物理化学学报最新文献

{"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 LiFePO₄ (LFPO) nanoparticles, derived from spent batteries, with g-C₃N₄ (CN) nanosheets, thereby creating an inorganic/organic S-scheme photocatalyst for the production of H₂O₂. <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 H₂O₂ formation are identified. Benefited from enhanced carrier separation, strong redox power, and multichannel H₂O₂ formation, the optimal composite shows an impressive H₂O₂-production rate of 3.22 mol g⁻¹ h⁻¹ under simulated solar irradiation. This research provides a potential method to investigate a sustainable H₂O₂ 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}

{"title":"Decoding SEI chemistry at the lithium-metal potential","authors":"Changsheng An,&nbsp;Tao Liu","doi":"10.1016/j.actphy.2025.100101","DOIUrl":"10.1016/j.actphy.2025.100101","url":null,"abstract":"","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100101"},"PeriodicalIF":10.8,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068022","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":"Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation","authors":"Lele Feng ,&nbsp;Xueying Bai ,&nbsp;Jifeng Pang ,&nbsp;Hongchen Cao ,&nbsp;Xiaoyan Liu ,&nbsp;Wenhao Luo ,&nbsp;Xiaofeng Yang ,&nbsp;Pengfei Wu ,&nbsp;Mingyuan Zheng","doi":"10.1016/j.actphy.2025.100100","DOIUrl":"10.1016/j.actphy.2025.100100","url":null,"abstract":"<div><div>Ethanol dehydrogenation is a vital elementary step in ethanol upgrading, for which Cu-based alloy catalysts are the most promising candidates. Nevertheless, elucidating the underlying reasons for the synergistic effect between alloying components and host metals remains challenging due to the intrinsic structural complexity and dynamic evolution of alloy catalysts under operational conditions. Herein, single-atom Pd modified Cu-MFI catalysts with well-defined structures were designed for ethanol dehydrogenation to acetaldehyde and hydrogen. Comprehensive characterizations using aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that Pd atoms are isolated by surrounding Cu atoms with a coordination number of 9–10, forming −0.36<em>e</em> charged single-atom sites and being uniformly dispersed on the surface of Cu catalysts. The newly generated Pd^{<em>δ</em>−} and Cu^<em>δ</em>+ sites synergistically reduced the activation energy barrier for C–H bond cleavage in ethanol. These sites simultaneously enhanced hydrogen adsorption and H–H bond coupling, leading to improved ethanol conversion and acetaldehyde productivity over Pd/Cu-MFI catalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100100"},"PeriodicalIF":10.8,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089963","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":"Decoding the interfacial competition between hydrogen evolution and CO2 reduction via edge-active-site modulation in photothermal catalysis","authors":"Jianan Hong,&nbsp;Chenyu Xu,&nbsp;Yan Liu,&nbsp;Changqi Li,&nbsp;Menglin Wang,&nbsp;Yanwei Zhang","doi":"10.1016/j.actphy.2025.100099","DOIUrl":"10.1016/j.actphy.2025.100099","url":null,"abstract":"<div><div>Solar-driven photothermal catalytic CO₂ conversion with H₂O is a promising approach to produce sustainable fuels and chemicals. However, the competition between hydrogen evolution reaction (HER) and CO₂ reduction reaction (CO₂RR) results in unsatisfactory product selectivity. Noble metal nanoparticles (NMNPs) are widely used cocatalysts to introduce active sites on semiconductors, with unique active sites at the metal-semiconductor interfacial edges playing a critical role in the competitive mechanisms. Herein, we prepared a series of NMNPs loaded on Al-doped SrTiO₃ with abundant interfacial edge sites for continuous photothermal catalytic CO₂ and H₂O conversion. Different NMNPs demonstrated distinct CO₂-induced effects on hydrogen evolution. The key intermediate interactions were investigated by <em>in situ</em> diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. The results