Journal of Materials Chemistry A最新文献

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Construction of phosphonitrile derivative-hybridized EPDM dense crosslinked networks for enhanced mechanics and ablation resistance 构建膦腈衍生物杂化三元乙丙橡胶致密交联网络,增强力学性能和抗烧蚀性能
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d5ta00056d
Shumeng Wang, Jian Wang, Xutao Ma, Zhaoqi Niu, Zongwu Zhang, Peibo Xu, Beixi Chen, Xiaoyan Ma, Shishan Yang, Xiao Hou
{"title":"Construction of phosphonitrile derivative-hybridized EPDM dense crosslinked networks for enhanced mechanics and ablation resistance","authors":"Shumeng Wang, Jian Wang, Xutao Ma, Zhaoqi Niu, Zongwu Zhang, Peibo Xu, Beixi Chen, Xiaoyan Ma, Shishan Yang, Xiao Hou","doi":"10.1039/d5ta00056d","DOIUrl":"https://doi.org/10.1039/d5ta00056d","url":null,"abstract":"With the development of aerospace technology, the thermal insulation layer between the engine casing and the propellant needs to have excellent mechanical and ablative resistance properties to meet higher environmental requirements. Herein, two novel reactive phosphonitrile derivatives containing P and N heteroatoms, namely, hexa(2-allylphenoxy) cyclotriphosphonitrile (HAPPCP) and hexa(3-ethynylphenylamino) cyclotriphosphonitrile (HEACP), were designed and synthesized to crosslink with EPDM for modulating its chain structure on a molecular scale, forming P- and N-atom hybridized EPDM dense crosslinked networks, which collectively improve the mechanical and ablative resistance. Results showed that HEACP was more effective for boosting the overall performance, accompanied by improvements of 64.6% and 89.2% in tensile strength and breaking elongation, respectively, and reductions of 52.6% and 33.1% in the linear ablation rate and mass ablation rate, respectively. The ablation-condensed phase, microscopic carbon crystal structure, and the gas-phase thermal barrier mechanism were investigated to elucidate the ablative resistance mechanism.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"37 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806259","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
Two-Dimensional Conductive Mesopore Engineering of Ultrahigh Content Covalent Sulfur-Doped Carbon for Superior Sodium Storage
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d5ta01526j
Jie He, Zhihao Sun, Lei Huang, Zijia Zhu, Wei Luo, Dongliang Chao, Fanxing Bu
{"title":"Two-Dimensional Conductive Mesopore Engineering of Ultrahigh Content Covalent Sulfur-Doped Carbon for Superior Sodium Storage","authors":"Jie He, Zhihao Sun, Lei Huang, Zijia Zhu, Wei Luo, Dongliang Chao, Fanxing Bu","doi":"10.1039/d5ta01526j","DOIUrl":"https://doi.org/10.1039/d5ta01526j","url":null,"abstract":"Ultrahigh content (>20 wt%) covalent sulfur-doped carbons (USC) exhibit significant potential as cathode materials for sodium-sulfur batteries. Despite sulfur-based redox reactions offering high capacity, their reaction kinetics is limited by poor activity of robust covalent C-S bond, and tardy ion and electron transport in carbon matrixes. Here, we report one novel 2D mesoporous USC vertically grown on Ti3C2 nanosheet (MesoUSC@Ti3C2) heterostructure, which shows a 2D hexagonal structure, a high surface area (~256 m2 g-1) and abundant covalent sulfur content (~26.2 wt% in USC). Spectroscopic characterizations and kinetics analysis reveal that the 2D conductive mesoporous engineering strategy efficiently activate C-S bonds, and accelerate ion and electron transfer, confering USC high capacity sodium ion storage with pseudocapacitive-like behavior. As a result, the obtained MesoUSC@Ti3C2 delivers a high capacity of 950 mAh g–1 at 0.1 A g–1 and superior rate performance of 463 mAh g–1 at 5 A g–1. This work opens up new ways to promote the practical applications of sulfur-doped carbon-based materials for advanced energy storage systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"25 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806266","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
Immobilize Simulated Am-Np-RE-Pu Product Waste from Trialkyl Phosphine Oxide process in Natural Granite-Based Aluminum Silicate Glass or Glass-Ceramic
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d4ta07751b
Jiaqin Wei, Xiaoyan Shu, Wenhong Han, Ran Tan, Mingfen Wen, Zhanqiang Li, Xirui Lu
