物理化学学报最新文献

{"title":"Covalent bond modulation of charge transfer for sensitive heavy metal ion analysis in a self-powered electrochemical sensing platform","authors":"Yun Chen ,&nbsp;Daijie Deng ,&nbsp;Li Xu ,&nbsp;Xingwang Zhu ,&nbsp;Henan Li ,&nbsp;Chengming Sun","doi":"10.1016/j.actphy.2025.100144","DOIUrl":"10.1016/j.actphy.2025.100144","url":null,"abstract":"<div><div>Rational design of photoelectric active materials for photoanodes in photocatalytic fuel cells is crucial for developing highly sensitive self-powered electrochemical sensors. Achieving directional migration and shortening transmission pathways of charge in photoanodes remains a fundamental challenge for enhancing the oxygen evolution reaction performance of photocatalytic fuel cells. Herein, tungsten species atomically dispersed on carbon-rich graphitic carbon nitride (W-CN-C) with the N–W–O covalent bond was designed as the photoanode for constructing a self-powered photocatalytic fuel cell sensing of heavy metal copper ions. W-CN-C was synthesized by self-assembly, exfoliation, and thermal-induced treatment processes. The N–W–O covalent bonds by anchoring tungsten atoms on carbon-rich carbon nitride served as an interfacial charge transport channel, facilitating the separation and migration of charge carriers. The carbon content increase by forming a carbon-rich structure can enhance π-electron delocalization in the W-CN-C, significantly broadening sunlight utilization range. The dispersed tungsten atoms provide effectively active sites, promoting the kinetics of the oxygen evolution reaction between the W-CN-C photoanode and electrolyte interface. The synergistic effects significantly enhance the visible light absorption ability and charge separation and transfer efficiency, improving the photoelectric conversion efficiency of W-CN-C photoanode, exhibiting superior oxygen evolution reaction performance, leading to the amplified open circuit potential in the photocatalytic fuel cell system based on excellent oxygen reduction reaction performance of the Pt@C electrocatalyst cathode. The specific identification probe for copper ions was effectively anchored on the W-CN-C photoanode to construct a self-powered photocatalytic fuel cell sensing platform for copper ions detection. The complex formed by copper ions with the probe hindered electron transport at the W-CN-C photoanode, altering the output detection signal of the photocatalytic fuel cell, thus demonstrating a broad detection range spanning five orders of magnitude (2.0× 10⁻² ∼ 9.2 × 10² nmolmol∙L⁻¹), a low limit of detection (7.0 pmol∙L⁻¹), high selectivity against common interferents, and applicability for detecting heavy metal copper ions in the aquatic environment. Furthermore, the platform allowed for self-powered and portable determination of copper ions using a multimeter as a signal output device, achieving a detection range of 0.25 ∼ 1.3 × 10² nmol∙L⁻¹ and a limit of 84 pmol∙L⁻¹. This work proposes an approach for developing a high-performance photoanode utilizing atomically dispersed metals to introduce covalent bonds as charge transfer channels, paving the way for highly sensitive self-powered electrochemical sensors for environmental monitoring.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100144"},"PeriodicalIF":13.5,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145359557","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":"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":"2025-07-30","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":"Construction of NH2-MIL-125/Na-doped g-C3N4 composite S-scheme heterojunction and its performance in photocatalytic hydrogen peroxide production","authors":"Fan Fan,&nbsp;Hao Xiu,&nbsp;Yuting Wang,&nbsp;Yongpeng Cui,&nbsp;Yajun Wang","doi":"10.1016/j.actphy.2025.100143","DOIUrl":"10.1016/j.actphy.2025.100143","url":null,"abstract":"<div><div>Heterogeneous structure building has proven to be an effective strategy for achieving efficient charge separation and improving photocatalytic performance. In this study, based on the synergistic optimization strategy of elemental doping and heterostructure construction, an S-scheme heterojunction photocatalyst (<em>x</em>% NMT/Na-CN) composed of titanium-based metal-organic framework (NH₂-MIL-125, abbreviated as NMT) and sodium-doped carbon