Carbon Energy最新文献

{"title":"Coordination Tailoring of Pt Single-Atom Catalysts at Room Temperature and Their Exceptional Performance in Hydrogen Evolution Reaction","authors":"Joo-Won Lee,&nbsp;Haleem Ud Din,&nbsp;Taehun Im,&nbsp;Chang-Kyu Hwang,&nbsp;Jong Min Kim,&nbsp;Jung-Hoon Lee,&nbsp;Sohee Jeong","doi":"10.1002/cey2.720","DOIUrl":"https://doi.org/10.1002/cey2.720","url":null,"abstract":"<p>Single-atom catalysts (SACs) have garnered interest in designing their ligand environments, facilitating the modification of single catalytic sites toward high activity and selectivity. Despite various synthetic approaches, it remains challenging to achieve a catalytically favorable coordination structure simultaneously with the feasible formation of SACs at low temperatures. Here, a new type of coordination structure for Pt SACs is introduced to offer a highly efficient hydrogen evolution reaction (HER) catalyst, where Pt SACs are readily fabricated by atomically confining PtCl₂ on chemically driven NO₂ sites in two-dimensional nitrogen-doped carbon nanosheets at room temperature. The resultant Pt SACs form the NO₂–Pt–Cl₂ coordination structure with an atomic dispersion, as revealed by X-ray spectroscopy and transmission electron microscopy investigations. Moreover, our first-principles density functional theory (DFT) calculations show strong interactions in the coordination by computing the binding energy and charge density difference between PtCl₂ and NO₂. Pt SACs, established on the NO₂-functionalized carbon support, demonstrate the onset potential of 25 mV, Tafel slope of 40 mV dec⁻¹, and high specific activity of 1.35 A mg_Pt⁻¹. Importantly, the Pt SACs also exhibit long-term stability up to 110 h, which is a significant advance in the field of single-atom Pt catalysts. The newly developed coordination structure of Pt SACs features a single Pt active center, providing hydrogen binding ability comparable to that of Pt(111), enhanced long-term durability due to strong metal-support interactions, and the advantage of room-temperature fabrication.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.720","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171191","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Extended Electrochemical Window Via Interfacial Microdomain Regulation by a Bicontinuous Microemulsion-Based Heterogel Electrolyte","authors":"Yuzhen Qian,&nbsp;Long Su,&nbsp;Hongyue Jing,&nbsp;Chunxiao Chai,&nbsp;Fengjin Xie,&nbsp;Xiaoyong Qiu,&nbsp;Jingcheng Hao","doi":"10.1002/cey2.697","DOIUrl":"https://doi.org/10.1002/cey2.697","url":null,"abstract":"<p>Regulating the freedom and distribution of H₂O molecules has become the decisive factor in enlarging the electrochemical stability window (ESW) of aqueous electrolytes. Compared with the water in a bulk electrolyte, H₂O molecules at the electrode–electrolyte interface tend to directly split under bias potential. Therefore, the composition and properties of the interfacial microenvironment are the crux for optimizing ESW. Herein, we developed a heterogel electrolyte with wide ESW (4.88 V) and satisfactory ionic conductivity (4.4 mS/cm) inspired by the bicontinuous architecture and surfactant self-assembly behavior in the ionic liquid microemulsion-based template. This electrolyte was capable of expanding the ESW through the dynamic oil/water/electrode interface ternary structure, which enriched the oil phase and assembled the hydrophobic surfactant tails at the interface to prevent H₂O molecules from approaching the electrode surface. Moreover, the surfactant Tween 20 and polymer network effectively suppressed the activity of H₂O molecules through H-bond interactions, which was beneficial in expanding the operating voltage range and improving the temperature tolerance. The prepared gel electrolyte demonstrated unparalleled adaptability in various aqueous lithium-based energy storage devices. Notably, the lithium-ion capacitor showed an extended operating voltage of 2.2 V and could provide a high power density of 1350.36 W/kg at an energy density of 6 Wh/kg. It maintained normal power output even in the challenging harsh environment, which enabled 11,000 uninterrupted charge–discharge cycles at 0°C. This work focuses on the regulation of the interfacial microdomain and the restriction of the degree of freedom of H₂O molecules to boost the ESW of aqueous electrolytes, providing a promising strategy for the advancement of energy storage technologies.