物理化学学报最新文献

{"title":"Exploring Zn doped NiBP microspheres as efficient and stable electrocatalyst for industrial-scale water splitting","authors":"Sumiya Akter Dristy,&nbsp;Md Ahasan Habib,&nbsp;Shusen Lin,&nbsp;Mehedi Hasan Joni,&nbsp;Rutuja Mandavkar,&nbsp;Young-Uk Chung,&nbsp;Md Najibullah,&nbsp;Jihoon Lee","doi":"10.1016/j.actphy.2025.100079","DOIUrl":"10.1016/j.actphy.2025.100079","url":null,"abstract":"<div><div>Green hydrogen holds great promise for the future energy ecosystem and designing alternative electrocatalysts is essential for industrial-scale green hydrogen production for high-current water splitting under industrial conditions. Herein, the Zn-doped NiBP microsphere electrocatalyst is fabricated <em>via</em> a multi-step process combining hydrothermal and electrochemical approaches, followed by post-annealing. The optimized Zn/NiBP electrode outperforms the majority of previously reported catalysts, with low overpotentials of 95 ​mV for HER (hydrogen evolution reaction) and 280 ​mV for OER (oxygen evolution reaction) at 100 ​mA ​cm⁻² in 1 ​mol ​L⁻¹ KOH. The bifunctional Zn/NiBP || Zn/NiBP demonstrates a 3.10 ​V cell voltage at 2000 ​mA ​cm⁻² in 1 ​mol ​L⁻¹ KOH, surpassing the benchmark Pt/C || RuO₂ systems. The Pt/C || Zn/NiBP hybrid system exhibits exceptionally low cell voltages of 2.50 and 2.30 ​V at 2000 ​mA ​cm⁻² in 1 and 6 ​mol ​L⁻¹ KOH respectively, demonstrating excellent overall water-splitting performance under challenging industrial conditions. Furthermore, the 2-E system shows remarkable stability over 120 ​h at 1000 ​mA ​cm⁻² in 1 and 6 ​mol ​L⁻¹ KOH, indicating the robust anti-corrosion properties of the Zn/NiBP microspheres. Zn-doped NiBP microspheres exhibit enhanced electrochemical conductivity, active surface area and intrinsic electrocatalytic activity due to synergistic interactions among Zn, Ni, B and P, enabling rapid charge transfer and superior electrocatalytic performance for efficient hydrogen generation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100079"},"PeriodicalIF":10.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143684740","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":"Accurate and efficient prediction of Schottky barrier heights in 2D semimetal/silicon heterojunctions","authors":"Haiyu Zhu ,&nbsp;Zhuoqun Wen ,&nbsp;Wen Xiong ,&nbsp;Xingzhan Wei ,&nbsp;Zhi Wang","doi":"10.1016/j.actphy.2025.100078","DOIUrl":"10.1016/j.actphy.2025.100078","url":null,"abstract":"<div><div>The accurate prediction of the Schottky barrier height (SBH) holds significant importance for optimizing the performance of semimetal/semiconductor heterojunction devices. Two-dimensional semimetal/semiconductor heterostructures have now been extensively studied experimentally. However, first-principles predictions of the corresponding SBH typically require solving the ab initio Hamiltonian in supercells containing more than 10³ atoms. This high computational complexity not only results in extremely low efficiency but also hinders the design and optimization of heterojunction devices. Herein, we apply density functional theory with a core-level energy alignment method for transition-metal-ditelluride semimetal/silicon junctions, which enables a reduction in supercell size by one order of magnitude. The predicted SBHs show excellent agreement with experiment. We further investigate different 2D semimetal compounds, finding that all candidates exhibit lower SBHs for holes than electrons, with thickness effects becoming negligible beyond three to five layers. This study presents an efficient framework for calculating SBH in complex heterostructures and provides theoretical guidance for the efficient design of high-performance 2D semimetal heterojunction devices.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100078"},"PeriodicalIF":10.8,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704031","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":"Facile synthesis of hierarchical Ti3C2/Bi12O17Br2 Schottky heterojunction with photothermal effect for solar–driven antibiotics photodegradation","authors":"Chao Liu ,&nbsp;Huan Yu ,&nbsp;Jiaming Li ,&nbsp;Xi Yu ,&nbsp;Zhuangzhi Yu ,&nbsp;Yuxi Song ,&nbsp;Feng Zhang ,&nbsp;Qinfang Zhang ,&nbsp;Zhigang Zou","doi":"10.1016/j.actphy.2025.100075","DOIUrl":"10.1016/j.actphy.2025.100075","url":null,"abstract":"<div><div>Photocatalytic technology is considered to be an efficient and green approach for removing tetracycline hydrochloride (TC) to meet the demands of sustainable development. Here, a facile stirring process was employed to construct Ti₃C₂/Bi₁₂O₁₇Br₂ (termed