物理化学学报最新文献

{"title":"Enhancing photocatalytic H2O2 production via dual optimization of charge separation and O2 adsorption in Au-decorated S-vacancy-rich CdIn2S4","authors":"Yanyan Zhao ,&nbsp;Zhen Wu ,&nbsp;Yong Zhang ,&nbsp;Bicheng Zhu ,&nbsp;Jianjun Zhang","doi":"10.1016/j.actphy.2025.100142","DOIUrl":"10.1016/j.actphy.2025.100142","url":null,"abstract":"<div><div>Photocatalytic oxygen reduction reaction (ORR) offers a mild and cost-effective approach for hydrogen peroxide (H₂O₂) production. However, its practical application is significantly hindered by rapid charge carrier recombination and insufficient O₂ adsorption capacity in photocatalysts. To address these limitations, we developed a strategy involving the creation of S-vacancy-rich CdIn₂S₄ (S_v–CIS) to facilitate charge separation and subsequent deposition of Au nanoparticles on its surface (Au–S_v–CIS) to strengthen O₂ adsorption. The results suggest that the optimized Au–S_v–CIS achieves a significantly increased H₂O₂ production yield of 2542 μmol⁻¹ h g⁻¹ in 10 %-ethanol/water solution, which is about 12.8 and 1.7 times higher than that of pure CIS and S_v–CIS. Comprehensive characterizations including photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent response, electrochemical impedance spectra, and femtosecond transient absorption spectroscopy confirm the improved charge dynamics of Au–S_v–CIS. In addition, temperature-programmed desorption of O₂ combined with density functional theory calculations conclusively demonstrates the superior O₂ adsorption capacity of Au–S_v–CIS. This work provides a design strategy for efficient solar–to–chemical energy conversion through cooperative photocatalyst engineering.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100142"},"PeriodicalIF":13.5,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144771838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution","authors":"Ruiyun Liu ,&nbsp;Ping Wang ,&nbsp;Xuefei Wang ,&nbsp;Feng Chen ,&nbsp;Huogen Yu","doi":"10.1016/j.actphy.2025.100137","DOIUrl":"10.1016/j.actphy.2025.100137","url":null,"abstract":"<div><div>Mo₂C MXene (Mo₂CT_x) exhibits exceptional hydrogen-evolution potential in photocatalysis due to the Pt-like electronic structure of surface Mo active sites. However, the Mo sites in Mo₂CT_x usually show excessively strong H-adsorption during HER, significantly limiting the intrinsic catalytic activity of Mo₂CT_x. To weaken the H-adsorption capacity of Mo active sites, a strategy of modulating <em>d</em>-orbital electron is implemented <em>via in-situ</em> constructing MoC-Mo₂C MXene heterojunction by a work-function-induced effect. The MoC-Mo₂CT_x heterojunction was synthesized by <em>in</em><em>-</em><em>situ</em> conversion of Mo₂C MXene into MoC <em>via</em> a Co-induced molten salt method, followed by coupling with TiO₂ through a simple ultrasonication-assisted method to prepare the MoC-Mo₂CT_x/TiO₂ photocatalyst. Photocatalytic tests showed that the optimal MoC-Mo₂CT_x/TiO₂ sample achieves an excellent hydrogen production rate of 1886 μmol h⁻¹ g⁻¹, representing 117.9 and 3.9 fold enhancements over TiO₂ and Mo₂CF_x/TiO₂ (Mo₂CF_x prepared by a conventional etchant NH₄F + HCl), respectively. Experimental and theoretical calculations substantiate that the work-function gradient between MoC and Mo₂C MXene induces electron transfer from MoC to Mo₂C MXene to weaken the H-adsorption of Mo active sites in Mo₂CT_x cocatalyst, thereby enhancing its HER activity. This research provides a new strategy of <em>in-situ</em> constructing Mo₂C MXene-based heterojunction for adjusting the H-adsorption capacity of Mo active sites.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100137"},"PeriodicalIF":13.5,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144738530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Carbon Doping and Cu Loading on Boron Nitride via Microwave Synthesis for Enhanced Atmospheric CO2 Photoreduction","authors":"Haotong Ma ,&nbsp;Mingyu Heng ,&nbsp;Yang Xu ,&nbsp;Wei Bi ,&nbsp;Yingchun Miao ,&nbsp;Shuning Xiao","doi":"10.1016/j.actphy.2025.100132","DOIUrl":"10.1016/j.actphy.2025.100132","url":null,"abstract":"<div><div>Photocatalytic CO₂ reduction under atmospheric concentrations remains highly challenging yet critical for practical carbon-neutral applications. In this study, a Cu-loaded, carbon-doped boron nitride (Cu/BCN) photocatalyst was synthesized by a microwave-assisted molten salt method. This approach enables simultaneous carbon incorporation into the BN lattice and selective deposition of Cu nanoparticles, forming an efficient heterostructure. The synergy between C doping and Cu loading modulates the band structure, enhances visible-light absorption, promotes charge separation, and improves CO₂ adsorption. The optimized Cu/BCN photocatalyst achieved a CO production rate of 30.62 μmol g⁻¹ h⁻¹ with 95.8 % selectivity under ambient CO₂ conditions. Combined experimental and DFT analyses confirm that the Cu/BCN interface facilitates charge transfer and lowers the energy barrier for ∗COOH formation. This work demonstrates a promising route toward efficient CO₂ utilization directly from air, offering a scalable strategy for atmospheric carbon conversion.