物理化学学报最新文献

{"title":"Modulating reactive oxygen species in O, S co-doped C3N4 to enhance photocatalytic degradation of microplastics","authors":"Yadan Luo ,&nbsp;Hao Zheng ,&nbsp;Xin Li ,&nbsp;Fengmin Li ,&nbsp;Hua Tang ,&nbsp;Xilin She","doi":"10.1016/j.actphy.2025.100052","DOIUrl":"10.1016/j.actphy.2025.100052","url":null,"abstract":"<div><div>Photocatalytic microplastic (MP) degradation <em>via</em> reactive oxygen species (ROS) is a considered environmentally friendly and sustainable approach for eliminating MP pollution in aquatic environments. However, it faces challenges due to the low migration and rapid recombination efficiency of charge carriers in photocatalysts. Herein, oxygen and sulfur co-doped carbon nitride (OSCN) nanosheets were synthesized through thermal polymerization coupled with a thermosolvent process. The O and S co-doping can reduce the bandgap and improve the light response of carbon nitride (C₃N₄). Meanwhile, O/S dopants effectively improve the delocalization of electron distribution, leading to increased carrier separation capacity, thereby promoting the formation of ROS and enhancing photocatalytic performance. Compared to C₃N₄, OSCN demonstrated significantly higher photocatalytic degradation and mineralization rates for MPs, including polyethylene (PE, traditional petroleum-based MPs) and polylactic acid (PLA, biodegradable bio-based MPs). Specifically, the mass loss of PE and PLA increased by 32.8 ​% and 34.1 ​%, respectively. Notably, ^•OH and ¹O₂ generated by OSCN synergistically catalyzed the degradation of PE, while ^•OH was the primary radical triggering the photolysis and hydrolysis of PLA. This study holds significant implications for the application of photocatalysis technology in the remediation of MP pollution in aquatic environments.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100052"},"PeriodicalIF":10.8,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143428896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Adjusting the electronic structure of Keggin-type polyoxometalates to construct S-scheme heterojunction for photocatalytic hydrogen evolution","authors":"Xinyu Miao ,&nbsp;Hao Yang ,&nbsp;Jie He ,&nbsp;Jing Wang ,&nbsp;Zhiliang Jin","doi":"10.1016/j.actphy.2025.100051","DOIUrl":"10.1016/j.actphy.2025.100051","url":null,"abstract":"<div><div>The sluggish electron migration rate and pronounced electron-hole recombination, pose significant obstacles to achieving high photocatalytic efficiency. The utilization of multiple catalysts for the construction of heterojunctions can effectively enhance charge separation. A series of Keggin-type hollow dodecahedral polyoxometalates were prepared <em>via</em> hydrothermal synthesis, and their molecular orbitals were modified through the addition of metal elements. The incorporation of metal elements modulated the electronic structure of polyoxometalates, effectively enhancing the electron aggregation capability of polyoxometalates. Single-component catalysts often face serious hole-electron recombination. In order to solve this problem, the scheme of constructing heterojunction is proposed to improve the electron transport efficiency. By immobilizing ZnCdS nanoparticles onto the polyoxometalate surface, the heterojunction architecture was engineered to significantly enhance the interfacial charge transfer capability. Density Functional Theory (DFT) calculations and the experimental results indicate that the modulation of metallic components renders the polyoxometalate a more favorable energy-level orbital. The catalytic mechanism of ZnCdS and KMoP S-scheme heterojunction was also verified. The formation of S-scheme heterojunctions further improves the electron transfer efficiency compared to other traditional heterojunctions, achieving efficient utilization of photo generated electrons and holes. Additionally, the S-scheme heterojunction shifts the catalystʼs <em>d</em>-band center closer to the Fermi level, thereby improving electrical conductivity. This article provides a new approach for energy level regulation of polyoxometalates and the design of S-scheme heterojunctions.