物理化学学报最新文献

{"title":"Opportunities and challenges of capacitive deionization for uranium extraction from seawater","authors":"Guoze Yan ,&nbsp;Bin Zuo ,&nbsp;Shaoqing Liu ,&nbsp;Tao Wang ,&nbsp;Ruoyu Wang ,&nbsp;Jinyang Bao ,&nbsp;Zhongzhou Zhao ,&nbsp;Feifei Chu ,&nbsp;Zhengtong Li ,&nbsp;Yusuke Yamauchi ,&nbsp;Saad Melhi ,&nbsp;Xingtao Xu","doi":"10.3866/PKU.WHXB202404006","DOIUrl":"10.3866/PKU.WHXB202404006","url":null,"abstract":"<div><div>Uranium is an indispensable resource for the nuclear industry, while land-based uranium mines are limited in content and unevenly distributed. Therefore, uranium extraction from seawater (UES) holds great potential for sustainable energy production. Capacitive deionization (CDI) technology, known for its low energy consumption, simple process, environmentally friendliness, and high adsorption efficiency, holds significant potential for UES. This paper reviews the development history, principles, classifications, and applications of CDI technology. In the section on development history, we provide a brief overview of the early development of CDI technology, emphasizing key milestones in its application to UES and recent optimization efforts. In the section on principle and categorization, we contextualize CDI technology within UES applications for a comprehensive introduction. Additionally, in the application section, we concentrate on current applications of CDI technology in UES. Furthermore, this paper elaborates on the current research status of CDI for UES and its advantages in terms of adsorptivity, selectivity, and economic benefits. In terms of adsorptivity, CDI technology demonstrates its efficiency in adsorbing uranium ions, achieved through meticulous optimization of electrode structure and material selection. With regard to selectivity, CDI technology selectively extracts uranium while mitigating interference from competing ions through adept modulation of electrode materials and operational parameters, thereby enhancing extraction efficiency. Economically, CDI technology stands out due to its hallmark features of low energy consumption and cost-effectiveness, facilitating high-efficiency uranium extraction and providing substantial economic advantages over alternative methods in the UES domain. Lastly, we discuss the challenge factors (competing ions, salinity, pH, and biofouling) of this technology in the uranium extraction process, aiming to explore the feasibility and economic benefits of UES by using the CDI technology and providing theoretical support for further optimization and promotion of CDI applications in UES. Additionally, we aim to address some of the current challenges of uranium extraction using CDI by incorporating materials informatics and providing an outlook on this matter. This paper provides practical insights into the development and industrial progress of CDI technology in UES, aiming to offer valuable references for the subsequent research on CDI seawater uranium extraction to contribute to the sustainable utilization of seawater resources.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 4","pages":"Article 100032"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093641","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":"Rational design of bimetallic oxide anodes for superior Li+ storage","authors":"Xueyu Lin ,&nbsp;Ruiqi Wang ,&nbsp;Wujie Dong ,&nbsp;Fuqiang Huang","doi":"10.3866/PKU.WHXB202311005","DOIUrl":"10.3866/PKU.WHXB202311005","url":null,"abstract":"&lt;div&gt;&lt;div&gt;The rapid advancement of scientific technology leads to a growing need for energy storage equipment in modern society. Lithium-ion batteries (LIBs) are extensively utilized in portable electronics, handy electric tools, medical electronics, and other industries due to their exceptional features such as high energy density, high power density, long lifespan, low self-discharge rate, wide operating temperature range and environmentally-friendly nature. However, the recent rapid development of mobile electronics and electric vehicles requires energy storage devices with even higher energy and power densities. To achieve this goal, it is essential to develop advanced electrode materials featuring high capacity, high rate capability, and long cycle life. The design of high-performance anode materials is an important aspect of constructing the ideal LIB devices. Besides the commercialized graphite, many metal oxides can also act as anode in the LIBs. In detail, the oxides that served as LIB anodes can be