revealed that bidentate carbonate (b-CO₃²⁻) tended to occupy the edge sites at the metal-semiconductor interfaces, competitively consuming the active sites for ∗H adsorption and altering the energy barrier of hydrogen evolution. The predominant site-blocking effect of b-CO₃²⁻ on Rh-loaded catalysts was verified through establishing a simplified geometric model to quantify the correlation of particle sizes, active site proportions and CO₂-induced hydrogen production variations. Controlling Rh nanoparticle size can tune the proportion of edge sites, which involves a trade-off between ∗H coverage and CO₂ activation and promotes the CO₂RR process toward methane production. This work initially unravels the interfacial competitive mechanism between HER and CO₂RR <em>via</em> edge-active-site modulation, hoping to provide valuable insights for the rational catalyst design and offer potential strategies to enhance CO₂ conversion efficiency.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100099"},"PeriodicalIF":10.8,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946630","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":"Machine learning-guided antireflection coatings architectures and interface modification for synergistically optimizing efficient and stable perovskite solar cells","authors":"Ying Liang ,&nbsp;Yuheng Deng ,&nbsp;Shilv Yu ,&nbsp;Jiahao Cheng ,&nbsp;Jiawei Song ,&nbsp;Jun Yao ,&nbsp;Yichen Yang ,&nbsp;Wanlei Zhang ,&nbsp;Wenjing Zhou ,&nbsp;Xin Zhang ,&nbsp;Wenjian Shen ,&nbsp;Guijie Liang ,&nbsp;Bin Li ,&nbsp;Yong Peng ,&nbsp;Run Hu ,&nbsp;Wangnan Li","doi":"10.1016/j.actphy.2025.100098","DOIUrl":"10.1016/j.actphy.2025.100098","url":null,"abstract":"<div><div>In recent years, single-junction perovskite solar cells (PSCs) have experienced unprecedented development, approaching the Shockley-Queisser (S-Q) theoretical efficiency limit, due to versatile optimization strategies targeting functional layers to minimize energy loss. The antireflection coating (ARC), as part of the light-management strategy, plays a critical role in reducing optical loss to achieve higher efficiency. The development of multifunctional ARC that can simultaneously enhance visible light transmittance while suppressing ultraviolet (UV) light transmission, along with excellent adhesion and wear resistance on glass substrates, remains a significant challenge in current research. Herein, we propose ultra-thin ARC made of multilayer dioxides, SiO₂–TiO₂–SiO₂ (STS) films, optimized using a machine learning approach with a Bayesian optimization algorithm. This process involved parameterized modeling of multilayer dioxide ARC, physical simulations using the Transfer Matrix Method (TMM), and evaluation of antireflective performance. The optimal configuration of STS ARC consists of 100 ​nm SiO₂, 10 ​nm TiO₂, and 10 ​nm SiO₂, increasing the transmittance of FTO glass by 9.2% in the 400–800 ​nm wavelength range. The ARC effectively enhances external quantum efficiency, achieving 96.94%, thereby increasing the short-circuit current density (<em>J</em>_SC) and power conversion efficiency (PCE) by 4%. PSCs with STS ARC retain 81.2% of their initial efficiency after continuous UV illumination for 300 ​h, while control devices degrade to approximately 69%, demonstrating effective UV filtration and improved operational stability. This ARC exhibit hardness exceeding 9H on the pencil hardness scale and achieve ISO class 0/ASTM class 5B in adhesion tests, meeting the outdoor durability requirements for PSCs. In addition to optical energy loss, the accumulation of defects on the surface of the perovskite layer induces non-radiative recombination energy loss and serves as initiation sites for lattice degradation. To address this, we use 3-amidinopyridinium iodide (3-PyADI) to passivate interface defects, further improving the PCE to 24.44%. The stability of the device remains at 93% of the initial PCE after 1000 ​h under atmospheric conditions. The proposed ARC and PSCs structure are expected to enhance optoelectronic performance and environmental stability, providing a promising and practical path for the development of PSCs.