Journal of Energy Chemistry最新文献

{"title":"Hydrogen spillover effect enhanced Cu2O/Cu/Mn2O3 catalyst for dual-electrode electrocatalytic hydrogen evolution","authors":"Wen-Kang Zhao ,&nbsp;Chang-Bao Han ,&nbsp;Zi-Qiang Ma ,&nbsp;Li-Hong Chang ,&nbsp;Jia-Yu Zheng ,&nbsp;Ming-Yang Hao ,&nbsp;De-Cai Fang ,&nbsp;Ya-Nuo Sun ,&nbsp;Shu-Feng Lin ,&nbsp;Hui Yan","doi":"10.1016/j.jechem.2025.02.026","DOIUrl":"10.1016/j.jechem.2025.02.026","url":null,"abstract":"<div><div>Replacing the oxygen evolution reaction (OER) with the anodic formaldehyde oxidation reaction (FOR) is crucial for achieving low-voltage dual-electrode hydrogen evolution. However, existing FOR catalysts face challenges such as low activity, high transition state barriers, and unclear reaction mechanisms. In this study, a three-dimensional nano-composite Cu₂O/Cu/Mn₂O₃ heterogeneous catalyst with enhanced hydrogen spillover effect was synthesized through hydrothermal and photosensitive oxidation treatment techniques. The catalyst consists of ∼20 nm Cu₂O/Cu and 30–70 nm Mn₂O₃ nanoparticles. The hydrogen spillover effect enhanced Cu₂O/Cu/Mn₂O₃ (1:1) electrocatalyst demonstrated outstanding FOR performance, with an anode potential of only 0.128 V at a current density of 100 mA cm⁻², significantly lower than that of the Cu₂O/Cu-CC catalyst (0.25 V) and the OER potential (1.726 V). Moreover, the Faraday efficiency of the Cu₂O/Cu/Mn₂O₃ (1:1) electrocatalyst reached ∼100%. The electrocatalyst’s FOR performance remains stable over 50 h without decay, and its hydrogen evolution reaction (HER) performance surpasses that of Cu and MnO<em>_x</em> electrocatalysts. Density functional theory (DFT) calculations suggested that the Cu₂O/Cu/Mn₂O₃ catalyst significantly lowers the energy barriers for C–H bond breaking (0.48 eV) and H–H bond formation (−0.99 eV) by promoting the hydrogen spillover effect. This study provides theoretical support for designing efficient and stable low-energy dual-electrode hydrogen evolution catalysts and validates their potential through experiments.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 291-301"},"PeriodicalIF":13.1,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143697201","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":"Overcoming low-temperature challenges in LIBs: the role of anion-rich solvation sheath in strong solvents","authors":"Xueqing Min,&nbsp;Li Wang,&nbsp;Yanzhou Wu,&nbsp;Zhiguo Zhang,&nbsp;Hong Xu,&nbsp;Xiangming He","doi":"10.1016/j.jechem.2025.02.027","DOIUrl":"10.1016/j.jechem.2025.02.027","url":null,"abstract":"<div><div>Lithium-ion batteries (LIBs) face significant limitations in low-temperature environments, with the slow interfacial de-solvation process and the hindered Li⁺ transport through the interphase layer emerging as key obstacles beyond the issue of ionic conductivity. This investigation unveils a novel formulation that constructs an anion-rich solvation sheath within strong solvents, effectively addressing all three of these challenges to bolster low-temperature performance. The developed electrolyte, characterized by an enhanced concentration of contact ion pairs (CIPs) and aggregates (AGGs), facilitates the formation of an inorganic-rich interphase layer on the anode and cathode particles. This promotes de-solvation at low temperatures and stabilizes the electrode–electrolyte interphase. Full cells composed of LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) and graphite, when equipped with this electrolyte, showcase remarkable cycle stability and capacity retention, with 93.3% retention after 500 cycles at room temperature (RT) and 95.5% after 120 cycles at −20 °C. This study validates the utility of the anion-rich solvation sheath in strong solvents as a strategy for the development of low-temperature electrolytes.