{"title":"Immobilize Simulated Am-Np-RE-Pu Product Waste from Trialkyl Phosphine Oxide process in Natural Granite-Based Aluminum Silicate Glass or Glass-Ceramic","authors":"Jiaqin Wei, Xiaoyan Shu, Wenhong Han, Ran Tan, Mingfen Wen, Zhanqiang Li, Xirui Lu","doi":"10.1039/d4ta07751b","DOIUrl":"https://doi.org/10.1039/d4ta07751b","url":null,"abstract":"The immobilization of nuclear waste can effectively reduce the possible harm of radioactive waste to human survival. In this study, preferred natural granite was used to prepare aluminosilicate glass or glass-ceramic for immobilizing simulated Am-Np-RE-Pu product waste from trialkyl phosphine oxide (TRPO) process. The phase evolution, microstructure, physical and chemical stability of the waste forms were researched. The results indicated that the waste cations mainly incorporated by the glass network or stable oxyapatite crystals. The lattice binding force and the interface effect inhibited the waste cations from escaping out of the glassy bulk. After 42d leaching, the normalized leaching rates of Ce, Nd, and La in glass-ceramic reached ~10-7 g m-2 d-1, ~10-8 g m-2 d-1, ~10-7 g m-2 d-1, respectively. This study demonstrated that the preferred natural granite showed considerable potential in effectively immobilize high-level radioactive waste rich in rare earth elements.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"29 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806261","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
Multimetallic assembly of concave-shaped rectangular Mn4 clusters as efficient hydrogen evolution electrocatalysts
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d5ta01854d
Chandan Sarkar, Aditi De, Arindam Gupta, Ranjay K. Tiwari, Tapan Sarkar, Jogendra Nath Behera, Sanjit Konar, Subrata Kundu, Manindranath Bera
{"title":"Multimetallic assembly of concave-shaped rectangular Mn4 clusters as efficient hydrogen evolution electrocatalysts","authors":"Chandan Sarkar, Aditi De, Arindam Gupta, Ranjay K. Tiwari, Tapan Sarkar, Jogendra Nath Behera, Sanjit Konar, Subrata Kundu, Manindranath Bera","doi":"10.1039/d5ta01854d","DOIUrl":"https://doi.org/10.1039/d5ta01854d","url":null,"abstract":"In this perspective, cluster-based molecular systems in which composition can be compared with electrocatalytic activity remain under-explored primarily because of the synthetic challenges. Thus, exploring novel electrocatalysts for water splitting with enhanced catalyst activity and stability are still a leading task. Manganese-grafted molecular clusters have garnered interest as models to design more precise replica, which in turn, tender a better perception into the probable pathways used in electrocatalysis. In this research, the design and synthesis of a novel class of fascinating concave-shaped Mn4 cluster materials of molecular formula Na[Mn4(L)2(μ-O)(μ-OH)(μ-p-O2CC6H4(Cl))2](ClO4)2(CH3OH)(H2O) (1), Na[Mn4(L)2(μ-O)(μ-OH)(μ-p-O2CC6H4(CH3))2](ClO4)2(CH3OH)(H2O)2 (2) and Na[Mn4(L)2(μ-O)(μ-OH)(μ-p-O2CC6H4(NO2))2](ClO4)2(H2O) (3), and their evaluation of magnetic exchange interactions and electrocatalytic efficacy for water splitting to generate molecular hydrogen (H3L = N,N'-bis[2-carboxybenzomethyl]-N,N'-bis[2-pyridylmethyl]-1,3-diaminopropan-2-ol; p-C6H4(Cl)(CO2H) = para-chlorobenzoic acid; p-C6H4(CH3)(CO2H) = para-methylbenzoic acid; p-C6H4(NO2)(CO2H) = para-nitrobenzoic acid) have been described. Clusters 1-3 have been characterized by a combined approach of microanalysis, FTIR, UV-Vis, PXRD, FESEM and single crystal X-ray crystallography. The X-ray crystallographic analyses of 1-3 disclose that their molecular structures consist of two crystallographically alike dimeric [Mn2L]3+ units, interconnected by one bridging oxide and hydroxide, and two bridging para-substituted benzoate linkers, forming concave-shaped rectangular motifs. Clusters 1-3 show the coexistence of ferromagnetic and antiferromagnetic exchange interactions as disclosed by low-temperature magnetic susceptibility studies, and the spin ground state (S = 2) of the clusters is correlated to the individuality of ancillary bridging ligands and structural arrangements of the [Mn4(L)2(μ-O)(μ-OH)(μ-p-O2CC6H4(R))2] cores [R = Cl (1), CH3 (2) and NO2 (3)]. All three Mn4 clusters exhibit excellent electrocatalytic activity for hydrogen evolution reaction (HER) with overpotential values of 284, 377 and 323 mV, and Tafel slopes of 184.34, 231.22 and 209.05 mV/dec for 1, 2 and 3, respectively to achieve a current density of 10 mA/cm2. As revealed by chronoamperometric investigation, 1-3 show outstanding stability with insignificant degradation of current density. Density functional theory (DFT) computations were employed to propose the mechanistic aspects of HER studies, suggesting that the Mn(III)-Ooxide-Mn(III) connectivity is the active site for HER. To our knowledge, 1-3 represent the first examples of MnIII4-based molecular clusters showing excellent electrocatalytic HER performance for the generation of molecular hydrogen.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"75 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806255","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