as TBOB) Schottky heterojunction with a hierarchical structure, in which the Bi₁₂O₁₇Br₂ component was closely deposited on the surface of Ti₃C₂. The TC photodegradation performance was estimated for all catalysts under simulated solar light. Compared with Bi₁₂O₁₇Br₂, TBOB materials exhibited the superior photodegradation activity due to the synergistic effect between Ti₃C₂ and Bi₁₂O₁₇Br₂, which could increase light harvesting capacity derived from Ti₃C₂ loading, promote the charge carrier separation due to the formed Schottky heterojunction, and facilitate surface reaction kinetics owing to the photothermal effect. Besides, some crucial influencing factors on the photocatalytic performance over TBOB composites were separately studied in detail. The free radical capture experiment and electron paramagnetic resonance (EPR) technique confirmed the predominant active species of •O₂⁻ and e⁻ for the TC photodegradation. Combined with experimental analysis and theoretical calculations, insight into the charge carrier transfer and photodegradation mechanisms were proposed. This study provides theoretical and experimental insights for the rational design of high-efficiency photothermal<strong>-</strong>assisted Ti₃C₂_-based photocatalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100075"},"PeriodicalIF":10.8,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143621186","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":"Efficient adsorption of hardness ions by a mordenite-loaded, nitrogen-doped porous carbon nanofiber cathode in capacitive deionization","authors":"Jun Huang ,&nbsp;Pengfei Nie ,&nbsp;Yongchao Lu ,&nbsp;Jiayang Li ,&nbsp;Yiwen Wang ,&nbsp;Jianyun Liu","doi":"10.1016/j.actphy.2025.100066","DOIUrl":"10.1016/j.actphy.2025.100066","url":null,"abstract":"<div><div>Water hardness, predominantly due to the presence of Ca²⁺ and Mg²⁺ ions, presents significant challenges to water quality and public health. Addressing this issue necessitates effective water softening, which remains a pivotal task in water treatment. Capacitive deionization (CDI) has emerged as a promising technology for selective hardness removal, leveraging the low-cost, non-toxic and environmentally friendly selective electrode materials. Electrospun nanofibers, characterized by their three-dimensional porous structure, offer good flexibility, high specific surface area and excellent electrical conductivity. Their components can be tailored to meet the specific requirements. In this study, we incorporated mordenite (MOR), noted for its excellent ion-exchange capacity, into self-supporting nitrogen-doped carbon nanofibers (N–CNF) via electrospinning a blend of polyacrylonitrile (PAN), urea, and MOR, followed by carbonization. The resulting mordenite-loaded N–CNF composite (MOR@N–CNF) exhibited good flexibility and high conductivity. Scanning electron microscopy and X-ray diffraction analysis confirmed the presence and uniform distribution of MOR within the CNF matrix. X-ray photo spectroscopy demonstrated an increase in nitrogen content in MOR@N–CNF. In addition, the MOR@N–CNF composite displayed enhanced hydrophilicity and an increased specific surface area. When used as a self-supporting electrode, MOR@N–CNF exhibited the electrochemical specific capacitance of 162.7 ​F/g, with the specific capacitance retention of 60% in a CaCl₂ solution. In an asymmetric CDI setup with activated carbon (AC) as the anode, the MOR@N–CNF cathode demonstrated outstanding adsorption capacities of 1501 and 1416 ​μmol/g for Mg²⁺ and Ca²⁺, respectively. The composite electrode exhibited high selectivity for Mg²⁺ and Ca²⁺ over Na⁺ with a selectivity factor of 9.7 and 8.9, respectively. These attributes endow the material with exceptional ability to discriminate between divalent and monovalent ions, thereby enhancing its potential for hardness removal. Furthermore, the electrode retained 78% of its adsorption capacity after 40 cycles, demonstrating robust cyclic stability, and ensuring long-term CDI operation. This work provides a new strategy for preparing ion-exchange material-based composite electrodes and highlights the potential of CDI technology in hard water softening.