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100098"},"PeriodicalIF":10.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068038","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":"Selective electrosorption of Cs(I) from high-salinity radioactive wastewater using CNT-interspersed potassium zinc ferrocyanide electrodes","authors":"Shuhong Xiang ,&nbsp;Lv Yang ,&nbsp;Yingsheng Xu ,&nbsp;Guoxin Cao ,&nbsp;Hongjian Zhou","doi":"10.1016/j.actphy.2025.100097","DOIUrl":"10.1016/j.actphy.2025.100097","url":null,"abstract":"<div><div>The management of ¹³⁷Cs-containing radioactive wastewater from the Fukushima nuclear accident (FNA) has garnered significant attention due to the challenge of its safe disposal. The presence of co-existing Na⁺ ions severely impedes Cs⁺ removal, exacerbating the costs associated with radioactive wastewater treatment. Recently, capacitive deionization (CDI) technology has demonstrated significant potential in this field. However, its application is limited by the lack of suitable electrode materials that exhibit high Cs⁺ selectivity. In this study, we developed a composite of carbon nanotubes (CNT) interspersed potassium zinc ferrocyanide (KZnFC-CNT), which was pre-activated <em>via</em> an electrochemical method, to serve as a CDI cathode for the selective electrosorption of Cs⁺ ions from saline radioactive wastewater. The KZnFC-CNT electrodes exhibited a maximum electrosorption capacity of 392.75 ​mg ​g⁻¹, with the highest electrosorption rate of 11.21 ​mg ​g⁻¹ ​min⁻¹. Furthermore, these electrodes exhibited remarkable selectivity, achieving a selectivity factor of 138.2 for Cs⁺ over Na⁺ in a Na⁺: Cs⁺ molar ratio of 100 : 1. X-ray diffraction, electrochemical analysis, and theoretical simulations revealed that the selective electrosorption of Cs⁺ is primarily governed by the ion exchange process between Cs⁺ and Na⁺ ions, as well as lattice phase transformations in KZnFC. This study presents an effective approach for the treatment of cesium-containing radioactive wastewater with high salinity.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100097"},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903951","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":"Advances in coating strategies for graphite anodes in lithium-ion batteries","authors":"Xintong Zhu ,&nbsp;Bin Cao ,&nbsp;Chong Yan ,&nbsp;Cheng Tang ,&nbsp;Aibing Chen ,&nbsp;Qiang Zhang","doi":"10.1016/j.actphy.2025.100096","DOIUrl":"10.1016/j.actphy.2025.100096","url":null,"abstract":"<div><div>As a critical component for achieving sustainable energy systems, secondary lithium-ion batteries (LIBs) have become the dominant electrochemical energy storage technology. Graphite has been widely employed as an anode material in rechargeable LIBs, where the formation of a solid electrolyte interphase (SEI) on graphite particles plays a pivotal role in realizing optimal Li⁺ ion storage performance. However, solvent co-intercalation with Li⁺ ions leads to volumetric expansion, unstable SEI formation, irreversible capacity loss, structural layer collapse, and even lithium dendrite formation. To overcome these challenges, surface coating modification has emerged as an effective strategy to enhance graphite anode performance. This review systematically summarizes recent progress in coating materials (including carbon materials, lithium-ion conductors, metal compounds, and polymers) fabricated through vapor-phase or liquid-phase deposition. Enormous research investigations demonstrate that rationally designed coating layers prevent direct electrolyte/graphite contact to inhibit solvent decomposition, regulate lithium-ion flux distribution to promote uniform deposition, and function as artificial SEI components to improve interphasial stability. This review provides both theoretical insights and practical considerations for future research and development of advanced graphite anode materials for lithium-ion batteries.