6ta06861h","url":null,"abstract":"Bifunctional oxygen electrocatalysts with low cost, high activity, and long-term durability hold critical significance for rechargeable zinc-air batteries (RZABs), yet the design of such catalysts still confronts enormous challenges. Herein, a novel bifunctional electrocatalyst consisted of NiFe metal-organic framework (NiFe-MOF) grown on carbon black with highly dispersed FeN4 single sites (NiFe-MOF/FeN4C) is reported for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) involved in liquid and flexible RZABs. The catalyst is prepared via the pyrolysis of hemin chloride adsorbed on carbon black, followed by the growth of NiFe-MOF through a hydrothermal method. The pyrolysis of hemin chloride produces single Fe atoms coordinated with four pyrrolic N atom onto carbon black. The grown NiFe-MOF has strong electronic interaction with the FeN4 sites. The cooperative effect between NiFe-MOF and FeN4C delivers outstanding bifunctional catalytic activity toward ORR and OER, with an ultrasmall potential gap of 0.64 V between half-wave potential of ORR and the potential at OER current density of 10 mA cm-2. Liquid RZAB assembled with NiFe-MOF/FeN4C shows an open-circuit potential (OCV) of 1.516 V, a peak power density of 173.2 mW cm-2, and outstanding cycling stability within 400 h (1200 cycles). The NiFe-MOF/FeN4C-based flexible solid-state RZAB also exhibits an OCV of 1.527 V, a peak power density of 103.1 mW cm-2, and stable operation at diverse bending angles. This work demonstrates a new strategy to improving the poor OER activity of single FeN4-based catalysts to obtain superior bifunctional OER and ORR catalysts for both liquid and flexible solid RZAB applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152049","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
Modification of Perovskite A-Site Cations to Achieve Near-Zero Oxygen Balance in High-Energy and Heat-Resistant Energetic Materials 改性钙钛矿a位阳离子在高能耐热含能材料中实现近零氧平衡
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta07378f
Caijin Lei,Yunfei An,Wei Hu,Jie Tang,Guangbin Cheng,Chuan Xiao,Hongwei Yang,Qinghua Zhang
{"title":"Modification of Perovskite A-Site Cations to Achieve Near-Zero Oxygen Balance in High-Energy and Heat-Resistant Energetic Materials","authors":"Caijin Lei,Yunfei An,Wei Hu,Jie Tang,Guangbin Cheng,Chuan Xiao,Hongwei Yang,Qinghua Zhang","doi":"10.1039/d6ta07378f","DOIUrl":"https://doi.org/10.1039/d6ta07378f","url":null,"abstract":"Perovskite-type energetic materials have emerged as promising alternatives to conventional nitro-rich heterocycles due to their rapid self-assembly and tunable performance. However, existing perovskite systems such as DAP-4 suffer from negative oxygen balance and high mechanical sensitivity. Herein, we report AMM-1, a novel ABX3 perovskite energetic material designed by replacing the A-site cation of DAP-4 with 3-(ammoniomethyl)morpholin-4-ium (H2amm 2+ ). This substitution reduces the carbon-to-oxygen ratio to achieve an oxygen balance of 1.8% and introduces additional N-H•••O hydrogen bonds (2.118 Å) that enhance mechanical stability. Moreover, AMM-1 exhibits excellent thermal stability (Td = 310 °C), low mechanical sensitivity (IS = 15 J, FS = 120 N). Its detonation velocity reaches 8700 m/s, surpassing conventional heatresistant explosives HNS (Dv: 7578 m/s) and TATB (Dv: 8033 m/s). This work demonstrates that A-site cation engineering is an effective strategy for developing high-performance, insensitive perovskite energetic materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"13 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152789","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
Fabricating highly active Ni/NiO bifunctional Janus heterojunctions for alkaline water electrolysis 制备高活性Ni/NiO双功能Janus异质结用于碱性电解
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-13 DOI: 10.1039/d6ta04765c
Shiyu Wen,Xiaoyan Guo,Yunfan Zhou,Yang Song,Yu Ying,Shun Yao,Shixiong Hao,Dong Cao,Daojian Cheng
{"title":"Fabricating highly active Ni/NiO bifunctional Janus heterojunctions for alkaline water electrolysis","authors":"Shiyu Wen,Xiaoyan Guo,Yunfan Zhou,Yang Song,Yu Ying,Shun Yao,Shixiong Hao,Dong Cao,Daojian Cheng","doi":"10.1039/d6ta04765c","DOIUrl":"https://doi.org/10.1039/d6ta04765c","url":null,"abstract":"Constructing Janus heterointerfaces is an effective strategy to change the electron cloud density of active sites, and thus largely optimizes the catalytic activity. Here, three types of transition metal/transition metal oxide nanoparticles with Janus heterointerfaces are constructed by an in situ separation of the active phase strategy. Notably, the Ni/NiO composite exhibits excellent activity in the basic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which only requires overpotentials of 57 and 237 mV to achieve 10 mA cm−2, respectively. Meanwhile, Ni/NiO assembled in an alkaline water electrolyzer shows 400 h durability under a current density of 500 mA cm−2, exhibiting negligible cell voltage loss. In situ measurement analyses reveal that the Ni/NiO heterointerfaces show a higher electron transfer rate in comparison to Co/CoO and Fe/Fe2O3, improving the kinetics of water splitting reaction. Further density functional theory calculations uncover that the electron transfer at Ni/NiO heterointerfaces optimizes the d-band center position of the Ni phase, leading to moderate adsorption energies for reactive intermediates, thereby facilitating the water splitting.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152795","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