classified into intercalation-type, conversion-type and conversion-alloying-type anodes based on their Li&lt;sup&gt;+&lt;/sup&gt; storage mechanisms. Due to their robust metal-oxygen bonds, intercalation-type anodes, such as &lt;em&gt;d&lt;/em&gt;&lt;sup&gt;0&lt;/sup&gt; metal oxides, exhibit stable cycling performance and high-rate capability. However, the limited valence change of intercalation-type metal ions often results in low theoretical capacities. In comparison, conversion-alloying type anodes, exemplified by &lt;em&gt;p&lt;/em&gt;-block metal oxides, offer high theoretical capacities and low Li&lt;sup&gt;+&lt;/sup&gt; extraction potential, making them suitable for high-energy-density LIBs. Nevertheless, the Li&lt;sup&gt;+&lt;/sup&gt; intercalation process induces severe phase agglomeration and volume expansion, leading to rapid capacity decay and poor rate capability. Therefore, these drawbacks severely limit the wild utilization s of metal oxide anodes in commercialized LIBs. Recently, substantial efforts have been made to design novel bimetallic oxide anodes. Among these anodes, the incorporation of intercalation-type or conversion-type motifs into conversion-alloying-type metal oxides enables the creation of bimetallic oxide anodes with optimized electronic and ionic conductivities. This approach has the potential to combine the advantages of high capacity, high-rate capability, and long cycle life in a single system. To uncover the underlying Li&lt;sup&gt;+&lt;/sup&gt; storage mechanisms, this review analyzes the bond situations and electronic structures of various metal oxides. Additionally, it introduces a new graphic representation of the Li&lt;sup&gt;+&lt;/sup&gt;-ion charge/discharge process using density of states (DOS) graphs. The multi-step lithium storage mechanisms in bimetallic oxide anodes are also discussed. Drawing on recent progress in the field, this review provides fundamental academic insights and practical perspectives for the development of high-capacity, high-rate, and robust bimetallic compound anodes","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 3","pages":"Article 100021"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143104721","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":"Architecting Inorganic/Organic S-Scheme Heterojunction of Bi4Ti3O12 Coupling with g-C3N4 for Photocatalytic H2O2 Production from Pure Water","authors":"Ke Li ,&nbsp;Chuang Liu ,&nbsp;Jingping Li ,&nbsp;Guohong Wang ,&nbsp;Kai Wang","doi":"10.3866/PKU.WHXB202403009","DOIUrl":"10.3866/PKU.WHXB202403009","url":null,"abstract":"<div><div>Hydrogen peroxide (H₂O₂) plays a significant role as an industrial chemical and potential energy carrier. However, common H₂O₂ photosynthesis catalysts face challenges such as limited solar spectrum absorption, severe agglomeration, and difficulty in reuse, hindering their widespread application. In this study, an inorganic/organic heterojunction photocatalyst comprising g-C₃N₄ nanosheets and Bi₄Ti₃O₁₂ nanofibers is synthesized using electrospinning assisted self-assembly methods. The Bi₄Ti₃O₁₂/g-C₃N₄ heterojunction exhibits significantly enhanced H₂O₂ yield of 1650 μmol∙g⁻¹∙h⁻¹ and efficient H₂O₂ photosynthesis directly from pure water. The improved performance is attributed to enhanced visible light absorption, charge separation efficiency, and boosting redox properties of photoinduced carriers in S-scheme heterojunctions. Additionally, the utilization of <em>in situ</em> X-ray photoelectron spectroscopy (ISXPS) enables the investigation of the S-scheme mechanism and dynamics of inorganic/organic Bi₄Ti₃O₁₂/g-C₃N₄ heterojunctions. This research presents a novel approach for designing inorganic/organic heterojunction photocatalysts for solar-driven H₂O₂ production.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (98KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2403009"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143144995","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":"Surface Sulfur Species Influence Hydrogenation Performance of Palladium-Sulfur Nanosheets","authors":"Weihan Zhang ,&nbsp;Menglu Wang ,&nbsp;Ankang Jia ,&nbsp;Wei Deng ,&nbsp;Shuxing Bai","doi":"10.3866/PKU.WHXB202309043","DOIUrl":"10.3866/PKU.WHXB202309043","url":null,"abstract":"<div><div>Olefins play a crucial role as fundamental raw materials in organic synthesis, particularly in the production of polyolefins and synthetic rubber. The conversion of alkynes to olefins is pivotal in both the polymer and fine