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Bandgap and adsorption engineering of carbon dots/TiO2 S-scheme heterojunctions for enhanced photocatalytic CO2 methanation 碳点/TiO2 s型异质结光催化CO2甲烷化的带隙与吸附工程
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-10 DOI: 10.1016/j.actphy.2025.100116
Wenlong Wang , Wentao Hao , Lang He , Jia Qiao , Ning Li , Chaoqiu Chen , Yong Qin
{"title":"Bandgap and adsorption engineering of carbon dots/TiO2 S-scheme heterojunctions for enhanced photocatalytic CO2 methanation","authors":"Wenlong Wang ,&nbsp;Wentao Hao ,&nbsp;Lang He ,&nbsp;Jia Qiao ,&nbsp;Ning Li ,&nbsp;Chaoqiu Chen ,&nbsp;Yong Qin","doi":"10.1016/j.actphy.2025.100116","DOIUrl":"10.1016/j.actphy.2025.100116","url":null,"abstract":"<div><div>S-scheme heterojunctions have garnered significant interest in photocatalytic CO<sub>2</sub> conversion to valuable products (e.g., CH<sub>4</sub>) due to their enhanced charge separation and robust redox capabilities. Carbon dots (CDs), with their tunable band structures and light absorption ranges, show particular promise in constructing efficient S-scheme photocatalytic systems. Nevertheless, the critical roles of CDs' band alignment and surface adsorption properties in determining heterojunction configuration, charge carrier kinetics, and ultimately CO<sub>2</sub> activation/product selectivity distribution remain insufficiently explored. Herein, we construct four CDs/TiO<sub>2</sub> heterojunctions using CDs synthesized from varied carbon sources, in which S-scheme heterojunctions were successfully constructed based on cost-effective coal pitch (C-GQDs, 1.75 nm), glucose (G-CQDs, 1.84 nm), and acetone (CQDs-X, 1.82 nm) carbon sources, whereas Type-I heterojunctions were formed by carbon black based CDs (GQDs-A, 1.92 nm). Systematic investigations reveal that both the band structure and adsorption characteristics of CDs play important roles in the charge transfer path and separation efficiency, CO<sub>2</sub> adsorption and activation capacities, and product selectivity in photocatalytic CO<sub>2</sub> reduction. Remarkably, the introduction of CDs significantly broadens the photo-response range compared to fresh TiO<sub>2</sub>, and in particular, the C-GQDs/TiO<sub>2</sub> exhibits exceptional performance with a CH<sub>4</sub> production rate of 32.7 μmol·g<sup>−1</sup>·h<sup>−1</sup>, surpassing TiO<sub>2</sub> by 6.3-fold and outperforming GQDs-A/TiO<sub>2</sub>, CQDs-X/TiO<sub>2</sub>, and G-CQDs/TiO<sub>2</sub> by factors of 3.8, 2.7, and 2.3, respectively. This heterojunction simultaneously achieves 72.6 % CH<sub>4</sub> selectivity and 98.1 % hydrocarbons selectivity (encompassing CH<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>4</sub>, and C<sub>3</sub>H<sub>8</sub>). In contrast, composites incorporating GQDs-A, CQDs-X, or G-CQDs exhibit substantially diminished CH<sub>4</sub> selectivity (&lt;40.0 %). The high CH<sub>4</sub> production rate and selectivity of C-GQDs/TiO<sub>2</sub> can be attributed to its unique S-scheme heterojunction structure, higher reduction potential, and well-matched CO<sub>2</sub> and H<sub>2</sub>O adsorption and activation capabilities. This study provides unique insights into the efficient photoreduction of CO<sub>2</sub> to CH<sub>4</sub> driven by the S-scheme heterojunction electron transfer pathway in CDs/TiO<sub>2</sub> photocatalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100116"},"PeriodicalIF":10.8,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144279475","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
Design of noble metal catalysts and reactors for the electrosynthesis of hydrogen peroxide 电合成过氧化氢贵金属催化剂及反应器设计
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-09 DOI: 10.1016/j.actphy.2025.100112
Kangjuan Cheng , Chunxiao Liu , Youpeng Wang , Qiu Jiang , Tingting Zheng , Xu Li , Chuan Xia
