Mo-based palmeirite oxide A2Mo3O8 is an emerging electrocatalyst, exhibiting a bipartite honeycomb lattice consisting of tetrahedral and octahedral sites with good conductivity. However, palmeirite as promising catalyst in electrocatalytic remains rarely touched. The rational design and clarification of the correlation between geometrical configuration modulation and electrocatalytic properties are challenging. Herein, an innovative strategy is reported to anchor thiospinel Co3S4 nanoparticles onto the surface of the Co2Mo3O8 nanosheet, which can trigger the spin electrons rearrangement, thus activating inert sites. According to the X-ray absorption spectroscopy, the Co2+─O─Co3+ bimetallic bridging sites with asymmetric bond polarization are constructed in the interface, which triggers a favorable spin transition of Co3+ from low to intermediate spin. Interestingly, the Co2Mo3O8/Co3S4 exhibits remarkable oxygen evolution reaction performance with an overpotential of 227 mV at 10 mA cm−2. At an industrial process temperature, it takes only 2.37 V for overall water splitting to obtain a large current density of 1 A cm−2. The theoretical calculation results confirm that lattice distortion-related spin transition optimizes the intermediate energy, thus enhancing the adsorption of the *OOH. This work highlights the potential of palmeirite for achieving industrial overall seawater splitting by geometrical configuration modulation and spin electrons rearrangement.
{"title":"Activating Inert Palmeirite Through Co Local-Environment Modulation and Spin Electrons Rearrangement for Superior Oxygen Evolution","authors":"Jia-xin Wen, Yi-ru Hao, Jiawen Sun, Yaqin Chen, Chunhao Li, Hui Xue, Jing Sun, Jianan Zhang, Qin Wang, Limin Wu","doi":"10.1002/aenm.202405555","DOIUrl":"https://doi.org/10.1002/aenm.202405555","url":null,"abstract":"Mo-based palmeirite oxide A<sub>2</sub>Mo<sub>3</sub>O<sub>8</sub> is an emerging electrocatalyst, exhibiting a bipartite honeycomb lattice consisting of tetrahedral and octahedral sites with good conductivity. However, palmeirite as promising catalyst in electrocatalytic remains rarely touched. The rational design and clarification of the correlation between geometrical configuration modulation and electrocatalytic properties are challenging. Herein, an innovative strategy is reported to anchor thiospinel Co<sub>3</sub>S<sub>4</sub> nanoparticles onto the surface of the Co<sub>2</sub>Mo<sub>3</sub>O<sub>8</sub> nanosheet, which can trigger the spin electrons rearrangement, thus activating inert sites. According to the X-ray absorption spectroscopy, the Co<sup>2+</sup>─O─Co<sup>3+</sup> bimetallic bridging sites with asymmetric bond polarization are constructed in the interface, which triggers a favorable spin transition of Co<sup>3+</sup> from low to intermediate spin. Interestingly, the Co<sub>2</sub>Mo<sub>3</sub>O<sub>8</sub>/Co<sub>3</sub>S<sub>4</sub> exhibits remarkable oxygen evolution reaction performance with an overpotential of 227 mV at 10 mA cm<sup>−2</sup>. At an industrial process temperature, it takes only 2.37 V for overall water splitting to obtain a large current density of 1 A cm<sup>−2</sup>. The theoretical calculation results confirm that lattice distortion-related spin transition optimizes the intermediate energy, thus enhancing the adsorption of the <sup>*</sup>OOH. This work highlights the potential of palmeirite for achieving industrial overall seawater splitting by geometrical configuration modulation and spin electrons rearrangement.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"194 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546010","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aqueous zinc-based batteries (AZBs) are emerging as a compelling candidate for large-scale energy storage systems due to their cost-effectiveness, environmental friendliness, and inherent safety. The design and development of high-performance AZBs have thus been the focus of considerable study efforts; yet, certain properties of electrode materials and electrolytes still limit their development. Here, a comprehensive overview and evaluation of the current progress, existing limitations, and potential solutions for electrode materials to achieve long-cycle stability and fast kinetics in AZBs is provided. Detailed analyses of the structural design, electrochemical behavior, and zinc-ion storage mechanisms of various materials are presented. Additionally, key issues and research directions related to the design of zinc anodes and the selection of electrolytes are systematically discussed to guide the future design of AZBs with superior electrochemical performance. Finally, this review provides a comprehensive outlook on the future development of AZBs, highlighting key challenges and opportunities, to foster their continued rapid advancement and broader practical applications in the field.