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 63-70"},"PeriodicalIF":13.1,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680066","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":"Topology-based machine learning for predicting curvature effects in metal-nitrogen-carbon single-atom catalysts","authors":"Ge-Hao Liang ,&nbsp;Heng-Su Liu ,&nbsp;Xi-Ming Zhang ,&nbsp;Jian-Feng Li ,&nbsp;Shisheng Zheng","doi":"10.1016/j.jechem.2025.02.022","DOIUrl":"10.1016/j.jechem.2025.02.022","url":null,"abstract":"<div><div>Metal-nitrogen-carbon (M-N-C) single-atom catalysts are widely utilized in various energy-related catalytic processes, offering a highly efficient and cost-effective catalytic system with significant potential. Recently, curvature-induced strain has been extensively demonstrated as a powerful tool for modulating the catalytic performance of M-N-C catalysts. However, identifying optimal strain patterns using density functional theory (DFT) is computationally intractable due to the high-dimensional search space. Here, we developed a graph neural network (GNN) integrated with an advanced topological data analysis tool—persistent homology—to predict the adsorption energy response of adsorbate under proposed curvature patterns, using nitric oxide electroreduction (NORR) as an example. Our machine learning model achieves high accuracy in predicting the adsorption energy response to curvature, with a mean absolute error (MAE) of 0.126 eV. Furthermore, we elucidate general trends in curvature-modulated adsorption energies of intermediates across various metals and coordination environments. We recommend several promising catalysts for NORR that exhibit significant potential for performance optimization via curvature modulation. This methodology can be readily extended to describe other non-bonded interactions, such as lattice strain and surface stress, providing a versatile approach for advanced catalyst design.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"105 ","pages":"Pages 608-616"},"PeriodicalIF":13.1,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143628231","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":"In-situ formed LiAlO2 coating enabling the prelithiated SiOx@C anode with enhanced initial coulombic efficiency and electrochemistry-active solid-state interfaces","authors":"Xiang Li ,&nbsp;Li Wang ,&nbsp;Zhengguo Gu ,&nbsp;Xuanhao Wu ,&nbsp;Feiyue Tu ,&nbsp;Naiwen Liang ,&nbsp;Xiaofan Liu ,&nbsp;Wenqing Ma ,&nbsp;Zhongchang Wang ,&nbsp;Lezhi Yang ,&nbsp;Lishan Yang","doi":"10.1016/j.jechem.2025.02.023","DOIUrl":"10.1016/j.jechem.2025.02.023","url":null,"abstract":"<div><div>The prelithiated SiO<em>_x</em> anode showcases markedly improved Li-storage capabilities compared to its unlithiated counterparts, yet it faces hurdles such as slurry gassing, electrolyte deterioration, and capacity fade attributed to residual alkali and an unstable electrolyte/anode interface. To tackle these challenges, we propose a strategic utilization of residual alkali by creating an in-situ <em>γ</em>-LiAlO₂ functional layer on the prelithiated SiO<em>_x</em>@C anode material. This is accomplished by incorporating a minor amount of Al₂O₃ into the SiO<em>_x</em>@C/LiH precursor mixture before the solid-phase prelithiation process. The resulting modified prelithiated SiO<em>_x</em>@C anode with in-situ formed electrolyte-isolating <em>γ</em>-LiAlO₂ layer exhibits no discernible slurry gas generation within 7 days and substantially mitigates side reactions with the electrolyte, thereby boosting the initial coulombic efficiency and cycling stability of the SiO<em>_x</em>@C anode. In half-cell evaluations, the prelithiated SiO<em>_x</em>@C anode demonstrates a high Li-storage capacity of 1323 mAh g⁻¹ and an impressive initial coulombic efficiency of 91.09%. When assessed in a 3.2 Ah 18,650 cylindrical battery, the prelithiated SiO<em>_x</em>@C anode showcases exceptional cyclability, retaining 81% of its capacity after 1000 cycles, underscoring its potential for practical applications. This study introduces a scalable and cost-effective prelithiation technique that propels the development and practical deployment of Si-based anodes by resolving persistent scientific challenges with the use of inexpensive additives.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 173-184"},"PeriodicalIF":13.1,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680001","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":"Constructing P–O bridge at heterogeneous interface to enhance built-in electric field to facilitate the surface reconstruction of carbon coated OER catalyst","authors":"Zhicheng Xu,&nbsp;Mingfeng Zhong,&nbsp;Pingan Liu,&nbsp;Zhijie Zhang","doi":"10.1016/j.jechem.2025.02.024","DOIUrl":"10.1016/j.jechem.2025.02.024","url":null,"abstract":"<div><div>Constructing heterostructures and facilitating surface reconstruction are effective ways to obtain excellent catalysts for the oxygen evolution reaction (OER). Surface