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100096"},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144070820","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":"Optimizing interfacial electric fields in carbon nitride nanosheet/spherical conjugated polymer S-scheme heterojunction for hydrogen evolution","authors":"Fanpeng Meng ,&nbsp;Fei Zhao ,&nbsp;Jingkai Lin ,&nbsp;Jinsheng Zhao ,&nbsp;Huayang Zhang ,&nbsp;Shaobin Wang","doi":"10.1016/j.actphy.2025.100095","DOIUrl":"10.1016/j.actphy.2025.100095","url":null,"abstract":"<div><div>Designing heterojunctions based on carbon nitride offers a promising pathway for enhancing photocatalytic efficiency. This study develops an all-organic S-scheme metal-free heterojunction uniquely composed of carbon nitride nanosheets (GCNNS) and a donor–acceptor conjugated polymer, poly p-aminobenzylidene-so-aniline (PASO), synthesized through a simple yet effective ball-milling technique. This heterojunction demonstrates excellent photocatalytic efficiency for hydrogen (H₂) evolution. The optimized GCNNS/PASO-10 sample attains an H₂ evolution rate of 10.12 ​mmol·g⁻¹·h⁻¹, which is about 5.9 times and 19.5 times greater than those of pure GCNNS and PASO, respectively. This improvement is due to the unique interfacial bonding, increased visible-light absorption, and efficient charge carrier separation facilitated by a strong internal electric field within the S-scheme. Theoretical calculations and characterization reveal that this heterojunction's S-scheme mechanism optimally aligns energy bands and promotes spatial charge separation, driving superior photocatalytic activity. This work presents the unique advantage of all-organic materials for heterojunction construction and provides insights into designing advanced S-scheme systems for sustainable energy conversion.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100095"},"PeriodicalIF":10.8,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870814","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":"Phosphazene-based flame-retardant artificial interphase layer for lithium metal batteries","authors":"Caiyun Jin,&nbsp;Zexuan Wu,&nbsp;Guopeng Li,&nbsp;Zhan Luo,&nbsp;Nian-Wu Li","doi":"10.1016/j.actphy.2025.100094","DOIUrl":"10.1016/j.actphy.2025.100094","url":null,"abstract":"&lt;div&gt;&lt;div&gt;The rapid development of emerging fields such as electric vehicles, drones, and robotics has driven the demand for secondary batteries with higher energy density and enhanced safety. The lithium metal anode (LMA) is widely regarded as an ideal anode material for next-generation rechargeable batteries due to its high specific capacity (3860 ​mA ​h·g&lt;sup&gt;−1&lt;/sup&gt;) and low redox potential (−3.04 ​V &lt;em&gt;vs.&lt;/em&gt; standard hydrogen electrode). However, LMA faces significant challenges, primarily the uncontrollable growth of dendrites and its inherent propensity for thermal runaway. To address these issues, this study proposes a novel silsesquioxane-functionalized hexaphenoxycyclotriphosphazene (HPCTP)-based porous polymer (SHPP) artificial interphase layer, synthesized via Friedel-Crafts alkylation, to achieve highly stable LMA performance. N&lt;sub&gt;2&lt;/sub&gt; adsorption/desorption analysis confirms that SHPP features a hierarchical nanoporous structure, with pores of approximately 0.5 and 0.6 ​nm that effectively restrict the mobility of PF&lt;sub&gt;6&lt;/sub&gt;&lt;sup&gt;−&lt;/sup&gt; anions. As a result, the Li-ion transference number increases from 0.29 in liquid electrolytes to 0.60, which helps suppress Li dendrite growth. Additionally, the rich nanoporous structure of SHPP significantly improves its wettability with the electrolyte. In situ thermogravimetric analysis coupled with Fourier transform infrared spectroscopy (TG-FTIR) reveals that SHPP decomposes at approximately 410 ​°C, generating phosphate radicals (PO•) that quench highly reactive hydroxyl (HO•) and