{"title":"Aqueous Zinc-Based Batteries: Active Materials, Device Design, and Future Perspectives","authors":"Yan Ran, Fang Dong, Shuhui Sun, Yong Lei","doi":"10.1002/aenm.202406139","DOIUrl":"https://doi.org/10.1002/aenm.202406139","url":null,"abstract":"Aqueous zinc-based batteries (AZBs) are emerging as a compelling candidate for large-scale energy storage systems due to their cost-effectiveness, environmental friendliness, and inherent safety. The design and development of high-performance AZBs have thus been the focus of considerable study efforts; yet, certain properties of electrode materials and electrolytes still limit their development. Here, a comprehensive overview and evaluation of the current progress, existing limitations, and potential solutions for electrode materials to achieve long-cycle stability and fast kinetics in AZBs is provided. Detailed analyses of the structural design, electrochemical behavior, and zinc-ion storage mechanisms of various materials are presented. Additionally, key issues and research directions related to the design of zinc anodes and the selection of electrolytes are systematically discussed to guide the future design of AZBs with superior electrochemical performance. Finally, this review provides a comprehensive outlook on the future development of AZBs, highlighting key challenges and opportunities, to foster their continued rapid advancement and broader practical applications in the field.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"41 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chen Wang, Roderick C. I. MacKenzie, Uli Würfel, Dieter Neher, Thomas Kirchartz, Carsten Deibel, Maria Saladina
Organic photovoltaics (OPV) are a promising solar cell technology well-suited to mass production using roll-to-roll processes. The efficiency of lab-scale solar cells has exceeded 20% and considerable attention is currently being given to understanding and minimizing the remaining loss mechanisms preventing higher efficiencies. While recent efficiency improvements are partly owed to reducing non-radiative recombination losses at open circuit, the low fill factor (FF) due to a significant transport resistance is becoming the Achilles heel of OPV. The term transport resistance refers to a voltage and light intensity-dependent charge collection loss in low-mobility materials. In this perspective, it is demonstrated that even the highest efficiency organic solar cells (OSCs) reported to-date have significant performance losses that can be attributed to transport resistance and that lead to high FF losses. A closer look at the transport resistance and the material properties influencing it is provided. How to experimentally characterize and quantify the transport resistance is described by providing easy to follow instructions. Furthermore, the causes and theory behind transport resistance are detailed. In particular, the relevant figures of merit (FoMs) and different viewpoints on the transport resistance are integrated. Finally, we outline strategies that can be followed to minimize these charge collection losses in future solar cells.
{"title":"Transport Resistance Dominates the Fill Factor Losses in Record Organic Solar Cells","authors":"Chen Wang, Roderick C. I. MacKenzie, Uli Würfel, Dieter Neher, Thomas Kirchartz, Carsten Deibel, Maria Saladina","doi":"10.1002/aenm.202405889","DOIUrl":"https://doi.org/10.1002/aenm.202405889","url":null,"abstract":"Organic photovoltaics (OPV) are a promising solar cell technology well-suited to mass production using roll-to-roll processes. The efficiency of lab-scale solar cells has exceeded 20% and considerable attention is currently being given to understanding and minimizing the remaining loss mechanisms preventing higher efficiencies. While recent efficiency improvements are partly owed to reducing non-radiative recombination losses at open circuit, the low fill factor (<i>FF</i>) due to a significant transport resistance is becoming the Achilles heel of OPV. The term transport resistance refers to a voltage and light intensity-dependent charge collection loss in low-mobility materials. In this perspective, it is demonstrated that even the highest efficiency organic solar cells (OSCs) reported to-date have significant performance losses that can be attributed to transport resistance and that lead