物理化学学报最新文献

{"title":"Insights into the Development of Copper-based Photocatalysts for CO2 Conversion","authors":"Zhiquan Zhang ,&nbsp;Baker Rhimi ,&nbsp;Zheyang Liu ,&nbsp;Min Zhou ,&nbsp;Guowei Deng ,&nbsp;Wei Wei ,&nbsp;Liang Mao ,&nbsp;Huaming Li ,&nbsp;Zhifeng Jiang","doi":"10.3866/PKU.WHXB202406029","DOIUrl":"10.3866/PKU.WHXB202406029","url":null,"abstract":"<div><div>Utilizing sunlight as a renewable energy source, photocatalysis offers a potential solution to global warming and energy shortages by converting CO₂ into useful solar fuels, including CO, CH₄, CH₃OH, and C₂H₅OH. Among the various formulations investigated, copper-based photocatalysts stand out as particularly appealing for CO₂ conversion due to their cost-effectiveness and higher abundance in comparison to catalysts based on precious metals. This literature review provides a thorough summary of the latest developments in copper-based photocatalysts used for CO₂ reduction reactions, including metallic copper, copper oxide, and cuprous oxide photocatalysts. The review also provides a categorical summary of the CO₂ reduction products and a detailed categorical discussion of the means of modulation and modification of each copper-based catalyst. Finally, this review highlights the existing challenges and proposes future research directions in the development of copper-based photocatalysts for CO₂ reduction, focusing on boosting energy utilization and improving product formation rates.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (70KB)</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 12","pages":"Article 2406029"},"PeriodicalIF":10.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143128682","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":"Modulating NH2 Lewis Basicity in CTF-NH2 through Donor-Acceptor Groups for Optimizing Photocatalytic Water Splitting","authors":"Zhao Lu ,&nbsp;Hu Lv ,&nbsp;Qinzhuang Liu ,&nbsp;Zhongliao Wang","doi":"10.3866/PKU.WHXB202405005","DOIUrl":"10.3866/PKU.WHXB202405005","url":null,"abstract":"<div><div>Photocatalytic water splitting (PWS) provides an optimal approach for the sustainable production of green hydrogen. NH₂-modified covalent triazine frameworks (CTFs-NH₂) hold potential in PWS due to robust light uptake, optimal charge separation, and considerable redox potential. However, the high surface reaction barriers hinder the efficiency of PWS owing to the conversion difficulty of intermediate products. Modulating the Lewis basicity of NH₂ on CTFs offers a feasible route for addressing this challenge. In this work, electron-donating ethyl (C₂H₅) and electron-withdrawing 5-fluoroethyl groups (C₂F₅) are introduced at the <em>para</em> position of amine groups, producing C₂H₅-CTF-NH₂ and C₂F₅-CTF-NH₂, to adjust the Lewis basicity of CTF-NH₂. Through DFT calculations, the optical properties, excited states, electronic structures, dipole moments, and surface reaction processes of the CTF-NH₂, C₂H₅-CTF-NH₂ and C₂F₅-CTF-NH₂ are simulated. The results indicate that the electron-withdrawing C₂F₅ group can decrease the electron density and Lewis basicity on NH₂, thereby lowering the energy barriers for hydrogen and oxygen evolution reactions, effectively ameliorating the PWS efficiency of CTF-NH₂. This work unveils an innovative approach for donor-acceptor-regulated CTFs for the application of PWS.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (76KB)</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 12","pages":"Article 2405005"},"PeriodicalIF":10.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143128699","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":"Defective ultrathin two-dimensional materials for photo-/electrocatalytic CO2 reduction: Fundamentals and perspectives","authors":"Runhua Chen ,&nbsp;Qiong Wu ,&nbsp;Jingchen Luo ,&nbsp;Xiaolong Zu ,&nbsp;Shan Zhu ,&nbsp;Yongfu Sun","doi":"10.3866/PKU.WHXB202308052","DOIUrl":"10.3866/PKU.WHXB202308052","url":null,"abstract":"<div><div>Photo-/electrocatalytic reduction of carbon dioxide (CO₂) to carbon-based fuel molecules driven by renewable energy is an attractive strategy for resource regeneration and energy storage, especially for achieving carbon peak and carbon-neutral goals. However, the high thermodynamic stability and chemical inertness of CO₂ molecules make the conversion efficiency and selectivity of reduction products very low, which further hinders its application. In addition, different CO₂ reduction products have similar reduction potential and usually