Chemistry of Materials最新文献

{"title":"Chiral Shape Engineering Combined with Bimetallic Nanostructures for High-Performance Plasmonic Sulfide Sensors","authors":"Han Lin, Kuniharu Ijiro, Hideyuki Mitomo","doi":"10.1021/acs.chemmater.4c03150","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03150","url":null,"abstract":"Combining chiral shape engineering with the plasmonic sensor features significantly enhances sensor performance and effectively avoids potential background interference. These advantages suggest that chiral nanoparticles could provide valuable insights into addressing defects or shortcomings in traditional plasmonic sensors. Herein, to address the common drawback of performance degradation due to line width broadening in plasmonic sulfide sensors during sulfidation, we designed a distinctive intrinsically chiral bimetallic core–shell plasmonic nanoparticle. The chiral gold core provided strong chiroptical activities, enriching the spectral features, including bipolar peaks and zero-crossing points, while the silver shell was used for sulfide sensing. Remarkably, this chiral plasmonic sulfide sensor demonstrated exceptional sensitivity and clarity. Specifically, the zero-crossing point in the circular dichroism spectrum serves as an easily recognizable tracking feature, leveraging the trend of line width broadening to enhance sensor responsiveness. Particularly, at a sulfide concentration of only 5 μM, the zero-crossing point shift reached up to 170 nm, with a maximum shift limit of 208 nm, surpassing all previously reported plasmonic sulfide sensors. Finally, the well-defined structure of this chiral-core sensing-shell design offers an alternative fabrication approach for expanding the chiral plasmonic sensing platform, allowing for flexible replacement of the shell material to meet specific sensing requirements.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"12 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077229","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":"Chiral Shape Engineering Combined with Bimetallic Nanostructures for High-Performance Plasmonic Sulfide Sensors","authors":"Han Lin,&nbsp;Kuniharu Ijiro and Hideyuki Mitomo*,&nbsp;","doi":"10.1021/acs.chemmater.4c0315010.1021/acs.chemmater.4c03150","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03150https://doi.org/10.1021/acs.chemmater.4c03150","url":null,"abstract":"<p >Combining chiral shape engineering with the plasmonic sensor features significantly enhances sensor performance and effectively avoids potential background interference. These advantages suggest that chiral nanoparticles could provide valuable insights into addressing defects or shortcomings in traditional plasmonic sensors. Herein, to address the common drawback of performance degradation due to line width broadening in plasmonic sulfide sensors during sulfidation, we designed a distinctive intrinsically chiral bimetallic core–shell plasmonic nanoparticle. The chiral gold core provided strong chiroptical activities, enriching the spectral features, including bipolar peaks and zero-crossing points, while the silver shell was used for sulfide sensing. Remarkably, this chiral plasmonic sulfide sensor demonstrated exceptional sensitivity and clarity. Specifically, the zero-crossing point in the circular dichroism spectrum serves as an easily recognizable tracking feature, leveraging the trend of line width broadening to enhance sensor responsiveness. Particularly, at a sulfide concentration of only 5 μM, the zero-crossing point shift reached up to 170 nm, with a maximum shift limit of 208 nm, surpassing all previously reported plasmonic sulfide sensors. Finally, the well-defined structure of this chiral-core sensing-shell design offers an alternative fabrication approach for expanding the chiral plasmonic sensing platform, allowing for flexible replacement of the shell material to meet specific sensing requirements.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 3","pages":"1221–1230 1221–1230"},"PeriodicalIF":7.2,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375862","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":"Quantification of Pore Connectivity in Hierarchically Porous Carbon by Percolation Effect Integrated Differential Hysteresis Scanning","authors":"Zhiheng Wang,&nbsp;Jiali Huang,&nbsp;Guancong Jiang,&nbsp;Tuo Ji,&nbsp;Han Lin,&nbsp;Liwen Mu and Jiahua Zhu*,&nbsp;","doi":"10.1021/acs.chemmater.5c0011410.1021/acs.chemmater.5c00114","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00114https://doi.org/10.1021/acs.chemmater.5c00114","url":null,"abstract":"<p >A thorough understanding of pore architecture is essential for grasping its effects on mass transfer processes in various applications, a challenge that has long persisted. Conventional gas sorption methods cannot provide direct insights into pore geometry, connectivity, and other detailed structural characteristics. Here, we present a robust percolation effect integrated differential hysteresis scanning (PE-DHS) method that quantitatively evaluates the size and quantity of different pore geometries in various porous materials through hysteresis loop scanning. Alongside a detailed measurement program and experimental procedures, we performed an in-depth analysis of the phase transition behaviors during the filling and emptying