ACS Applied Energy Materials最新文献

{"title":"Effect of Transition-Metal Doping in Bismuth Titanate Nanostructures for Enhancing the Photocatalytic Efficiency in the Photodegradation of BPA and Photocatalytic CO2 Hydrogenation","authors":"Isha Arora,&nbsp;, ,&nbsp;Seema Garg*,&nbsp;, ,&nbsp;Andras Sapi,&nbsp;, ,&nbsp;Mohit Yadav,&nbsp;, ,&nbsp;Anastasiia Efremova,&nbsp;, ,&nbsp;Ákos Szamosvölgyi,&nbsp;, ,&nbsp;Sumant Upadhyay,&nbsp;, ,&nbsp;Uttam Gupta,&nbsp;, ,&nbsp;Pravin Popinand Ingole,&nbsp;, and ,&nbsp;M.M. Abdullah,&nbsp;","doi":"10.1021/acsaem.5c01873","DOIUrl":"https://doi.org/10.1021/acsaem.5c01873","url":null,"abstract":"<p >The present study aims to evaluate the photocatalytic efficiency of transition metal-modified bismuth titanate (BT) for the photocatalytic degradation of a recalcitrant pollutant “bisphenol A” (BPA) and photocatalytic CO₂ hydrogenation. Concentration studies of dopants (nickel, Ni; cobalt, Co; and iron, Fe) have been carried out at two distinct concentrations (0.1–0.2 mol %). Transition-metal dopants into the BT lattice modify its electronic structure and charge-carrier dynamics, leading to enhanced photocatalytic efficacy of pristine bismuth titanate. Among the doped samples, Ni-doped BT exhibited the highest photocatalytic efficiency, achieving superior degradation of BPA (approximately 61%) and highest CO₂ conversion (32.8%) and reduction to C₁ products, selectively carbon monoxide (CO) and methane (CH₄), attributed to its optimal band gap and improved electron–hole separation. Moreover, iron doping further led to the proximal degradation of BPA (55%) and 32.1% CO₂ conversion, followed by 52% degradation of BPA and 28.8% CO₂ conversion by cobalt-doped BT. This current investigation explores the impact of transition-metal modification on BT nanocrystals. Factors such as interfacial charge transfer, band gap adjustments, and surface area played a role in achieving high CO₂ conversion and a notable increase in CH₄ production compared to pristine BT.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13485–13498"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104035","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":"Clean Production of 3,4-Dihydronaphthalen-1(2H)-one via the Photocatalytic Selective Oxidation of Tetraline: A High Value-Added Utilization of Naphthalene","authors":"Kuanhong Cao,&nbsp;, ,&nbsp;Xiaoyu Zhou,&nbsp;, ,&nbsp;Shanming Lu*,&nbsp;, ,&nbsp;Lei Yu*,&nbsp;, and ,&nbsp;Juan Du*,&nbsp;","doi":"10.1021/acsaem.5c02219","DOIUrl":"https://doi.org/10.1021/acsaem.5c02219","url":null,"abstract":"<p >Naphthalene, a major environmental pollutant, is generated in large quantities as a byproduct during the distillation of coal tar and petroleum in the energy chemical industry. Presently, the common harmless treatment of the chemical is to partially hydrogenate it into 1,2,3,4-tetrahydronaphthalene (tetraline), which is an industrial solvent. This work reports a novel technique that can further enhance the economic added value for naphthalene treatment, i.e., the photocatalytic selective oxidation of tetraline into 3,4-dihydronaphthalen-1(2<i>H</i>)-one. The reaction was performed under environment-friendly conditions using boron-doped polymer carbon nitride as a catalyst, affording a good product yield at 81%. The morphology, structure, and optical properties of the catalyst show that the synergistic effect of boron doping and nitrogen defects is the decisive reason for obtaining excellent photocatalytic performance.