face severe hydrogen evolution competition under aqueous system conditions, which makes the selectivity of specific reduction products unable to be effectively controlled. To overcome these bottlenecks, researchers have been working for many years to develop efficient photo/electrocatalysts to enhance the activity and product selectivity of CO₂ reduction. Thanks to the ultrathin thickness and large specific surface area, ultrathin two-dimensional materials possess highly active sites with high density and high uniformity, which can effectively regulate the key thermodynamic and kinetic factors of CO₂ photo-/electroreduction reactions. As a typical two-dimensional material, the defective ultrathin two-dimensional materials can provide a large number of electron-rich catalytic sites to efficiently adsorb and highly activate CO₂ molecules, which can effectively reduce the reaction barrier, thus accelerating CO₂ reduction and enhancing product selectivity. Moreover, the local atomic and electronic structure of the defects can effectively stabilize the intermediate of CO₂ reduction reactions, thus further optimizing the kinetics of CO₂ reduction reactions. Furthermore, the surface defects are beneficial to the mass and electron transfer in the catalytic process, thus further improving the catalytic activity of the catalysts. In this review, we overview the latest research progress in CO₂ photo-/electrocatalytic reduction using defective ultrathin two-dimensional materials, including the controllable synthesis and fine structure characterization of defective ultrathin two-dimensional materials; the modulation effect of defect structure on the local atomic and electronic structure; the advantages of defective ultrathin two-dimensional materials for CO₂ reduction. We also discuss the challenges and opportunities of defective ultrathin two-dimensional materials for future development of CO₂ photo-/electrocatalytic reduction. It is expected that this review will provide a guide for designing highly efficient CO₂ reduction systems.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 3","pages":"Article 100019"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143104726","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":"Recent advances in iron-based heterostructure anode materials for sodium ion batteries","authors":"Yu Guo,&nbsp;Zhiwei Huang,&nbsp;Yuqing Hu,&nbsp;Junzhe Li,&nbsp;Jie Xu","doi":"10.3866/PKU.WHXB202311015","DOIUrl":"10.3866/PKU.WHXB202311015","url":null,"abstract":"<div><div>Sodium ion batteries (SIBs), characterized by high energy density, prolonged cycle life, and cost-effectiveness, have garnered substantial attention as scalable energy storage devices. However, the primary challenge facing SIBs is the identification of suitable electrode materials capable of accommodating sodium ions reversibly and sustainably. To transition SIBs from the experimental stage to practical applications, the identification of electrode materials exhibiting satisfactory electrochemical performance is imperative. Iron (Fe), as a widely utilized metal element, exhibits considerable potential for application as anode materials in SIBs due to its abundance, cost-effectiveness, and high specific capacity. Nonetheless, Fe-based electrode materials suffer from low conductivity and significant volume changes during charge and discharge processes, leading to poor rate performance and cyclic stability, thereby restricting their widespread application in SIBs. Various modification strategies, such as nanosizing electrode materials, heteroatom doping, heterostructure construction, and combination with fast ion conductors, have been reported to address these challenges. Importantly, engineering Fe-based electrode materials with heterogeneous structures, integrating two or more components <em>via</em> van der Waals forces or chemical bonds, is crucial for creating intricate heterogeneous interfaces. These interfaces generate self-built electric fields that expedite ion transport, enhance reaction kinetics, and mitigate structural damage due to volume changes during cycling, thereby significantly improving the overall electrochemical performance of Fe-based materials in SIBs. Given the rapid advancements in the utilization of Fe-based materials in SIBs, a comprehensive review is necessary to not only summarize recent progress but also provide insight and guidance on their application in SIBs. This review offers a detailed overview of the research progress on Fe-based anode materials with heterostructure in SIBs. Emphasis is placed on synthesis methods, characterization techniques, and energy storage mechanisms of heterostructure Fe-based electrode materials. Additionally, the sodium ion storage characteristics, modification strategies, and strengthening mechanisms of Fe-based materials, including Fe-based oxides, sulfides, phosphides, selenides, as well as dual-anion Fe-based anode materials, are summarized. Finally, the remaining challenges and future development prospects of Fe-based heterostructure anode materials are discussed, aiming to promote the rapid development and practical application of these materials for SIBs.