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100051"},"PeriodicalIF":10.8,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143428898","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Rationally designed ZnFe1.2Co0.8O4/BiVO4 S-scheme heterojunction with spin-polarization for the elimination of antibiotic","authors":"Jinwang Wu ,&nbsp;Qijing Xie ,&nbsp;Chengliang Zhang ,&nbsp;Haifeng Shi","doi":"10.1016/j.actphy.2025.100050","DOIUrl":"10.1016/j.actphy.2025.100050","url":null,"abstract":"<div><div>Recently, the regulation of electronic spin polarization has attracted considerable interest as an effective strategy to mitigate the rapid recombination of photo-generated charges. However, current research predominantly targets individual photocatalysts, where the efficiency of charge separation still has significant room for improvement. Herein, a ZnFe_1.2Co_0.8O₄ (ZFCO) and BiVO₄ (BVO) S-scheme heterojunction was developed, which synergistically promoted charge separation through the S-scheme heterojunction and spin polarization, and further enhanced the photocatalytic performance in removing organic pollutants under an external magnetic field. Experimental results revealed that under sole light irradiation, ZB-1.5 (ZFCO : BVO ​= ​3 : 2) demonstrated optimal performance, with a reaction rate constant (<em>k</em>) for tetracycline (TC) degradation of 0.0146 ​min⁻¹. Under light irradiation and magnetic field conditions, the reaction rate constant (<em>k</em>) of ZB-1.5 for TC degradation increased to 0.0175 ​min⁻¹, indicating enhanced photocatalytic performance. DFT calculations indicated that ZFCO exhibited the spin polarization. Photoluminescence measurements demonstrated that the S-scheme heterojunction structure improved the charge separation efficiency. In addition, possible degradation pathways and toxicity were assessed, indicating successful detoxification. This work provides some useful insights into utilizing S-scheme heterojunctions to develop photocatalysts with efficient separation of photo-generated charges.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 5","pages":"Article 100050"},"PeriodicalIF":10.8,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102411","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Research on Cu-based and Pt-based catalysts for hydrogen production through methanol steam reforming","authors":"Xue Liu ,&nbsp;Lipeng Wang ,&nbsp;Luling Li ,&nbsp;Kai Wang ,&nbsp;Wenju Liu ,&nbsp;Biao Hu ,&nbsp;Daofan Cao ,&nbsp;Fenghao Jiang ,&nbsp;Junguo Li ,&nbsp;Ke Liu","doi":"10.1016/j.actphy.2025.100049","DOIUrl":"10.1016/j.actphy.2025.100049","url":null,"abstract":"<div><div>Methanol steam reforming (MSR) is a critical pathway for on-board hydrogen production from methanol, playing a significant role in clean energy applications. The catalytic performance in MSR reactions directly influences hydrogen yield and byproduct composition, with Cu-based and Pt-based catalysts extensively studied for their high efficiency. The catalytic mechanism primarily involves the cleavage of C–H and O–H bonds in methanol and water molecules. The activity of Cu-based catalysts depends on the ratio and synergistic interaction of Cu⁰ and Cu⁺ ​active sites, while Pt-based catalysts operate through Pt⁰, Pt^δ+ or Pt²⁺ active sites, in conjunction with oxygen vacancies. However, the electron transfer and interaction mechanisms between active metals and supports remain contentious, impacting the metal oxidation states, adsorption sites, and reaction pathway selectivity. This is particularly evident in the pathways for methanol dehydrogenation and intermediate product formation (e.g., formaldehyde, formic acid, and methyl formate), which lack a unified understanding. This review systematically examines the unitary and synergistic roles of Cu⁰ and Cu⁺ ​sites, explores the direct and synergistic pathways of Pt-based catalysts, and analyzes the effects of additives such as In₂O₃ on Pt site modulation and oxygen vacancy generation. By integrating catalytic performance evaluations with mechanistic insights, strategies are proposed to enhance catalyst activity and stability. This comprehensive review not only advances the understanding of MSR mechanisms but also provides a theoretical foundation and research direction for the development of high-performance catalysts for on-board hydrogen production.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 5","pages":"Article 100049"},"PeriodicalIF":10.8,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pt single-atom-functionalized 2D Al-TCPP MOF nanosheets for enhanced photodynamic antimicrobial therapy","authors":"Shiyang He ,&nbsp;Dandan Chu ,&nbsp;Zhixin Pang ,&nbsp;Yuhang Du ,&nbsp;Jiayi Wang ,&nbsp;Yuhong Chen ,&nbsp;Yumeng Su ,&nbsp;Jianhua Qin ,&nbsp;Xiangrong Pan ,&nbsp;Zhan Zhou ,&nbsp;Jingguo Li ,&nbsp;Lufang Ma ,&nbsp;Chaoliang Tan","doi":"10.1016/j.actphy.2025.100046","DOIUrl":"10.1016/j.actphy.2025.100046","url":null,"abstract":"<div><div>The pressing challenges posed by infectious diseases caused by pathogenic microbial infections have necessitated the development of advanced antimicrobial strategies. Among the promising avenues, photodynamic therapy (PDT) has emerged as a promising approach due to its non-invasive and targeted nature. Although it has been widely used in antibacterial therapy, there are still obstacles in precisely regulating the structure of photosensitizers to achieve satisfactory photodynamic