Oxide-functionalized CuPc interfaces enable the development of efficient and stable inverted perovskite solar cells 氧化物功能化CuPc界面使高效稳定的倒钙钛矿太阳能电池得以发展
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-12 DOI: 10.1039/d6ta05903a
Xin Chen,Wenjie Cheng,Qingyuan Li,Zhibo Lin,Yaolong Xin,Jie Xu,Abuduwaili Mijiti,Lin Zheng,Xuan Wu,Yuhan Liu,Yong Peng,Li Yang,Jinbao Zhang
{"title":"Oxide-functionalized CuPc interfaces enable the development of efficient and stable inverted perovskite solar cells","authors":"Xin Chen,Wenjie Cheng,Qingyuan Li,Zhibo Lin,Yaolong Xin,Jie Xu,Abuduwaili Mijiti,Lin Zheng,Xuan Wu,Yuhan Liu,Yong Peng,Li Yang,Jinbao Zhang","doi":"10.1039/d6ta05903a","DOIUrl":"https://doi.org/10.1039/d6ta05903a","url":null,"abstract":"Inverted perovskite solar cells (PSCs) have achieved efficiencies exceeding 27%; however, their inferior operational stability is severely constrained by the hole contact interfaces. Herein, we propose an oxide-modified copper phthalocyanine (CuPc) hole transport layer (HTL), constructed via an Al2O3-coated CuPc bilayer architecture. The introduction of the Al2O3 interlayer effectively suppresses interfacial carrier recombination and greatly boosts the open-circuit voltage. Moreover, we employ (3-aminopropyl)triethoxysilane (APTES) for surface modification of Al2O3, which facilitates the preparation of homogeneous interlayers with superior uniformity. The orderly arranged terminal amino groups on APTES enable efficient passivation of perovskite interfacial defects and mitigate non-radiative charge recombination. By leveraging molecular-guided interface engineering, our devices attained a power conversion efficiency (PCE) of 23.62%, setting a new efficiency record for PSCs employing CuPc as the sole HTL. Most encouragingly, the resultant devices exhibit exceptional operational stability. The unencapsulated devices retain 98.1% of their original efficiency after 3000 h of continuous aging. This work verifies the great viability of molecularly guided interface engineering and provides insightful strategies for fabricating high-efficiency, durable perovskite solar cells.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152054","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
Influence of arylene diimide linker aromaticity on the electrochemical performance of redox-active metal–organic framework cathodes for lithium-ion storage 芳烯二亚胺连接剂芳香性对锂离子存储用氧化还原活性金属-有机骨架阴极电化学性能的影响
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-12 DOI: 10.1039/d6ta05048d
Catarina Ribeiro,Amol Kumar,Jonathan Caroni,Gioele García-Pinar,A. Nuno Guerreiro,João Rocha,M. Helena Braga,Joaquín Calbo,Sascha Ott,Manuel Souto
{"title":"Influence of arylene diimide linker aromaticity on the electrochemical performance of redox-active metal–organic framework cathodes for lithium-ion storage","authors":"Catarina Ribeiro,Amol Kumar,Jonathan Caroni,Gioele García-Pinar,A. Nuno Guerreiro,João Rocha,M. Helena Braga,Joaquín Calbo,Sascha Ott,Manuel Souto","doi":"10.1039/d6ta05048d","DOIUrl":"https://doi.org/10.1039/d6ta05048d","url":null,"abstract":"Organic electrode materials represent an attractive alternative to inorganic cathodes because they are based on abundant elements and offer tunable electrochemical performance through molecular design. Among them, metal–organic frameworks (MOFs) incorporating redox-active organic linkers have attracted considerable attention as electrode materials for metal-ion batteries. Herein, a series of isoreticular redox-active MOFs based on pyromellitic diimide (PMDI), naphthalene diimide (NDI), and perylene diimide (PDI) linkers were investigated as cathode materials for lithium-ion storage to elucidate the influence of arylene diimide aromaticity on electrochemical performance. Among the Zn-XDI (XDI = PMDI, NDI, PDI) MOFs, Zn-PDI and Zn-NDI exhibited excellent cycling stability, retaining 98% and 87% of their initial capacities after 500 cycles at 2C, respectively, whereas Zn-PMDI showed poor capacity retention, highlighting the importance of the aromatic core in stabilizing reduced states. Post-mortem X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction and Raman studies confirmed the preservation of the framework structure of Zn-PDI and Zn-NDI after extended cycling. Density functional theory (DFT) calculations revealed that increasing the aromatic core size in the Zn-XDI series stabilizes the reduced states, lowers the LUMO energy, enhances electron affinity, and facilitates Li+ uptake through the carbonyl oxygen atoms. These findings establish a direct relationship between linker aromaticity and electrochemical performance and provide molecular-level design principles for the development of high-performance redox-active MOF cathodes for sustainable energy storage.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151941","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