nitride (Na-CN) was constructed by a simple impregnation method. The energy band structure of the catalysts was modulated by intra-layer doping of Na, which introduced nitrogen defects and improved the separation efficiency of photogenerated charges. In addition, the composite of Na-CN and NMT formed an S-scheme heterojunction, which further improved the photogenerated charge separation efficiency while retaining the strong redox ability of the composite catalyst. Owing to the synergistic effect of Na doping and NMT composite, the photocatalytic H₂O₂ production rate of 15 % NMT/Na-CN in isopropanol solution was as high as 2474.6 μmol g⁻¹ h⁻¹, which was 38 times higher than that of unmodified bulk carbon nitride. This work offers a novel approach to realize the efficient production of H₂O₂ from carbon nitride-based photocatalysts based on the doping-heterojunction synergistic optimization strategy.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 2","pages":"Article 100143"},"PeriodicalIF":13.5,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145360972","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":"Unveiling the direct-to-indirect bandgap transition mechanism in the photocatalytic hydrogen evolution of ZnxCd1−xS solid solution","authors":"Huoshuai Huang ,&nbsp;Zhidong Wei ,&nbsp;Jiawei Yan ,&nbsp;Jiasheng Chi ,&nbsp;Qianxiang Su ,&nbsp;Mingxia Chen ,&nbsp;Zhi Jiang ,&nbsp;Yangzhou Sun ,&nbsp;Wenfeng Shangguan","doi":"10.1016/j.actphy.2025.100141","DOIUrl":"10.1016/j.actphy.2025.100141","url":null,"abstract":"<div><div>Solid solution strategy could improve the photocatalytic performance thermodynamically, yet the study focusing on the carrier dynamics of the solid solution catalysts was equally important. Herein, a series of Zn_<em>x</em>Cd_{1−<em>x</em>}S solid solutions were successfully synthesized based on band structure regulation, and the carrier dynamics were investigated by femtosecond transient absorption spectroscopy (TAS) and DFT, which unveiled a variation of the mixed direct-to-indirect bandgap transition mechanism in Zn_<em>x</em>Cd_{1−<em>x</em>}S solid solution. The indirect bandgap exhibited a lower photocarrier recombination rate and, more importantly, could also serve as a trapping center for photocarrier, thus promoting the efficiency of charge separation. Consequently, Zn_<em>x</em>Cd_{1−<em>x</em>}S solid solutions achieved an approximately eleven-fold enhancement in the hydrogen evolution rate (1426.66 μmol h⁻¹) relative to that of bare CdS (129.83 μmol h⁻¹) under visible light (&gt;420 nm). This work proposed that the enhanced photocatalytic performance could originate from both thermodynamic and kinetic aspects simultaneously, and that the alteration of the photocarrier transition mechanism is one of the main factors affecting the kinetics.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100141"},"PeriodicalIF":13.5,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195916","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":"2025-07-25","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":"Waste medical mask-derived carbon quantum dots enhance the photocatalytic degradation of polyethylene terephthalate (PET) over BiOBr/g-C3N4 S-scheme heterojunction","authors":"Shiyi Chen,&nbsp;Jialong Fu,&nbsp;Jianping Qiu,&nbsp;Guoju Chang,&nbsp;Shiyou Hao","doi":"10.1016/j.actphy.2025.100135","DOIUrl":"10.1016/j.actphy.2025.100135","url":null,"abstract":"<div><div>The coronavirus disease 2019 (COVID-19) pandemic has increased the necessity of medical masks, and to date, many waste masks have been discarded without being reprocessed, causing environmental harm. PET, a commonly used plastic product, presents certain hurdles to its natural degradation. In this work, waste medical masks were converted into carbon quantum dots (MCQDs) with blue fluorescence emissions using a simple solvothermal process and then doped into BiOBr/g-C₃N₄ composite material to construct S-scheme heterojunctions for PET degradation. Density functional theory (DFT) calculations revealed that an interfacial electric field (IEF) was formed between g-C₃N₄ and BiOBr. The findings demonstrate that the MCQDs, as a cocatalyst for electron transmission and storage, encourage S-scheme heterojunctions to further separate photogenerated electrons and holes. Levofloxacin (LEV) was