物理化学学报最新文献

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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
Efficient interfacial charge transfer of CeO2/Bi19Br3S27 S-scheme heterojunction for boosted photocatalytic CO2 reduction CeO2/Bi19Br3S27 S-scheme异质结高效界面电荷转移促进光催化CO2还原
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-19 DOI: 10.1016/j.actphy.2025.100065
Peng Li , Yuanying Cui , Zhongliao Wang , Graham Dawson , Chunfeng Shao , Kai Dai
{"title":"Efficient interfacial charge transfer of CeO2/Bi19Br3S27 S-scheme heterojunction for boosted photocatalytic CO2 reduction","authors":"Peng Li ,&nbsp;Yuanying Cui ,&nbsp;Zhongliao Wang ,&nbsp;Graham Dawson ,&nbsp;Chunfeng Shao ,&nbsp;Kai Dai","doi":"10.1016/j.actphy.2025.100065","DOIUrl":"10.1016/j.actphy.2025.100065","url":null,"abstract":"<div><div>Improving the separation efficiency of photogenerated charge carriers to significantly enhance the redox capability of photocatalysts remains a major challenge in the field of photocatalysis. To address this issue, this study successfully synthesized a CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> S-scheme heterojunction catalyst using a hydrothermal method, aiming to enhance the photocatalytic performance of the catalyst. The synthesis of the CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> composite not only improved the separation efficiency of photogenerated charge carriers but also endowed the catalyst with stronger redox capabilities and greater driving force, significantly boosting its photocatalytic performance. Experimental results showed that the CO production rate of the CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> composite catalyst reached 13.5 ​μmol ​g<sup>−1</sup> ​h<sup>−1</sup>, which is 5.19 times higher than that of the pure Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> catalyst and 2.81 times higher than that of the pure CeO<sub>2</sub> catalyst. This significant enhancement indicates that the CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> composite catalyst exhibited stronger catalytic performance in CO generation reactions. Furthermore, CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> catalyst achieved a CH<sub>4</sub> production rate of 4.3 ​μmol ​g<sup>−1</sup> ​h<sup>−1</sup>, which is 3.1 times higher than that of the CeO<sub>2</sub> catalyst and 2.7 times higher than that of the Bi19Br3S27 catalyst, further confirming its superior performance in CH<sub>4</sub> generation reactions. These results demonstrate that the CeO<sub>2</sub>/Bi<sub>19</sub>Br<sub>3</sub>S<sub>27</sub> composite catalyst not only shows significant improvements in CO and CH<sub>4</sub> production rates but also exhibits excellent photocatalytic performance, highlighting its potential application in the field of photocatalysis. This study provides new insights into improving the separation efficiency of photogenerated charges and offers valuable references for the future development of highly efficient photocatalytic materials. By constructing the S-scheme heterojunction structure, the recombination of photogenerated charge carriers can be effectively suppressed, thereby enhancing the efficiency of photocatalytic reactions and providing a new solution for sustainable energy utilization.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100065"},"PeriodicalIF":10.8,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520443","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
Hierarchical MoS2/Ti3C2Tx heterostructure with excellent photothermal conversion performance for solar-driven vapor generation 具有优异光热转换性能的层叠MoS2/Ti3C2Tx异质结构,用于太阳能驱动蒸汽产生
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-06 DOI: 10.1016/j.actphy.2025.100053
Kun Rong , Cuilian Wen , Jiansen Wen , Xiong Li , Qiugang Liao , Siqing Yan , Chao Xu , Xiaoliang Zhang , Baisheng Sa , Zhimei Sun
{"title":"Hierarchical MoS2/Ti3C2Tx heterostructure with excellent photothermal conversion performance for solar-driven vapor generation","authors":"Kun Rong ,&nbsp;Cuilian Wen ,&nbsp;Jiansen Wen ,&nbsp;Xiong Li ,&nbsp;Qiugang Liao ,&nbsp;Siqing Yan ,&nbsp;Chao Xu ,&nbsp;Xiaoliang Zhang ,&nbsp;Baisheng Sa ,&nbsp;Zhimei Sun","doi":"10.1016/j.actphy.2025.100053","DOIUrl":"10.1016/j.actphy.2025.100053","url":null,"abstract":"<div><div>Metallic 1T Molybdenum disulfide (1T-MoS<sub>2</sub>) exhibits enhanced full spectral light absorption and prominent electrical conductivity, making it ideal for photothermal applications in conjunction with Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> MXene. Despite the challenges in increasing the 1T-MoS<sub>2</sub> proportion within MoS<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> heterostructures and