{"title":"Constructing 3D crosslinked CeO2 nanosheet/graphene architectures anchored with Pd nanoparticles for boosted formic acid and methanol oxidation performance","authors":"Cuizhen Yang, Tingyao Wang, Tianyi Wang, Hao Yuan, Hongxing Li, Haiyan He, Dongming Liu, Huajie Huang","doi":"10.1039/d5qi00420a","DOIUrl":"https://doi.org/10.1039/d5qi00420a","url":null,"abstract":"In recent years, there is growing interest in direct formic acid fuel cells and direct methanol fuel cells due to the diminishing energy resources and escalating environmental concerns, which stimulates the rapid development of advanced anode catalysts towards the formic acid and methanol oxidation reactions. This study outlines an efficient bottom-up approach for the controllable fabrication of three-dimensional (3D) crosslinked CeO2 nanosheet/graphene architectures anchored with Pd nanoparticles (Pd/CeO2-G) via a solvothermal co-building process. The existence of 3D graphene skeletons introduces numerous pore channels for the fast transportation of reactants and electrons, while the incorporation of CeO2 nanosheets provides abundant oxygen vacancies to stabilize Pd species as well as reduce the CO adsorption on active surfaces. As a result, the as-synthesized Pd/CeO2-G architectures exhibit impressive electrocatalytic formic acid and methanol oxidation properties including large electrochemically active surface areas, high mass activities, and exceptional long-term stability, which make them more competitive than traditional Pd catalysts supported by carbon black, carbon nanotube, and graphene matrices.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"1 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multi-structured and Ligand Modified NiFe LDH with Self-Optimization for Efficient Oxygen Evolution Reaction.","authors":"Zi-Ye Liu, Jiu-Jiu Ge, Ji-Ming Hu","doi":"10.1039/d5qi00296f","DOIUrl":"https://doi.org/10.1039/d5qi00296f","url":null,"abstract":"Nickel foam (NF) self-supported NiFe LDH electrodes have been widely studied for their excellent oxygen evolution reaction (OER) performance. However, these electrodes synthesized via conventional electrodeposition or hydrothermal methods are still unsatisfactory because they have insufficient specific surface area and suboptimal activity. In this study, we report on NF-supported NiFe LDH electrodes directly derived from NF-supported-bimetallic MOF-74(NiFe). The as-prepared NiFe LDH shows a hierarchical structure and inherit the molecule-level porosity of MOF-74 precursor. The as-prepared electrode undergoes self-optimization during the OER process, significantly increasing the electrochemical active surface area and providing numerous catalytic sites. In addition, the 2, 5-dihydroxyterephthalate (DHTP) ligand, released from MOF-74 during its dissociation, enables to chemically modify NiFe LDH. The ligand well promotes the formation of Ni(III) and resists Cl⁻ corrosion. For these reasons, LDH-MOF74@NF superiors to almost all other NiFe LDH@NF electrodes as previously reported in literature, exhibiting excellent OER performance and high durability in both KOH and KOH/NaCl solutions with overpotentials of 244 mV and 254 mV at 100 mA cm-2, respectively.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"9 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Novel Strategy to Prepare Pure Cu4TiSe4 and Its High-Pressure Raman and Thermoelectric Performance Investigation","authors":"Guangfeng Zhang, Tonghan Yang, Wei He, Zhikai Zhu, Hui Luo, Shuohai Fang, Chang-Zhong Liao","doi":"10.1039/d5qi00707k","DOIUrl":"https://doi.org/10.1039/d5qi00707k","url":null,"abstract":"Low lattice thermal conductivity is crucial for enhancing the dimensionless figure of merit (ZT) which is primarily responsible for determining the energy conversion efficiency of thermoelectric materials. Cu4TiSe4 exhibits ultra-low lattice thermal conductivity at room temperature. However, achieving a pure single phase has been challenging in prior research due to the high volatility of Se. This study presents a novel approach for obtaining single-phase Cu4TiSe4 through the use of Cu2Se/TiSe2 precursors coupled with spark plasma sintering. Phase purity and structure were