{"title":"Design of noble metal catalysts and reactors for the electrosynthesis of hydrogen peroxide","authors":"Kangjuan Cheng ,&nbsp;Chunxiao Liu ,&nbsp;Youpeng Wang ,&nbsp;Qiu Jiang ,&nbsp;Tingting Zheng ,&nbsp;Xu Li ,&nbsp;Chuan Xia","doi":"10.1016/j.actphy.2025.100112","DOIUrl":"10.1016/j.actphy.2025.100112","url":null,"abstract":"<div><div>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is an eco-friendly oxidant vital for chemical synthesis, water treatment, and disinfection. However, the conventional anthraquinone production method is energy-intensive, generates waste, and requires hazardous transport of concentrated H<sub>2</sub>O<sub>2</sub>. Electrochemical H<sub>2</sub>O<sub>2</sub> synthesis <em>via</em> a two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) has emerged as a sustainable alternative, enabling renewable-powered, decentralized production under mild conditions. Noble metal catalysts outperform alternatives in acidic media, demonstrating superior stability and selectivity. Despite these advantages, several technical challenges must be addressed to enable industrial-scale implementation. The primary challenge lies in optimizing catalyst performance to achieve both high activity and selectivity for the 2e<sup>−</sup> pathway while suppressing the competing 4e<sup>−</sup> pathway that produces water. This requires precise control of the catalyst’s electronic and surface structures. Additionally, the development of cost-effective reactor systems that can maintain high performance at scale presents another significant hurdle. Current research focuses on improving mass transport, current distribution, and product separation while minimizing energy consumption.</div><div>This review provides a comprehensive examination of recent progress in the 2e<sup>−</sup> ORR, with particular emphasis on noble metal catalysts and reactor engineering. We begin by discussing the fundamental principles and reaction mechanisms underlying the 2e<sup>−</sup> ORR, emphasizing the role of material design in optimizing catalytic performance. Noble-metal catalysts are categorized into four types, namely, pure metals, alloys, compounds, and single-atom catalysts, with a critical evaluation of their performance based on theoretical and experimental findings. The second part of the review focuses on reactor design strategies for practical applications. We evaluate reactor designs, including H-cells, flow cells, membrane electrode assemblies, and solid-state electrolyte cells, with a focus on their mass transport and scalability characteristics. Particular emphasis is placed on gas diffusion electrodes for improved oxygen accessibility and innovative <em>in situ</em> product separation methods. Finally, we discuss the remaining challenges and future directions, including the need for reduced noble metal loading, improved long-term stability, and system integration with renewable energy sources. The review concludes by highlighting the tremendous potential of electrochemical H<sub>2</sub>O<sub>2</sub> production to transform industrial oxidation processes while contributing to the development of sustainable chemical manufacturing.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100112"},"PeriodicalIF":10.8,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144364490","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
Rationally assembling different surface functionalized carbon dots for enhanced near-infrared tumor photothermal therapy 合理组装不同表面功能化碳点用于增强近红外肿瘤光热治疗
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-04 DOI: 10.1016/j.actphy.2025.100109
Xue Wu , Yupeng Liu , Bingzhe Wang , Lingyun Li , Zhenjian Li , Qingcheng Wang , Quansheng Cheng , Guichuan Xing , Songnan Qu
{"title":"Rationally assembling different surface functionalized carbon dots for enhanced near-infrared tumor photothermal therapy","authors":"Xue Wu ,&nbsp;Yupeng Liu ,&nbsp;Bingzhe Wang ,&nbsp;Lingyun Li ,&nbsp;Zhenjian Li ,&nbsp;Qingcheng Wang ,&nbsp;Quansheng Cheng ,&nbsp;Guichuan Xing ,&nbsp;Songnan Qu","doi":"10.1016/j.actphy.2025.100109","DOIUrl":"10.1016/j.actphy.2025.100109","url":null,"abstract":"<div><div>Carbon dots (CDs) have emerged as promising photothermal agents for near-infrared (NIR)-mediated tumor therapy due to their excellent biocompatibility and tunable optical properties. However, it is still unclear how to precisely control their assembly behavior to enhance NIR absorption and photothermal conversion efficiency. In this work, we present a hyper-assembled electron donor/acceptor CDs complex (S-d/a-CDs), constructed by integrating electron-donating CDs (d-CDs) with electron-withdrawing CDs (a-CDs). This configuration significantly enhances the NIR absorption capacity of S-d/a-CDs. Under 740 nm laser irradiation, S-d/a-CDs achieve a remarkable photothermal conversion efficiency (PTCE) of 65.8 %. S-d/a-CDs exhibit negligible cytotoxicity and effective tumor accumulation capacity through intravenous administration, enabling complete tumor elimination after NIR laser irradiation. To our knowledge, this study is the first to exploit synergistic assembles of two types of CDs for photo-physical property engineering, establishing a groundbreaking paradigm for the development of advanced NIR-triggered photothermal materials.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100109"},"PeriodicalIF":10.8,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144270331","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
