ACS Applied Energy Materials最新文献

{"title":"Highly Active Water-Splitting Electrocatalyst Developed by the Creation of Oxygen Vacancies in a Perovskite Oxide","authors":"Md. Sofiul Alom,&nbsp;Narayan Acharya,&nbsp;Antonis N. Andriotis,&nbsp;Madhu Menon and Farshid Ramezanipour*,&nbsp;","doi":"10.1021/acsaem.4c0282110.1021/acsaem.4c02821","DOIUrl":"https://doi.org/10.1021/acsaem.4c02821https://doi.org/10.1021/acsaem.4c02821","url":null,"abstract":"<p >Using both experimental and computational approaches, we have demonstrated a major enhancement of electrocatalytic activity for both half-reactions of water splitting, i.e., the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline conditions, through the incorporation of oxygen vacancies in the perovskite oxide La₂FeNiO₆ (LaFe_0.5Ni_0.5O₃). Density functional theory (DFT) calculations predicted that the incorporation of oxygen vacancies would lead to the reinforcement of several electronic parameters, namely, the proximity of the <i>d</i>-band center to the Fermi level, closer separation between <i>p</i> and <i>d</i> bands, and greater hybridization of those bands, all of which are known to be descriptors of electrocatalytic properties. Therefore, DFT simulations predicted that the electrocatalytic activity should be enhanced due to the presence of oxygen vacancies. This was thoroughly confirmed by the experiment, where the reduced material containing oxygen vacancies, termed LaFe_0.5Ni_0.5O₃-R, showed remarkably lower overpotentials for both HER and OER. This was particularly notable for OER, where the overpotential decreased by nearly 100 mV, reaching η₁₀ = 330 mV, comparable to those of noble metal catalysts such as IrO₂ and RuO₂. In addition, for both HER and OER, the mass activity and reaction kinetics were enhanced upon the creation of oxygen vacancies. Furthermore, a significant increase in turnover frequency (TOF), by nearly 8-fold, was achieved. In addition, electrochemical impedance spectroscopy indicated that the charge-transport properties were enhanced, leading to facile electron transfer for both HER and OER. The excellent match between computational predictions and experimental results is notable.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3369–3378 3369–3378"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-Diffusivity Measurement of Eutectic F7LiNaK with and without Additives Using Quasi-Elastic Neutron Scattering","authors":"G. S. Rakib,&nbsp;Shao-Chun Lee,&nbsp;Melissa A. Rose,&nbsp;Rebecca Mills,&nbsp;Daniel Pajerowski,&nbsp;Y Z and Brent J. Heuser*,&nbsp;","doi":"10.1021/acsaem.4c0324910.1021/acsaem.4c03249","DOIUrl":"https://doi.org/10.1021/acsaem.4c03249https://doi.org/10.1021/acsaem.4c03249","url":null,"abstract":"<p >The atomic scale relaxation dynamics of eutectic F⁷LiNaK (46.5 LiF–11.5 NaF–42 KF mol %, Li-7 enriched) were measured using quasi-elastic neutron scattering (QENS) over a temperature range of 500–750 °C. The effect of adding 0.988 mol % cerium, 0.499 mol % cesium, and 1.21 mol % zirconium individually to the dynamics of F⁷LiNaK was also investigated. The relaxation process in both pure and doped F⁷LiNaK molten salts was fit with a stretched exponential function and the temperature dependence follows an Arrhenius behavior over a wavevector transfer range of 0.4 Å^–1 &lt; <i>Q</i> &lt; 0.9 Å^–1. The measured activation energy for self-diffusion is <i>E</i>_a = 0.77 ± 0.02 eV/atom for pure molten F⁷LiNaK. The QENS response with additives added to F⁷LiNaK was also fit with a stretched exponential and the associated Arrhenius behavior was characterized with activation energies of <i>E</i>_a = 0.88 ± 0.01 eV/atom for zirconium (1.21 mol %), <i>E</i>_a = 1.02 ± 0.02 eV/atom for cerium (0.988 mol %), and <i>E</i>_a = 0.71 ± 0.03 eV/atom for cesium (0.499 mol %). The measured diffusivities are compared to those simulated with a neural network force field model by Lee et al. [<contrib-group><span>Lee, S.-C.</span></contrib-group> Comparative Studies of the Structural and Transport Properties of Molten Salt FLiNaK Using the Machine-Learned Neural Network and Reparametrized Classical Forcefields. <cite><i>J. Phys. Chem. B</i></cite> <span>2021</span>, <em>125</em>(37), 10562–10570].