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13877–13883"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104021","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":"Amide-Bonded 2,4,6-Tris(carboxyphenyl)-1,3,5-triazine with B-Doped Carbon Nitride Z-Scheme Heterojunction for Efficient Photocatalytic Hydrogen Production","authors":"Tania Tofaz,&nbsp;, ,&nbsp;Jing-Han Li,&nbsp;, ,&nbsp;Shuai Chen,&nbsp;, ,&nbsp;Hao-Yang Ding,&nbsp;, ,&nbsp;Ikram Ullah,&nbsp;, and ,&nbsp;An-Wu Xu*,&nbsp;","doi":"10.1021/acsaem.5c00682","DOIUrl":"https://doi.org/10.1021/acsaem.5c00682","url":null,"abstract":"<p >Graphitic carbon nitride (g-C₃N₄, termed as CN) has emerged as a suitable photocatalyst strategy for hydrogen production from water splitting. However, it suffers from fast recombination of photogenerated carriers, poor visible light absorption, and low photocatalytic performance. Herein, we employ urea and NaBH₄ as precursors for boron-doped CN (BCN) and then graft with 2,4,6-tris(carboxyphenyl)-1,3,5-triazine (TPT) named as BCN/TPT nanocomposites via the solvothermal method. Several characterization techniques, such as X-ray diffraction, Fourier transform infrared, X-ray photoelectron spectroscopy, and Raman spectra, have thoroughly examined the BCN/TPT heterostructure’s construction, photophysical characteristics, and charge transfer. The covalent interactions in BCN and TPT facilitate the extension of the π-conjugated system and spatial separation of electrons and holes, which in turn augments photocatalytic hydrogen production from water splitting under visible light (λ ≥ 420 nm). The optimal BCN/TPT-15 composite shows the highest H₂ evolution rate of 193.67 μmol h^–1, which is nearly 6 and 17 times greater than BCN (30.33 μmol h^–1) and CN (11.33 μmol h^–1). In addition, the optimal sample achieves an apparent quantum yield (AQY) of 7.93% at λ = 420 nm with an excellent photocatalytic stability of 16 h. This study presents an amide-bonded strategy for developing high-performance Z-scheme heterojunction photocatalysts for efficient solar-driven H₂ production.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13207–13214"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104123","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 Alkaline Oxygen Evolution at Industrial Current Densities with Hierarchical Electrode Architecture Overcoming Mass Transport Limitations","authors":"Lin Yuan,&nbsp;, ,&nbsp;Aikifa Raza,&nbsp;, ,&nbsp;Faisal AlMarzooqi,&nbsp;, and ,&nbsp;TieJun Zhang*,&nbsp;","doi":"10.1021/acsaem.5c01595","DOIUrl":"https://doi.org/10.1021/acsaem.5c01595","url":null,"abstract":"<p >Alkaline oxygen evolution reaction (OER) crucial for green hydrogen production can be primarily enhanced by electrode nanostructuring to increase active-site density and boost catalytic activity. However, above 0.5 A cm^–2, this enhancement is limited by insufficient O₂ transport due to the challenge of counteracting Marangoni-stabilized retention of large O₂ bubbles, and impaired OH^– transport resulting from excessive nucleation-site density. Herein, we demonstrate a three-tier hierarchical electrode architecture that overcomes the mass transport limitations while enhancing catalytic activity via nanocrystalline NiFe layered double hydroxide nanosheets. Pore confinement-induced Laplace pressure gradients enforce bubble self-ejection, which reduces departure diameters to sub-50 μm and bubble ohmic overpotential by 61.5%. Confining nucleation to single nanocavity in microcavities with large spacings reduces nucleation density by 89.6% and eliminates OH^– transport blockage. The proposed approach enables ultralow transport and total OER overpotentials of 62 mV and 280 mV at 1.0 A cm^–2, dropping by 75.5% and 46.1%, respectively.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13306–13317"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c01595","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104020","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":"Temperature-Resilient Monolithic Perovskite/Silicon Tandems Enabling Crystalline Front TCO Integration","authors":"Ahmed Ali Said,&nbsp;, ,&nbsp;Lorenzo Mardegan,&nbsp;, ,&nbsp;Esma Ugur,&nbsp;, ,&nbsp;Zhaoning Song,&nbsp;, ,&nbsp;Pia Dally,&nbsp;, ,&nbsp;Bumin Yildirim,&nbsp;, ,&nbsp;Drajad S. Utomo,&nbsp;, ,&nbsp;Arsalan Razzaq,&nbsp;, ,&nbsp;Deniz Turkay,&nbsp;, ,&nbsp;Christian M. Wolff,&nbsp;, ,&nbsp;Monica Morales-Masis,&nbsp;, ,&nbsp;Yanfa Yan,&nbsp;, ,&nbsp;Henk J. Bolink,&nbsp;, ,&nbsp;Erkan Aydin*,&nbsp;, and ,&nbsp;Stefaan De Wolf*,&nbsp;","doi":"10.1021/acsaem.5c02044","DOIUrl":"https://doi.org/10.1021/acsaem.5c02044","url":null,"abstract":"<p >Front transparent conductive oxides (TCOs) that combine