process in pores of diverse shapes, offering a systematic explanation of the guiding mechanisms and the derivation of relevant formulas for PE-DHS. Additionally, we selected two samples with distinct <i>d</i>_pore and <i>d</i>_win characteristics to validate our analysis. A series of wood-based carbon materials with varying delignified pretreatment were chosen to test the analytical capabilities of PE-DHS on more complex and disordered pore networks with wider pore size distribution. Based on PE-DHS analysis, we introduced an index called the mean diameter/window ratio (MDWR) to quantify the degree of constriction in each cavity, thereby transforming conventional pore size distribution into a two-dimensional representation. Moving forward, the PE-DHS method is anticipated to become accessible to all and applicable to various materials with complex pore structures.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 4","pages":"1337–1348 1337–1348"},"PeriodicalIF":7.2,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478320","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":"Dibenzyl Diselenide as a Monitorable, Atom-Efficient Se Source for the Synthesis of Cu3PSe4 Nanoparticles","authors":"Luke T. MacHale, Nathan A. Neisius, Erin R. Snyder, Richard G. Finke, Amy L. Prieto","doi":"10.1021/acs.chemmater.4c02719","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02719","url":null,"abstract":"Complex ternary composition nanoparticles (NPs) are highly desired for a range of potential applications, but their syntheses often rely on empirical syntheses rather than designed, ideally mechanism-based, syntheses. Here, we focus on colloidal Cu₃PSe₄ nanoparticles as a model system, one we have previously prepared from Cu_3–<i>x</i>P and solid Se. However, in that prior system quantitatively following the conversion of solid Se into the Cu₃PSe₄ product is problematic, in turn meaning that the balanced reaction stoichiometry and, hence, mechanistic insights remain elusive. Herein, we show that dibenzyl diselenide (Bn₂Se₂) has considerable utility in the synthesis of Cu₃PSe₄ NPs. Using Cu_3–<i>x</i>P plus 2 equiv of Bn₂Se₂ yields Cu₃PSe₄ as the main NP product. The benzyl moiety (PhCH₂−), coupled with NMR and gas chromatography–mass spectrometry (GC-MS) handles, establishes that benzyl loss and toluene (PhCH₃) gain are a monitorable proxy for net Se⁰₂ delivery when the facile, net two H^• donor 9,10-dihydroanthracene is added. The experiments performed and the results obtained help to further lay the groundwork for the expanded use of Bn₂Se₂ as a Se⁰₂ delivery reagent for the syntheses of Se-containing materials. More broadly, the results herein support the use of molecular precursors, chosen based on previously established chemistry, that allow trackable, quantifiable reaction products in NP and related material syntheses.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"122 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083173","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":"Polymorphic YTiGe Intermetallic Electride Created by Hydrogenation and Dehydrogenation","authors":"Shuhao Chen,&nbsp;Siyuan Ren,&nbsp;Md Salman Khan,&nbsp;Dong Cheol Lim,&nbsp;Nahyun Lee,&nbsp;Hyungsub Kim,&nbsp;Thu-Thuy Hoang,&nbsp;Junhyeok Bang and Sung Wng Kim*,&nbsp;","doi":"10.1021/acs.chemmater.4c0321910.1021/acs.chemmater.4c03219","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03219https://doi.org/10.1021/acs.chemmater.4c03219","url":null,"abstract":"<p >Electrides are emerging materials with unique structural features of a positively charged lattice framework and interstitial anionic electrons trapped in structural cavities, exhibiting exceptional functionalities. Thermodynamic and electronic stabilities of the electrides are mainly dominated by the existence of anionic electrons and their structural arrangements that are interdependent with the lattice frameworks. Different arrays of anionic electrons in a fixed chemical formula can provide unexpected properties but are hardly found in electrides. Here, we demonstrate the stable polymorphic forms of intermetallic YTiGe electride at ambient pressure via hydrogenation and subsequent dehydrogenation processes. We find that hydrogenation leads to a phase transition from the <i>P4/nmm</i> structured YTiGe electride to the <i>I4/mmm</i> structured YTiGeH_1.5 hydride. Importantly, it was experimentally confirmed that the <i>I4/mmm</i> structure was retained, even after complete dehydrogenation. Our theoretical calculations demonstrate that the anionic electrons are localized in both tetrahedral Y₄ and octahedral Y₂Ti₄ cavities, indicating that <i>P4/nmm</i> and <i>I4/mmm</i> structured YTiGe compounds are polymorphic electrides. This polymorphic YTiGe electride system shows distinct magnetic properties, where a higher magnetic moment is obtained in the <i>I4/mmm</i> structured YTiGe due to a higher concentration of quasi-atomic anionic electrons. These results accentuate hydrogenation–dehydrogenation processes for exploring polymorphic electrides as functional materials.