</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3638–3646 3638–3646"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675735","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"In Situ Synthesis of Phosphate-Based CelloMOF as a Promising Separator for Li–Ion Batteries","authors":"Anass Ait Benhamou*,&nbsp;ElMehdi Moumen,&nbsp;Mohamed Aqil,&nbsp;Rachid Amine,&nbsp;Hiba El Fallah,&nbsp;Seoung-Bum Son,&nbsp;Soumia Boukind,&nbsp;Mounir El Achaby,&nbsp;Samir El Hankari,&nbsp;Jones Alami,&nbsp;Mouad Dahbi* and Houssine Sehaqui*,&nbsp;","doi":"10.1021/acsaem.4c0290810.1021/acsaem.4c02908","DOIUrl":"https://doi.org/10.1021/acsaem.4c02908https://doi.org/10.1021/acsaem.4c02908","url":null,"abstract":"<p >Nowadays, battery separators play a critical role in determining the sustainability, electrochemical efficiency, and safety of lithium-ion batteries (LIBs). In this contribution, we developed fire-resistant composite membranes called CelloMOF by in situ grafting of metal-organic framework, ZIF-67, onto phosphorylated cellulose nanofibers (P-CNFs) followed by a vacuum filtration process akin to papermaking. The hybrid ZIF-67@P-CNF membrane exhibits superior properties than a polyolefin-based commercial separator (CS) in terms of enhanced thermal and dimensional stability, flame-retardant properties, better surface wettability, and improved electrolyte uptake. Thermal dimensional stability tests revealed that the ZIF-67@P-CNF separator maintained its structure even at 200 °C, whereas CS suffered severe shrinkage, potentially leading to internal short circuits. Combustion tests showed a peak heat release rate (PHRR) of 34.5 W/g and a total heat release (THR) of 1.61 kJ/g for ZIF-67@P-CNF, significantly lower than the PHRR (1111.82 W/g) and THR (40.89 kJ/g) of CS. The composite separator also demonstrated significantly improved wettability, with a contact angle of 32 ± 1.04°, compared to 92 ± 1.07° for CS, highlighting its hydrophilic nature. Electrochemical evaluations in LiFePO₄/Li half-cells indicated a higher discharge capacity of 149 mA h g^–1 at 0.2 C and superior capacity retention of 86% after 50 cycles, outperforming CS (145 mA h g^–1 and 84%, respectively). These results underscore the potential of the ZIF-67@P-CNF membrane to advance safe, high-performance LIBs by addressing critical challenges in thermal stability, flame retardancy, and electrolyte compatibility.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3379–3391 3379–3391"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675693","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation of a Difunctional Electrolyte Engineered for Capacitor Batteries","authors":"Zhenhao Luo,&nbsp;Xuefang Chen*,&nbsp;Xibang Chen,&nbsp;Jintao Li,&nbsp;Xuhong Wang,&nbsp;Songtong Zhang,&nbsp;Xiayu Zhu,&nbsp;Wenjie Meng,&nbsp;Jingyi Qiu,&nbsp;Jing Wang* and Hai Ming*,&nbsp;","doi":"10.1021/acsaem.4c0326310.1021/acsaem.4c03263","DOIUrl":"https://doi.org/10.1021/acsaem.4c03263https://doi.org/10.1021/acsaem.4c03263","url":null,"abstract":"<p >Recently, the rapid advancement of electric vehicles has resulted in a growing demand for enhanced battery performance, particularly in application scenarios that necessitate fast (dis)charging properties and ultralong cycle life. The capacitor lithium-ion batteries, which fully leverage the synergistic advantages of a double electric layer and redox reaction storage mechanisms of lithium-ion batteries to optimize both energy and power properties, are poised to play a significant role to meet these requirements. Herein, this paper designs a difunctional electrolyte and investigates its effects on the electrochemical behaviors within a capacitor lithium-ion battery. The objective of this study is to develop functional electrolytes for capacitor lithium-ion batteries tailored for carbon-rich systems with dual energy storage mechanisms. The capacitor lithium-ion battery comprising LiNi_0.6Co_0.2Mn_0.2O₂-activated carbon (cathode)||hard carbon (anode) demonstrates attractive performance, while utilizing a difunctional electrolyte system of LiPF₆ and tetraethylammonium tetrafluoroborate. With the additives of vinylidene carbonate and fluorinated ethylene carbonate, the batteries exhibit commendable reversible capacities of 111.5 and 116 mAh/g at 180 mA/g, respectively, with capacity retention rate exceeding 90% after 100 cycles. Consequently, this research provides both theoretical and technical support for the advancement of capacitor lithium-ion batteries characterized by a wide operating temperature range, extended lifespan, and enhanced safety.