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100132"},"PeriodicalIF":10.8,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694549","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation","authors":"Shumin Zhang ,&nbsp;Yaqi Wang ,&nbsp;Zelin Wang ,&nbsp;Libo Wang ,&nbsp;Changsheng An ,&nbsp;Difa Xu","doi":"10.1016/j.actphy.2025.100136","DOIUrl":"10.1016/j.actphy.2025.100136","url":null,"abstract":"<div><div>Coupling H₂O₂ production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn₂S₄/g-C₃N₄ (ZIS_{1−<em>x</em>}/UCN) S-scheme heterojunction photocatalyst was constructed by <em>in situ</em> growing ZIS_{1−<em>x</em>} nanosheets on porous ultrathin UCN. The designed ZIS_{1−<em>x</em>}/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS_{1−<em>x</em>}/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H₂O₂ production rate of 2902.2 μmol g⁻¹ h⁻¹ and 91.3 % tetracycline (50 mg L⁻¹) degradation efficiency. This H₂O₂ performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 μmol g⁻¹ h⁻¹). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), <em>in situ</em> irradiation X-ray photoelectron spectroscopy (ISI-XPS), and <em>in situ</em> X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100136"},"PeriodicalIF":13.5,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Membrane-anchoring nanoengineered carbon dots as a pyroptosis amplifier for robust tumor photodynamic-immunotherapy","authors":"Tiejin Chen ,&nbsp;Xiaokuang Xue ,&nbsp;Jian Li ,&nbsp;Minhui Cui ,&nbsp;Yongliang Hao ,&nbsp;Mianqi Xue ,&nbsp;Haihua Xiao ,&nbsp;Jiechao Ge ,&nbsp;Pengfei Wang","doi":"10.1016/j.actphy.2025.100113","DOIUrl":"10.1016/j.actphy.2025.100113","url":null,"abstract":"<div><div>Photodynamic therapy (PDT), as a FDA-approved therapeutic modality, has witnessed substantial advancements in the field of oncology. However, the conventional PDT may suffer poor prognosis due to the transient nature of ROS, excessive phototoxicity, and inducing traditional apoptosis. In this study, a nanoengineered carbon dots (NCDs) was constructed through electrostatic interaction between a positive-charged carbon dots photosensitizers (PCDs) and new indocyanine green (IR820). The introduction of IR820 at variable ratios could change the surface charge and amphiphilic characteristics of NCDs, thereby modulating the membrane-anchoring capability of NCDs. Besides, the J-aggregation of IR820 led to a redshift of fluorescence from NIR-I to NIR-II region, thereby achieving NIR-II imaging. Furthermore, the photoactivity of PCDs was quenched by IR820, with subsequent restoration of PDT occurring contingent on the photobleaching of IR820 <em>via</em> 750 nm laser irradiation. Finally, both <em>in vitro</em> and <em>in vivo</em> studies had demonstrated that under a cascaded laser irradiation, the membrane-targeted NCDs could effectively induce cell pyroptosis, thereby eradicating tumors with minimal side effects while simultaneously activating immune responses to inhibit tumor lung metastasis. This study developed a multifunctional nanoengieering carbon dots and offered novel perspectives for tumor photodynamic-immunotherapy with enhanced controllability, improved efficacy and high security.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100113"},"PeriodicalIF":10.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144307587","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ga-doped Cu/γ-Al2O3 bifunctional interface sites promote the direct hydrogenation of CO2 to DME","authors":"Xiaorui Chen ,&nbsp;Xuan Luo ,&nbsp;Tongming Su ,&nbsp;Xinling Xie ,&nbsp;Liuyun Chen ,&nbsp;Yuejing Bin ,&nbsp;Zuzeng Qin ,&nbsp;Hongbing Ji","doi":"10.1016/j.actphy.2025.100126","DOIUrl":"10.1016/j.actphy.2025.100126","url":null,"abstract":"<div><div>The reaction of CO₂ catalytic hydrogenation to dimethyl ether (DME) usually relies on a Cu-containing metal oxide/molecular sieve system; however, the migration of copper species to molecular sieves is unavoidable during the reaction, leading to the loss of Cu⁰ sites and acidic sites. In this work, a Cu/<em>x</em>%Ga-γ-Al₂O₃ bifunctional catalyst was synthesized <em>via</em> the coprecipitation method. Ga was doped into the γ-Al₂O₃ lattice at a low concentration, forming interfacial active sites with surface Cu⁰ species to achieve the hydrogenation of CO₂ to DME. Experimental studies combined with DFT calculations demonstrate that the catalyst remains stable for 180 h and that the Ga-doped Cu/γ-Al₂O₃ interface sites exhibit catalytic effects on CO₂ hydrogenation to CH₃OH and CH₃OH dehydration to produce DME. The doping of Ga increases the specific surface area of the catalyst, reduces the particle size of Cu⁰, enhances the number of acidic and basic sites on the catalyst, and promotes the adsorption of H₂ and CO₂. In addition, a new reaction pathway for DME synthesis was proposed. This work removes the dehydrated component of a traditional Cu-based bifunctional catalyst, enabling two reactions to occur at the same active sites, thus providing a new strategy for the design of novel dimethyl ether synthesis bifunctional catalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100126"},"PeriodicalIF":10.