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.697","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Tellurium-Free, Sustainable Thermoelectric Device for Mid-Temperature Waste Heat Recovery","authors":"Vaskuri C. S. Theja,&nbsp;Vaithinathan Karthikeyan,&nbsp;Sanjib Nayak,&nbsp;Gopalan Saianand,&nbsp;Vellaisamy A. L. Roy","doi":"10.1002/cey2.689","DOIUrl":"https://doi.org/10.1002/cey2.689","url":null,"abstract":"<p>Famatinite (Cu₃SbS₄, <i>p</i>-type) and chalcopyrite (CuFeS₂, <i>n</i>-type) are well-recognized sustainable minerals with good intermediate-temperature thermoelectric performance. In this article, we utilize the inherent thermoelectric properties of these compounds to demonstrate real-time operational performance as a coupled thermoelectric generator (TEG) for waste heat recovery applications. First, we synthesized the polycrystalline and nano-grained famatinite and chalcopyrite materials with high purity through a sustainable synthesis process of mechanical alloying followed by hot pressing. A maximum output power of ~5 mW by the developed TEG was demonstrated while harvesting from a waste heat source of 723 K. Furthermore, the TEG performance via computational simulations for varied thermal gradients was validated. Our results highlight the sustainable development of thermoelectric power generator from earth-abundant minerals having strong stability and capacity to convert waste heat to electricity, which opens a new direction for fabricating a low-cost TEG for intermediate-temperature applications.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.689","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"LiZn/LiAlO2/Li2O-Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping","authors":"Huaming Qian,&nbsp;Xifei Li,&nbsp;Qinchuan Chen,&nbsp;Jingjing Wang,&nbsp;Xiaohua Pu,&nbsp;Wei Xiao,&nbsp;Yanyan Cao,&nbsp;Mengxin Bai,&nbsp;Wenbin Li,&nbsp;Zhengdong Ma,&nbsp;Guiqiang Cao,&nbsp;Ruixian Duan,&nbsp;Gaini Zhang,&nbsp;Kaihua Xu,&nbsp;Kun Zhang,&nbsp;Wei Yan,&nbsp;Jiujun Zhang","doi":"10.1002/cey2.714","DOIUrl":"https://doi.org/10.1002/cey2.714","url":null,"abstract":"<p>ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO-derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li₂O products upon lithiation of ZnO. However, the striking differences in the lithiophilicity between Li₂O and LiZn would result in a high overpotential during cycling. In this research, the Al₂O₃/<i>n</i>ZnO (<i>n</i> ≥ 1) hybrid layers were precisely fabricated by atomic layer deposition (ALD) to regulate the lithiophilicity of ZnO phase and Li₂O/LiZn configuration—determining the actual Li loading amount and Li plating/stripping processes. Theoretically, the Li adsorption energy (<i>E</i>_a) values of LiZn and Li₂O in the LiZn/Li₂O configuration are separately predicted as −2.789 and −3.447 eV. In comparison, the <i>E</i>_a values of LiZn, LiAlO_2, and Li₂O in the LiZn/LiAlO₂/Li₂O configuration upon lithiation of Al₂O₃/8ZnO layer are calculated as −2.899, −3.089, and −3.208 eV, respectively. Importantly, a novel introduction of LiAlO₂ into the LiZn/Li₂O configuration could enable the hierarchical Li plating/stripping and reduce the overpotentials during cycling. Consequently, the Al₂O₃/8ZnO-derived hybrid Li-metal anode could exhibit electrochemical performances superior to these of ZnO-derived Li anode in both symmetrical and full cells paired with a LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) cathode.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.714","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171285","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Interface Engineering Toward Surface-Activated Catalysts for Advanced Li–CO2 Batteries","authors":"Yanze Song,&nbsp;Bingyi Lu,&nbsp;Zhiwen Min,&nbsp;Haotian Qu,&nbsp;Yingqi Liu,&nbsp;Rui Mao,&nbsp;Yanli Chen,&nbsp;Yuanmiao Sun,&nbsp;Guangmin Zhou","doi":"10.1002/cey2.692","DOIUrl":"https://doi.org/10.1002/cey2.692","url":null,"abstract":"<p>Lithium–carbon dioxide (Li–CO₂) batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality. However, bidirectional catalysts design for improving the sluggish CO₂ reduction reaction (CO₂RR)/CO₂ evolution reaction (CO₂ER) kinetics remains a huge challenge. In this work, an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation, which significantly improves the electrocatalytic activity for both CO₂RR and CO₂ER. Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface, which leads to optimized binding affinity towards reactants and preferred Li₂CO₃ decomposition behavior, enabling excellent catalytic activity during CO₂ redox. Benefiting from the enhanced charge transfer ability, the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%. This work provides an attractive strategy to construct robust catalysts by interface engineering, which could inspire further design of superior bidirectional catalysts for Li–CO₂ batteries.