The role of hydroxyl species in the alkaline hydrogen evolution reaction over transition metal surfaces 羟基在过渡金属表面碱性析氢反应中的作用
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-03 DOI: 10.1016/j.actphy.2025.100111
Ruizhi Duan , Xiaomei Wang , Panwang Zhou , Yang Liu , Can Li
{"title":"The role of hydroxyl species in the alkaline hydrogen evolution reaction over transition metal surfaces","authors":"Ruizhi Duan ,&nbsp;Xiaomei Wang ,&nbsp;Panwang Zhou ,&nbsp;Yang Liu ,&nbsp;Can Li","doi":"10.1016/j.actphy.2025.100111","DOIUrl":"10.1016/j.actphy.2025.100111","url":null,"abstract":"<div><div>Understanding the activity-determining factors governing the alkaline hydrogen evolution reaction (HER) on transition metal catalysts is indispensable for water electrolysis with renewable energy. However, it remains a critical challenge. Although hydroxyl adsorption has been proposed to influence alkaline HER performance, its exact mechanistic role and quantitative correlations remain elusive. Here, we systematically investigate the alkaline HER on ten transition metal surfaces using density functional theory (DFT), revealing that hydroxyl adsorption critically modulates both pathway selection and reaction energy barrier. However, hydroxyl adsorption energy alone cannot fully explain the anomalous activity of certain catalysts, especially Pt. To address this, we introduce a multi-parameter coupled descriptor (ECS) that integrates electron occupancy (E), adsorption configuration (C), and surface crystallographic (S), enabling a qualitative evaluation of catalytic activity. This descriptor successfully elucidates previously unexplained activity trends and demonstrates a good correlation with over 10 experimental datasets, including those involving single-atom alloy (SAA) catalysts, indicating its robustness beyond pure metals. Our findings provide a descriptor based on the key species of hydroxyl for rational catalyst design and screening, and offer a fundamental framework for advancing the development of high-performance alkaline HER catalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100111"},"PeriodicalIF":10.8,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144270419","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
Enhanced photocatalytic synthesis of H2O2 by triplet electron transfer at g-C3N4@BN van der Waals heterojunction interface 在g-C3N4@BN范德华异质结界面上通过三重态电子转移增强H2O2的光催化合成
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-28 DOI: 10.1016/j.actphy.2025.100107
Qi Wu, Changhua Wang, Yingying Li, Xintong Zhang
{"title":"Enhanced photocatalytic synthesis of H2O2 by triplet electron transfer at g-C3N4@BN van der Waals heterojunction interface","authors":"Qi Wu,&nbsp;Changhua Wang,&nbsp;Yingying Li,&nbsp;Xintong Zhang","doi":"10.1016/j.actphy.2025.100107","DOIUrl":"10.1016/j.actphy.2025.100107","url":null,"abstract":"<div><div>The van der Waals heterojunctions demonstrate exceptional advantages due to their outstanding charge separation capabilities and remarkable flexibility in tuning electronic properties. This study explores the potential application of the 2D/2D g-C<sub>3</sub>N<sub>4</sub>@BN van der Waals heterojunction in the photocatalytic synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). Based on this heterojunction, we investigated the energy transfer process between triplet excitons and singlet oxygen, emphasizing the importance of catalyst structure for charge separation and the stable generation of triplet electrons. By constructing a charge transfer pathway, the built-in electric field within the heterojunction effectively drives the directional migration of charge carriers, significantly extending their lifetime. We employed two modification strategies to regulate the excited state electronic properties of the catalyst, including adjusting the interlayer arrangement to enhance charge transport capability and halogen modification to improve the light responsiveness of materials. Experimental validation indicates that the representative chlorinated-CN@BN effectively suppresses exciton recombination compared to CN, extending the lifetime of excited-state carriers by 3.52 times. Furthermore, the photocatalytic yield of H<sub>2</sub>O<sub>2</sub> is improved by 2.73 times. This study provides a theoretical basis for developing novel photocatalysts and inspires the design of catalysts for direct synthesis of H<sub>2</sub>O<sub>2</sub> from oxygen.