chemical industries. However, this process faces significant challenges in terms of equilibrium selectivity and activity. The inherent low solubility of hydrogen, coupled with the thermodynamic ease of hydrogenating intermediate olefins compared to alkynes, contributes to a decline in olefin selectivity due to further hydrogenation leading to alkanes. Palladium-based catalysts, widely used for hydrogenation, exhibit robust hydrogen adsorption but lack selectivity. Researchers commonly modify catalyst structures by introducing other metals or nonmetals to create intermetallic compounds, aiming to enhance olefin selectivity. This study focuses on synthesizing palladium-sulfur nanosheets (Pd-S NSs) using various sulfur sources to explore the impact of surface S species on the catalytic efficiency of selectively hydrogenating alkynes. Among these, Pd-S-PT NSs/C, utilizing 1,4-benzenedithiol (PT) as the sulfur source, demonstrated high styrene selectivity (92.3%–96.7%) following phenylacetylene hydrogenation for 2 h, showing notable selectivity for different alkynes’ end-groups. Contrastingly, Pd-S-TU NSs/C, with thiourea (TU) as the sulfur source, exhibited poor olefin selectivity (72.4%). X-ray photoelectron spectroscopy (XPS) revealed that the improved olefin selectivity in Pd-S-PT NSs/C was attributed to hindered electron transfer from Pd to S, as well as the presence of surface S⁰ species, maintaining high hydrogenation activity while avoiding over-hydrogenation induced by oxidized S species (S⁴⁺). <em>In situ</em> diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) demonstrated weak styrene adsorption on Pd-S-PT NSs, inhibiting further hydrogenation to ethylbenzene. The ease of styrene desorption on Pd-S-PT NSs, indicated by reduced adsorption strength with increasing desorption temperature, highlighted high olefin selectivity. Conversely, stronger styrene adsorption on Pd-S-TU NSs facilitated additional hydrogenation to produce ethylbenzene, suggesting that the presence of additional S⁴⁺ species hindered improved styrene selectivity. This study not only introduces efficient catalysts for olefin hydrogenation but also advances fundamental research on precisely controlling catalytic processes, particularly focusing on the nuanced control of catalytic surfaces.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (150KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2309043"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145013","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 ZnCoP/CdLa2S4 Schottky Heterojunctions for Enhancing Photocatalytic Hydrogen Evolution","authors":"Jianyin He ,&nbsp;Liuyun Chen ,&nbsp;Xinling Xie ,&nbsp;Zuzeng Qin ,&nbsp;Hongbing Ji ,&nbsp;Tongming Su","doi":"10.3866/PKU.WHXB202404030","DOIUrl":"10.3866/PKU.WHXB202404030","url":null,"abstract":"<div><div>Photocatalytic hydrogen evolution by heterojunction photocatalysts is considered an effective way to address environmental and energy crises. In this work, a novel ZnCoP/CdLa₂S₄ Schottky heterojunction was prepared <em>via</em> a physical mixing method assisted by water bath heating and used to enhance the efficiency of photocatalytic hydrogen production. Owing to the higher work function and metallic conductivity of ZnCoP, the photoinduced electrons can transfer from CdLa₂S₄ to ZnCoP through the ZnCoP/CdLa₂S₄ interface, which suppresses the recombination of photoinduced electrons and holes. Moreover, the Schottky heterojunction formed at the interface between ZnCoP and CdLa₂S₄ inhibits electron backflow from ZnCoP to CdLa₂S₄, which further promotes the separation of electron-hole pairs. Meanwhile, the ZnCoP/CdLa₂S₄ heterojunction exhibited enhanced visible light absorption compared to CdLa₂S₄. In addition, ZnCoP acts as an electron acceptor and hydrogen evolution active site. The synergistic effect of the tight ZnCoP/CdLa₂S₄ interface, the higher work function and metallic conductivity of ZnCoP, and the formation of Schottky junctions significantly enhance the photocatalytic hydrogen production evolution performance of CdLa₂S₄. When the amount of ZnCoP was 30 wt% (wt%, mass fraction), the 30ZCP/CLS composite showed the highest photocatalytic performance, and the hydrogen production rate reached 10.26 mmol·g⁻¹·h⁻¹ under visible light irradiation and with Na₂S and Na₂SO₃ as sacrificial agents, which was 7.7 times that of CdLa₂S₄. Combined with the activity data and characterization results, a potential mechanism for photocatalytic hydrogen production over ZnCoP/CdLa₂S₄ Schottky heterojunctions was proposed.