Journal of Energy Chemistry最新文献

{"title":"Research progress of polarized perovskite type ferroelectric materials for photocatalytic hydrogen production","authors":"Rong Yan ,&nbsp;Chunyan Du ,&nbsp;Hanbo Yu ,&nbsp;Jingyi Jiang ,&nbsp;Jiao Cao ,&nbsp;Guanlong Yu ,&nbsp;Wei Dong ,&nbsp;Yulv Zou ,&nbsp;Huaiyuan Peng ,&nbsp;Yu Yang ,&nbsp;Tian Ao ,&nbsp;Tong Sun ,&nbsp;Yiyi Deng","doi":"10.1016/j.jechem.2025.03.051","DOIUrl":"10.1016/j.jechem.2025.03.051","url":null,"abstract":"<div><div>To address the global energy shortage, hydrogen production as a green energy source has become one of the most prominent research topics over the past decade. Novel and promising ferroelectric materials, exhibiting unique spontaneous polarization capabilities, have shown great potential in the field of photocatalytic hydrogen evolution. Among these materials, perovskites represent a significant group of ferroelectrics, possessing both excellent ferroelectric properties and photocatalytic performance. By focusing on perovskites, we analyze the advantages of their built-in electric field for photocatalytic hydrogen evolution, integrating the domain wall structures of ferroelectrics. Furthermore, we summarize how to fully exploit the unique characteristics of ferroelectrics and highlight recent advancements in their application to photocatalytic hydrogen evolution.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 87-102"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838169","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":"Crosslinked ionogels containing a Li-conducting inorganic phase as electrolyte for lithium-metal batteries","authors":"Matteo Gandolfo ,&nbsp;Mattia Longo ,&nbsp;Thomas Diemant ,&nbsp;Silvia Bodoardo ,&nbsp;Dominic Bresser ,&nbsp;Julia Amici","doi":"10.1016/j.jechem.2025.03.056","DOIUrl":"10.1016/j.jechem.2025.03.056","url":null,"abstract":"<div><div>In the quest for the development of safer lithium-metal batteries (LMBs), the integration of inorganic fillers and ionic liquids into polymer matrices has emerged as a promising strategy to enhance safety, ionic conductivity and battery performance. This study introduces a novel composite ionogel (IG) synthesized through a facile one-pot method, incorporating butyl methacrylate (BMA) and poly(ethylene glycol) diacrylate (PEGDA) with the ionic liquid 1-butyl-1-methylpyrrolidinium bis(fluorosulfonyl)imide (PYR₁₄FSI) and garnet Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) nanoparticles. A distinctive feature of the approach is the use of an organosilane functionalization of the LLZTO nanoparticles, which ensures their full integration into the polymer matrix during free-radical polymerization. Moreover, this method effectively eliminates the Li₂CO₃ passivation layer that typically forms on the surface of the LLZTO nanoparticles, thus, further contributing to an enhanced performance. As a result, a LMB with the functionalized LLZTO IG electrolyte delivered more than 160 mA h g⁻¹ with a very good capacity retention of 97.7% after 400 cycles in Li|IG|LFP cells.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 221-232"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143843651","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":"Screening dual variable-valence metal oxides doped calcium-based material for calcium looping thermochemical energy storage and CO2 capture with DFT calculation","authors":"Youhao Zhang ,&nbsp;Yi Fang ,&nbsp;Zhiwei Chu ,&nbsp;Zirui He ,&nbsp;Jianli Zhao ,&nbsp;Kuihua Han ,&nbsp;Yingjie Li","doi":"10.1016/j.jechem.2025.03.052","DOIUrl":"10.1016/j.jechem.2025.03.052","url":null,"abstract":"<div><div>The reaction characteristics of calcium-based materials during calcium looping (CaL) process are pivotal in the efficiency of CaL thermochemical energy storage (TCES) and CO₂ capture systems. Currently, metal oxide doping is the primary method to enhance the reaction characteristics of calcium-based materials over multiple cycles. In particular, co-doping with variable-valence metal oxides (VVMOs) can effectively increase the oxygen vacancy content in calcium-based materials, significantly improving their cyclic reaction characteristics. However, there are so numerous VVMOs co-doping schemes