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 4","pages":"1600–1608 1600–1608"},"PeriodicalIF":7.2,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478321","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":"High Oxide-Ion Conduction in Rb-Containing Oxides","authors":"Yuta Yasui, Kazuaki Jojima, Kotaro Fujii, Kazuhiro Mori, Masatomo Yashima","doi":"10.1021/acs.chemmater.4c03148","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03148","url":null,"abstract":"Oxide-ion conductors are essential for clean energy applications, such as solid oxide fuel cells (SOFCs). Since the Rb⁺ ion is the second largest available cation, some Rb-containing oxides are expected to have low activation energy for oxide-ion conductivity and high oxide-ion conductivity at low temperatures. However, Rb-containing oxide-ion conductors are very rare. Herein, we report the high oxide-ion conductivity of the palmierite-type Rb₅BiMo₄O₁₆ (e.g., 2.3 mS cm^–1 at 560 °C), which was discovered by a combined technique of computer screening through bond-valence-based energy calculations of 475 compositions of Rb-containing oxides, synthesis, and characterization of the structural and transport properties. Rb₅BiMo₄O₁₆ exhibits a high oxide-ion conductivity of 0.14 mS cm^–1 at 300 °C, which is 29 times higher than that of yttria-stabilized zirconia (YSZ) at 300 °C and comparable to the leading oxide-ion conductors with tetrahedral moieties. The high ionic conductivity below 480 °C is mainly due to the low activation energy for ionic conductivity, which can be attributed to the large free volume of Rb₅BiMo₄O₁₆. The extremely large anisotropic thermal motion of oxygen atoms and the rotational motion of MoO₄ tetrahedra are also responsible for the high conductivity. Rb₅BiMo₄O₁₆ is stable at high temperatures under a CO₂ flow, under a wet air flow, and under a wet 5% H₂ in a N₂ flow, and at about 21 °C in water. Rb₅<i>R</i>Mo₄O₁₆ materials (<i>R</i>: La, Pr, Nd, Sm, Gd, Tb, and Er) also exhibit significant conductivity. The discovery of Rb-containing oxides with high conductivity and high stability would open a new avenue for oxide-ion conductors.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"207 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077235","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":"Risks of Nanoscale Byproducts Generated during the Interzeolite Transformation for Cesium Sequestration","authors":"Seokju Hong,&nbsp; and ,&nbsp;Wooyong Um*,&nbsp;","doi":"10.1021/acs.chemmater.4c0264710.1021/acs.chemmater.4c02647","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02647https://doi.org/10.1021/acs.chemmater.4c02647","url":null,"abstract":"<p >The development of radionuclide-sequestering materials should be directed toward eliminating all possibilities of radionuclide release based on a comprehensive understanding of all chemical reactions. Here, we report that undesired chemical reactions occurring during the interzeolite transformation for Cs sequestration and the resulting minor amounts of nanoscale byproducts can increase the release of Cs. Most studies developing radionuclide-sequestering materials have not examined the presence of byproducts and whether they affect the release of radionuclides; however, we demonstrated for the first time that these neoformed byproducts not only increase the release of radionuclides but also delay the rate of interzeolite transformation into Cs-sequestering pollucite. Moreover, we report that pore characteristics and the high specific surface area of the byproducts can greatly distort the results of the Cs release from Cs-sequestering pollucite. We found that the mechanism of undesired chemical reactions was due to the charge-compensating Ca ions present in the parent zeolite, and we suggest a strategy to minimize the release of Cs through a design that suppresses the generation of byproducts by pre-eliminating Ca ions before interzeolite transformation. We expect our study to raise awareness that minor amounts of byproducts generated during the synthesis and development of radionuclide-sequestering host material can negatively affect the sequestration of radionuclides. Also, we accentuate the requirement for a strategic design to prevent the risks that could increase the release of radionuclides in advance.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 3","pages":"1001–1012 1001–1012"},"PeriodicalIF":7.2,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143376413","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":"Risks of Nanoscale Byproducts Generated during the Interzeolite Transformation for Cesium Sequestration","authors":"Seokju Hong, Wooyong Um","doi":"10.1021/acs.chemmater.4c02647","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02647","url":null,"abstract":"The development of radionuclide-sequestering materials should be directed toward eliminating all possibilities of radionuclide release based on a comprehensive understanding of all chemical reactions. Here, we report that undesired chemical reactions occurring during the interzeolite transformation for Cs sequestration and the resulting minor amounts of nanoscale byproducts can increase the release of Cs. Most studies developing radionuclide-sequestering materials have not examined the presence of byproducts and whether they affect the release of radionuclides; however, we demonstrated for the first time that these neoformed byproducts not only increase the release of radionuclides but also delay the rate of interzeolite transformation into Cs-sequestering pollucite. Moreover, we report that pore characteristics and the high specific surface area of the byproducts can greatly distort the results of the Cs release from Cs-sequestering pollucite. We found that the mechanism of undesired chemical reactions was due to the charge-compensating Ca ions present in the parent zeolite, and we suggest a strategy to minimize the release of Cs through a design that suppresses the generation of byproducts by pre-eliminating Ca ions before interzeolite transformation. We expect our study to raise awareness that minor amounts of byproducts generated during the synthesis and development of radionuclide-sequestering host material can negatively affect the sequestration of radionuclides. Also, we accentuate the requirement for a strategic design to prevent the risks that could increase the release of radionuclides in advance.