the incomplete understanding of the mechanisms governing their formation and properties, herein, a combined theoretical and experimental framework has been established, suggesting that the metallic characteristics of Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> and 1T-MoS<sub>2</sub> could significantly improve photothermal performance through strong interlayer interactions and efficient electron transport. The hierarchical MoS<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> heterostructure has been fabricated through a one-step hydrothermal synthesis method with enhanced 1T-MoS<sub>2</sub> proportion, which achieves multilayered wrinkled architecture resulting from the in-situ growth of MoS<sub>2</sub> on Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> nanosheets. Notably, a remarkable peak photoheating temperature of 107 ​°C under an 808 ​nm laser with an intensity of 0.5 ​W·cm<sup>−2</sup> is realized, demonstrating its exceptional photothermal conversion capability. By incorporated into a polyvinylidene difluoride membrane, the MoS<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> heterostructure functions as an efficient self-floating solar-driven steam generator, reaching an evaporation rate of 1.79 ​kg·m<sup>−2</sup>·h<sup>−1</sup> and an evaporation efficiency of 96.4% under one solar irradiance. This study proposes a versatile strategy for the MoS<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub><em>x</em></sub> heterostructure, offering the potential for sustainable solar-driven vapor generation technologies.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100053"},"PeriodicalIF":10.8,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463762","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 of functional nanomaterials for screen-printed photoelectrochemical biosensors 丝网印刷光电化学生物传感器功能纳米材料的研究进展
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-02-01 DOI: 10.3866/PKU.WHXB202310046
Meiqing Yang , Lu Wang , Haozi Lu , Yaocheng Yang , Song Liu
{"title":"Recent advances of functional nanomaterials for screen-printed photoelectrochemical biosensors","authors":"Meiqing Yang ,&nbsp;Lu Wang ,&nbsp;Haozi Lu ,&nbsp;Yaocheng Yang ,&nbsp;Song Liu","doi":"10.3866/PKU.WHXB202310046","DOIUrl":"10.3866/PKU.WHXB202310046","url":null,"abstract":"<div><div>Photoelectrochemical (PEC) biosensors have attracted intensive attention due to their advantages, including low background, high sensitivity, high specificity and rapid response. In recent years, the introduction of disposable screen-printed electrodes (SPE) has greatly facilitated the development of PEC biosensors, making screen-printed PEC biosensors a promising analytical tool for various applications. Photoactive nanomaterials play a crucial role in the construction of screen-printed PEC biosensors as they can be used not only as photoelectric conversion platforms but also as loading platforms for recognition elements. However, pure photoactive materials usually suffer from some drawbacks, such as inherent toxicity, wide bandgap, and high electron-hole pair recombination rate. Therefore, it is necessary to improve the photoelectric properties of these materials through various design strategies. Moreover, to obtain highly sensitive screen-printed PEC biosensors, it is usually necessary to combine the high-performance photoelectrodes with various signal amplification strategies. In view of this, we provide the first systematic summary of photoactive materials for screen-printed PEC biosensors in this paper, classifying them into four main categories: metal oxides, metal chalcogenides, carbon nanomaterials and bismuth-based nanomaterials. Meanwhile, we focus on the design strategies for photoactive materials, including morphology modulation, elemental doping, and heterostructure construction. In addition, we introduce signal amplification strategies, such as the enzyme label amplification (ELA) strategy, polymerase chain reaction (PCR) strategy, rolling circle amplification (RCA) strategy, and hybridization chain reaction (HCR) strategy, through representative screen-printed PEC immunosensors and screen-printed PEC aptasensors. Finally, we discuss the current challenges and prospects of screen-printed PEC biosensors. We hope to provide readers with a comprehensive understanding of the recent advances in screen-printed PEC biosensors and provide a feasible guidance for the future development of this field.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 2","pages":"Article 100018"},"PeriodicalIF":10.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143097009","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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