that the experimental screening process is complex, consuming considerable time and economic costs. Density functional theory (DFT) calculations have been widely used to reveal the impact of metal oxide doping on the cyclic reaction characteristics of calcium-based materials, with calculation results showing good agreement with experimental conclusions. Nevertheless, there is still a lack of research on utilizing DFT to screen calcium-based materials, and a systematic research methodology has not yet been established. In this study, a systematic DFT-based screening methodology for calcium-based materials was proposed. A series of key parameters for DFT calculations including CO₂ adsorption energy, oxygen vacancy formation energy, and sintering resistance were proposed. Furthermore, a preliminary mathematical model to predict the CaL TCES and CO₂ capture performance of calcium-based materials was introduced. The aforementioned DFT method was employed to screen for VVMOs co-doped calcium-based materials. The results revealed that Mn and Ce co-doped calcium-based materials exhibited superior DFT-predicted reaction characteristics. These DFT predictions were validated through experimental assessments of cyclic thermochemical energy storage, CO₂ capture, and relevant characterization. The outcomes demonstrate a high degree of consistency among DFT-based predictions, experimental results, and characterization. Hence, the DFT-based screening methodology for calcium-based materials proposed herein is a viable solution, poised to offer theoretical insights for the efficient design of calcium-based materials.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 170-182"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838174","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":"Innovations in catalysis towards efficient electrochemical reduction of CO2 to C1 chemicals","authors":"Sheraz Ahmed ,&nbsp;Muhammad Shakir Hussain ,&nbsp;Muhammad Kashif Khan ,&nbsp;Jaehoon Kim","doi":"10.1016/j.jechem.2025.03.055","DOIUrl":"10.1016/j.jechem.2025.03.055","url":null,"abstract":"<div><div>The electrochemical CO₂ reduction reaction (CO₂RR) is considered a promising technology for converting atmospheric CO₂ into valuable chemicals. It is a significant way to mitigate the shortage of fossil energy and store excessive renewable electricity in fuels to maintain carbon neutrality. Considering the substantially reduced cost of clean electricity, C₁ molecule unitization has emerged as a competitive strategy for room-temperature electrolysis. However, the practical implementation of CO₂RR has been hindered by low desired product selectivity, high overpotential, and undesirable hydrogen evolution reactions (HER). Consequently, it is imperative to execute a timely assessment of advanced strategies in CO₂RR, with emphasis on catalytic design strategies, understanding of structure–activity relationships, and deactivation of catalysts. In this context, it is imperative to investigate the intrinsic active sites and reaction mechanisms. This review focuses on the design of novel catalysts and their active sites via operando techniques. The combination of advanced characterization techniques and theoretical calculations provides a high-throughput way to obtain a deeper understanding of the reaction mechanism. Furthermore, optimization of the interplay between the catalyst surface and reaction intermediate disturbs the linear correlation between the adsorption energies of the intermediates, resulting in a convoluted cascade system. The appropriate strategies for CO₂RR, challenges, and future approaches are projected in this review to stimulate major innovations. Moreover, the plausible research directions are discussed for producing C₁ chemicals via electrochemical CO₂RR at room temperature.