performance. Herein, Pt single-atoms (SAs) are deposited on two-dimensional (2D) Al-TCPP metal-organic framework (MOF) nanosheets, creating Pt/Al-TCPP as the photosensitizer to boost reactive oxygen species (ROS) production for enhanced photodynamic antimicrobial therapy. By integrating Pt SAs onto 2D Al-TCPP MOF nanosheets, we not only improve the dispersion and stability of Pt atoms but also harness the synergistic effect between the MOF's crystal porous structure and Pt SAs, optimizing its light-trapping ability. This unique structure enhances the bridging unit between Pt SA and the porphyrin linker, facilitating efficient charge transfer and separation during illumination, ultimately boosting ROS production. In addition to the inherent photodynamic performance of Pt SAs, they can also increase the adsorption of oxygen, facilitate electron transfer, and improve charge separation, thus enhancing photodynamic ROS generation efficiency. Therefore, the Pt/Al-TCPP photosensitizer shows much greater efficacy in generating ROS under a 660 ​nm laser irradiation compared to Al-TCPP. Both <em>in vitro</em> and <em>in vivo</em> experiments demonstrate that the Pt/Al-TCPP nanosheets can effectively eliminate bacteria and promote wound healing in a short time at low doses under laser irradiation. This study underscores the advantages of integrating Pt SAs with Pt/Al-TCPP nanosheets and offers a highly effective photosensitizer for bacterial infections. The results pave the way for novel strategies in the antibacterial realm, highlighting the potential of Pt/Al-TCPP nanosheets as a promising therapeutic agent for efficient wound healing.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 5","pages":"Article 100046"},"PeriodicalIF":10.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164819","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-precision and reliable thermal conductivity measurement for graphene films based on an improved steady-state electric heating method","authors":"Jiahao Lu ,&nbsp;Xin Ming ,&nbsp;Yingjun Liu ,&nbsp;Yuanyuan Hao ,&nbsp;Peijuan Zhang ,&nbsp;Songhan Shi ,&nbsp;Yi Mao ,&nbsp;Yue Yu ,&nbsp;Shengying Cai ,&nbsp;Zhen Xu ,&nbsp;Chao Gao","doi":"10.1016/j.actphy.2025.100045","DOIUrl":"10.1016/j.actphy.2025.100045","url":null,"abstract":"<div><div>The graphene film with high thermal conductivity has garnered considerable attention in recent years as an ideal material for dissipating heat in high-power electronic devices. Thermal conductivity is a crucial parameter for evaluating its fundamental performance. High-precision measurement holds significant importance for understanding its basic properties, fabrication optimization, and industrial applications. However, it is difficult to simultaneously achieve efficient, accurate, and reliable measurements with existing commercial thermal conductivity testing methods. The development of a convenient, high-precision, and reliable measurement approach remains a great challenge. Here, we introduce a thermal conductivity testing methodology with superior accuracy and excellent efficiency based on an improved steady-state electric heating method, refined through the optimization of heat transfer principles, experimental operation, and data analysis, supported by finite element simulation. The accuracy of measurements is affected by four factors: heat loss calibration, sample size, device design, and data treatment. The experimental results show that the heat loss caused by heat radiation and heat convection affects the temperature distribution and the measurements of the sample, which should be strictly controlled by sample size and temperature rise. Reasonable screening and preprocessing of data are also necessary to improve measurement accuracy. Through the comparative analysis of the temperature distribution and thermal conductivity measurements of samples under different conditions, we propose feasible operational guidance and a standardized testing protocol to minimize measurement error. The measurement error is less than 3.0%, and uncertainty is reduced to 0.5%. Simulation results confirm that the response time of this method is down to milliseconds, correlating well with the experiment, which can effectively improve test efficiency. Considering the combined merits of high accuracy, repeatability, and fast response, the improved steady-state electric heating method offers useful guidance for the accurate evaluation of the thermal conductivity of materials and crucial technical support for research and application in thermal management.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 5","pages":"Article 100045"},"PeriodicalIF":10.