used as a molecular probe to visually compare the catalytic activities of various catalysts. These catalysts with different photocatalytic activity were then used to degrade PET. The findings demonstrate that the degradation efficiency of PET over the BiOBr/g-C₃N₄/3MCQDs in seawater is 39.88 ± 1.04 % (weight loss), which is 1.37 times higher than that of BiOBr/g-C₃N₄, and also better than those reported in most of the literature. Free radical capture tests, electrostatic field orbital trap high-resolution gas chromatography-mass spectrometry (HRGC-MS), and ultra-performance liquid chromatography-mass spectrometry (UPLC-MS) experiments uncovered and briefly revealed the key products in the photocatalytic degradation of PET, as well as the relevant mechanism of photocatalytic degradation of PET. The degradation products are expected to become precursors for the further production of polymers and medicines, <em>etc</em>. This study offers fresh perspectives for the creation of innovative photocatalysts for the ecologically benign breakdown of PET, which helps to further lessen environmental damage caused by microplastics (MPs) and enhance resource sustainability.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100135"},"PeriodicalIF":13.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195915","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":"2025-07-24","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":"Red-emitting carbon dots prepared from Epipremnum Aureum leaves extract for biological imaging","authors":"Renyi Shao ,&nbsp;Khurram Abbas ,&nbsp;Vladimir Yu Osipov ,&nbsp;Haimei Zhu ,&nbsp;Yuan Li ,&nbsp;Usama ,&nbsp;Hong Bi","doi":"10.1016/j.actphy.2025.100134","DOIUrl":"10.1016/j.actphy.2025.100134","url":null,"abstract":"<div><div>Carbon dots (CDs) have been widely applied in fluorescence imaging both <em>in vitro</em> and <em>in vivo</em>. However, key challenges remain to be addressed, including the poor specificity of CDs as biological markers and their relatively low fluorescence quantum yield (QY) in the red emission region. In this study, we synthesized red fluorescent carbon dots (designated as EA-CDs, <em>λ</em>_ex/<em>λ</em>_em = 400 nm/660 nm) using a natural plant-derived precursor ethanol extract from <em>Epipremnum aureum</em> leaves <em>via</em> a one-pot solvothermal method. The EA-CDs exhibit a small particle size (average diameter: 3.9 nm), high fluorescence QY (15.4 % in ethanol at <em>λ</em>_em = 660 nm), low toxicity (both <em>in vitro</em> and <em>in vivo</em>), and favorable lipophilicity (oil-water partition coefficient Log<em>P</em> &gt; 0), making them suitable for biological fluorescence imaging and labeling applications. Experimental results indicate that these red-emitting CDs can not only effectively label plant cell membranes, but also serve as an intestinal fluorescence imaging probe in zebrafish models. This suggests their potential as a universal red-emissive bio-membrane dye with high QY. Furthermore, this work pioneers a novel application approach for ornamental plants like <em>Epipremnum aureum</em>.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 2","pages":"Article 100134"},"PeriodicalIF":13.5,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145360973","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":"Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO2 hydrogenation","authors":"Qinhui Guan ,&nbsp;Yuhao Guo ,&nbsp;Na Li ,&nbsp;Jing Li ,&nbsp;Tingjiang Yan","doi":"10.1016/j.actphy.2025.100133","DOIUrl":"10.1016/j.actphy.2025.100133","url":null,"abstract":"<div><div>In the realm of photocatalytic CO₂ hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In₂O₃ composites (denoted as IO@5A-<em>x</em>wt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO₂ to CO, achieving a CO production rate of 2610.55 μmol g⁻¹ h⁻¹, which is 19 times higher than that of pristine In₂O₃. Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 h and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO₂ adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H₂O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100133"},"PeriodicalIF":13.5,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144749480","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":"2025-07-18","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}