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100066"},"PeriodicalIF":10.8,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143551997","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":"Recent advances in synergistic catalytic valorization of CO2 and hydrocarbons by heterogeneous catalysis","authors":"Honghong Zhang ,&nbsp;Zhen Wei ,&nbsp;Derek Hao ,&nbsp;Lin Jing ,&nbsp;Yuxi Liu ,&nbsp;Hongxing Dai ,&nbsp;Weiqin Wei ,&nbsp;Jiguang Deng","doi":"10.1016/j.actphy.2025.100073","DOIUrl":"10.1016/j.actphy.2025.100073","url":null,"abstract":"<div><div>The escalating frequency of extreme weather events globally has necessitated immediate action to mitigate the impacts and threats posed by excessive greenhouse gas emissions, particularly carbon dioxide (CO₂). Consequently, reducing CO₂ emissions has become imperative, with decarbonization techniques being extensively investigated worldwide to achieve net-zero emissions. From an energy perspective, CO₂ represents an abundant and low-cost carbon resource that can be converted into high-value chemical products through reactions with hydrocarbons, including alkanes, alkenes, aromatic hydrocarbons, and polyolefins. Through hydrogen transfer, CO₂ can be reduced to CO, accompanied by the formation of H₂O. CO₂ and hydrocarbons can also be transformed into syngas (CO and H₂) <em>via</em> dry reforming. Furthermore, CO₂ can be incorporated into hydrocarbon molecules, resulting in carbon chain growth, such as the production of alcohols, carboxylic acids, and aromatics. However, due to the thermodynamic stability and kinetic inertness of CO₂, as well as the high bond energy and low polarity of hydrocarbon C–H bonds, the conversion of CO₂ and hydrocarbons remains a highly challenging and demanding strategic objective. This review focuses on the synergistic catalytic valorization of CO₂ and hydrocarbons using heterogeneous catalysts, summarizing recent advancements in coupling CO₂ with various hydrocarbons. It also examines relevant kinetic models, including Langmuir-Hinshelwood and Eley-Rideal mechanisms. For catalyst design, bifunctional catalysts with distinct active sites can independently activate these two reactive molecules, and the modulation of acid-base properties, oxygen vacancies, and interfacial interactions represents an effective strategy to optimize catalytic performance. Finally, future directions for advancing CO₂-hydrocarbon co-utilization technologies are proposed, along with recommendations for low-carbon development strategies.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100073"},"PeriodicalIF":10.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143592144","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":"Modulating the d-band center of NNU-55(Fe) for enhanced CO2 adsorption and photocatalytic activity","authors":"Xueqi Yang ,&nbsp;Juntao Zhao ,&nbsp;Jiawei Ye ,&nbsp;Desen Zhou ,&nbsp;Tingmin Di ,&nbsp;Jun Zhang","doi":"10.1016/j.actphy.2025.100074","DOIUrl":"10.1016/j.actphy.2025.100074","url":null,"abstract":"<div><div>Photocatalytic reduction of carbon dioxide (CO₂) has emerged as an effective technology to transform CO₂ into valuable chemicals. Metal-organic frameworks (MOFs) show great promise due to their adjustable structures, huge specific surface areas, excellent catalytic properties, and remarkable photo responsiveness. Herein, the MOF material NNU-55(Fe) was employed for the photocatalytic transformation of CO₂ into carbon monoxide (CO). Through electronic modulation of the active metal center (Fe–N4) <em>via</em> inorganic anionic ligand tuning, the photocatalytic performance of NNU-55(Fe) MOFs can be easily regulated. Notably, NO₃⁻-coordinated NNU-55(Fe) demonstrated superior catalytic performance compared to SO₄²⁻- and Cl⁻-coordinated catalysts, achieving a CO production of 124 ​μmol·g⁻¹ within 3 ​h. The stronger electron donation capacity of NO₃⁻ leads to an improved electron density of Fe centers, which lowers the Fe <em>d</em>-band center and enhances the bonding orbital occupancy in the adsorption system, thereby increasing the adsorption strength of CO₂ and reduction activity. This study highlights a simple strategy for altering the catalytic activity and electrical structure of MOFs by altering the coordinated inorganic ligands of metal sites, offering a novel approach to developing efficient photocatalytic materials.