Breaking the trade-off in CrN thermoelectrics Ti doping: from room-temperature fabricated films to device-level performance 打破CrN热电Ti掺杂的权衡:从室温制备薄膜到器件级性能
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-12 DOI: 10.1039/d6ta04854d
Junya Kurahashi,Yi Shuang,Yuji Sutou
{"title":"Breaking the trade-off in CrN thermoelectrics Ti doping: from room-temperature fabricated films to device-level performance","authors":"Junya Kurahashi,Yi Shuang,Yuji Sutou","doi":"10.1039/d6ta04854d","DOIUrl":"https://doi.org/10.1039/d6ta04854d","url":null,"abstract":"Thermoelectric thin films capable of efficient energy conversion under low-temperature processing conditions are highly desirable for next-generation energy harvesting applications. Here, we report a Ti-doping strategy to modulate carrier transport in CrN thin films and achieve enhanced thermoelectric performance without high-temperature deposition. A maximum power factor of 5.26 µW cm−1 K−2, 250 times higher than undoped CrN, is realized by Ti doping at room temperature. Beyond material-level optimization, device-level evaluations demonstrate that the n-type Ti doped CrN device delivers high power output, while in-plane devices exhibit enhanced voltage generation arising from the combined Seebeck effect. Notably, the achieved power density is comparable to that of state-of-the-art thermoelectric thin films such as chalcogenide-based materials, despite the absence of high-temperature or epitaxy processing. These results establish nitride-based thin films as a competitive platform for thermoelectric energy conversion and provide a viable pathway toward high-performance devices compatible with scalable and flexible fabrication processes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"167 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152052","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
Electrodeposited Bismuth Nanomaterials as Binder Free and Scalable Catalysts for Highly Selective CO 2 to Formate Conversion 电沉积铋纳米材料作为无粘结剂和可扩展催化剂的高选择性co2到甲酸盐的转化
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-10-12 DOI: 10.1039/d6ta04799h
Anil Kumar Sihag,Yashraj Kumar Singh,Esraa Kotob,Sarah Zulfa Khairunnisa,Markus Ostermann,Olga Guselnikova,Markus Valtiner,Maryam Abdinejad,Christian M. Pichler
{"title":"Electrodeposited Bismuth Nanomaterials as Binder Free and Scalable Catalysts for Highly Selective CO 2 to Formate Conversion","authors":"Anil Kumar Sihag,Yashraj Kumar Singh,Esraa Kotob,Sarah Zulfa Khairunnisa,Markus Ostermann,Olga Guselnikova,Markus Valtiner,Maryam Abdinejad,Christian M. Pichler","doi":"10.1039/d6ta04799h","DOIUrl":"https://doi.org/10.1039/d6ta04799h","url":null,"abstract":"The design of binder-free catalyst materials that can be manufactured in a scalable manner and utilized in gas diffusion electrodes (GDEs) remains a critical bottleneck for further advancement of the CO2-to-formate electrolysis. Here, direct chronopotentiometric electrodeposition from a choline chloride:ethylene glycol deep eutectic solvent (DES) was applied to manufacture conformal, nanowirelike bismuth catalyst layers on commercial GDE substrates (Bi/GDE). These materials demonstrate a significantly improved catalytic activity per mass, compared with the conventional aqueous deposition method, as they showed uncompromised catalytic activity at a 6-times lower mass loading. Insight into the electrochemical surface restructuring mechanism was gained by combining ICP– MS dissolution analysis with in situ Raman spectroscopy. It could be shown, that both, DES and aqueous-derived, catalysts undergo an identical Bi2O3 → Bi2O2CO3 → Bi0 restructuring sequence, converging to a common hierarchical nanoflower active phase morphology with equivalent charge-transfer resistance, demonstrating that the activated state, not the initial morphology, governs selectivity. Both catalysts deliver high formate Faradaic efficiencies at 100 mA cm−2 (96.8% for the DES- and 93.7% for the aqueous-derived electrode), with the DES electrode achieving a mass-normalised activity for formate production of 166.9 mA mg−Bi1. The electrodeposition process could be scaled to 150 cm2 substrates while maintaining a formate Faradaic efficiency of 95.5%. Operation at 100 mA cm−2 is extended to 48 h of total elapsed time, corresponding to 32 h of cumulative electrolysis, through a periodic electrolysis swing protocol that mitigates GDE flooding, identified as the primary degradation pathway, while intrinsic catalyst stability showed no decline. This work establishes DES electrodeposition directly on GDE as a material-efficient and inherently scalable route to high-performance Bi/GDE catalysts, and reveals electrochemical activation history as the key design parameter for CO2-to-formate conversion.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"68 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152050","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
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