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100107"},"PeriodicalIF":10.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144243514","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
Valorization strategies for electrodegradation of nitrogenous wastes in sewage 污水中含氮废物电降解的评价策略
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-28 DOI: 10.1016/j.actphy.2025.100108
Minglei Sun, Zhong-Yong Yuan
{"title":"Valorization strategies for electrodegradation of nitrogenous wastes in sewage","authors":"Minglei Sun,&nbsp;Zhong-Yong Yuan","doi":"10.1016/j.actphy.2025.100108","DOIUrl":"10.1016/j.actphy.2025.100108","url":null,"abstract":"<div><div>The interconversion of N<sub>2</sub> and N-containing compounds is central to the natural nitrogen cycle, one of the most important global biogeochemical cycles, which plays a crucial role in sustaining life across all organisms. Nitrogen pollution in surface water bodies, caused by the indiscriminate discharge of industrial and domestic wastewater, has become a global environmental concern. The excessive accumulation of nitrogenous wastes poses a serious threat to human health and disrupts the natural nitrogen cycle. Traditional water purification methods, such as chemical redox processes, physical adsorption, and biological treatments, often face limitations, including high energy consumption, low efficiency, large space requirements, prolonged treatment times, sludge generation, and high operating costs. Emerging electrochemical degradation techniques offer promising solutions for efficiently degrading nitrogenous wastes. These electrochemical technologies demonstrate advantages in cost-effectiveness, environmental friendliness, high efficiency, and broad applicability, while also presenting opportunities to generate added value during the electrodegradation processes. Nitrogen-containing wastes in wastewater can be classified into electrophiles (e.g., nitrate and nitrite) and nucleophiles (e.g., ammonia nitrogen, hydrazine, and urea) according to their redox properties. Based on the different properties of nitrogenous wastes, coupling corresponding electrochemical degradation reactions with tailored electrochemical energy storage and conversion devices provides opportunities for additional energy and value generation. Herein, advanced insights into valorization strategies during the electrodegradation processes of representative nitrogenous wastes in sewage are subtly provided, where the approaches for enhanced value output efficiency are highlighted, including (i) coupling the electroreduction of electrophilic pollutants with Zn-electrophile batteries to achieve energy output and simultaneous chemical production, (ii) coupling electro-oxidation of nucleophilic pollutants with hybrid direct fuel cells to realize energy output, (iii) applying hybrid water electrolysis systems assisted with nucleophilic wastes for energy-saving and clean H<sub>2</sub> production, (iv) assembling Zn-nucleophile batteries for energy storage and hydrogen production, and (v) producing valuable chemicals via C-N coupling processes. The cell design, coupled with selection criteria and optimizing strategies of advanced electrodes and cell configuration, is highlighted. Finally, an in-depth analysis of current challenges and future prospects is provided to deepen the understanding of advanced electrochemical cells and bridge the gap between experimental trials and practical applications with respect to mechanism investigation, electrode design and evaluation, and cell design.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100108"},"PeriodicalIF":10.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144205004","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
Sulfur-doped carbon dots: a novel bifunctional electrolyte additive for high-performance aqueous zinc-ion batteries 硫掺杂碳点:高性能水锌离子电池的新型双功能电解质添加剂