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100074"},"PeriodicalIF":10.8,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577793","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":"Efficient capacitive desalination over NCQDs decorated FeOOH composite","authors":"Yihan Xue ,&nbsp;Xue Han ,&nbsp;Jie Zhang,&nbsp;Xiaoru Wen","doi":"10.1016/j.actphy.2025.100072","DOIUrl":"10.1016/j.actphy.2025.100072","url":null,"abstract":"<div><div>Capacitive deionization (CDI) is emerging as a novel technology for seawater purification, with the electrode material playing a crucial role in desalination performance. In this study, we designed a nitrogen-doped carbon quantum dots decorated iron oxide hydroxide (NCQDs/FeOOH) composite by a facile hydrothermal strategy and investigated as the CDI cathode for desalination application. Microstructural analyses reveal that the composite features a relatively uniform nanoparticle-assembled network, hierarchical pore alignment, and abundant porosity. Electrochemical tests confirm its outstanding capacitance property and conductivity. In an initial NaCl aqueous solution of 2000 ​mg ​L⁻¹ ​at an applied potential of 1.4 ​V, the GAC_NaCl of NCQDs/FeOOH hybrid electrode reaches 56.52 ​mg ​g⁻¹, along with the remarkable cycling durability. Furthermore, CV (cyclic voltammetry) and <em>ex situ</em> XPS (X-ray photoelectron spectroscopy) characterizations indicate the predominantly pseudocapacitive desalination mechanism.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100072"},"PeriodicalIF":10.8,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143563801","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":"Hollow structured photocatalysts","authors":"Fangxuan Liu ,&nbsp;Ziyan Liu ,&nbsp;Guowei Zhou ,&nbsp;Tingting Gao ,&nbsp;Wenyu Liu ,&nbsp;Bin Sun","doi":"10.1016/j.actphy.2025.100071","DOIUrl":"10.1016/j.actphy.2025.100071","url":null,"abstract":"<div><div>Photocatalysis technology, utilizing solar-driven reactions, is poised to emerge as a reliable strategy to alleviate environmental and energy pressures. Thus, whether the photocatalytic performance is excellent depends on the reasonable design of photocatalysts. By considering factors such as morphology engineering, band gap engineering, co-catalyst modification, and heterojunction construction, the photocatalysts with superior performance can be developed. Inspired by this unique characteristic, photocatalysts with a hollow structure endow numerous advantages in photocatalyst design, including enhanced multiple refraction and reflection of light, reduced transport distance of photo-induced carriers, and provided plentiful surface reaction sites. Herein, we systematically review the latest progress of hollow structured photocatalysts and summarize the diversity from geometric morphology, internal structure, and chemical composition. Specifically, the synthetic strategies of hollow structured photocatalysts are highlighted, including hard template, soft template, and template free methods. Furthermore, a series of hollow structured photocatalysts have also been described in detail, such as metal oxide, metal sulfide, metal-organic framework, and covalent organic framework. Subsequently, we present the potential applications of hollow structured photocatalysts in photocatalytic pollutant degradation, H₂ production, H₂O₂ production, CO₂ reduction, and N₂ fixation. Simultaneously, the relevant relationship between hollow structure and photocatalytic performance is deeply discussed. Toward the end of the review, we introduce the challenges and prospects in the future development direction of hollow structured photocatalysts. The review can provide inspiration for better designing hollow structured photocatalysts to meet the needs of environmental remediation and energy conversion.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100071"},"PeriodicalIF":10.8,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143551996","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":"Waste plastics promoted photocatalytic H2 evolution over S-scheme NiCr2O4/twinned-Cd0.5Zn0.5S homo-heterojunction","authors":"Jingzhuo Tian ,&nbsp;Chaohong Guan ,&nbsp;Haobin Hu ,&nbsp;Enzhou Liu ,&nbsp;Dongyuan Yang","doi":"10.1016/j.actphy.2025.100068","DOIUrl":"10.1016/j.actphy.2025.100068","url":null,"abstract":"<div><div>The simultaneous enhancement of separation and utilization of bulk and surface charges is crucial for achieving efficient photocatalytic H₂ evolution reactions. In this study, NiCr₂O₄/T-CZS composites were fabricated by incorporating NiCr₂O₄ nanosheets onto the surface of twinned Cd_0.5Zn_0.5S (T-CZS) nanoparticles using a solvent evaporation strategy. After optimization, the 6% NiCr₂O₄/T-CZS exhibited an impressive hydrogen (H₂) evolution rate (<em>r</em>_H2) of 81.4 ​mmol·h⁻¹·g⁻¹ when employing polylactic acid (PLA) plastic as a sacrificial agent in NaOH solution. The reason behind this can be mainly attributed to the fact that T-CZS consists of wurtzite Cd_0.5Zn_0.5S (WZ-CZS) and zinc blende Cd_0.5Zn_0.5S (ZB-CZS) with slight band structure differences, thereby facilitating rapid bulk phase and interface charge separation due to the S-scheme charge transfer routes between WZ-CZS and ZB-CZS, as well as T-CZS and NiCr₂O₄. Moreover, this system can effectively retain electrons with strong reducing ability for efficient H₂ evolution reaction (HER) and generate hot electrons through the localized surface plasmon resonance (LSPR) effect of NiCr₂O₄, which enhances the absorption of UV–Vis–NIR light energy, thereby facilitating the HER process. What's more, NaOH solution can indirectly promote the HER kinetics by enhancing the oxidative driving force of holes. Additionally, other metal chromates (MCr_<em>x</em>O_<em>y</em>), such as CoCr₂O₄, AgCrO₂, Bi₆CrO₁₂, BaCrO₄, ZnCr₂O₄, CdCr₂O₄, CuCr₂O₄ <em>etc.