Recent progress in functional applications of polymer foams
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d4ta09226k
Xianhang Yan, Guoqun Zhao, Zhiping Chen, Lei Zhang
{"title":"Recent progress in functional applications of polymer foams","authors":"Xianhang Yan, Guoqun Zhao, Zhiping Chen, Lei Zhang","doi":"10.1039/d4ta09226k","DOIUrl":"https://doi.org/10.1039/d4ta09226k","url":null,"abstract":"Porous structures are ubiquitous in nature, and such structures are the result of natural selection, their functional attributes of lightweight and high strength provide the basis for the continuation of plant and animal life. Inspired by this, researchers have also endowed materials with superior properties and more functional attributes through porosification. Among the common porous materials, polymer foam materials, as a typical porous class of three-dimensional materials with the characteristics of lightweight, flexibility, controllable structure, and a wide range of applications, have made amazing progress in recent years in the fields of structural lightweight, energy conversion, and photothermal effect. We systematically summarize the pore characteristics and different preparation methods of polymer foams and elaborate on their diversified functionalized applications in the fields of energy storage, electromagnetic interference shielding, sensors, adsorption capture, and thermal management. The focus is on revealing its morphological structure, application mechanism, and physicochemical properties as functionalized devices. This review summarizes the potential drawbacks and possible solutions of polymer foams for functionalized applications, as well as reflections on their future innovative directions for the development of the field.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"59 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806262","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
An ultra-strong multilayer structural bacterial cellulose film by biosynthesis for high-performance electromagnetic interference shielding
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d5ta00095e
Guoqiang Chen, Yibing Zhang, Ying Han, Qingtao Li, Lei Wang, Haibo Zhang
{"title":"An ultra-strong multilayer structural bacterial cellulose film by biosynthesis for high-performance electromagnetic interference shielding","authors":"Guoqiang Chen, Yibing Zhang, Ying Han, Qingtao Li, Lei Wang, Haibo Zhang","doi":"10.1039/d5ta00095e","DOIUrl":"https://doi.org/10.1039/d5ta00095e","url":null,"abstract":"Structural materials represent the future development direction for electromagnetic interference (EMI) shielding materials, enabling the effective integration of multiple functions into a single material. Nonetheless, the traditional assembly processes remain a significant challenge in coordinating the mechanical properties and functionality of structural materials. In this study, we introduce a biological synthesis method for fabricating multilayered electromagnetic interference (EMI) shielding materials using bacterial cellulose (BC), which are developed by entangling AgNWs, CNT, and Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> with continuously secreted cellulose nanofibers during <em>in situ</em> fermentation. The BC/AgNWs and BC/CNT/Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> composites could function as the reflection and absorption layers for electromagnetic waves, respectively, thereby simultaneously achieving superior mechanical performance and electromagnetic wave absorption capabilities. Benefiting from the biosynthesis strategy, the tensile strength of the BC/AgNWs/CNT/Fe<small><sub>3</sub></small>O<small><sub>4</sub></small> multilayer film reached 327 MPa, which is higher than that of almost all previously reported multilayer electromagnetic shielding materials. Meanwhile, multilayer structural design improves impedance matching, contributing to the high EMI shielding performance (69.2 dB) and high absorption effectiveness ratio (83.1%). This study presents a novel strategy for producing multilayer structural materials through <em>in situ</em> biosynthesis, demonstrating significant utility in the field of stealth technology and electromagnetic interference protection for electronic packaging materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"38 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806263","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
Recyclable, Conductive Alginate-Based Hydrogels with High Stretchability and Low Electrical Hysteresis for Wireless Wearable Sensors 用于无线可穿戴传感器的具有高拉伸性和低电滞后性的可回收导电藻酸盐基水凝胶
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d4ta08909j