high conductivity with broadband transparency are essential to minimize resistive and optical losses in perovskite/silicon tandem solar cells. While indium zinc oxide (IZO) is a commonly used front electrode, its amorphous nature leads to undesired absorption losses near the band edge, thereby constraining the tandem current. Here, we explore the use of crystalline Zr-doped indium oxide (IZrO), featuring a higher transparency at its band edge, to replace IZO as the front electrode. Full crystallization of IZrO requires postannealing at temperatures &gt;190 °C, which raises concerns around its compatibility with typically employed charge transport layers and the perovskite layer itself. Our work reveals that hole- and electron-selective contacts (NiO_<i>x</i>/MeO-2PACz and C₆₀/SnO₂, respectively) as used in our tandems endure such temperatures. Conversely, the wide bandgap CsFAMAPbI_<i>x</i>Br_3–<i>x</i> perovskite composition, deposited by solution and sequential hybrid processes, degrades upon high-temperature annealing. Notably, we identified substantial differences between the solution- and hybrid-processed perovskites through comprehensive analysis, where the latter exhibited higher temperature resilience. As a result, only hybrid-processed perovskite/silicon tandem devices partially retained their initial power conversion efficiency after high-temperature annealing. Our work underlines the urgency to develop high-temperature-resilient perovskites to advance perovskite/silicon tandem photovoltaics to their full performance potential, and, arguably, to improve their overall reliability under thermal stress.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13722–13731"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104022","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":"Ultraviolet-Induced Formation of Silver Nanoparticles Anchored by the Conductive-Viscous Polypyrene–Polydopamine Copolymer on CFx Surface for High-Power Li/CFx Battery","authors":"Yifan Liu*,&nbsp;, ,&nbsp;Jiacheng He,&nbsp;, ,&nbsp;Jiali Du,&nbsp;, ,&nbsp;Shengnan Yang,&nbsp;, ,&nbsp;Yong Fan,&nbsp;, ,&nbsp;Shahab Ahmad,&nbsp;, and ,&nbsp;Xian Jian*,&nbsp;","doi":"10.1021/acsaem.5c01905","DOIUrl":"https://doi.org/10.1021/acsaem.5c01905","url":null,"abstract":"<p >The high energy density lithium/carbon fluoride (Li/CF_<i>x</i>) battery meets the challenge of limited high-rate discharge performance due to the low intrinsic conductivity of CF_<i>x</i>. Herein, an inorganic/organic (Ag/PPy-PDA) synergistic conductivity strategy is developed to suppress CF_<i>x</i> polarization, addressing the ultrahigh rate of CF_<i>x</i> batteries for the high F content. Bioinspired by mussel surface chemistry, UV-mediated synthesis of Ag nanoparticles on CF_<i>x</i> surfaces is achieved through a polypyrene–polydopamine (PPy-PDA) copolymer-assisted reduction of a silver ammonia solution. During UV irradiation, the copolymer serves a dual function: stabilizing C–F bonds against alkaline degradation in silver ammonia solutions and hindering the defluorination under UV exposure. Detailed mechanistic studies reveal synergistic adhesive growth and surface-protection effects, enabling the precise Ag nanoparticle assembly on CF_<i>x</i>. The as-designed CF_<i>x</i>@PPy-PDA@Ag composite possesses the advantage of a high F/C ratio, excellent inorganic/organic conductive path, and good wettability of the electrolyte. Therefore, the optimal Li/CF_<i>x</i> battery (CF_<i>x</i>@PPy-PDA@Ag-10%) achieved a high discharge rate of 15000 mA·g^–1, delivering a high-power density of 22,404.37 W·kg^–1. This inorganic/organic (Ag/PPy-PDA) synergistic conductivity strategy lights up the high-rate Li/CF_<i>x</i> batteries with a high F/C ratio. A DFT calculation is conducted for CF_<i>x</i>, and the result shows that the conductivity is significantly improved, and the interaction between C–F bonds was significantly weakened after the Ag NPs are deposited on the surface.