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Applications of generative artificial intelligence in battery research: Current status and prospects","authors":"Hengrui Zhang,&nbsp;Xijun Xu,&nbsp;Xun-Lu Li,&nbsp;Xiangwen Gao","doi":"10.1016/j.actphy.2025.100115","DOIUrl":"10.1016/j.actphy.2025.100115","url":null,"abstract":"<div><div>With the rapid development of renewable energy and electric vehicles, batteries, as the core components of electrochemical energy storage systems, have become a global focus in both scientific research and industrial sectors due to their critical impact on system efficiency and safety. However, the complex multi-physics reactions within batteries make traditional mathematical models inadequate for comprehensively revealing their mechanisms. The key to solving this problem lies in introducing data-driven approaches, which have laid a solid foundation for battery research and development through extensive accumulation of experimental data and extraction of effective information. Generative artificial intelligence (GAI), leveraging its powerful latent pattern learning and data generation capabilities, has already found widespread applications in protein structure prediction, material inverse design, and data augmentation, demonstrating its broad application prospects. Applying GAI to battery research workflows with diverse battery data resources could provide innovative solutions to challenges in battery research. In this perspective, we introduce the core principles and latest advancements of generative models (GMs), including Generative Adversarial Network (GAN), Variational Auto-Encoder (VAE), and Diffusion Model (DM), which can learn the latent distribution of the input samples to generate new data by sampling from it. Applications of GAI in battery research are then reviewed. For battery materials design, by learning material compositions, structures, and properties, GM can generate novel candidate materials with desired properties through conditional constraints, significantly extending the chemical space to be explored. For electrode microstructure characterization, GM can serve as a bridge for interconversion and integration of different image data, enhance the quality of microscopic characterization, and generate realistic synthetic data. For battery state estimation, GM can perform data augmentation and feature extraction on battery datasets, which benefits the model performance for battery state estimation. Lastly, we discuss the challenges and future development directions in terms of data governance and model design, including data quality and diversity, data standardization and sharing, usability of synthetic data, interpretability of GM, and foundational models for battery research. For the innovation and advancement of battery technology, this perspective offers theoretical references and practical guidelines for implementing GAI as an effective tool in battery research workflows by discussing its status and prospects in this field.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100115"},"PeriodicalIF":10.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472367","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Integrating high surface area and electric conductivity in activated carbon by in-situ formation of a less-defective carbon network during selective chemical etching","authors":"Jing Zhang ,&nbsp;Su Zhang ,&nbsp;Qiqi Li ,&nbsp;Linken Ji ,&nbsp;Yutong Li ,&nbsp;Yukang Ren ,&nbsp;Xiaobei Zang ,&nbsp;Ning Cao ,&nbsp;Han Hu ,&nbsp;Peng Liang ,&nbsp;Zhuangjun Fan","doi":"10.1016/j.actphy.2025.100114","DOIUrl":"10.1016/j.actphy.2025.100114","url":null,"abstract":"<div><div>Activated carbons are widely used as electrode materials for supercapacitors owing to their large surface area, good electric conductivity, and outstanding electrochemical stability. Improving the electric conductivity of activated carbon is crucial for promoting its electrochemical energy storage, but it is hard to achieve because well-developed pores usually break the continuous conductive network. To solve this problem, researchers have developed several methods, such as the selection of highly-conjugated carbon precursors, high-temperature post-treatment, compositing with highly conductive nanocarbons, and local catalytic graphitization. However, these methods generally suffer from high cost, low efficiency, and the sacrifice of specific surface area. Herein, we propose a selective chemical etching strategy to prepare activated carbon with both high surface area and electric conductivity using a mixture of pitch and polyacrylonitrile (PAN) as