confirmed by Rietveld XRD analysis and TEM. High-pressure Raman studies revealed that a blue shift of the vibration mode towards high frequency was observed, and a pressure-induced transition of local structure occurs at ~10 GPa. XPS analysis confirmed consistent chemical states between bulk and nano-structured Cu4TiSe4, indicating robust structural stability. Remarkably, bulk Cu4TiSe4 exhibits an ultra-low thermal conductivity of 0.1019 W·m-1·K-1 at room temperature, while the nanostructured Cu4TiSe4 achieved record-low value of 0.0503 W·m-1·K-1. This work establishes a rapid synthesis method for high-purity polycrystalline single-phase Cu4TiSe4, providing novel synthesis strategy and advancing the development of thermoelectric materials with low lattice thermal conductivity.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"25 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154274","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Iyan Subiyanto, Winda Devina, Segi Byun, Hyunuk Kim
{"title":"Facile template-guided synthesis of conformal Bi2O3-coated LiMn2O4 hollow microspheres for enhanced stability of lithium-ion battery cathodes","authors":"Iyan Subiyanto, Winda Devina, Segi Byun, Hyunuk Kim","doi":"10.1039/d5qi00918a","DOIUrl":"https://doi.org/10.1039/d5qi00918a","url":null,"abstract":"Manganese-based cathodes have gained significant attention for lithium-ion batteries (LIBs) due to their cost-effectiveness, safety, and environmental compatibility. Among them, LiMn<small><sub>2</sub></small>O<small><sub>4</sub></small> (LMO) is a promising candidate due to its high operating voltage (4.0 V) and three-dimensional lithium-ion transport pathways. However, its practical application is limited by Mn dissolution, induced by the disproportionation of Mn<small><sup>3+</sup></small>, leading to capacity fading and structural degradation. Surface coating strategies have been widely investigated to address this issue, with oxide coatings providing enhanced electrochemical stability while maintaining the intrinsic properties of LMO. Here, a Bi<small><sub>2</sub></small>O<small><sub>3</sub></small>-coated LiMn<small><sub>2</sub></small>O<small><sub>4</sub></small> hollow microsphere (BiLMOhms) was synthesized via a solution-based templated self-assembly method. This approach enables the formation of an ultrathin (2 nm) conformal Bi<small><sub>2</sub></small>O<small><sub>3</sub></small> coating, ensuring uniform coverage while preserving the LMO hollow structure. The Bi<small><sub>2</sub></small>O<small><sub>3</sub></small> layer improves the electrochemical performance by stabilizing the cathode-electrolyte interface, enhancing lithium-ion transport, and increasing the Mn<small><sup>4+</sup></small>/Mn<small><sup>3+</sup></small> ratio, thereby reducing Jahn-Teller distortion and suppressing Mn dissolution. Electrochemical characterization reveals that BiLMOhms exhibits superior cycling stability compared to pristine LMO. In half-cell tests, BiLMOhms retains 80.1% of its capacity after 1000 cycles, significantly higher than the 45.8 % retention of pristine LMO. Moreover, in a full-cell configuration with a graphite anode, BiLMOhms achieves a capacity retention of 89.5% after 100 cycles at 1C, compared to 38.4% for pristine LMO. The coating effectively mitigates capacity degradation while facilitating ionic transport at the cathode-electrolyte interface. This study demonstrates a cost-effective and scalable synthesis strategy for stabilizing Mn-based cathodes in next-generation fast-charging LIBs.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"49 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154098","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"pH-modulated Activation of Pendant Amine Leading to Rapid Electrocatalytic H2 Production by a Molecular Copper Complex in Acidic Water","authors":"Naseer Ahmed Shah, Thinles Dolkar, Suhana Karim, Jumana Ishrat, Chandan Das, Srewashi Das, ARITRO SINHA ROY, Kalishankar Bhattacharyya, Arnab Dutta","doi":"10.1039/d5qi00963d","DOIUrl":"https://doi.org/10.1039/d5qi00963d","url":null,"abstract":"A modular multidentate ligand scaffold is crafted by strategically incorporating three pyridines (NPy) and three