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.692","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Novel Sn-Doped NASICON-Type Na3.2Zr2Si2.2P0.8O12 Solid Electrolyte With Improved Ionic Conductivity for a Solid-State Sodium Battery","authors":"Muhammad Akbar,&nbsp;Iqra Moeez,&nbsp;Young Hwan Kim,&nbsp;Mingony Kim,&nbsp;Jiwon Jeong,&nbsp;Eunbyoul Lee,&nbsp;Ali Hussain Umar Bhatti,&nbsp;Jae-Ho Park,&nbsp;Kyung Yoon Chung","doi":"10.1002/cey2.717","DOIUrl":"https://doi.org/10.1002/cey2.717","url":null,"abstract":"<p>Solid electrolytes face challenges in solid-state sodium batteries (SSSBs) because of limited ionic conductivity, increased interfacial resistance, and sodium dendrite issues. In this study, we adopted a unique Sn⁴⁺ doping strategy for Na_3.2Zr₂Si_2.2P_0.8O₁₂ (NZSP) that caused a partial structural transition from the monoclinic (<i>C</i>2/<i>c</i>) phase to the rhombohedral (<i>R</i>-3<i>c</i>) phase in Na_3.2Zr_1.9Sn_0.1Si_2.2P_0.8O₁₂ (NZSnSP1). X-ray diffraction (XRD) patterns and high-resolution transmission electron microscopy analyses were used to confirm this transition, where rhombohedral NZSnSP1 showed an increase in the Na2–O bond length compared with monoclinic NZSnSP1, increasing its triangular bottleneck areas and noticeably enhancing Na⁺ ionic conductivity, a higher Na transference number, and lower electronic conductivity. NZSnSP1 also showed exceptionally high compatibility with Na metal with an increased critical current density, as evidenced by symmetric cell tests. The SSSB, fabricated using Na_0.9Zn_0.22Fe_0.3Mn_0.48O₂ (NZFMO), Na metal, and NZSnSP1 as the cathode, anode, and the solid electrolyte and separator, respectively, maintains 65.86% of retention in the reversible capacity over 300 cycles within a voltage range of 2.0–4.0 V at 25°C at 0.1 C. The in-situ X-ray diffraction and X-ray absorption analyses of the P and Zr K-edges confirmed that NZSnSP1 remained highly stable before and after electrochemical cycling. This crystal structure modification strategy enables the synthesis of ideal solid electrolytes for practical SSSBs.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.717","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Recent Advances in Sn-Based Heterojunction-Type Anode Materials for Alkali-Ion Batteries","authors":"Hui Li,&nbsp;Zhiqiang Liu,&nbsp;Lei Li,&nbsp;Yehong Zhang,&nbsp;Zeheng Li,&nbsp;Huixin Lan,&nbsp;Zhenhe Zhu,&nbsp;Yuchen Wu,&nbsp;Jiajia Li,&nbsp;Chuanbo Zheng,&nbsp;Jun Lu","doi":"10.1002/cey2.703","DOIUrl":"https://doi.org/10.1002/cey2.703","url":null,"abstract":"<p>The urgent demand for clean energy solutions has intensified the search for advanced storage materials, with rechargeable alkali-ion batteries (AIBs) playing a pivotal role in electrochemical energy storage. Enhancing electrode performance is critical to addressing the increasing need for high-energy and high-power AIBs. Next-generation anode materials face significant challenges, including limited energy storage capacities and complex reaction mechanisms that complicate structural modeling. Sn-based materials have emerged as promising candidates for AIBs due to their inherent advantages. Recent research has increasingly focused on the development of heterojunctions as a strategy to enhance the performance of Sn-based anode materials. Despite significant advances in this field, comprehensive reviews summarizing the latest developments are still sparse. This review provides a detailed overview of recent progress in Sn-based heterojunction-type anode materials. It begins with an explanation of the concept of heterojunctions, including their fabrication, characterization, and classification. Cutting-edge research on Sn-based heterojunction-type anodes for AIBs is highlighted. Finally, the review summarizes the latest advancements in heterojunction technology and discusses future directions for research and development in this area.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.703","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Modulating the Local Charge Distribution of Single-Atomic Ru Sites for an Efficient Hydrogen Evolution Reaction","authors":"Youyu Long,&nbsp;Lingfeng Yang,&nbsp;Min Xi,&nbsp;Yifan Zhao,&nbsp;Hua Zhang,&nbsp;Tingting Liu,&nbsp;Anran Chen,&nbsp;Xuguang An,&nbsp;Guangzhi Hu,&nbsp;Zitao Ni","doi":"10.1002/cey2.690","DOIUrl":"https://doi.org/10.1002/cey2.690","url":null,"abstract":"<p>Ruthenium (Ru)-based electrocatalysts show great promise as substitutes for platinum (Pt) for the alkaline hydrogen evolution reaction (HER) because of their efficient water dissociation capabilities. Nevertheless, the strong adsorption of Ru–OH intermediates (Ru-OH_ad) blocks the active site, leading to unsatisfactory HER performance. In this study, we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP–CoP heterostructure-anchored Ru single-atom site catalyst (Ru-FeP-CoP/NPC). The obtained catalyst shows a low overpotential (28 mV at 10 mA cm⁻²) and a high mass activity (9.29 A mg⁻¹ at 100 mV), surpassing the performance of commercial Pt/C by a factor of 46. Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH⁻ blockages, accelerating water dissociation and facilitating hydrogen adsorption/desorption, thus enhancing HER activity. This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.690","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171460","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Locking Surface Dimensionality for Endurable Interface in Perovskite Photovoltaics","authors":"Xu Zhang,&nbsp;Yixin Luo,&nbsp;Xiaonan Wang,&nbsp;Ke Zhao,&nbsp;Pengju Shi,&nbsp;Yuan Tian,&nbsp;Jiazhe Xu,&nbsp;Libing Yao,&nbsp;Jingyi Sun,&nbsp;Qingqing Liu,&nbsp;Wei Fan,&nbsp;Rui Wang,&nbsp;Jingjing Xue","doi":"10.1002/cey2.718","DOIUrl":"https://doi.org/10.1002/cey2.718","url":null,"abstract":"<p>Surface passivation with organic ammoniums improves perovskite solar cell performance by forming 2D/quasi-2D structures or adsorbing onto surfaces. However, complexity from mixed phases can trigger phase transitions, compromising stability. The control of surface dimensionality after organic ammonium passivation presents significant importance to device stability. In this study, we developed a poly-fluorination strategy for surface treatment in perovskite solar cells, which enabled a high and durable interfacial phase purity after surface passivation. The locked surface dimensionality of perovskite was achieved through robust interaction between the poly-fluorinated ammoniums and the perovskite surface, along with the steric hindrance imparted by fluorine atoms, reducing its reactivity and penetration capabilities. The high hydrophobicity of the poly-fluorinated surface also aids in moisture resistance of the perovskite layer. The champion device achieved a power conversion efficiency (PCE) of 25.2% with certified 24.6%, with 90% of its initial PCE retained after approximately 1200 h under continuous 1-sun illumination, and over 14,400 h storage stability and superior stability under high-temperature operation.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 4","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.718","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143884060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Built-In Electric Field Effects Tailoring Solvation Sheath and Desolvation Processes of Solvated Zn2+ Toward Stable Aqueous Rocking-Chair Zinc-Ion Batteries","authors":"Peng Cai,&nbsp;Xin He,&nbsp;Kangli Wang,&nbsp;Zidong Zhang,&nbsp;Qingyuan Wang,&nbsp;Yumeng Liu,&nbsp;Haomiao Li,&nbsp;Min Zhou,&nbsp;Wei Wang,&nbsp;Kai Jiang","doi":"10.1002/cey2.691","DOIUrl":"https://doi.org/10.1002/cey2.691","url":null,"abstract":"<p>Currently, although some progress has been made in infancy-stage rocking-chair aqueous zinc-ion batteries (AZIBs), more discussions have focused only on the different electrochemical performances displayed by different material types rather than the intrinsic ion transport migration electrochemistry. Herein, we for the first time delve into the mechanism of tailoring the solvation sheath and desolvation processes at the electrode/electrolyte interfaces to enhance the structural stabilities in the deep discharge states. In this work, the TiO₂ front interfaces are induced on electrochemically active but unstable TiSe₂ host materials to construct unique TiO₂/TiSe₂–C heterointerfaces. According to X-ray absorption near edge structure (XANES), differential electrochemical mass spectrometry (DEMS), and electrochemical quartz crystal microbalance (EQCM), the intercalated species are transformed from [Zn(H₂O)₆]²⁺ to [Zn(H₂O)₂]²⁺ due to the built-in electric fields (BEFs) effects, further accelerating the ion transfer kinetics. Furthermore, owing to the absence of high-energy desolvation solvents released from desolvation processes, hydrogen evolution reaction (HER) energy barriers, Ti–Se bond strength, and structural stabilities are significantly improved, and the initial CE and HER overpotentials of the TiO₂/TiSe₂–C heterointerfaces increased from 13.76% to 84.7%, and from 1.04 to 1.30 V, respectively, and the H₂ precipitation current density even at −1.3 V decreased by 73.2%. This work provides valuable insights into the complex interface electrochemical mechanism of tailoring the solvation sheath and desolvation processes toward rocking-chair zinc-ion batteries.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.691","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}