to high <i>FF</i> losses. A closer look at the transport resistance and the material properties influencing it is provided. How to experimentally characterize and quantify the transport resistance is described by providing easy to follow instructions. Furthermore, the causes and theory behind transport resistance are detailed. In particular, the relevant figures of merit (FoMs) and different viewpoints on the transport resistance are integrated. Finally, we outline strategies that can be followed to minimize these charge collection losses in future solar cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546096","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daowei Gao, Juan Chen, Yanao Zhang, Yunrui Li, Lidan Zhu, Yipin Lv, Yuchen Qin, Jiawei Zhang, Yuming Dong, Yongfa Zhu, Yao Wang
Constructing high-efficiency platinum (Pt)-based catalysts for methanol oxidation reaction (MOR) by suppressing the intermediate COads generation is strongly desired and remains a grand challenge. Herein, the concept of holding O-bridged triple sites is documented to strengthen “non-CO” pathway selectivity by forming HCOO− species during MOR. The obtained Ga-O-PtPd triple sites via grafting the single-atomic Ga sites on PtPd nanosheets achieves a high current density of 3.05 mAcm−2 of MOR, which is 5.65 times higher than commercial Pt/C (0.54 mAcm−2), as well as remarkably stability and COads poison resistance. The CO diffuse reflectance infrared Fourier transform spectroscopy (CO-DRIFTS) results reveal that Ga-O-PtPd triple sites present a weak CO binding ability, reducing the generation of COads intermediate. In addition, the Ga-O-PtPd-based Zn-methanol-air batteries present an excellent activity and stability compared with commercial catalysts.
{"title":"Oxygen-Bridged Ga-O-PtPd Triple Sites Boost Methanol-Assisted Rechargeable Zn-Air Batteries Through Suppressing COads Generation","authors":"Daowei Gao, Juan Chen, Yanao Zhang, Yunrui Li, Lidan Zhu, Yipin Lv, Yuchen Qin, Jiawei Zhang, Yuming Dong, Yongfa Zhu, Yao Wang","doi":"10.1002/aenm.202500421","DOIUrl":"https://doi.org/10.1002/aenm.202500421","url":null,"abstract":"Constructing high-efficiency platinum (Pt)-based catalysts for methanol oxidation reaction (MOR) by suppressing the intermediate CO<sub>ads</sub> generation is strongly desired and remains a grand challenge. Herein, the concept of holding O-bridged triple sites is documented to strengthen “non-CO” pathway selectivity by forming HCOO<sup>−</sup> species during MOR. The obtained Ga-O-PtPd triple sites via grafting the single-atomic Ga sites on PtPd nanosheets achieves a high current density of 3.05 mAcm<sup>−2</sup> of MOR, which is 5.65 times higher than commercial Pt/C (0.54 mAcm<sup>−2</sup>), as well as remarkably stability and CO<sub>ads</sub> poison resistance. The CO diffuse reflectance infrared Fourier transform spectroscopy (CO-DRIFTS) results reveal that Ga-O-PtPd triple sites present a weak CO binding ability, reducing the generation of CO<sub>ads</sub> intermediate. In addition, the Ga-O-PtPd-based Zn-methanol-air batteries present an excellent activity and stability compared with commercial catalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Achieving commercial viability for organic solar cells (OSCs) requires non-toxic, non-halogenated solvent processing. However, poor solubility and suboptimal morphology of commonly used active layer materials have been limiting their non-halogenated solvent applications for high-performance OSCs. This study introduces a novel random terpolymer, PM7-TTz50, designed to overcome these challenges. By incorporating 50 mol% of a co-planar thiophene-thiazolothiazole (TTz) unit into the PM7 backbones, the resulting terpolymer achieves enhanced solubility in eco-friendly solvents. Furthermore, PM7-TTz50's strong aggregation tendency, coupled with high-boiling-point solvent processing—which prolongs aggregate/crystal growth—enhances molecular stacking and ordering. This approach supports efficient charge transport and minimizes non-radiative recombination, yielding power conversion efficiencies (PCEs) exceeding 19% and over 16% w/o solvent additives. Additionally, PM7-TTz50 demonstrates broad compatibility with various non-fullerene acceptors (NFAs), leading to enhanced material uniformity and reproducibility in device fabrication.