imines along with a pendant tertiary amine (Ntert) around a mononuclear copper centre. This unique design leads to the generation of a molecular copper complex C1 with a dynamically adaptive coordination environment, where the multiple proton and electron movements can be accommodated. Complex C1 demonstrates rapid hydrogen generation from water across a wide pH range (pH 1.0–7.0), with a markedly enhanced catalytic performance under acidic conditions. At pH 1.0, C1 achieves high turnover numbers (TONs) of 1014 ± 10 within 1 hour and 2980 ± 20 over 3 hours. In operando spectroelectrochemical investigations, in conjunction with density functional theory (DFT) calculations, reveal a unique pH-dependent structural flexibility of the ligand scaffold around the Cu centre in C1. In near-neutral to slightly acidic media (pH 3.0-7.0), the protonation of an NPy group (pKa1~ 11.6) following its cleavage from Cu linkage provides the primary protonation site, which is essential for Cu-complex driven H2 production catalysis. The Ntert group (pKa2~ 2.8), positioned in the outer coordination sphere of Cu, gets involved in highly acidic conditions (pH < 3.0). Here, this pendant amine acts as the initial protonation site and alters the course of the catalysis by unleashing an energetically downhill reaction pathway consisting of spontaneous electron and proton transfer steps. This pH-specific participation of the pendant Ntert functionality is key for the escalated HER activity by C1 under strongly acidic conditions, which is rarely observed for Cu-based molecular complexes. Complementary surface and solution-phase analyses confirm the molecular integrity of the complex, supporting a homogeneous catalytic mechanism operative throughout the hydrogen evolution process.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"15 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144130215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaohui Guo, Jiangcheng Zhang, Xin Yu, hu yao, Wang XiaYu, Qiuhan Cao, Xiaoyi Dong
{"title":"Core-Shell Ru/NiOx@graphene Composite Aerogel as efficient Bifunctional Electrocatalysts for Overall Water Splitting","authors":"Xiaohui Guo, Jiangcheng Zhang, Xin Yu, hu yao, Wang XiaYu, Qiuhan Cao, Xiaoyi Dong","doi":"10.1039/d5qi00912j","DOIUrl":"https://doi.org/10.1039/d5qi00912j","url":null,"abstract":"The development of bifunctional catalysts with excellent catalytic properties is the main task for alkaline electrolytic water, and hence the construction of a novel crystalline/amorphous heterojunction catalysts is proved to be an effective strategy to realize bifunctional electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction(OER). In this paper, uniformly dispersed and highly active Ru/NiOx heterojunction anchored on the GA composites (Ru/NiOx@GA) were successfully synthesized by freeze-drying and calcination process. The results of XRD, TEM, and XPS tests show that there were strong interactions in the Ru/NiOx heterojunction and graphene, and the NiOx in the outer layer exert a squeezing effect on the Ru in the inner layer that generate charge transfer from Ni to Ru. As such, the Ru/NiOx@GA only requires a overpotentials of only 34 mV (HER) and 237 mV (OER) when reaching a current density of 10 mA cm-2 in 1 M KOH electrolyte, as well as display a roust cycling stability of over 200 h. A low decomposition voltage of 1.53 V and a high Faraday efficiency of 100% were obtained for the assembled overall water splitting (OWS) device. All these are attributed to the synergistic effect of between Ru/NiOx heterojunction resulting in charge-enriched Ru sites and oxidation state-corrected Ni site, as well as high conductivity of GA. This study highlights the unique advantages of the synergistic effect of both crystalline/amorphous heterojunctions and GA, which provides a new way to prepare GA-based materials for advanced multifunctional electrocatalytic applications.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"19 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kathryn Margaret Lawson, Tyler L Spano, Jordan M Roach, Connor J Parker, Sara Isbill, Andrew Miskowiec