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (98KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2404030"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145963","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":"Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation","authors":"You Wu ,&nbsp;Chang Cheng ,&nbsp;Kezhen Qi ,&nbsp;Bei Cheng ,&nbsp;Jianjun Zhang ,&nbsp;Jiaguo Yu ,&nbsp;Liuyang Zhang","doi":"10.3866/PKU.WHXB202406027","DOIUrl":"10.3866/PKU.WHXB202406027","url":null,"abstract":"<div><div>Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H₂O₂). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized <em>via</em> the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H₂O₂ production efficiency of 4.07 mmol·g⁻¹·h⁻¹, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and <em>in situ</em> irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (72KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406027"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145015","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":"Improved Photo-Carrier Transfer by an Internal Electric Field in BiOBr/Nrich C3N5 3D/2D S-Scheme Heterojunction for Efficiently Photocatalytic Micropollutant Removal","authors":"Changjun You ,&nbsp;Chunchun Wang ,&nbsp;Mingjie Cai ,&nbsp;Yanping Liu ,&nbsp;Baikang Zhu ,&nbsp;Shijie Li","doi":"10.3866/PKU.WHXB202407014","DOIUrl":"10.3866/PKU.WHXB202407014","url":null,"abstract":"<div><div>Photocatalytic wastewater decontamination techniques hold eminent promise in mitigating environmental deterioration, yet the lack of distinctive photocatalysts prevents their further large-scale application. Herein, an S-scheme heterojunction photocatalyst BiOBr/C₃N₅ (BBN) was fabricated for efficiently dislodging micropollutants under visible light. Among the BBN samples, the optimal BBN-2 demonstrated exceptional activity in photocatalytic TC removal with a rate constant of 0.0139 min^‒1, which surpassed that of pure BiOBr and C₃N₅ by 0.6 and 2.8 times, respectively. The spatially segregated photoredox sites and efficient photo-carrier separation propelled by an internal electric field are found to play a cardinal role in promoting photoreaction kinetics. Moreover, BBN-2 exhibited remarkable resistance to environmental interference and stability, retaining a high activity level after five runs. Through active radical detection, •O₂^‒, h⁺ and •OH were identified as the primary active species in the photocatalytic reaction process. This research would encourage the exploration of C₃N₅-based photocatalysts for environmental protection.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (91KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407014"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145019","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":"Accelerated Interfacial Electron Transfer in Perovskite Solar Cell by Ammonium Hexachlorostannate Modification and fs-TAS Investigation","authors":"Jizhou Liu ,&nbsp;Chenbin Ai ,&nbsp;Chenrui Hu ,&nbsp;Bei Cheng ,&nbsp;Jianjun Zhang","doi":"10.3866/PKU.WHXB202402006","DOIUrl":"10.3866/PKU.WHXB202402006","url":null,"abstract":"<div><div>Organic-inorganic halide perovskite solar cells (PSCs) have received widespread attention due to their outstanding photovoltaic performance and straightforward preparation process. However, charge recombination at the interface is a crucial factor limiting further enhancement of the power conversion efficiency (PCE) of the PSCs. In this study, we report the interfacial modification between the electron transport layer and the perovskite film (PSK) using ammonium hexachlorostannate (AH) crystals synthesized <em>via</em> the room temperature spin-coating method. AH as an inorganic tin-based perovskite material, can passivate defects in the PSK and establish a better lattice match, thereby enhancing the quality and crystallinity of the PSK. Kelvin probe force microscopy results confirm that AH promotes the directional migration of photogenerated electrons. Femtosecond transient absorption spectroscopy results verify that AH effectively shortens the lifetime of electron extraction and facilitates interfacial electron transfer. Based on the benefits of AH modification, AH-based PSCs exhibit higher PCE and reduced hysteresis effect.