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-23 DOI: 10.1016/j.actphy.2025.100106
Qianli Ma, Tianbing Song, Tianle He, Xirong Zhang, Huanming Xiong
{"title":"Sulfur-doped carbon dots: a novel bifunctional electrolyte additive for high-performance aqueous zinc-ion batteries","authors":"Qianli Ma,&nbsp;Tianbing Song,&nbsp;Tianle He,&nbsp;Xirong Zhang,&nbsp;Huanming Xiong","doi":"10.1016/j.actphy.2025.100106","DOIUrl":"10.1016/j.actphy.2025.100106","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Aqueous zinc-ion batteries (AZIBs) have gained considerable attention as next-generation energy storage devices due to their inherent safety, environmental friendliness, and cost-effectiveness. However, their widespread application is severely hampered by uncontrolled zinc dendrite growth and detrimental side reactions (e.g., hydrogen evolution, corrosion, and passivation), which lead to reduced Coulombic efficiency and shortened cycle life. Current strategies to improve zinc anode stability mainly focus on artificial interface coatings, electrode structure design, and electrolyte optimization. Among these approaches, electrolyte additive engineering is considered the most promising for practical applications due to its simplicity, low cost, and excellent scalability. Nevertheless, conventional additives (including metal ions, polymers, and surfactants) typically address only single issues (either dendrite suppression or side reaction mitigation), failing to achieve synergistic effects. In this work, we developed sulfur-doped carbon dots (S-CDs) as a novel bifunctional electrolyte additive to significantly enhance AZIB performance. The carbon dot additive was synthesized via a facile calcination method, followed by systematic characterization of its structure and properties using methods such as fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and density functional theory (DFT) calculations. Comprehensive electrochemical evaluations were conducted to investigate the influence of S-CDs on zinc deposition behavior and overall battery performance. Experimental results demonstrate the successful synthesis of sulfur-doped carbon dots with abundant surface functional groups. During battery operation, the strong binding affinity between S-CDs and Zn&lt;sup&gt;2+&lt;/sup&gt; effectively reconstructs the Zn&lt;sup&gt;2+&lt;/sup&gt; solvation shell, reducing water molecule content and thereby minimizing electrode corrosion and side reactions caused by interfacial active water molecules. Moreover, the S-CDs induce the formation of stable (002) crystallographic planes that continuously renew during plating/stripping cycles, with particularly pronounced effects under high current densities, significantly enhancing the structural stability of the electrode. The synergistic effect of these dual functions leads to remarkable improvement in zinc electrode performance and ultimately endows the battery with ultra-long cycling life. Benefiting from the positive effects of the carbon dot additive, the symmetric cell achieves exceptional stability for nearly 2000 h at a high current density of 10 mA cm&lt;sup&gt;−2&lt;/sup&gt;, far outperforming conventional electrolyte systems. Furthermore, both Zn||NH&lt;sub&gt;4&lt;/sub&gt;V&lt;sub&gt;4&lt;/sub&gt;O&lt;sub&gt;10&lt;/sub&gt; and Zn||MnO&lt;sub&gt;2&lt;/sub&gt; full cells exhibit superior electrochemical performance and significantly enhanced cycling stability, confirming the excellent compatibility of the carbon dot additiv","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100106"},"PeriodicalIF":10.8,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144230290","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
S-scheme heterojunction g-C3N4/Bi2WO6 highly efficient degradation of levofloxacin: Performance, mechanism and degradation pathway S-scheme异质结g-C3N4/Bi2WO6高效降解左氧氟沙星:性能、机理及降解途径
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-21 DOI: 10.1016/j.actphy.2025.100105
Menglan Wei, Xiaoxia Ou, Yimeng Wang, Mengyuan Zhang, Fei Teng, Kaixuan Wang