{"title":"Thermal Decomposition of Neptunyl Ammonium Nitrate: Mechanistic Insights and Structural Characterization of the Np2O5 Intermediate Phase","authors":"Kathryn Margaret Lawson, Tyler L Spano, Jordan M Roach, Connor J Parker, Sara Isbill, Andrew Miskowiec","doi":"10.1039/d5qi01015b","DOIUrl":"https://doi.org/10.1039/d5qi01015b","url":null,"abstract":"Neptunium (Np) possesses a rich and unique chemistry that often diverges from other actinide elements yet remains relatively underexplored compared with the other light actinides. A resurgence of interest in Np has been spurred by the application of <small><sup>237</sup></small>Np for plutonium-238 (<small><sup>238</sup></small>Pu) production for use in radioisotope thermoelectric generators (RTGs), necessitating evaluation of Np chemical reactions and materials. The work presented here studied the thermal decomposition of neptunyl ammonium nitrate (NH<small><sub>4</sub></small>Np<small><sup>VI</sup></small>O<small><sub>2</sub></small>(NO<small><sub>3</sub></small>)<small><sub>3</sub></small>) for synthesis of neptunium dioxide (NpO<small><sub>2</sub></small>), which is the target material used for production of <small><sup>238</sup></small>Pu. Additionally, structural characterization of the intermediate solid Np pentoxide (Np<small><sub>2</sub></small>O<small><sub>5</sub></small>) was performed. Advanced solid-state characterization techniques, including simultaneous thermal analysis (STA), powder X-ray diffraction (pXRD), Raman spectroscopy, and density functional theory (DFT) modeling have been combined to study the reaction pathways. Analysis revealed that NH<small><sub>4</sub></small>Np<small><sup>VI</sup></small>O<small><sub>2</sub></small>(NO<small><sub>3</sub></small>)<small><sub>3</sub></small> thermally decomposes to a proposed neptunyl nitrate intermediate, followed by Np<small><sub>2</sub></small>O<small><sub>5</sub></small> and finally NpO<small><sub>2</sub></small>, all within the temperature range of 150℃–600℃. Further characterization of the pentoxide intermediate provided the first Raman spectra of pure-phase Np<small><sub>2</sub></small>O<small><sub>5</sub></small> and associated DFT modeling confirmed Raman peak assignments for this phase. These findings provide mechanistic information to advance production of the critical radioisotope 238Pu and advance the state of knowledge on Np materials chemistry using modern characterization techniques.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"31 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Kinetics enhancement of hierarchical hollow boride microspheres for double-high aqueous Zn-based batteries","authors":"Shiyu Gu, Yaqi Wu, Liyuan Liu, Yang Li, Zihan Yang, Xiaodan Xia, Jinling Zhao, Qingliang Lv, Dehong Chen, Zhenyu Xiao","doi":"10.1039/d5qi00595g","DOIUrl":"https://doi.org/10.1039/d5qi00595g","url":null,"abstract":"The unsatisfactory kinetics of the cathode electrode material are the key factor hampering the achievement of double-high performance (both high energy and high power) in aqueous Zn-based batteries. In this work, an amorphous Co-doped Ni<small><sub>2</sub></small>B hollow microsphere has been successfully constructed by a controllable etching process using a bimetallic MOF precursor. The unique hierarchical hollow structure and amorphous phase can provide more accessible active centers, abundant channels and a shortened diffusion path for enhanced redox kinetics. Therefore, the obtained CNB sample exhibits an ultra-high capacity of 2173 F g<small><sup>−1</sup></small> (301.8 mA h g<small><sup>−1</sup></small>) at a current density of 1 A g<small><sup>−1</sup></small> and can still maintain an initial value of 87.0% when the current density increases to 10 A g<small><sup>−1</sup></small>, achieving outstanding rate performance of CNB. Furthermore, a CNB//rGO–Zn aqueous zinc battery device is fabricated, which exhibits a high energy density of 454.7 W h kg<small><sup>−1</sup></small> at a high power density of 0.46 kW kg<small><sup>−1</sup></small>. In addition, the CNB//rGO–Zn device can maintain 80.01% of its initial value at a current density of 6 A g<small><sup>−1</sup></small> after 6600 cycles, revealing outstanding stability. Meanwhile, the energy storage mechanism is explored using <em>ex situ</em> XPS spectroscopy and <em>ex situ</em> TEM mapping, demonstrating that the energy storage mechanism of the CNB//rGO–Zn device involves a mixed process of the Faraday redox reaction of Co/Ni elements and the adsorption and desorption of Zn species. The CNB//rGO–Zn soft-packed device can operate an electronic thermometer for over 8 hours after several seconds of charging time, revealing its outstanding application prospect.