reconstruction is a dynamic process that is affected by the built-in electric field of the heterostructure. In this study, P/N co-doped carbon-coated Ni-Co/Ni-CoO heterostructure was prepared by in situ acid etching, aniline polymerization, and pyrolysis. This method can form a tightly connected heterogeneous interface. It was found that introducing P–O bonds in the carbon shell can increase its work function, thereby enhancing the built-in electric field between the carbon shell and the core catalyst. Detailed characterizations confirm that the P–O bridge at the heterogeneous interface can provide an electron flow highway from the core to the shell. The generated carbon defects generated by P leaching during surface reconstruction also have strong electron-absorbing capacity. These effects promote the conversion of Co²⁺ to Co³⁺, thereby providing more highly active sites. The resulting catalyst shows significantly enhanced activity and stability. This study demonstrates the promoting effect of the built-in electric field on the surface reconstruction of the catalyst and emphasizes the importance of the construction of tightly connected heterogeneous interface, which is instructive for the design of excellent OER catalysts.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 123-132"},"PeriodicalIF":13.1,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143679935","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":"Secondary growth of three-dimensional lead halide perovskite during the alkylammonium salts induced “in-situ healing” strategy","authors":"Jiao Ma,&nbsp;Xiaohan Yu,&nbsp;Yuhuan Xiao,&nbsp;De’en Guo,&nbsp;Mei Fang,&nbsp;Han Huang,&nbsp;Conghua Zhou","doi":"10.1016/j.jechem.2025.02.025","DOIUrl":"10.1016/j.jechem.2025.02.025","url":null,"abstract":"<div><div>Two-dimensional (2D) precursor molecules-based surface treatment on three-dimensional (3D) lead halide perovskite (PVSK) has achieved huge successes, the in-depth understanding of the modification mechanism remains an urgent need. Here the effect of alkyl-chain length on the reaction dynamics between alkylammonium salts (XI) and 3D PVSK matrix is studied, through examination of surface morphological and crystallographic properties of the 3D PVSK matrix. It is observed that the average crystallite size of 3D PVSK increases as XI is either spin-coated on 3D PVSK or penetrated through carbon-electrode (during the “in-situ healing” process). Secondary growth is observed for 3D PVSK, which is related to ion-exchanging reactions. Prolonging alkyl-chain length favors the secondary growth. Besides, the formation dynamics of 2D PVSK are studied. Adding alkyl-chain length increases the yields. The observations are thoroughly discussed with respect to the steric-hindrance effect held by alky-chains of XI molecule. The improved crystallization of 3D PVSK and increased yields of 2D PVSK help accelerate charge extraction and reduce recombination across the interface between PVSK and carbon-electrode (CE). Tuning alkyl-chain length of XI molecules, and the mass ratio between XI molecules and carbon black could mitigate the “in-situ healing” effect. Power conversion efficiency (<em>PCE</em>) of the carbon-electrode-based hole-conductor-free planar perovskite solar cells has been upgraded from 14% to 17%, and further upgraded to 20.4% by utilizing relatively thick CEs. Thanks to the hydrophobicity of long alkyl-chains owned by XI molecules, prolonged stability has been achieved on unsealed devices at the high-moisture environment (RH ≈ 85%), meanwhile, shelf-stability up to 6400 h has been achieved. This study deepens the understanding of the 2D precursor-basing modification strategies.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 71-80"},"PeriodicalIF":13.1,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143680008","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":"Reduced humidity sensitivity of the perovskite fabrication via intermediate treatment enabling stable perovskite solar cells","authors":"Hongyu Xu ,&nbsp;Qixuan Zhong ,&nbsp;Yongqiang Ji ,&nbsp;Qiuyang Li ,&nbsp;Haoming Yan ,&nbsp;Yu Chen ,&nbsp;Rui Zhu ,&nbsp;Lichen Zhao","doi":"10.1016/j.jechem.2025.02.014","DOIUrl":"10.1016/j.jechem.2025.02.014","url":null,"abstract":"<div><div>High-efficiency formamidinium lead iodide (FAPbI₃)-based perovskite solar cells (PSCs) typically involve annealing in humid air during the