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (104KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2402006"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143144996","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":"Improving Photocatalytic H2O2 Production over iCOF/Bi2O3 S-Scheme Heterojunction in Pure Water via Dual Channel Pathways","authors":"Yang Xia ,&nbsp;Kangyan Zhang ,&nbsp;Heng Yang ,&nbsp;Lijuan Shi ,&nbsp;Qun Yi","doi":"10.3866/PKU.WHXB202407012","DOIUrl":"10.3866/PKU.WHXB202407012","url":null,"abstract":"<div><div>Solar photocatalysis is a green, economical, and sustainable method for H₂O₂ synthesis, which has been regarded as the most promising alternative to the traditional anthraquinone oxidation method. However, single-component photocatalyst exhibits moderate activity owing to the limited light-harvesting range, fast charge recombination and inadequate redox capacity. Moreover, the addition of sacrificial agents is required in the reaction system. Herein, we present the development of an S-scheme heterojunction, achieved through photodepositing Bi₂O₃ nanoparticles (BO) on ionic covalent organic framework nanofiber (iCOF). The optimized photocatalyst iCOF/BO10 shows the highest H₂O₂ production performance in pure water, achieving an H₂O₂ yield of 9.76 mmolꞏg⁻¹ꞏh⁻¹ with an apparent quantum yield (AQY) of 5.5% at 420 nm. This photocatalytic performance is approximately 2.2 and 5.6 times as high as that of pristine iCOF and BO, respectively. In-depth characterizations including <em>in situ</em> irradiated XPS, DFT-calculations, active species trapping experiments and <em>in situ</em> DRIFTS, reveal that the obtained sample not only facilitates charge carrier separation and enhances light absorption capability, but also maximizes the redox ability to concurrently achieve indirect 2e⁻ ORR and 4e⁻ WOR for H₂O₂ production. Additionally, the generated O₂ from the 4e⁻ WOR is capable of accelerating the reaction kinetics for H₂O₂ formation <em>via</em> the indirect 2e⁻ ORR pathway, enabling overall photocatalytic H₂O₂ synthesis. This work provides a new insight into creating innovative catalysts for achieving high-efficiency photosynthesis of H₂O₂.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (84KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407012"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145020","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":"Highly Efficient InOOH/ZnIn2S4 Hollow Sphere S-Scheme Heterojunction with 0D/2D Interface for Enhancing Photocatalytic CO2 Conversion","authors":"Jiaxing Cai ,&nbsp;Wendi Xu ,&nbsp;Haoqiang Chi ,&nbsp;Qian Liu ,&nbsp;Wa Gao ,&nbsp;Li Shi ,&nbsp;Jingxiang Low ,&nbsp;Zhigang Zou ,&nbsp;Yong Zhou","doi":"10.3866/PKU.WHXB202407002","DOIUrl":"10.3866/PKU.WHXB202407002","url":null,"abstract":"<div><div>S-scheme heterojunction system represents a highly efficient strategy for photocatalytic applications as it can simultaneously facilitate photogenerated charge carrier separation and enhance the reduction-oxidation potentials of the photocatalyst. Despite its gigantic potential, the photocatalytic CO₂ conversion efficiency of the S-scheme heterojunction remains limited mainly attributed to the sluggish interfacial charge carrier migration and poor light utilization efficiency. Herein, we prepare an InOOH/ZnIn₂S₄ hollow sphere S-scheme heterojunction with 0D/2D contact interface for enhancing photocatalytic CO₂ conversion performance. Specifically, the hollow sphere morphology can cause the multireflection of incident light within the photocatalyst leading to enhanced light absorption of the photocatalyst. In addition, the 0D/2D contact interface can facilitate the photogenerated charge carrier migration transfer over the InOOH/ZnIn₂S₄ S-scheme heterojunction. Furthermore, combining <em>in situ</em> irradiated X-ray photoelectron spectroscopy (ISIXPS) characterization and radicals trapping test, it is affirmed the accumulation of photogenerated holes and electrons respectively on InOOH and ZnIn₂S₄, which is beneficial for the effective utilization of photogenerated charge carriers. As a result, the photocatalytic CO₂ conversion performance of the optimized InOOH/ZnIn₂S₄ is <em>ca.</em> 25.8 times higher than that of pristine ZnIn₂S₄. Our reported results demonstrate a facile yet effective strategy for enhancing the interfacial photogenerated charge carrier migration and light utilization efficiency of S-scheme heterojunction.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (98KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407002"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145034","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}