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3663–3675 3663–3675"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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-Performance Cathodes for Alkaline Water Electrolysis in a Zero-Gap Setting: Ni–Sn/Ni Foam Prepared by Galvanostatic Electrodeposition","authors":"Jelena D. Gojgić*,&nbsp;Aleksandar Petričević,&nbsp;Thomas Rauscher,&nbsp;Christian Immanuel Bernäcker,&nbsp;Thomas Weißgärber,&nbsp;Rastko Vasilić,&nbsp;Luka Pavko,&nbsp;Marjan Bele,&nbsp;Francisco Ruiz-Zepeda,&nbsp;Milutin Smiljanić,&nbsp;Nejc Hodnik,&nbsp;Mila N. Krstajić Pajić* and Vladimir D. Jović,&nbsp;","doi":"10.1021/acsaem.4c0314010.1021/acsaem.4c03140","DOIUrl":"https://doi.org/10.1021/acsaem.4c03140https://doi.org/10.1021/acsaem.4c03140","url":null,"abstract":"<p >In an attempt to obtain fully functional cathode materials for zero-gap alkaline water electrolysis, Ni foam substrates with various pore diameters were modified through galvanostatic electrodeposition of Ni–Sn alloys as an easily scalable procedure. To optimize the production process for each substrate, Ni–Sn alloys were electrodeposited at five different constant current densities. The obtained cathodes were primarily subjected to hydrogen evolution in 1 M KOH to evaluate their activity, while the best-performing samples were further investigated in 30 wt % KOH at 70 °C in a three- and two-electrode arrangement. Detailed electrochemical impedance spectroscopy analysis of hydrogen evolution reaction (HER) conducted with a three electrode arrangement indicated two semicircles on the Nyquist plots that confirmed that the adsorption of intermediate (<i>H</i>_ads) is potential dependent. Relevant HER parameters such as exchange current density and relaxation time showed exceptional performance of optimized electrodes. During zero-gap single cell tests with bare Ni foam used as the anode, onset voltages for Ni–Sn cathodes were around 1.64 V (for bare foams, 1.99 V), with cell voltage at 1 A cm^–2 being as low as 2.03 V (for bare foams, 2.57 V). The cathodes were also subjected to a long-term stability test, showing excellent activity preservation. Great stability, low cell voltage, and low production cost confirm their suitability for industrial applications. Top-view as well as cross-section electron microscopy analysis have shown that the entire foam surface was evenly covered with Ni–Sn coating. The composition of the investigated coatings was within the range of Ni_(1+<i>x</i>)Sn (0 &lt; <i>x</i> &lt; 0.5) metastable phase and practically independent of deposition current density. Aberration-corrected scanning transmission electron microscopy revealed that the so-called metastable phase is in fact the Ni₃Sn₂ phase, which is shown for the first time for electrodeposited Ni–Sn alloys.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3570–3580 3570–3580"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unraveling Energy Transfer Dynamics and Exciton Diffusion in Multicomponent Metal–Organic Frameworks","authors":"Joel Cornelio*,&nbsp;Isabella Wagner,&nbsp;Sam Otter,&nbsp;Kai Chen,&nbsp;Justin M. Hodgkiss and Shane G. Telfer,&nbsp;","doi":"10.1021/acsaem.5c0050110.1021/acsaem.5c00501","DOIUrl":"https://doi.org/10.1021/acsaem.5c00501https://doi.org/10.1021/acsaem.5c00501","url":null,"abstract":"<p >Luminescence in metal–organic frameworks (MOFs) typically has one of three fundamental origins: emission from ligands, metal clusters, and encapsulated guests. Photophysical processes such as energy transfer or charge transfer can further modulate the emission profile. However, as the MOF structure becomes more complex, it can become increasingly difficult to pinpoint the origin of the emission. Herein, we report on the energy transfer behavior of multicomponent zinc-based frameworks from the MUF-77 family, which combine three luminescent, aromatic ligands and Zn₄O nodes. Each ligand has distinct photophysics and energy transfer behavior upon photoexcitation. Time-resolved photoluminescence spectroscopy on the nanosecond and picosecond time scales reveals the specific interligand energy pathways that influence the emission profile. Fluence-dependent measurements uncover both bimolecular and