物理化学学报最新文献

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Facile synthesis of hierarchical Ti3C2/Bi12O17Br2 Schottky heterojunction with photothermal effect for solar–driven antibiotics photodegradation 具有光热效应的分层Ti3C2/Bi12O17Br2 Schottky异质结的简单合成及其在太阳能驱动抗生素光降解中的应用
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-03-08 DOI: 10.1016/j.actphy.2025.100075
Chao Liu , Huan Yu , Jiaming Li , Xi Yu , Zhuangzhi Yu , Yuxi Song , Feng Zhang , Qinfang Zhang , Zhigang Zou
{"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 Ti<sub>3</sub>C<sub>2</sub>/Bi<sub>12</sub>O<sub>17</sub>Br<sub>2</sub> (termed as TBOB) Schottky heterojunction with a hierarchical structure, in which the Bi<sub>12</sub>O<sub>17</sub>Br<sub>2</sub> component was closely deposited on the surface of Ti<sub>3</sub>C<sub>2</sub>. The TC photodegradation performance was estimated for all catalysts under simulated solar light. Compared with Bi<sub>12</sub>O<sub>17</sub>Br<sub>2</sub>, TBOB materials exhibited the superior photodegradation activity due to the synergistic effect between Ti<sub>3</sub>C<sub>2</sub> and Bi<sub>12</sub>O<sub>17</sub>Br<sub>2</sub>, which could increase light harvesting capacity derived from Ti<sub>3</sub>C<sub>2</sub> 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 •O<sub>2</sub><sup>−</sup> and e<sup>−</sup> 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 Ti<sub>3</sub>C<sub>2</sub><sub>-</sub>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}
引用次数: 0
Efficient adsorption of hardness ions by a mordenite-loaded, nitrogen-doped porous carbon nanofiber cathode in capacitive deionization 负载丝光沸石的氮掺杂多孔碳纳米纤维阴极在电容去离子过程中对硬度离子的高效吸附
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-03-06 DOI: 10.1016/j.actphy.2025.100066
Jun Huang , Pengfei Nie , Yongchao Lu , Jiayang Li , Yiwen Wang , Jianyun Liu
{"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 Ca<sup>2+</sup> and Mg<sup>2+</sup> 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 CaCl<sub>2</sub> 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 Mg<sup>2+</sup> and Ca<sup>2+</sup>, respectively. The composite electrode exhibited high selectivity for Mg<sup>2+</sup> and Ca<sup>2+</sup> over Na<sup>+</sup> 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}
引用次数: 0
Recent advances in synergistic catalytic valorization of CO2 and hydrocarbons by heterogeneous catalysis 非均相催化作用下CO2和烃类协同催化增值的研究进展
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-03-04 DOI: 10.1016/j.actphy.2025.100073
Honghong Zhang , Zhen Wei , Derek Hao , Lin Jing , Yuxi Liu , Hongxing Dai , Weiqin Wei , Jiguang Deng
{"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 (CO<sub>2</sub>). Consequently, reducing CO<sub>2</sub> emissions has become imperative, with decarbonization techniques being extensively investigated worldwide to achieve net-zero emissions. From an energy perspective, CO<sub>2</sub> 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, CO<sub>2</sub> can be reduced to CO, accompanied by the formation of H<sub>2</sub>O. CO<sub>2</sub> and hydrocarbons can also be transformed into syngas (CO and H<sub>2</sub>) <em>via</em> dry reforming. Furthermore, CO<sub>2</sub> 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 CO<sub>2</sub>, as well as the high bond energy and low polarity of hydrocarbon C–H bonds, the conversion of CO<sub>2</sub> and hydrocarbons remains a highly challenging and demanding strategic objective. This review focuses on the synergistic catalytic valorization of CO<sub>2</sub> and hydrocarbons using heterogeneous catalysts, summarizing recent advancements in coupling CO<sub>2</sub> 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 CO<sub>2</sub>-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}
引用次数: 0
Modulating the d-band center of NNU-55(Fe) for enhanced CO2 adsorption and photocatalytic activity 调节NNU-55(Fe)的d波段中心增强CO2吸附和光催化活性
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-03-01 DOI: 10.1016/j.actphy.2025.100074
Xueqi Yang , Juntao Zhao , Jiawei Ye , Desen Zhou , Tingmin Di , Jun Zhang