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"96 3 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Boosting the growth kinetics of extra-large pore zeolite ZEO-1","authors":"Haijun Yu, Wen-Jing Zhang, Yiqing Sun, Guangying Fu, Doudou Cai, Nourrdine Chaouati, Ludovic Pinard, Mohammad FAHDA, Feng Shao, Peng Lu, Valentin Valtchev","doi":"10.1039/d5qi00709g","DOIUrl":"https://doi.org/10.1039/d5qi00709g","url":null,"abstract":"The first stable aluminosilicate zeolite with extra-large pores, ZEO-1, marks the great breakthrough in zeolite community after decades of exploration and endeavors, opening possibilities for processing bulky substrates. However, the long synthesis cycle and relatively low reproducibility hinders the wide application of this intriguing material. Here, we report the synthesis of ZEO-1 zeolite using a tentatively so-called “deficient fluoride approach”, i.e., a small amount of fluoride sources was introduced to the gel rendering the stoichiometrically unbalanced charge of the cation and anion from the OSDA and fluoride sources. Using this approach, faster crystallization and higher reproducibility of ZEO-1 zeolite were achieved compared to the originally reported protocol. The physicochemical properties of the obtained products were analyzed using comprehensive characterizations, including PXRD, SEM, TEM, ICP-OES, TG, MAS NMR, FTIR, etc. The crystallization kinetics of ZEO-1 were performed by following up and characterizing the extracted products obtained at different temporal stages. The plausible role of fluoride in boosting the crystallization of ZEO-1 zeolite was discussed. The catalytic performance of alkylation of phenol with tert-butanol was evaluated and compared with other large and extra-large pore zeolites.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"40 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144096998","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Synergistic electrolyte engineering with TEABH4 additive: achieving oriented deposition and ultralong cycling in magnesium metal batteries","authors":"Qi Sun, Shaohua Luo, Wei Zhao, Xin Yan, Rui Huang, Yicheng Lin, Qiuyue Liu, Shengxue Yan, Xiaoping Lin","doi":"10.1039/d5qi00609k","DOIUrl":"https://doi.org/10.1039/d5qi00609k","url":null,"abstract":"Simple magnesium salt Mg(CF<small><sub>3</sub></small>SO<small><sub>3</sub></small>)<small><sub>2</sub></small>-based electrolytes often exhibit elevated charge-transfer resistance at the electrode interface owing to surface adsorption phenomena. Herein, to overcome this limitation, tetraethylammonium borohydride (TEABH<small><sub>4</sub></small>) was used as a moisture scavenger to chemically control the moisture content. Moreover, the uniform coverage of TEA<small><sup>+</sup></small> cations on the Mg anode surface regulated the Mg<small><sup>2+</sup></small> reduction rate and enabled the epitaxial growth of magnesium metal deposited along the (002) crystal plane. Electrochemical evaluation showed that the modified electrolyte (MAT-G2) remained stable for over 3500 hours at a current density of 1 mA cm<small><sup>−2</sup></small> and a capacity of 0.5 mA h cm<small><sup>−2</sup></small>. Additionally, the fabricated Mg||Cu cells achieved a high coulombic efficiency of 97.3% (over 2500 cycles). The critical current density of the cells reached 5.5 mA cm<small><sup>−2</sup></small>, achieving the highest value reported in similar works. This study underscores the critical role of eliminating water contamination and optimizing ion-transport kinetics in enhancing the performance of magnesium metal batteries.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"130 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097288","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}