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"2017 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077232","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":"High Oxide-Ion Conduction in Rb-Containing Oxides","authors":"Yuta Yasui,&nbsp;Kazuaki Jojima,&nbsp;Kotaro Fujii,&nbsp;Kazuhiro Mori and Masatomo Yashima*,&nbsp;","doi":"10.1021/acs.chemmater.4c0314810.1021/acs.chemmater.4c03148","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03148https://doi.org/10.1021/acs.chemmater.4c03148","url":null,"abstract":"<p >Oxide-ion conductors are essential for clean energy applications, such as solid oxide fuel cells (SOFCs). Since the Rb⁺ ion is the second largest available cation, some Rb-containing oxides are expected to have low activation energy for oxide-ion conductivity and high oxide-ion conductivity at low temperatures. However, Rb-containing oxide-ion conductors are very rare. Herein, we report the high oxide-ion conductivity of the palmierite-type Rb₅BiMo₄O₁₆ (e.g., 2.3 mS cm^–1 at 560 °C), which was discovered by a combined technique of computer screening through bond-valence-based energy calculations of 475 compositions of Rb-containing oxides, synthesis, and characterization of the structural and transport properties. Rb₅BiMo₄O₁₆ exhibits a high oxide-ion conductivity of 0.14 mS cm^–1 at 300 °C, which is 29 times higher than that of yttria-stabilized zirconia (YSZ) at 300 °C and comparable to the leading oxide-ion conductors with tetrahedral moieties. The high ionic conductivity below 480 °C is mainly due to the low activation energy for ionic conductivity, which can be attributed to the large free volume of Rb₅BiMo₄O₁₆. The extremely large anisotropic thermal motion of oxygen atoms and the rotational motion of MoO₄ tetrahedra are also responsible for the high conductivity. Rb₅BiMo₄O₁₆ is stable at high temperatures under a CO₂ flow, under a wet air flow, and under a wet 5% H₂ in a N₂ flow, and at about 21 °C in water. Rb₅<i>R</i>Mo₄O₁₆ materials (<i>R</i>: La, Pr, Nd, Sm, Gd, Tb, and Eu) also exhibit significant conductivity. The discovery of Rb-containing oxides with high conductivity and high stability would open a new avenue for oxide-ion conductors.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 3","pages":"1231–1243 1231–1243"},"PeriodicalIF":7.2,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03148","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bifunctional Noble Metal-Free Ternary Chalcogenide Electrocatalysts for Overall Water Splitting","authors":"Shantanu Singh,&nbsp;Ahamed Irshad,&nbsp;Germany Diaz De la Cruz,&nbsp;Boyang Zhao,&nbsp;Billal Zayat,&nbsp;Yongjun Kwon,&nbsp;Qiaowan Chang,&nbsp;Sri R. Narayan and Jayakanth Ravichandran*,&nbsp;","doi":"10.1021/acs.chemmater.4c0168410.1021/acs.chemmater.4c01684","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01684https://doi.org/10.1021/acs.chemmater.4c01684","url":null,"abstract":"<p >Hydrogen has been identified as a clean, zero-carbon, sustainable, and promising energy source for the future, and electrochemical water splitting for hydrogen production is an emission-free and efficient energy conversion technology. A major limitation of this approach is the unavailability of efficient, abundant, and inexpensive catalysts, which prompts the need for new catalytic materials. Here, we report the synthesis and electrocatalytic properties of a novel transition-metal-based ternary chalcogenide family, LaMS₃ (M = Mn, Fe, Co, and Ni). These materials exhibit bifunctional catalytic activity toward the two half-reactions of the water-splitting process, with LaNiS₃ being the most active material for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). The LaMS₃ compounds show long-term stability with negligible change in the overpotential at a constant current density of 10 mA cm^–2 over 18 h of measurements. As compared to the corresponding ternary oxides, the LaMS₃ materials exhibit higher activity and significantly lower Tafel slopes. These materials demonstrate overpotentials comparable to those of commercial catalysts at a current density of 300 mA cm^–2. The ability to catalyze both half-reactions of water electrolysis makes these materials promising candidates for bifunctional catalysts and presents a new avenue to search for high-efficiency electrocatalysts for water splitting.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 3","pages":"823–832 823–832"},"PeriodicalIF":7.2,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143376414","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}