Yulia Shara Sembiring, Truong Tien Truong Vo, Siti Aisyah Nurmaulia Entifar, Anky Fitrian Wibowo, Jung Ha Kim, Nisa Aqilla Ellenahaya Entifar, Jang Hyeok Lee, Si Won Baek, Soo In Lee, Min Seong Kim, Sang Min Jeon, Jincheol Kim, Junghwan Oh, Yong Hyun Kim
{"title":"Recyclable, Conductive Alginate-Based Hydrogels with High Stretchability and Low Electrical Hysteresis for Wireless Wearable Sensors","authors":"Yulia Shara Sembiring, Truong Tien Truong Vo, Siti Aisyah Nurmaulia Entifar, Anky Fitrian Wibowo, Jung Ha Kim, Nisa Aqilla Ellenahaya Entifar, Jang Hyeok Lee, Si Won Baek, Soo In Lee, Min Seong Kim, Sang Min Jeon, Jincheol Kim, Junghwan Oh, Yong Hyun Kim","doi":"10.1039/d4ta08909j","DOIUrl":"https://doi.org/10.1039/d4ta08909j","url":null,"abstract":"Soft electronics based on conductive hydrogels hold considerable promise for advanced wearable technologies. However, these systems face critical challenges, particularly in mitigating electronic waste and ensuring electrical stability. In this study, we present a highly stretchable and recyclable hydrogel composed of the natural polymer alginate (ALG) as the matrix and the lab-synthesized poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) as a conductive filler, ionically crosslinked using CaCl2. The ALG/PEDOT:PSS hydrogel exhibited a stretchability of 138% and a low hysteresis of 6.65% while maintaining stable electrochemical properties over 400 stretching cycles achieved without relying on a synthetic polymer matrix. The integration of ALG with the conductive PEDOT:PSS created conductive pathways and strengthened the intermolecular interactions, resulting in a modest 1.6-fold increase in resistance under 100% strain. Skin-adaptable sensors fabricated from this hydrogel effectively detected large human movements and small activities in real-time. The sensors demonstrated notable electrical responsiveness (65.01 kΩ), good sensitivity (GF: 0.58), rapid response (0.59 s), and recovery times (0.57 s), even after recycling. Furthermore, the integration of the hydrogel into wireless sensor systems afforded a consistent and reliable performance for real-time movement monitoring. These findings highlight the potential of the fabricated hydrogel for high-performance, stretchable electronic devices, particularly due to its excellent recyclability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"2 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806264","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
Trimetallic spinel NiCo2−xMoxO4 oxygen evolution catalyst enabling bias-free solar water splitting with inverted perovskite solar cells 三金属尖晶石 NiCo2-xMoxO4 氧进化催化剂使倒置包晶太阳能电池实现无偏压太阳能水分离
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d4ta08267b
Mahmoud G. Ahmed, Yi Fei Phang, Ying Fan Tay, Anupam Sadhu, Pritish Mishra, Akhmad Herman Yuwono, Lydia H. Wong
{"title":"Trimetallic spinel NiCo2−xMoxO4 oxygen evolution catalyst enabling bias-free solar water splitting with inverted perovskite solar cells","authors":"Mahmoud G. Ahmed, Yi Fei Phang, Ying Fan Tay, Anupam Sadhu, Pritish Mishra, Akhmad Herman Yuwono, Lydia H. Wong","doi":"10.1039/d4ta08267b","DOIUrl":"https://doi.org/10.1039/d4ta08267b","url":null,"abstract":"Efficient spinel oxide catalysts are pivotal for driving the oxygen evolution reaction (OER) for hydrogen production <em>via</em> solar-driven water splitting. Designing trimetallic spinel oxides with high-valence metal ions which leach out to promote surface reconstruction is an effective strategy to maximize active sites for the OER. Herein, we report a trimetallic spinel oxide, NiCo<small><sub>2−<em>x</em></sub></small>Mo<small><sub><em>x</em></sub></small>O<small><sub>4</sub></small> as an efficient OER catalyst, generating 10 mA cm<small><sup>−2</sup></small> at a low overpotential of 250 mV, and demonstrating stability for over 25 h. Experimental and spectroscopic results indicate that the partial leaching of Mo ions from tetrahedral sites in the electrolyte facilitates Ni<small><sup>2+</sup></small> oxidation to Ni<small><sup>3+</sup></small>, leading to the formation of an active nickel (oxy)hydroxide with numerous catalytic sites. Furthermore, integrating this spinel oxide in a 2-electrode water electrolyzer coupled with an inverted p-i-n perovskite solar cell enables bias-free solar water splitting with a solar-to-hydrogen efficiency of 8.8%. This work underscores the efficacy of using high-valence metal ions as effective dopants in activating spinel oxide pre-catalysts for the OER, thereby broadening their application in solar-driven water splitting technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"108 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806253","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