{"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 (CO<sub>2</sub>) has emerged as an effective technology to transform CO<sub>2</sub> 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 CO<sub>2</sub> 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, NO<sub>3</sub><sup>−</sup>-coordinated NNU-55(Fe) demonstrated superior catalytic performance compared to SO<sub>4</sub><sup>2−</sup>- and Cl<sup>−</sup>-coordinated catalysts, achieving a CO production of 124 ​μmol·g<sup>−1</sup> within 3 ​h. The stronger electron donation capacity of NO<sub>3</sub><sup>−</sup> 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 CO<sub>2</sub> 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}
引用次数: 0
Efficient capacitive desalination over NCQDs decorated FeOOH composite NCQDs修饰FeOOH复合材料的高效电容式海水淡化
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-28 DOI: 10.1016/j.actphy.2025.100072
Yihan Xue , Xue Han , Jie Zhang, Xiaoru Wen
{"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<sup>−1</sup> ​at an applied potential of 1.4 ​V, the GAC<sub>NaCl</sub> of NCQDs/FeOOH hybrid electrode reaches 56.52 ​mg ​g<sup>−1</sup>, 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}
引用次数: 0
Hollow structured photocatalysts 空心结构光催化剂
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-27 DOI: 10.1016/j.actphy.2025.100071
Fangxuan Liu , Ziyan Liu , Guowei Zhou , Tingting Gao , Wenyu Liu , Bin Sun
{"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, H<sub>2</sub> production, H<sub>2</sub>O<sub>2</sub> production, CO<sub>2</sub> reduction, and N<sub>2</sub> 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}
引用次数: 0
Waste plastics promoted photocatalytic H2 evolution over S-scheme NiCr2O4/twinned-Cd0.5Zn0.5S homo-heterojunction 废塑料在S-scheme NiCr2O4/孪晶- cd0.5 zn0.5 s均质异质结上促进光催化析氢
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-25 DOI: 10.1016/j.actphy.2025.100068
Jingzhuo Tian , Chaohong Guan , Haobin Hu , Enzhou Liu , Dongyuan Yang
{"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 H<sub>2</sub> evolution reactions. In this study, NiCr<sub>2</sub>O<sub>4</sub>/T-CZS composites were fabricated by incorporating NiCr<sub>2</sub>O<sub>4</sub> nanosheets onto the surface of twinned Cd<sub>0.5</sub>Zn<sub>0.5</sub>S (T-CZS) nanoparticles using a solvent evaporation strategy. After optimization, the 6% NiCr<sub>2</sub>O<sub>4</sub>/T-CZS exhibited an impressive hydrogen (H<sub>2</sub>) evolution rate (<em>r</em><sub>H2</sub>) of 81.4 ​mmol·h<sup>−1</sup>·g<sup>−1</sup> 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<sub>0.5</sub>Zn<sub>0.5</sub>S (WZ-CZS) and zinc blende Cd<sub>0.5</sub>Zn<sub>0.5</sub>S (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 NiCr<sub>2</sub>O<sub>4</sub>. Moreover, this system can effectively retain electrons with strong reducing ability for efficient H<sub>2</sub> evolution reaction (HER) and generate hot electrons through the localized surface plasmon resonance (LSPR) effect of NiCr<sub>2</sub>O<sub>4</sub>, 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<sub><em>x</em></sub>O<sub><em>y</em></sub>), such as CoCr<sub>2</sub>O<sub>4</sub>, AgCrO<sub>2</sub>, Bi<sub>6</sub>CrO<sub>12</sub>, BaCrO<sub>4</sub>, ZnCr<sub>2</sub>O<sub>4</sub>, CdCr<sub>2</sub>O<sub>4</sub>, CuCr<sub>2</sub>O<sub>4</sub> <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 H<sub>2</sub> 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}
引用次数: 0
Strategies for enhancing capacity and rate performance of two-dimensional material-based supercapacitors 提高二维材料基超级电容器容量和速率性能的策略
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-24 DOI: 10.1016/j.actphy.2025.100063
Huayan Liu, Yifei Chen, Mengzhao Yang, Jiajun Gu
{"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}
引用次数: 0
Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde 设计热力学稳定的贵金属单原子光催化剂,用于乙醇高效非氧化转化为高纯氢和增值乙醛
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-21 DOI: 10.1016/j.actphy.2025.100067
Yuchen Zhou , Huanmin Liu , Hongxing Li , Xinyu Song , Yonghua Tang , Peng Zhou