{"title":"Balance Processing and Molecular Packing via Structural Disordering in a Random Terpolymer for Over 19% Efficiency Non-Halogenated Solvent Organic Solar Cells","authors":"Jingnan Wu, Fengbo Sun, Feng Hua, Wenwen Hou, Xinxin Xia, Xia Guo, Donghong Yu, Ergang Wang, Yongfang Li, Maojie Zhang","doi":"10.1002/aenm.202500024","DOIUrl":"https://doi.org/10.1002/aenm.202500024","url":null,"abstract":"Achieving commercial viability for organic solar cells (OSCs) requires non-toxic, non-halogenated solvent processing. However, poor solubility and suboptimal morphology of commonly used active layer materials have been limiting their non-halogenated solvent applications for high-performance OSCs. This study introduces a novel random terpolymer, PM7-TTz50, designed to overcome these challenges. By incorporating 50 mol% of a co-planar thiophene-thiazolothiazole (TTz) unit into the PM7 backbones, the resulting terpolymer achieves enhanced solubility in eco-friendly solvents. Furthermore, PM7-TTz50's strong aggregation tendency, coupled with high-boiling-point solvent processing—which prolongs aggregate/crystal growth—enhances molecular stacking and ordering. This approach supports efficient charge transport and minimizes non-radiative recombination, yielding power conversion efficiencies (PCEs) exceeding 19% and over 16% w/o solvent additives. Additionally, PM7-TTz50 demonstrates broad compatibility with various non-fullerene acceptors (NFAs), leading to enhanced material uniformity and reproducibility in device fabrication.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"211 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tian Wang, Ya Xiao, Shaocong Tang, Weiwei Xiang, Jae Su Yu
Anode-free aqueous zinc (Zn) metal batteries (AFZMBs) possess an optimal battery architecture configuration because no excess Zn source is involved in the charge/discharge processes, rendering it feasible to enhance the energy density of batteries. However, rapid capacity fading due to the unstable anode-side current collector/electrolyte interfacial chemistry, which results in Zn dendrite growth, impedes their practical application, especially in quasi-solid-state AFZMBs. Herein, a robust bilayer interphase design strategy between a gel electrolyte and a copper current collector is proposed to achieve high-energy and stable quasi-solid-state AFZMBs. Utilizing the upper mass transfer layer to regulate rapid Zn ion transport and the lower zincophilic electron transfer layer to induce initial uniform Zn nucleation and balance the surface electric field, uniform dendrite-free Zn deposition and prominent reversibility are achieved. Therefore, the robust bilayer interphase design strategy significantly improves the cycling stability of quasi-solid-state Zn//I2 batteries. Additionally, the fabricated quasi-solid-state AFZMBs employing a pre-intercalated VO2 cathode deliver attractive energy and power densities (186.1 Wh kg−1/470 W kg−1 and 145.3 Wh kg−1/1.74 kW kg−1, based on the active material). Moreover, the successful extension of the bilayer interphase design to flexible AFZMBs offers a promising pathway for the development of wearable electronic devices.
{"title":"Unlocking Quasi-Solid-State Anode-Free Zinc Metal Batteries Through Robust Bilayer Interphase Engineering","authors":"Tian Wang, Ya Xiao, Shaocong Tang, Weiwei Xiang, Jae Su Yu","doi":"10.1002/aenm.202500430","DOIUrl":"https://doi.org/10.1002/aenm.202500430","url":null,"abstract":"Anode-free aqueous zinc (Zn) metal batteries (AFZMBs) possess an optimal battery architecture configuration because no excess Zn source is involved in the charge/discharge processes, rendering it feasible to enhance the energy density of batteries. However, rapid capacity fading due to the unstable anode-side current collector/electrolyte interfacial chemistry, which results in Zn dendrite growth, impedes their practical application, especially in quasi-solid-state AFZMBs. Herein, a robust bilayer interphase design strategy between a gel electrolyte and a copper current collector is proposed to achieve high-energy and stable quasi-solid-state AFZMBs. Utilizing the upper mass transfer layer to regulate rapid Zn ion transport and the lower zincophilic electron transfer layer to induce initial uniform Zn nucleation and balance the surface electric field, uniform dendrite-free Zn deposition and prominent reversibility are achieved. Therefore, the robust bilayer interphase design strategy significantly improves the cycling stability of quasi-solid-state Zn//I<sub>2</sub> batteries. Additionally, the fabricated quasi-solid-state AFZMBs employing a pre-intercalated VO<sub>2</sub> cathode deliver attractive energy and power densities (186.1 Wh kg<sup>−1</sup>/470 W kg<sup>−1</sup> and 145.3 Wh kg<sup>−1</sup>/1.74 kW kg<sup>−1</sup>, based on the active material). Moreover, the successful extension of the bilayer interphase design to flexible AFZMBs offers a promising pathway for the development of wearable electronic devices.