the precursor. Through systematic investigation of the activation behavior of pure pitch, pure PAN, and the composite precursors, we demonstrate that the PAN-derived carbon contains amorphous and crystallized components. During activation, the amorphous carbon is primarily etched away due to its high reactivity, leading to the in-situ formation of less-defective carbon as the entire conductive network. The optimized sample shows a surface area of 2773 m² g⁻¹ and 2.6 times increased electric conductivity of 912 S m⁻¹, outperforming most of the reported activated carbons. Furthermore, the strong cross-linking between pitch and PAN molecules through pre-oxidation leads to a higher activated carbon yield of 58 % than the pure pitch activated carbon (34 %). The optimized cross-linking structure also allows the activator K⁺ to be adsorbed more easily in the carbon precursor, which enhances the activation efficiency. As a result, the embedded PAN simultaneously constructs a conductive network and promotes activation efficiency, leading to the integration of high electric conductivity and surface area of the activated carbon. For aqueous supercapacitor application, at the high electrode mass loading of 10 mg cm⁻², the optimized material shows remarkable areal capacitance (2.8 F cm⁻² at 1 A g⁻¹) and good rate performance (41 % retention at 50 A g⁻¹). The corresponding device shows high energy densities (10.9 Wh·kg⁻¹) and remarkable cycle stability (100 % retention after 50000 cycles). The reason is that good electric conductivity enables high surface area utilization, significantly improved electric double-layer formation and ion transport kinetics. This work demonstrates the significant potential of highly conductive activated carbon for practical applications and provides novel insights into the design of conductive activated carbon for advanced energy storage.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100114"},"PeriodicalIF":10.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144298269","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"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 (H₂O₂) 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 H₂O₂. Electrochemical H₂O₂ synthesis <em>via</em> a two-electron oxygen reduction reaction (2e⁻ 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⁻ pathway while suppressing the competing 4e⁻ 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⁻ ORR, with particular emphasis on noble metal catalysts and reactor engineering. We begin by discussing the fundamental principles and reaction mechanisms underlying the 2e⁻ 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 H₂O₂ 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":"2025-10-01","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}

{"title":"3D/2D ReSe2/ZnCdS S-scheme photocatalyst with efficient interfacial charge separation for optimized hydrogen production","authors":"Jiaqi Yang ,&nbsp;Xuqiang Hao ,&nbsp;Jiejie Jing ,&nbsp;Yuqiang Hao ,&nbsp;Zhiliang Jin","doi":"10.1016/j.actphy.2025.100131","DOIUrl":"10.1016/j.actphy.2025.100131","url":null,"abstract":"<div><div>The rational construction of step-scheme (S-scheme) heterojunctions has been demonstrated as an effective strategy to optimize interfacial charge carrier separation dynamics in semiconductor photocatalysts. In this work, a hierarchical ReSe₂/ZnCdS S-scheme heterojunction with well-defined architectures was successfully synthesized <em>via</em> an ultrasonication-assisted synthetic strategy, achieving precise nanostructure control and enhanced interfacial coupling for optimized photogenerated charge dynamics. The disordered nanoflower-like ReSe₂ architecture enhances light-harvesting efficiency and the density of surface reaction sites, and significantly suppresses ZnCdS nanoparticle aggregation. The optimized 5 % ReSe₂/ZnCdS composite exhibits an exceptional hydrogen evolution rate of 13.96 mmol g⁻¹ h⁻¹ under visible light irradiation, representing a 5.91-fold enhancement over pristine ZnCdS (2.36 mmol g⁻¹ h⁻¹) and outperforming most conventional heterojunction systems. The outstanding photocatalytic performance is attributed to the formation of the ReSe₂/ZnCdS S-scheme heterojunction, which promotes the separation of photogenerated electrons and holes, enhancing the photo-redox capacity. Combining <em>in-situ</em> XPS analysis and DFT calculations further conforms the S-scheme charge transfer mechanism at the heterointerface of ReSe₂/ZnCdS. Furthermore, Gibbs free energy calculations of hydrogen adsorption confirm that ReSe₂ as the predominant catalytic center provides more favorable hydrogen adsorption kinetics than ZnCdS. This work provides a universal framework to design ZnCdS-based S-scheme heterojunctions for high-efficiency photocatalytic hydrogen evolution.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100131"},"PeriodicalIF":10.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694605","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}