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13576–13585"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104018","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":"Unveiling the Superior Rate Performance of Sodiated Manganese Oxides for Ca-Ion Hybrid Supercapacitors","authors":"Aneesh Anand Nechikott,&nbsp;, ,&nbsp;Anjeline Williams,&nbsp;, ,&nbsp;Pitchai Ragupathy,&nbsp;, and ,&nbsp;Prasant Kumar Nayak*,&nbsp;","doi":"10.1021/acsaem.5c00996","DOIUrl":"https://doi.org/10.1021/acsaem.5c00996","url":null,"abstract":"<p >Sodiated manganese oxides are promising electrode materials for hybrid supercapacitors, which possess higher gravimetric capacitance (<i>C</i>_g) in aqueous electrolytes containing divalent cations compared to that of monovalent cations. This study explores the electrochemical capacitive performances of hydrothermally synthesized sodiated manganese oxide (NaMnO₂) in the aqueous electrolytes of 0.5 M Mg(NO₃)₂ (MNE) and 0.5 M Ca(NO₃)₂ (CNE) containing divalent cations of Mg²⁺ and Ca²⁺ ions. The <i>C</i>_g values of NaMnO₂ (NMO) are found to be 432 F g^–1 (583 mF cm^–2) and 308 F g^–1 (462 mF cm^–2), respectively, in MNE and CNE electrolytes when cycled at 0.6 A g^–1. Very impressively, the prepared NMO exhibits <i>C</i>_g values of 166 F g^–1 (249 mF cm^–2) and 115 F g^–1 (155 mF cm^–2) in CNE and MNE electrolytes, respectively, at a very high specific current (<i>I</i>_s) of 10 A g^–1, indicating its high-rate performance in the CNE electrolyte. The variation in the electrochemical performance of the NMO between Mg²⁺ and Ca²⁺ is correlated to the charge density, size of the hydrated ions, and desolvation energy. Furthermore, AC||NMO hybrid capacitors are fabricated, which deliver a higher <i>C</i>_g of 63.3 F g^–1 in MNE compared to that of 54.0 F g^–1 in the CNE electrolyte at 0.2 A g^–1. The hybrid devices exhibit energy densities (<i>E</i>_d) of 35.0 Wh kg^–1 and 30.6 Wh kg^–1 at 0.2 kW kg^–1, whereas they are found to be 4.2 and 12.4 Wh kg^–1 in Mg²⁺ and Ca²⁺-based electrolytes, respectively, at a power density (<i>P</i>_d) of 7 kW kg^–1, thus demonstrating its high energy and high-power characteristics in an aqueous Ca(NO₃)₂ electrolyte.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13215–13230"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104039","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":"Energy-Saving H2 Production through H2S Electrolysis Accompanying Solid Sulfur Recovery Using a Ni3S2/Ni3N Heterostructure as the Electrocatalyst","authors":"Nibedita Sinha,&nbsp;, ,&nbsp;Chandni Das,&nbsp;, ,&nbsp;Santanu Pal,&nbsp;, and ,&nbsp;Poulomi Roy*,&nbsp;","doi":"10.1021/acsaem.5c01952","DOIUrl":"https://doi.org/10.1021/acsaem.5c01952","url":null,"abstract":"<p >The thermodynamically feasible electrochemical sulfion oxidation reaction (SOR) is advantageous for degrading the toxic H₂S pollutant into the value-added chemical sulfur but often suffers from catalyst passivation due to blockage of electroactive sites by accumulation of solid sulfur. The strategic design of electrocatalysts with enhanced electrochemical activity and improved sulfur tolerance is thereby crucial to fully harness the benefits of the SOR. In this work, we developed nickel sulfide nanorods decorated with nickel nitride nanoparticles directly grown on conductive nickel foam as an efficient trifunctional electrocatalyst for the SOR, oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Optimized Ni₃S₂/Ni₃N showed lower electrode potentials of 0.25, 1.487, and 0.89 V to achieve a benchmark current density of 10 mA cm^–2 for the SOR, OER, and HER, respectively. The hybrid H₂S electrolysis setup employing a Ni₃S₂/Ni₃N electrocatalyst drastically reduced the cell potential by 1.24 V compared to that of conventional water electrolysis at a current density of 200 mA cm^–2. Having said that, heterostructure formation not only enhances the activity for the SOR but also helps to avoid sulfur poisoning, enabling the electrocatalyst to sustain for 100 long hours at a high current density of 100 mA cm^–2. Consequently, the approach with the developed electrocatalyst has the ability to reduce the energy consumption by 59.22%, which can make rigorous, economically viable H₂ production driven by solar energy.