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 622-649"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870412","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":"Entropy tuning and artificial CEI synergistically enhance the stability and kinetics of P2-type layered oxide cathode for high-voltage sodium-ion batteries","authors":"Yingxinjie Wang ,&nbsp;Ziying Zhang ,&nbsp;Kejian Tang ,&nbsp;Yongchun Li ,&nbsp;Guohao Li ,&nbsp;Jie Wang ,&nbsp;Zhenjun Wu ,&nbsp;Nan Zhang ,&nbsp;Xiuqiang Xie","doi":"10.1016/j.jechem.2025.03.054","DOIUrl":"10.1016/j.jechem.2025.03.054","url":null,"abstract":"<div><div>P2-type layered oxide Na_2/3Ni_1/3Mn_2/3O₂ (NM) is a promising cathode material for sodium-ion batteries (SIBs). However, the severe irreversible phase transition, sluggish Na⁺ diffusion kinetics, and interfacial side reactions at high-voltage result in grievous capacity degradation and inferior electrochemical performance. Herein, a dual-function strategy of entropy tuning and artificial cathode electrolyte interface (CEI) layer construction is reported to generate a novel P2-type medium-entropy Na_0.75Li_0.1Mg_0.05Ni_0.18Mn_0.66Ta_0.01O₂ with NaTaO₃ surface modification (LMNMT) to address the aforementioned issues. In situ X-ray diffraction reveals that LMNMT exhibits a near zero-strain phase transition with a volume change of only 1.4%, which is significantly lower than that of NM (20.9%), indicating that entropy tuning effectively suppresses irreversible phase transitions and enhances ion diffusion. Kinetic analysis and post-cycling interfacial characterization further confirm that the artificial CEI layer promotes the formation of a stable, thin NaF-rich CEI and reduces interfacial side reactions, thereby further enhancing ion transport kinetics and surface/interface stability. Consequently, the LMNMT electrode exhibits outstanding rate capability (46 mA h g⁻¹ at 20 C) and cycling stability (89.5% capacity retention after 200 cycles at 2 C) within the voltage range of 2–4.35 V. The LMNMT also exhibits superior all-climate performance and air stability. This study provides a novel path for the design of high-voltage cathode materials for SIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 241-251"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143843572","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":"Abundant adsorption and catalytic sites of the CoS2/MoS2 heterostructure for enhanced reversible kinetics in polysulfide conversion","authors":"Qian He ,&nbsp;Weikun Chen ,&nbsp;Bin Fan ,&nbsp;Qingya Wei ,&nbsp;Yingping Zou","doi":"10.1016/j.jechem.2025.03.050","DOIUrl":"10.1016/j.jechem.2025.03.050","url":null,"abstract":"<div><div>The practical application of lithium-sulfur (Li-S) batteries is hindered by the sluggish redox kinetics of sulfur, significant volume expansion, and the shuttle effect of lithium polysulfides (LiPSs). To address these challenges, this study utilizes hollow carbon spheres (HCS) as a matrix, incorporating a heterojunction of transition metal sulfides (CoS₂/MoS₂) as the sulfur host. The HCS, with their ultrahigh specific surface area, effectively mitigate structural damage to the cathode caused by sulfur’s volume expansion during charge and discharge cycles. Meanwhile, the CoS₂/MoS₂ heterojunction provides abundant chemical adsorption and reaction sites, which accelerate the redox kinetics of sulfur and alleviating the shuttle effect of LiPSs. Density functional theory (DFT) calculations reveal that the coupling effect at the CoS₂/MoS₂ heterointerface significantly enhances charge transfer and adsorption interactions between CoS₂/MoS₂ and LiPSs. Experimental results demonstrate that Li-S batteries with S/CoS₂/MoS₂@HCS composites as the cathode exhibit an exceptionally low capacity decay rate of only 0.023% per cycle after 1200 cycles at 2.0 C. Even with high sulfur loading (7.9 mg cm⁻²) and a low electrolyte-to-sulfur (E/S) ratio (6.0 μL mg⁻¹), the battery achieves an outstanding areal capacity of 6.86 mA h cm⁻². This study develops a highly efficient CoS₂/MoS₂ heterojunction within HCS for the adsorption and conversion of LiPSs, providing valuable insights into the design of high-performance cathode materials for Li-S batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 570-581"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143865206","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":"Electronic modulation of amorphous/crystalline NiFe LDH by atomic Pt loading enabling industrial hydrogen production in alkaline water and seawater","authors":"Boxue Wang ,&nbsp;Zhongge Luo ,&nbsp;Huachuan Sun ,&nbsp;Mingpeng Chen ,&nbsp;Yumin Zhang ,&nbsp;Xinru Zhao ,&nbsp;Guoyang Qiu ,&nbsp;Bin Xiao ,&nbsp;Tong Zhou ,&nbsp;Qinjie Lu ,&nbsp;Dequan Li ,&nbsp;Yuewen Wu ,&nbsp;Yuxiao Zhang ,&nbsp;Jianhong Zhao ,&nbsp;Jin Zhang ,&nbsp;Hao Cui ,&nbsp;Feng Liu ,&nbsp;Tianwei He ,&nbsp;Qingju Liu","doi":"10.1016/j.jechem.2025.03.053","DOIUrl":"10.1016/j.jechem.2025.03.053","url":null,"abstract":"<div><div>The reasonable development and design of high-efficiency and low-cost electrocatalysts for hydrogen evolution reaction (HER) under industrial current densities are imperative for achieving carbon neutrality, while also posing challenges. In this study, an efficient electrocatalyst is successfully constructed through electrodeposition methods, which consists of monodispersed Pt loaded on amorphous/crystalline nickel–iron layered double hydroxide (Pt-SAs/ac-NiFe LDH). The Pt-SAs/ac-NiFe LDH demonstrates an elevated mass activity of 17.66 A mg_Pt⁻¹ and a significant turnover frequency of 17.90 s⁻¹ for HER in alkaline conditions under the overpotential of 100 mV. Meanwhile, for alkaline freshwater and seawater, Pt-SAs/ac-NiFe LDH exhibits ultra-low overpotentials of 141 and 138 mV to reach 1000 mA cm⁻², respectively. Remarkably, it maintains stable operation for 100 h at 500 mA cm⁻², showcasing its robustness and reliability. <em>In situ</em> Raman spectra reveal that Pt single atoms (Pt-SAs) accelerate interfacial water dissociation, thereby enhancing the HER kinetics in Pt-SAs/ac-NiFe LDH. Furthermore, theoretical calculation results show significant electronic interaction between the Pt-SAs and the ac-NiFe LDH support. The interaction significantly enhances water adsorption and dissociation, and balances the adsorption/desorption of hydrogen intermediates, ultimately improving HER performance. This research provides a viable method for designing efficient HER catalysts for water electrolysis in alkaline freshwater and seawater under industrial current densities.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 427-439"},"PeriodicalIF":13.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864921","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":"Developing inorganic-rich interphases through single-solvent siloxane electrolytes with weak solvation characteristics for high-voltage Ni-rich batteries","authors":"Yuanqin Li ,&nbsp;Lijiao Quan ,&nbsp;Jiarong He ,&nbsp;Lidan Xing ,&nbsp;Weishan Li","doi":"10.1016/j.jechem.2025.03.044","DOIUrl":"10.1016/j.jechem.2025.03.044","url":null,"abstract":"<div><div>Enhancing the energy density of lithium-ion batteries through high-voltage cathodes holds great promise. However, traditional carbonate-based electrolytes face significant challenges due to limited oxidative stability and poor compatibility with high-nickel materials. This study introduces a novel electrolyte that combines bis(triethoxysilyl) methane (DMSP) as the sole solvent with lithium bis(fluorosulfonyl) imide (LiFSI) as the lithium salt. This formulation significantly improves the stability of LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathodes and graphite anodes. The capacity retention of the NCM811 electrode increases from 5% to 95% after 1000 cycles at 1 C (3.0–4.5 V), while that of the graphite anode is improved from 22% to 92% after 400 cycles at 0.2 C (0.005–3.0 V). The NCM811//graphite pouch cell exhibits enhanced retention, rising from 12% to 66% at 25 °C and from 3% to 65% at 60 °C after 300 cycles at 0.2 C. Spectroscopic characterization and theoretical calculations reveal that the steric hindrance of the Si–O–CH₃ groups in DMSP creates a weakly solvating structure, promoting the formation of Li⁺-FSI⁻ ion pairs and aggregation clusters, which enriches the electrode interphase with LiF, Li₃N, and Li₂SO₃. Furthermore, DMSP with abundant Si–O effectively enhances the elasticity of the interphase layer, scavenging harmful substances such as HF and suppressing gas evolution and transition metal dissolution. The simplicity of the DMSP-based electrolyte formulation, coupled with its superior performance, ensures scalability for large-scale manufacturing and practical application in the high-voltage battery. This work provides critical insights into improving interfacial chemistry and addressing compatibility issues in high-voltage Ni-rich cathodes.