{"title":"Designing thermodynamically stable noble metal single-atom photocatalysts for highly efficient non-oxidative conversion of ethanol into high-purity hydrogen and value-added acetaldehyde","authors":"Yuchen Zhou ,&nbsp;Huanmin Liu ,&nbsp;Hongxing Li ,&nbsp;Xinyu Song ,&nbsp;Yonghua Tang ,&nbsp;Peng Zhou","doi":"10.1016/j.actphy.2025.100067","DOIUrl":"10.1016/j.actphy.2025.100067","url":null,"abstract":"<div><div>The intrinsic surface atomic configuration of photocatalyst without unstable or difficult-to-generate atomic vacancies often limits the formation of effective interaction between metal single atom (MSA) cocatalyst and photocatalyst, thus inhibiting the stability and performance improvement of single-atom photocatalysts. In this study, we present a convenient and cost-effective photochemical oxygen reduction reaction (ORR) mechanism to prepare thermodynamically stable noble metal single-atom cocatalysts on TiO<sub>2</sub> photocatalyst under mild condition (only consuming water and oxygen at 101,325 ​Pa and 25 ​°C). The first-principles simulation firstly theoretically reveals that the intrinsic surface configuration of TiO<sub>2</sub> can only produce unstable Pt–O<sub>2</sub> structure. However, ORR occurring on TiO<sub>2</sub> can not only provide one foreign oxygen to coordinate with Pt single atom (PtSA), but also induce one surface lattice oxygen to move toward PtSA, promoting the formation of one thermodynamically stable Pt–O<sub>4</sub> species, demonstrated by the experimental synthesis of PtSA on TiO<sub>2</sub> in oxygen atmosphere instead of inert atmosphere. The obtained stable PtSA-TiO<sub>2</sub> photocatalysts exhibit a photocatalytic rate of 320.4 ​mmol·g<sup>−1</sup>·h<sup>−1</sup> for the coproduction of high-purity hydrogen and value-added acetaldehyde with a selectivity of 99.65%, three-fold higher than the activity of Pt nanoparticles-loaded TiO<sub>2</sub>. This strategy is further extended to other noble metals, such as Rh and Pd.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100067"},"PeriodicalIF":10.8,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510948","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}
引用次数: 0
Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn2S4 photocatalyst for H2O2 production and benzylamine oxidation S-scheme ZnO/CdIn2S4光催化剂中超快电子转移的飞秒瞬态吸收光谱研究
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-19 DOI: 10.1016/j.actphy.2025.100064
Yi Yang , Xin Zhou , Miaoli Gu , Bei Cheng , Zhen Wu , Jianjun Zhang
{"title":"Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn2S4 photocatalyst for H2O2 production and benzylamine oxidation","authors":"Yi Yang ,&nbsp;Xin Zhou ,&nbsp;Miaoli Gu ,&nbsp;Bei Cheng ,&nbsp;Zhen Wu ,&nbsp;Jianjun Zhang","doi":"10.1016/j.actphy.2025.100064","DOIUrl":"10.1016/j.actphy.2025.100064","url":null,"abstract":"<div><div>Photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production is a crucial process for clean energy conversion, involving the reduction of O<sub>2</sub> through two electrons. However, this process is often hampered by the sluggish water oxidation involving the photogenerated holes. To address this challenge, we have constructed a dual-functional S-scheme ZnO/CdIn<sub>2</sub>S<sub>4</sub> heterojunction systerm coupling the H<sub>2</sub>O<sub>2</sub> generation with a value-added benzylamine (BA) oxidation reaction. In this dual-functional photocatalytic system, photogenerated electrons in CdIn<sub>2</sub>S<sub>4</sub> efficiently reduce O<sub>2</sub> to produce H<sub>2</sub>O<sub>2</sub>, while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine. Leveraging the advantages of the S-scheme heterojunction, the optimized ZnO/CdIn<sub>2</sub>S<sub>4</sub> photocatalyst displays an enhanced H<sub>2</sub>O<sub>2</sub> production rate (386 ​μmol·L<sup>−1</sup>·h<sup>−1</sup>) and BA oxidation fraction (81 ​%) than pure ZnO or CdIn<sub>2</sub>S<sub>4</sub>. Femtosecond transient absorption (fs-TA) spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band (CB) to the CdIn<sub>2</sub>S<sub>4</sub> valence band (VB) upon photoexcitation of the ZnO/CdIn<sub>2</sub>S<sub>4</sub> composite. Besides, timely depletion of VB holes in ZnO and CB electrons in CdIn<sub>2</sub>S<sub>4</sub> can accelerate the interfacial electron transfer in the ZnO/CdIn<sub>2</sub>S<sub>4</sub> S-scheme heterojunction. The innovative design of the ZnO/CdIn<sub>2</sub>S<sub>4</sub> S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100064"},"PeriodicalIF":10.8,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143550475","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}
引用次数: 0
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