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Indium sulfide (In2S3) as water splitting photocatalyst has been broadly investigated due to its narrow bandgap (2.0–2.3 eV) and optimized opto-electronic properties. However, In2S3 still suffers from a rapid photogenerated charge carrier recombination rate. In addition, the main group metals (such as In) lack active d-orbital electrons for catalysis, thus limits activation of intermediates during catalytic water splitting reaction. Herein, to overcome the above limitations of In2S3, In2S3/TiO2 heterojunction with sulfur defects are constructed by temperature control strategy. The sulfur vacancy (Sv) can induce the electron density transformation of In 5p-orbital from localized states to delocalized states, which efficiently enhances the chemical affinity to *OOH. Thus, the p-orbital interaction between In and O atoms greatly facilitates the rate-determining step (*OOH → *+O2), realizing a high O2 yield rate of 10.00 µmol cm−2 h−1 at 1.23 V versus RHE. Furthermore, the heterogeneous structure also can enhance interfacial electric field (IEF) and stability for promoting oxygen generation. This work provides an efficient pathway to improve photoelectrochemical (PEC) activity by manipulating p-orbital electron delocalization of main group metals through defect engineering.
{"title":"Tailoring p-Orbital Electron Delocalization Induced by Sulfur Defect Engineering for Enhancing Photoelectrochemical Water Splitting Performance","authors":"Yixuan Gao, Zhaoli Liu, Hua Lu, Weiliang Sun, Juanjuan Wei, Wen Liu","doi":"10.1002/aenm.202403752","DOIUrl":"https://doi.org/10.1002/aenm.202403752","url":null,"abstract":"Indium sulfide (In<sub>2</sub>S<sub>3</sub>) as water splitting photocatalyst has been broadly investigated due to its narrow bandgap (2.0–2.3 eV) and optimized opto-electronic properties. However, In<sub>2</sub>S<sub>3</sub> still suffers from a rapid photogenerated charge carrier recombination rate. In addition, the main group metals (such as In) lack active <i>d</i>-orbital electrons for catalysis, thus limits activation of intermediates during catalytic water splitting reaction. Herein, to overcome the above limitations of In<sub>2</sub>S<sub>3</sub>, In<sub>2</sub>S<sub>3</sub>/TiO<sub>2</sub> heterojunction with sulfur defects are constructed by temperature control strategy. The sulfur vacancy (Sv) can induce the electron density transformation of In 5<i>p</i>-orbital from localized states to delocalized states, which efficiently enhances the chemical affinity to <sup>*</sup>OOH. Thus, the <i>p</i>-orbital interaction between In and O atoms greatly facilitates the rate-determining step (<sup>*</sup>OOH → <sup>*</sup>+O<sub>2</sub>), realizing a high O<sub>2</sub> yield rate of 10.00 µmol cm<sup>−2</sup> h<sup>−1</sup> at 1.23 V versus RHE. Furthermore, the heterogeneous structure also can enhance interfacial electric field (IEF) and stability for promoting oxygen generation. This work provides an efficient pathway to improve photoelectrochemical (PEC) activity by manipulating <i>p</i>-orbital electron delocalization of main group metals through defect engineering.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"54 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In article number 2305169, Kaizhao Wang, Jin Hu, Shizhao Xiong, and co-workers have established a composite zinc anode with an in situ generated liquid metal interface and revealed the correlation between the physico-chemical properties of gallium and the electrodeposition behaviour of zinc. This study reveals the role of gallium's liquid interface on the morphological evolution of electrodeposited zinc and provides guidance for the future design and optimisation of high-performance aqueous zinc-metal batteries.