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102410","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Corrigendum to “Mechanistic insights into water-mediated CO2 electrochemical reduction reactions on Cu@C2N catalysts: A Theoretical study” [Acta Physico-Chimica Sinica (2024) 40, 2303040]","authors":"Hanyu Xu ,&nbsp;Xuedan Song ,&nbsp;Qing Zhang ,&nbsp;Chang Yu ,&nbsp;Jieshan Qiu","doi":"10.1016/j.actphy.2024.100043","DOIUrl":"10.1016/j.actphy.2024.100043","url":null,"abstract":"","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 5","pages":"Article 100043"},"PeriodicalIF":10.8,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Performance and electrochemical asymmetry optimization of hydrogen electrode supported reversible solid oxide cell","authors":"Qianwen Han,&nbsp;Tenglong Zhu,&nbsp;Qiuqiu Lyu,&nbsp;Mahong Yu,&nbsp;Qin Zhong","doi":"10.3866/PKU.WHXB202309037","DOIUrl":"10.3866/PKU.WHXB202309037","url":null,"abstract":"<div><div>Solid oxide cell (SOC) is a typical multi-layer thin film ceramic device consisting of oxygen electrodes, electrolytes, and hydrogen electrodes. The currently widely used structure is a single cell supported by a Ni-YSZ (Nickel-Yttria Stabilized Zirconia) hydrogen electrode, with YSZ (Yttria Stabilized Zirconia) serving as the electrolyte. This configuration achieves electrolyte filmization, while also reducing the operating temperature of the cell. However, it introduces significant diffusion resistance within the hydrogen electrode, which is considered the main reason for the electrochemical asymmetry in reversible solid oxide cell (R–SOC). This study prepared hydrogen electrodes with varying porosity and investigated the impact of diffusion resistance of hydrogen electrodes on R–SOC asymmetry. On this basis, <em>in-situ</em> hydrothermal growth technology was employed to prepare ultra-thin and dense GDC (Gd₂O₃ doped CeO₂) barrier layers, compared with conventional screen-printed barrier layers to explore the effect of electrolyte ohmic resistance on electrochemical asymmetry. Experimental findings revealed that the electrolyte ohmic resistance is also a significant factor affecting the electrochemical asymmetry of reversible SOC, and the synergistic mechanism of the diffusion resistance of hydrogen electrodes and the ohmic resistance of thin film electrolytes on this asymmetry was elucidated. The experimental results show that increasing the hydrogen electrode porosity and reducing the electrolyte ohmic resistance can both enhance the R–SOC performance, particularly improving SOEC electrolysis performance, and both have the effect of reducing asymmetry. At 750 °C, 50 % H₂O, and ±0.3 V bias conditions, the single cell with a large-pore hydrogen electrode and a thin film barrier layer exhibited a discharge current density of 0.752 A cm⁻² and an electrolysis current density of 0.635 A cm⁻². Compared to the single cell with a small pore hydrogen electrode and an ordinary screen-printed barrier layer, the discharge and electrolysis performance of the cell have been improved by ∼37 % and ∼140 %, respectively. At the same time, the current density asymmetry of the cell (Δ<em>j</em>) under these conditions was only 0.117 A cm⁻², reduced by 58 % compared to a small porosity hydrogen electrode single cell and 24 % compared to a large ohmic resistance single cell. In addition, the study noted that R–SOC asymmetry increases with operating temperature and decreases with higher steam content in the fuel on the hydrogen electrode side. These findings hold significant reference value the design, preparation, and reversible operation of high-performance hydrogen electrode supported thin film electrolyte SOC single cell structures.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 1","pages":"Article 100005"},"PeriodicalIF":10.8,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Catalytic effect of H3PW12O40 on hydrogen storage of MgH2","authors":"Ran Yu ,&nbsp;Chen Hu ,&nbsp;Ruili Guo ,&nbsp;Ruonan Liu ,&nbsp;Lixing Xia ,&nbsp;Cenyu Yang ,&nbsp;Jianglan Shui","doi":"10.3866/PKU.WHXB202308032","DOIUrl":"10.3866/PKU.WHXB202308032","url":null,"abstract":"<div><div>Developing hydrogen energy to replace carbon-rich fossil fuels is the future direction of energy technology, but there is still a lack of safe and efficient hydrogen storage technology. Hydrogen storage in solid medium is a relatively safe way to store hydrogen, among which magnesium hydride (MgH₂) is one of the most promising solid hydrogen storage materials. MgH₂ has the advantages of high hydrogen storage density, low cost and good reversibility of hydrogen absorption and release. However, improving its poor thermodynamic and slow kinetic characteristics are still challenging. Catalysts derived from polyoxometalates have been successfully used for catalyzing hydrogen evolution reaction, oxidation of organic compounds, desulfurization reaction, and so on. However, these catalysts have