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13631–13644"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104067","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":"Synergistic Redox Modulation in Hollow Mesoporous Frameworks for High-Performance Symmetric and Asymmetric Supercapacitors","authors":"Kajal Panchal,&nbsp;, ,&nbsp;Kritika S. Sharma,&nbsp;, ,&nbsp;Naresh Rajpurohit,&nbsp;, and ,&nbsp;Dinesh Kumar*,&nbsp;","doi":"10.1021/acsaem.5c01931","DOIUrl":"https://doi.org/10.1021/acsaem.5c01931","url":null,"abstract":"<p >Transition metal vanadates (TMVs) are promising candidates for high-performance supercapacitor electrode materials owing to their rich redox chemistry, synergistic interactions and cost-effectiveness. However, their practical application is still limited by poor intrinsic conductivity, sluggish ion transport, restricted accessibility of redox-active sites, and structural instability, which collectively hinder the simultaneous attainment of high energy density and long-cycle-life.Herein, an approach based on the “mesopore-confined synergistic redox modulation” is proposed to concurrently enhance conductivity, increase the density of accessible redox-active sites, and improve structural stability. This is achieved by synthesizing a cerium-incorporated cobalt vanadate (CVO@3Ce) hollow mesoporous structure via a glycerol-assisted soft template method. The resulting material, when employed in both aqueous symmetric supercapacitors (ASS) and asymmetric supercapacitors (AAS), delivers energy densities of 34.72 and 47.77 Wh kg^–1, respectively, with capacitance retention of 75.08% (ASS) and 81.20% (AAS) after 10,000 cycles. This work demonstrates an effective strategy for designing high-energy, long-cycle-life electrodematerials for high-performance supercapacitors.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13561–13575"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104122","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":"Molecular Complex as a Charge-Transfer Agent at the Lithium Interface for Dendrite-Free Cycling","authors":"Ipsita Pal,&nbsp;, ,&nbsp;Aditya Rawal*,&nbsp;, and ,&nbsp;Dipan Kundu*,&nbsp;","doi":"10.1021/acsaem.5c02097","DOIUrl":"https://doi.org/10.1021/acsaem.5c02097","url":null,"abstract":"<p >The practical realization of lithium metal batteries (LMBs)─long hailed for their high theoretical energy density─continues to be impeded by the persistent challenge of lithium dendrite formation, which compromises safety and cycling stability. In this study, we introduce 5,10,15,20-tetrakis(pentafluorophenyl)porphyrin (TPP) as an electrolyte additive to suppress dendritic lithium growth. The porphyrin additive forms an in situ lithium-TPP complex at the Li metal interface, which facilitates the interfacial charge transfer and homogenizes the Li⁺ flux, thereby stabilizing the lithium metal deposition. Symmetric cells incorporating 20 mM TPP in a commercial electrolyte, with a thin polymeric separator that offers minimal resistance to dendritic penetration, exhibit stable cycling for over 1000 h at 0.5 mA cm^–2 without short-circuiting and stable voltage response under increasing current, significantly outperforming the reference cell without the TPP-containing electrolyte, which suffers rapid short-circuit failure. Scanning electron microscopy reveals a compact lithium morphology with the TPP-modified electrolyte, while <i>operando</i> solid-state ⁷Li NMR spectroscopy during symmetric Li-cell cycling confirms the suppression of dendrite formation. Full cells using Li₄Ti₅O₁₂ cathodes demonstrate 90% capacity retention over 150 cycles, with a Coulombic efficiency of 99.9%. These results highlight the potential of porphyrin-based additives in enabling safe and long-lasting lithium metal batteries, and may inspire broader exploration of molecular complexes as a dynamic interphase in next-generation energy storage systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13763–13773"},"PeriodicalIF":5.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104038","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}