Regulating the Electronic States of NiSe2 by Cr-doping to Promote Formation of Active Phase for High Catalytic Performance of Urea Oxidation Reaction
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-09 DOI: 10.1039/d5ta01694k
Shao-Lan Zheng, Huimin Xu, Chen-Jin Huang, Hongrui Zhu, Chen-Yu Song, Ruo-Zheng Xiong, Gao-Ren Li
{"title":"Regulating the Electronic States of NiSe2 by Cr-doping to Promote Formation of Active Phase for High Catalytic Performance of Urea Oxidation Reaction","authors":"Shao-Lan Zheng, Huimin Xu, Chen-Jin Huang, Hongrui Zhu, Chen-Yu Song, Ruo-Zheng Xiong, Gao-Ren Li","doi":"10.1039/d5ta01694k","DOIUrl":"https://doi.org/10.1039/d5ta01694k","url":null,"abstract":"At present, urea oxidation reaction (UOR), as a small molecule oxidation reaction, can replace anodic oxygen evolution reaction (OER) and has become a research hotspot in the field of efficient and economical hydrogen production through water electrolysis. However, the kinetics of UOR is still slow compared to hydrogen evolution reaction (HER) and involves the adsorption and desorption of various intermediates. It is essential to develop efficient and stable UOR catalysts. In this paper, Cr-doped NiSe2 (Cr0.25-NiSe2) was synthesized as high-performance catalyst for UOR by hydrothermal and selenization methods. The doping of Cr in NiSe2 can regulate electron distribution of Ni, weaken the adsorption of intermediates on NiSe2, and accelerates the reaction kinetics of UOR. In-situ Raman tests show that Cr doping is conducive to surface reconstruction of NiSe2, and the crystalline NiOOH with high catalytic activity is generated at a low potential, which is helpful to improve the performance. In addition, the strong electron absorption ability of the Cr6+ generated by partial oxidation of Cr3+ ions during the UOR can effectively stabilize high valence active sites of the catalyst. Based on the above advantages, the prepared Cr0.25-NiSe2 as a catalyst for UOR only requires a potential of 1.37 V vs. RHE at 100 mA cm-2 in 1.0 M KOH+0.33 M urea solution, with an overpotential negative shift of 270 mV compared to OER. Furthermore,the Cr0.25-NiSe2 showed excellent catalytic stability for UOR, with a catalytic activity retention of 96.8% after 100 h of cyclic testing at 10 mA cm-2.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"4 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143805984","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
Sn-Doped Co-P-Based Trifunctional Electrocatalysts for Accelerating Water Splitting and Hydrogen Generation Concurrent with Ethylene Glycol Electrooxidation
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2025-04-08 DOI: 10.1039/d4ta07773c
Tanu Bagaria, Sougata Saha, Swapan K. Pati, Anustup Sadhu, Bharati Debnath
{"title":"Sn-Doped Co-P-Based Trifunctional Electrocatalysts for Accelerating Water Splitting and Hydrogen Generation Concurrent with Ethylene Glycol Electrooxidation","authors":"Tanu Bagaria, Sougata Saha, Swapan K. Pati, Anustup Sadhu, Bharati Debnath","doi":"10.1039/d4ta07773c","DOIUrl":"https://doi.org/10.1039/d4ta07773c","url":null,"abstract":"Hydrogen (H2) production via water electrolysis is crucial for meeting future energy demands, but developing highly active electrocatalysts through simple and quick methods remains challenging. We introduce a highly active, stable trifunctional Sn-doped Co-P (Sn-Co-P-x; where x represents % of Sn into the system), fabricated using the electrodeposition technique which possesses superior hydrogen evolution reaction (HER) activity, with a significantly low overpotential of 40 mV and remarkable oxygen evolution reaction (OER) efficiency having overpotentials of 220 mV at 10 mA/cm2. This catalyst outperforms commercial HER (Pt/C) and OER (IrO2) catalysts at higher current densities. The Sn-Co-P-5 achieves a cell voltage of 1.51 V to reach a current density of 10 mA/cm2 during water splitting. Moreover, H2 production is further boosted by replacing the OER with the oxidation of ethylene glycol (EG) and a cell voltage of 1.32 V is achieved at 10 mA/cm2. Theoretical insights confirm that incorporating Sn into the Co-P system facilitates water adsorption and H2 evolution, attributed to the heightened positive charge on the Co atoms. The downshift of the d-band center in the Sn-Co-P system as compared to Co-P facilitates hydrogen desorption and enhances the overall water-splitting process. This work shows great potential for developing innovative and highly efficient trifunctional electrocatalysts for future applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"31 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143805983","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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