fabrication process of perovskite films. However, the combined effects of humidity and relatively high temperature often result in the uncontrollable formation of a detrimental PbI₂ phase in the perovskite films. As a result, the annealing process of perovskite films is highly sensitive to the relative humidity fluctuations of the environment. Under solar illumination, the undesired PbI₂ tends to decompose, accelerating the degradation of perovskite materials and severely compromising the light stability of PSCs. This issue is particularly critical for the buried interface and bulk of the perovskite films, as these regions absorb the majority of the incident light. Pre-treatment and post-treatment strategies are generally confined to address the PbI₂ issues at the buried interface and on the surface of the perovskite films, respectively. However, effectively addressing the effects of excess PbI₂ at buried interface and grain boundaries within bulk in a single step remains challenging. In this study, we propose an intermediate-treatment strategy using phthalylglycyl chloride (PTC), which involves treating the wet films with PTC prior to annealing during the formation process of the perovskite films. This approach protects the grain boundaries of polycrystalline perovskite films in advance, effectively preventing moisture-induced degradation of the perovskites and thus significantly broadening the relative humidity window of annealing process. Our results demonstrate that this strategy can successfully suppress the formation of PbI₂ at the grain boundaries and buried interface of perovskite films, thereby eliminating the PbI₂-induced degradation pathways. Our strategy significantly reduces the sensitivity to humidity fluctuations during annealing for fabricating stable PSCs, ensuring more consistent fabrication of stable PSCs. Consequently, the resulting PSCs achieve a champion power conversion efficiency of 26.1% and demonstrate excellent light stability.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 133-141"},"PeriodicalIF":13.1,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143679936","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 hybrid platinum-based electrocatalyst: leveraging multi-site synergy and tailored electrochemical microenvironment for efficient oxygen reduction reaction","authors":"Haibin Wang ,&nbsp;Yuanyuan Cong ,&nbsp;Yi Wang ,&nbsp;Chunlei Li ,&nbsp;Mengling Liu ,&nbsp;Qiuping Zhao ,&nbsp;Xueliang Wang ,&nbsp;Junying Tian","doi":"10.1016/j.jechem.2025.02.018","DOIUrl":"10.1016/j.jechem.2025.02.018","url":null,"abstract":"<div><div>Platinum (Pt)-based single atoms and alloys represent reasonable structures to reduce the cost of electrocatalysts for the oxygen reduction reaction (ORR). However, the poor oxygen adsorption of single Pt atoms and the unfavorable surface microenvironment of alloy electrodes limit their practical applications. To address these issues, we have engineered a synergistic hybrid structure by anchoring PtNi alloys onto defective carbon (DC) modified with Pt and Ni single atoms, followed by surface modification with 2,6-diacetylpyridine (DAP) molecules. The mass activity (MA) of the optimized DAP-PtNi/Pt&amp;Ni-SAC electrocatalyst reaches 1678.9 mA mg_Pt⁻¹, which is 10.21 times that of commercial JM Pt/C (164.5 mA mg_Pt⁻¹). Moreover, after 20,000 accelerated durability tests (ADTs), DAP-PtNi/Pt&amp;Ni-SAC shows only a 7.9% loss in MA, demonstrating its outstanding stability. Structural characterization and theoretical calculations reveal that the interaction of Ni single atoms and PtNi alloys enhances the adsorption stability of O₂ molecules at Pt single atoms, facilitating a 4-electron ORR pathway. Meanwhile, DAP molecules adsorbed on Pt alloy sites associate with various oxygen-containing intermediates and protons through electrostatic interactions, promoting their combination. This synergistic effect between the intrinsic structure and the electrochemical microenvironment optimizes the ORR pathway in an overall manner, thus improving the kinetics of ORR.