not been applied to the hydrogen storage materials yet. In this paper, H₃PW₁₂O₄₀ is selected as a representative of polyoxometalates and its catalytic effect on hydrogen storage is studied. MgH₂-<em>x</em>H₃PW₁₂O₄₀ (<em>x</em> ​= ​7 ​%, 10 ​%, 13 ​%, mass percentage) and pure MgH₂ samples are prepared by mechanical ball milling method. Among them, MgH₂-10H₃PW₁₂O₄₀ exhibits the optimal performance in both kinetic characteristic and hydrogen storage capacity. It can rapidly absorb 6.25 ​% hydrogen within 1 ​min at 250 ​°C and release 6.54 ​% hydrogen within 15 ​min at 300 ​°C, while ball-milled MgH₂ only releases 1.2 ​% hydrogen within 30 ​min at 300 ​°C. At the same time, the activation energy of the composite decreases to 106.08 ​kJ ​mol⁻¹, which is 46.23 ​kJ ​mol⁻¹ lower than MgH₂. The catalytic effect of H₃PW₁₂O₄₀ on the hydrogen storage properties of MgH₂ mainly comes from three aspects. Firstly, the addition of H₃PW₁₂O₄₀ helps to avoid the agglomeration of MgH₂ during the ball milling process, which makes the MgH₂ particles become smaller after ball milling, thus increasing the specific surface area of the interaction with hydrogen. Secondly, the addition of H₃PW₁₂O₄₀ makes MgH₂ produce a large number of defects and lattice distortion during ball milling, which provides more channels for hydrogen diffusion. Thirdly, the catalytic components of WO₃ and W are <em>in situ</em> formed during the ball milling process. They can be used as active components to accelerate the electron migration process, which promotes the cleavage of the Mg―H bond and the adsorption and dissociation of hydrogen.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 1","pages":"Article 100001"},"PeriodicalIF":10.8,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143154597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-stable aqueous zinc metal anodes enabled by an oriented ZnQ zeolite protective layer with facile ion migration kinetics","authors":"Shanghua Li ,&nbsp;Malin Li ,&nbsp;Xiwen Chi ,&nbsp;Xin Yin ,&nbsp;Zhaodi Luo ,&nbsp;Jihong Yu","doi":"10.3866/PKU.WHXB202309003","DOIUrl":"10.3866/PKU.WHXB202309003","url":null,"abstract":"<div><div>Aqueous zinc ion batteries (ZIBs) are regarded as one of the most promising energy storage systems due to their reliable safety, low cost, high volumetric capacity, and environmental friendliness. However, the utilization of Zn metal anode in aqueous electrolyte commonly encounters complex water-induced side reactions and uncontrollable dendrite growth issues. Constructing a protective layer on the surface of Zn anode is an effective strategy to alleviate side reactions and dendrite growth, achieving the stable operation of ZIBs with prolonged cycling life. However, the utilization of protective layers will increase interfacial resistance and result in high polarization in most cases. Thus, developing a desirable artificial protective layer with high ion migration kinetics is a significant task, enabling a fast Zn²⁺ ion flux for homogeneous deposition with low polarization. Considering that porous aluminosilicate zeolite with a low Si/Al ratio can accommodate abundant framework-associated cations as charge carriers for conduction, herein, we prepared an oriented protective layer on the Zn anode using Zn-ion-exchanged Q zeolite with <strong>BPH</strong> topology (ZnQ@Zn), achieving a stable Zn anode with high ion migration kinetics. The ZnQ zeolite plates parallelly lay on the surface of Zn foil with the <em>c</em> axis normal to the substrate plane. The three-dimensional ordered channels and the oriented arrangement of ZnQ zeolite plates provide facile ion migration pathways for Zn²⁺ ions, and the coordination of framework-associated Zn²⁺ ions with water in zeolite channels also enables fast ion conduction kinetics and high corrosion resistance. Therefore, ZnQ@Zn exhibits enhanced ion conduction kinetics with reduced energy barriers for desolvation, charge transfer, and diffusion processes, resulting in a uniform ion flux to suppress dendrite growth. Consequently, the ZnQ@Zn symmetric cell displays an ultra-low voltage hysteresis of 27 ​mV with a long lifespan of over 1100 ​h at 1 ​mA ​cm⁻² and 1 ​mAh ​cm⁻². Moreover, the ZnQ@Zn//NaV₃O₈·1.5H₂O full cell delivers a superior long-term cycling performance with a high capacity retention of 96% after 1800 cycles at 8 ​A ​g⁻¹. This work provides a new sight for constructing protective layers with fast ion migration kinetics to achieve high-stable Zn anodes, and extends the application of zeolite-based ion-conductive materials in energy storage devices.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 1","pages":"Article 100003"},"PeriodicalIF":10.8,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143154598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}