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 18-30"},"PeriodicalIF":13.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143834572","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":"Amorphous fluorinated interphase enables fast Li-ion kinetics in sulfide-based all-solid-state lithium metal batteries","authors":"Ao-Long Yue ,&nbsp;Hong Yuan ,&nbsp;Shi-Jie Yang ,&nbsp;Jiang-Kui Hu ,&nbsp;Xi-Long Wang ,&nbsp;Di-Chen Wu ,&nbsp;Zi-Hao Zuo ,&nbsp;Bo-Dong Bi ,&nbsp;Zhong-Heng Fu ,&nbsp;Jia-Qi Huang","doi":"10.1016/j.jechem.2025.03.048","DOIUrl":"10.1016/j.jechem.2025.03.048","url":null,"abstract":"<div><div>Sulfide-based all-solid-state lithium metal batteries (ASSLMBs) have garnered significant attention due to their potential for high energy density and enhanced safety. However, their practical application is hindered by challenges such as uneven lithium (Li) deposition and the growth of Li dendrites. In this contribution, we propose an amorphous fluorinated interphase (AFI), composed of amorphous LiF and lithiated graphite, to regulate the interfacial Li-ion transport kinetics through in-situ interface chemistry. Amorphous LiF, which exhibits a significantly enhanced Li-ion diffusion compared to its crystalline counterpart, works synergistically with lithiated graphite to promote both short-range and long-range Li-ion transport kinetics at the Li/electrolyte interface. As a result, the Li anode with AFI demonstrates a remarkably enhanced critical current density of 1.6 mA cm⁻² and an extended cycle life exceeding 1100 h. The Li||LiNi_0.6Co_0.2Mn_0.2O₂ full cell also achieves a high discharge capacity of 125.7 mA h g⁻¹ and retains 71.2% of its initial capacity after 200 cycles. This work provides valuable insights into the rational design of artificial anodic interphase to regulate interfacial Li-ion transport kinetics in ASSLMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 277-284"},"PeriodicalIF":13.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143847372","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":"High-performance water-in-salt electrolyte-enabled zinc-graphite batteries with bromine dual electrochemical processes","authors":"Sirugaloor Thangavel Senthilkumar ,&nbsp;Maryam Mouselly ,&nbsp;Javad B.M. Parambath ,&nbsp;Anis Allagui ,&nbsp;Hussain Alawadhi","doi":"10.1016/j.jechem.2025.03.047","DOIUrl":"10.1016/j.jechem.2025.03.047","url":null,"abstract":"<div><div>As an alternative to lithium-ion batteries, aqueous zinc-graphite batteries (ZnGBs) are being explored as safer and low-cost options with the expectation of scalability to large energy storage systems. However, the currently adopted polyatomic and metal complex anion intercalation process at the graphite electrode in ZnGB exhibits poor electrochemical performances. Alternatively, incorporating halogen anions offers exceptional electrochemical performance to graphite electrodes due to their redox process. In this work, ZnGBs are assembled using a LiCl/ZnCl₂/KBr-based water-in-salt electrolyte, which efficiently supplies bromide (Br⁻) ions for conversion into Br<em>_x</em>⁻ and facilitates Br₂ intercalation at the graphite electrode. The conversion and intercalation of bromine together enable the ZnGB to achieve a discharge capacity of 2.73 mAh/cm² with 91.0% of coulombic efficiency (CE) while supporting high current density operations of up to 150 mA/cm². With high energy density (4.56 Wh/cm²), high power density (199.5 mW/cm²), and excellent rate capability (∼93.0% CE at 150 mA/cm²), the ZnGB is shown to operate efficiently for as much as 800 cycles. Beguilingly, an anode-free ZnGB offers enhanced stability for up to 1100 cycles without performance decay, matching the electrochemical performance of Zn metal electrodes. This work provides insights into the bromine reaction mechanism at graphite electrodes and the role of surface exfoliation in enabling efficient Br<em>_x</em>⁻ formation, along with Br₂ intercalation, for achieving high-performance ZnGBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 345-356"},"PeriodicalIF":13.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858834","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}