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"105 ","pages":"Pages 560-569"},"PeriodicalIF":13.1,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629341","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":"Safety assessment of overcharged batteries and a novel passive warning method based on relaxation expansion force","authors":"Long Chen ,&nbsp;Shaohong Zeng ,&nbsp;Jiahua Li ,&nbsp;Kuijie Li ,&nbsp;Ruixin Ma ,&nbsp;Jizhen Liu ,&nbsp;Weixiong Wu","doi":"10.1016/j.jechem.2025.02.016","DOIUrl":"10.1016/j.jechem.2025.02.016","url":null,"abstract":"<div><div>Due to batteries inconsistencies and potential faults in battery management systems, slight overcharging remains a common yet insufficiently understood safety risk, lacking effective warning methods. To illuminate the degradation behavior and failure mechanism of various overcharged states (100% SOC, 105% SOC, 110% SOC, and 115% SOC), multiple advanced in-situ characterization techniques (accelerating rate calorimeter, electrochemical impedance spectroscopy, ultrasonic scanning, and expansion instrument) were utilized. Additionally, re-overcharge-induced thermal runaway (TR) tests were conducted, with a specific emphasis on the evolution of the expansion force signal. Results indicated significant degradation at 110% SOC, including conductivity loss, loss of lithium inventory, and loss of active material accompanied by internal gas generation. These failure behaviors slow down the expansion force rate during re-overcharging, reducing the efficacy of active warnings that depend on rate thresholds of expansion force. Specifically, the warning time for 115% SOC battery is only 144 s, which is 740 s shorter than that for fresh battery, and the time to TR is advanced by 9 min. Moreover, the initial self-heating temperature (<em>T</em>₁) is reduced by 62.4 °C compared to that of fresh battery, reaching only 70.8 °C. To address the low safety of overcharged batteries, a passive overcharge warning method utilizing relaxation expansion force was proposed, based on the continued gas generation after stopping charging, leading to a sustained increase in force. Compared to active methods that rely on thresholds of expansion force rate, the passive method can issue warnings 115 s earlier. By combining the passive and active warning methods, guaranteed effective overcharge warning can be issued 863–884 s before TR. This study introduces a novel perspective for enhancing the safety of batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"105 ","pages":"Pages 595-607"},"PeriodicalIF":13.1,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143628122","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":"Root-inspired self-healing binder enabling robust micron-sized SiO electrodes with durable lithium storage stability","authors":"Weihua Wang ,&nbsp;Sha Li ,&nbsp;Wenyi Li ,&nbsp;Siyi Jing ,&nbsp;Yudai Huang ,&nbsp;Huiqun Wang ,&nbsp;Huiping Yang ,&nbsp;Xuan Wang ,&nbsp;Ling Huang ,&nbsp;Yuxiang Mao ,&nbsp;Shiyu Luo ,&nbsp;Li Zhang","doi":"10.1016/j.jechem.2025.02.019","DOIUrl":"10.1016/j.jechem.2025.02.019","url":null,"abstract":"<div><div>Silicon monoxide (SiO) is highly attractive as an anode material for high-energy lithium-ion batteries (LIBs) due to its significantly higher specific capacity. However, its practical application is hindered by substantial volume expansion during cycling, which leads to material pulverization and an unstable solid electrolyte interphase (SEI) layer. Inspired by the natural root fixation in soil, we designed a root-like topological structure binder, cassava starch-citric acid (CS-CA), based on the synergistic action of covalent and hydrogen bonds. The abundant –OH and –COOH groups in CS-CA molecules effectively form hydrogen bonds with the –OH groups on the SiO surface, significantly enhancing the interfacial interaction between CS-CA and SiO. The root-like topological structure of CS-CA with a high tolerance alleviates the mechanical stress generated by the volume changes of SiO. More encouragingly, the hydrogen bond action among CS-CA molecules produces a self-healing effect, which is advantageous for repairing damaged electrodes and preserving their structural integrity. As such, the CS-CA/SiO electrode exhibits exceptional cycling performance (963.1 mA h g⁻¹ after 400 cycles at 2 A g⁻¹) and rate capability (558.9 mA h g⁻¹ at 5 A g⁻¹). This innovative, topologically interconnected, root-inspired binder will greatly advance the practical application of long-lasting micron-sized SiO anodes.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 151-160"},"PeriodicalIF":13.1,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143679938","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}