oxygen (O•) radicals produced during the thermal decomposition of ester-based electrolytes, effectively mitigating thermal runaway risks. Thermal analysis and ignition tests confirm the outstanding thermal stability and flame-retardant properties of SHPP. Semi-in situ X-ray photoelectron spectroscopy (XPS) analysis indicates that the solid electrolyte interphase (SEI) on bare Li metal is predominantly organic and undergoes significant compositional fluctuations during cycling. In contrast, the SEI formed on SHPP-Li is enriched with Li phosphide (Li&lt;sub&gt;3&lt;/sub&gt;P), which enhances ionic conductivity, and Li fluoride (LiF), which improves chemical stability, resulting in a compositionally stable SEI throughout cycling. SHPP not only facilitates interfacial Li-ion transport but also promotes the formation of a chemically robust interphase. In situ optical microscopy and semi-in situ field-emission scanning electron microscopy (FE-SEM) images demonstrate that the SHPP artificial interphase effectively suppresses Li dendrite growth, enabling uniform Li deposition. As a result, SHPP-Li||SHPP-Li symmetric cells exhibit stable cycling for 1600 ​h at 0.5 ​mA ​cm&lt;sup&gt;−2&lt;/sup&gt; and 0.5 ​mA ​h·cm&lt;sup&gt;−2&lt;/sup&gt;. Furthermore, SHPP-Li||LiNi&lt;sub&gt;0·8&lt;/sub&gt;Co&lt;sub&gt;0·1&lt;/sub&gt;Mn&lt;sub&gt;0·1&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; full cells maintain a high capacity retention of 76.8% after 500 cycles at 1 ​&lt;em&gt;C&lt;/em&gt; (1 ​&lt;em&gt;C&lt;/em&gt; ​= ​190 ​mA ​g&lt;sup&gt;−1","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100094"},"PeriodicalIF":10.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870840","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":"Green H2O2 synthesis via melamine-foam supported S-scheme Cd0.5Zn0.5In2S4/S-doped carbon nitride heterojunction: Synergistic interfacial charge transfer and local photothermal effect","authors":"Weikang Wang ,&nbsp;Yadong Wu ,&nbsp;Jianjun Zhang ,&nbsp;Kai Meng ,&nbsp;Jinhe Li ,&nbsp;Lele Wang ,&nbsp;Qinqin Liu","doi":"10.1016/j.actphy.2025.100093","DOIUrl":"10.1016/j.actphy.2025.100093","url":null,"abstract":"<div><div>Green photocatalytic synthesis of hydrogen peroxide (H₂O₂) represents a promising alternative to the energy-intensive anthraquinone process, yet it is hindered by rapid carrier recombination and insufficient redox capacity in sacrificial-agent-free systems. This work reports a melamine-foam (MF) supported sulfur (S)-doped carbon nitride (SCN)/S vacancy-modified Cd_0.5Zn_0.5In₂S₄ (CZIS) S-scheme heterojunction (CZIS/SCN/MF) <em>via</em> an <em>in situ</em> chemical bath-hydrothermal method for sacrificial-agent-free H₂O₂ photosynthesis. The S-scheme charge transfer mechanism was confirmed by <em>in situ</em> irradiated X-ray photoelectron spectroscopy, free-radical trapping electron paramagnetic resonance, femtosecond transient absorption spectra and theoretical calculations. Specifically, the sulfur doping could modulate the local charge distribution of the carbon nitride framework to reinforce the interfacial built-in electric field for the CZIS/SCN S-scheme heterojunction. Meanwhile, the calcination-induced S-vacancies in CZIS could serve as photoelectron traps, promoting charge separation, and reserving photoinduced holes for H₂O oxidation, thereby achieving sacrificial-agent-free H₂O₂ synthesis. Coupled with the photothermal effect of MF's three-dimensional porous framework, the CZIS/SCN/MF catalyst with optimized S-doping density and SCN dosage delivers an H₂O₂ production rate of 3.46 ​mmol ​g⁻¹ h⁻¹ in pure water, surpassing most of the sacrificial-agent-free systems. This study proposes a novel strategy for synergistic interfacial charge regulation and energy conversion enhancement in sacrificial-agent-free photocatalytic systems.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100093"},"PeriodicalIF":10.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870901","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}