</em>, were employed to enhance the activity of T-CZS too. The results show that above homo-heterojunction composites can integrate waste plastic degradation and photocatalytic H₂ evolution effectively based on their S-scheme bulk phase and interface charge separation mechanisms. This work provides new insights into energy and environmental challenges.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100068"},"PeriodicalIF":10.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143550476","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":"Strategies for enhancing capacity and rate performance of two-dimensional material-based supercapacitors","authors":"Huayan Liu,&nbsp;Yifei Chen,&nbsp;Mengzhao Yang,&nbsp;Jiajun Gu","doi":"10.1016/j.actphy.2025.100063","DOIUrl":"10.1016/j.actphy.2025.100063","url":null,"abstract":"&lt;div&gt;&lt;div&gt;With the profound transformation of the global energy landscape and the rapid advancement of portable electronic devices and electric vehicle industries, there is an increasingly urgent demand for high-performance energy storage devices. Among the available energy storage technologies, supercapacitors stand out due to their rapid charge/discharge capabilities, excellent cycling stability, and high power density, enabling reliable long-term operation as well as efficient energy conversion and storage. A fundamental challenge in contemporary energy storage research remains the enhancement of supercapacitor energy density while maintaining their inherent high power density capabilities. Two-dimensional (2D) materials have emerged as promising candidates for constructing high-performance supercapacitor electrodes. Materials such as graphene, transition metal nitrides and/or carbides (MXenes), and transition metal dichalcogenides possess unique layered structures with atomic thickness, exceptional surface areas, high theoretical capacities, and remarkable mechanical flexibility. These characteristics make them particularly suitable for developing next-generation energy storage devices. However, the inherent van der Waals interactions between nanosheets frequently result in restacking phenomena, significantly impeding ion transport and consequently limiting both practical capacity and rate performance. Thus, rational materials design and precise electrode architecture engineering are imperative for overcoming these performance limitations. This review first explores modification strategies for enhancing the electrochemical performance of 2D materials. Studies have shown that diverse modification approaches, including surface functionalization, defect engineering, and heterogeneous structure construction, can effectively increase active sites, enhance conductivity, and improve pseudocapacitive characteristics. These modifications lead to substantial improvements in both areal and volumetric capacitance of electrode materials. Notably, efforts to increase supercapacitor energy density typically necessitate higher active material mass loading, which inherently results in more complex and extended ion transport pathways within the electrode structure, thereby compromising rate performance. In addressing this challenge, we evaluate conventional methodologies for establishing ion transport channels in high mass loading electrodes, including template-based approaches, external field-induced assembly techniques, and three-dimensional (3D) printing processes. However, these traditional methods typically generate pore structures at the micrometer or sub-micrometer scale, making it challenging to simultaneously achieve optimal rate performance and volumetric capacitance. To concurrently optimize areal capacitance, volumetric capacitance, and rate performance, this review emphasizes recent innovative approaches for constructing nanoscale porous architect","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100063"},"PeriodicalIF":10.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474882","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}