{"title":"S-scheme heterojunction g-C3N4/Bi2WO6 highly efficient degradation of levofloxacin: Performance, mechanism and degradation pathway","authors":"Menglan Wei,&nbsp;Xiaoxia Ou,&nbsp;Yimeng Wang,&nbsp;Mengyuan Zhang,&nbsp;Fei Teng,&nbsp;Kaixuan Wang","doi":"10.1016/j.actphy.2025.100105","DOIUrl":"10.1016/j.actphy.2025.100105","url":null,"abstract":"<div><div>g-C<sub>3</sub>N<sub>4</sub>/Bi<sub>2</sub>WO<sub>6</sub> (MCN/BWO) heterojunction photocatalysts were synthesized <em>via</em> a one-step hydrothermal method for the degradation of levofloxacin (LEV). Under simulated sunlight irradiation, the degradation rate of LEV by MCN/BWO with a molar ratio of 1 : 1 reached 98.14 %, which was attributed to the formation of an S-scheme heterojunction between MCN and BWO. <em>In situ</em> XPS analysis and surface work function measurements confirmed that the electron transfer pathway follows the S-scheme heterojunction mechanism. The internal electric field (IEF) generated by the S-scheme heterojunction in the MCN/BWO system facilitates direct transfer of photogenerated electrons (e<sup>−</sup>) from the conduction band (CB) of BWO to the valence band (VB) of MCN. This process enables efficient separation of photogenerated electron-hole (e<sup>−</sup>-h<sup>+</sup>) pairs, with h<sup>+</sup> accumulating on the VB of BWO and e<sup>−</sup> accumulating on the CB of MCN. Free radical trapping experiments demonstrated that the superoxide free radical (·O<sub>2</sub><sup>−</sup>) and h<sup>+</sup> were the primary active species. Besides exhibiting superior photocatalytic performance, the catalyst maintained excellent stability over three consecutive cycles. To elucidate the degradation mechanism, liquid chromatography-mass spectrometry (LC-MS) and quantitative structure-activity relationship (QSAR) analysis were employed to identify degradation pathways, intermediates, and potential toxicity. This study provides a theoretical foundation for wastewater treatment applications.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100105"},"PeriodicalIF":10.8,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144185151","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
Improving hydrogen peroxide photosynthesis over inorganic/organic S-scheme photocatalyst with LiFePO4 LiFePO4改善过氧化氢在无机/有机s型光催化剂上的光合作用
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-20 DOI: 10.1016/j.actphy.2025.100104
Jingping Li, Suding Yan, Jiaxi Wu, Qiang Cheng, Kai Wang
{"title":"Improving hydrogen peroxide photosynthesis over inorganic/organic S-scheme photocatalyst with LiFePO4","authors":"Jingping Li,&nbsp;Suding Yan,&nbsp;Jiaxi Wu,&nbsp;Qiang Cheng,&nbsp;Kai Wang","doi":"10.1016/j.actphy.2025.100104","DOIUrl":"10.1016/j.actphy.2025.100104","url":null,"abstract":"<div><div>With the rapid development of new energy industries, the utilization of waste batteries has attracted the attention of researchers. Developing a hydrogen peroxide photosynthesis system with battery recycling materials as photocatalysts presents a significant challenge. In this study, an ultrasonic self-assembly technique is employed to integrate LiFePO<sub>4</sub> (LFPO) nanoparticles, derived from spent batteries, with g-C<sub>3</sub>N<sub>4</sub> (CN) nanosheets, thereby creating an inorganic/organic S-scheme photocatalyst for the production of H<sub>2</sub>O<sub>2</sub>. <em>In situ</em> analyses using X-ray photoelectron spectroscopy (XPS) and Kelvin probe force microscopy (KPFM) demonstrate that the interaction between LFPO and CN facilitates the development of an internal electric field (IEF), which in turn gives rise to a distinctive S-scheme charge transfer mechanism. Combining electron spin resonance spectroscopy, radical-trapping experiments, and <em>in situ</em> DRIFTS spectra, three pathways for H<sub>2</sub>O<sub>2</sub> formation are identified. Benefited from enhanced carrier separation, strong redox power, and multichannel H<sub>2</sub>O<sub>2</sub> formation, the optimal composite shows an impressive H<sub>2</sub>O<sub>2</sub>-production rate of 3.22 mol g<sup>−1</sup> h<sup>−1</sup> under simulated solar irradiation. This research provides a potential method to investigate a sustainable H<sub>2</sub>O<sub>2</sub> photosynthesis pathway by designing S-scheme heterojunctions from spent battery materials.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100104"},"PeriodicalIF":10.8,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144230288","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
Decoding SEI chemistry at the lithium-metal potential 解码锂金属电位下的SEI化学
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-05-09 DOI: 10.1016/j.actphy.2025.100101
Changsheng An, Tao Liu
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