higher-order recombination in MUF-77. The long lifetimes and low bimolecular recombination rate point to modest exciton diffusion alongside higher-order exciton-charge annihilation in these systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3951–3962 3951–3962"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675713","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hot Pressing Argyrodite Solid Electrolyte Powders Results in >2 mS cm–1 Ionic Conductivity at 20 °C and <1 MPa Operating Pressure","authors":"Karl Larson,&nbsp;Yang Wang,&nbsp;Bhuvsmita Bhargava,&nbsp;Ravindra Kumar Bhardwaj,&nbsp;Osma Gomez,&nbsp;Adam Antar,&nbsp;Gary W. Rubloff,&nbsp;David Zitoun,&nbsp;Alexander C. Kozen,&nbsp;Sang Bok Lee and Paul Albertus*,&nbsp;","doi":"10.1021/acsaem.5c0002010.1021/acsaem.5c00020","DOIUrl":"https://doi.org/10.1021/acsaem.5c00020https://doi.org/10.1021/acsaem.5c00020","url":null,"abstract":"<p >The formation of Li₆PS₅Cl argyrodite solid electrolyte pellets typically involves compaction at ∼20 °C and hundreds of megapascal of pressure, and the resulting pellets usually need &gt;10 MPa operating pressure to achieve ionic conductivities &gt;1 mS cm^–1 at 25 °C and/or sputtered metal electrodes. This work demonstrates a key advance achieved with pellet fabrication at 150 °C and 300 MPa with foil electrodes: &gt;2 mS cm^–1 ionic conductivity at 20 °C with &lt;1 MPa operating pressure. Scanning electron microscopy reveals fused grains present in samples pressed at 150 °C but not in those at 20 °C. X-ray photoelectron spectroscopy and diffraction analysis show no significant difference in crystal structure or surface composition between 150 and 20 °C pressed samples, and the pellet densities are nearly identical. The ionic conductivity of 150 °C pressed samples is nearly invariant with operating pressure, while that at 20 °C has a strong operating pressure dependence. Nanoindentation on pellet surfaces shows a higher elastic modulus for the 150 vs 20 °C pellets. Overall, these results suggest that fabrication at 150 °C results in grain–grain fusion and motivate further study of the fabrication parameter space (e.g., pressure, temperature, time, and contacts) to find routes to &lt;1 MPa operation of argyrodite structures.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3754–3763 3754–3763"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675741","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient Organic Solar Cells Enabled by Structurally Modified Quinoxaline-Based Small Molecule Acceptors with Brominated End Groups","authors":"Wanting Yao,&nbsp;Xiaoyu Zhang,&nbsp;Zezhou Liang,&nbsp;Haimei Wu,&nbsp;Jiahao Liu,&nbsp;Tianyi Zhao,&nbsp;Yuchen Zhou,&nbsp;Weiping Wang,&nbsp;Shujuan Liu,&nbsp;Baofeng Zhao,&nbsp;Zhiyuan Cong,&nbsp;Qinghao Yang* and Chao Gao*,&nbsp;","doi":"10.1021/acsaem.5c0009910.1021/acsaem.5c00099","DOIUrl":"https://doi.org/10.1021/acsaem.5c00099https://doi.org/10.1021/acsaem.5c00099","url":null,"abstract":"<p >Scientific interest in organic solar cells (OSCs) has increased significantly in recent years. This surge is largely due to advances in A-DA′D-A-type small molecule acceptors (SMAs), which have played a key role in improving the power conversion efficiency (PCE) of OSC devices. Nevertheless, there is a prevailing need to continue exploring avenues that would further elevate the performance of OSCs, particularly improving their open-circuit voltage (<i>V</i>_OC). The structural modification of the fused-ring electron-withdrawing A′ unit with the quinoxaline unit is an approach that holds considerable promise for enhancing the <i>V</i>_OC and PCE of A-DA′D-A type molecules. Furthermore, it has been demonstrated that the incorporation of bromine atoms into SMAs can result in the synthesis of highly prospective SMAs. This is attributable to the fact that bromine atoms possess lower electronegativity, larger atomic dimensions, and a comparatively more straightforward and cost-effective synthetic procedure compared to the commonly used fluorine and chlorine atoms. To develop promising brominated SMAs to enhance the <i>V</i>_OC of OSCs, two alkoxypheny-substituted quinoxaline-based A-DA′D-A molecules (<b>BQ-2FBr</b> and <b>BQ-2Cl-FBr</b>) were synthesized, with the former sealed with (5-bromo-4-fluoro-3-oxy-2,3-dihydro-1<i>H</i>-indole-1-ylidene)malonitrile (FBr-INCN) unit and the latter sealed with 2-(5,6-dichloro-3-oxo-2,3-dihydro-1<i>H</i>-inden-1-ylidene)malonitrile (2Cl-INCN) and FBr-INCN units simultaneously. The symmetrical molecule <b>BQ-2FBr</b> possesses an elevated LUMO energy level, while the asymmetrical molecule <b>BQ-2Cl-FBr</b> displays a broadened absorption spectrum with a high extinction coefficient and better molecular stacking property. When combined with PM6, the <b>BQ-2FBr</b> device achieves a very good <i>V</i>_OC of 0.944 V and a moderate PCE of 10.11%. Despite a decline in the <i>V</i>_OC of the PM6:<b>BQ-2Cl-FBr</b> device to 0.928 V, simultaneous enhancement in the short circuit current density (<i>J</i>_SC) and fill factor (FF) was observed. This resulted in an augmented PCE of 11.54%, a development primarily attributed to the improved charge collection and exciton dissociation properties, suppression of charge recombination, enhancement of molecular stacking property and better morphology of the blend film, and acceleration of exciton diffusion time. This work describes the important influence of distinct brominated terminal groups on the photovoltaic performance of alkoxyphenyl-substituted quinoxalinyl A-DA′D-A SMAs, which may offer a useful structural guideline for the development of promising SMAs for high-efficiency and large <i>V</i>_OC OSCs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3866–3876 3866–3876"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675835","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effects of Metal-Cation Doping on Photocatalytic H2 Evolution Activity of Layered Perovskite Oxynitride K2LaTa2O6N","authors":"Hideya Tsuchikado,&nbsp;Shuji Anabuki,&nbsp;Ovidiu Cretu,&nbsp;Yuki Kinoshita,&nbsp;Masashi Hattori,&nbsp;Yuta Shiroma,&nbsp;Dongxiao Fan,&nbsp;Megumi Okazaki,&nbsp;Takuto Soma,&nbsp;Fumitaka Ishiwari,&nbsp;Shunsuke Nozawa,&nbsp;Toshiyuki Yokoi,&nbsp;Michikazu Hara,&nbsp;Koji Kimoto,&nbsp;Akira Yamakata,&nbsp;Akinori Saeki and Kazuhiko Maeda*,&nbsp;","doi":"10.1021/acsaem.4c0313110.1021/acsaem.4c03131","DOIUrl":"https://doi.org/10.1021/acsaem.4c03131https://doi.org/10.1021/acsaem.4c03131","url":null,"abstract":"<p >Aliovalent cation doping into a heterogeneous photocatalyst affects several of its physicochemical properties, including its morphological characteristics, optical absorption behavior, and charge carrier dynamics, causing a drastic change in its photocatalytic activity. In the present work, we investigated the effects of aliovalent cation doping on the visible-light H₂-evolution photocatalytic activity of the Ruddlesden–Popper layered perovskite oxynitride K₂LaTa₂O₆N. The photocatalytic activity toward H₂ evolution from an aqueous NaI solution was found to be enhanced by an increase in the specific surface area of the K₂LaTa₂O₆N photocatalyst, which could be realized upon doping with lower-valence cations (e.g., Mg²⁺, Al³⁺, and Ga³⁺). Among the dopants examined at 1 mol % doping, Ga resulted in the highest activity. The activity of the Ga-doped specimen was further improved with increasing Ga concentration, where the maximal activity was obtained at 10 mol %, corresponding to an apparent quantum yield of 2.7 ± 0.4% at 420 nm from aqueous methanol. This number is the highest reported for a layered oxynitride photocatalyst. In the Ga-doped K₂LaTa₂O₆N, a trade-off was observed between the Ga concentration and the photocatalytic activity. Although doping with Ga reduced the particle size of K₂LaTa₂O₆N and suppressed undesirable charge recombination, it led to an enlarged bandgap, unsuitable for visible-light absorption.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3541–3552 3541–3552"},"PeriodicalIF":5.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaem.4c03131","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675690","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Welcoming New Associate Editors to ACS Applied Energy Materials: Professor Huanping Zhou and Professor Ayan Datta","authors":"Yiying Wu,&nbsp; and ,&nbsp;Chengmei Zhong,&nbsp;","doi":"10.1021/acsaem.5c0048610.1021/acsaem.5c00486","DOIUrl":"https://doi.org/10.1021/acsaem.5c00486https://doi.org/10.1021/acsaem.5c00486","url":null,"abstract":"","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2660–2662 2660–2662"},"PeriodicalIF":5.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}