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 3","pages":"Article 100022"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143104722","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":"Progress on self-powered photodetectors based on low-dimensional materials","authors":"Yuhang Zhang ,&nbsp;Weiwei Zhao ,&nbsp;Hongwei Liu ,&nbsp;Junpeng Lü","doi":"10.3866/PKU.WHXB202310004","DOIUrl":"10.3866/PKU.WHXB202310004","url":null,"abstract":"&lt;div&gt;&lt;div&gt;In recent years, there has been a growing interest in self-powered photodetectors, which can detect light without needing an external power supply. This unique feature makes them highly attractive for addressing the current energy shortage and the future demand for miniaturized devices. Among various design approaches for self-powered photodetectors, the use of low-dimensional materials holds great promise. Low-dimensional nanomaterials offer several advantages for self-powered photodetectors. They can be assembled into large area ordered structures such as ultra-thin layers, nanowire arrays, and quantum dot superlattices. Additionally, their atomic-level thickness provides a large specific surface area and facilitates integration with other materials. By combining different low-dimensional materials with complementary enhancements in bandgap, carrier transport rate, and light collection efficiency, the performance of self-powered photodetectors can be significantly improved. These devices can be scaled down to micro-nano levels while taking advantage of the adjustable bandgap, wide spectral response, high carrier migration rate, and high light absorption efficiency offered by low-dimensional materials. This article introduces the performance metrics of photodetectors, including photoresponsivity, noise equivalent power, detectivity, and response time. It then discusses the latest advancements in self-powered photodetectors based on 0D, 1D, and 2D materials. In the section on 0D material self-powered photodetectors, the device structure design using 0D materials as heterojunction components and doping materials is presented, highlighting their respective advantages. The section on 1D material self-powered photodetectors summarizes three main device structure types: planar, vertical, and core-shell, along with their individual advantages. The focus is placed on the content related to 2D material self-powered photodetectors. Graphene, transition metal dichalcogenides (TMDs), and black phosphorus are the most widely used 2D materials, and their preparation methods and the latest advancements in self-powered photodetectors are discussed. The controllable diversity in electrical properties resulting from interlayer interactions in two-dimensional materials offers great potential for new principles and multifunctional electronic devices. Finally, the article summarizes and discusses the key challenges and future development directions for self-powered photodetectors based on low-dimensional materials. In summary, the utilization of low-dimensional materials in self-powered photodetectors presents a promising direction for the development of advanced optoelectronic devices. By utilizing the unique properties of these materials, such as their atomic-level thickness, large specific surface area, and controllable electrical properties, significant advancements can be made in the field of self-powered photodetectors. The challenges associated with","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 3","pages":"Article 100020"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143104723","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":"Progress and perspective of perovskite thin single crystal photodetectors","authors":"Yao Ma,&nbsp;Xin Zhao,&nbsp;Hongxu Chen,&nbsp;Wei Wei,&nbsp;Liang Shen","doi":"10.3866/PKU.WHXB202309045","DOIUrl":"10.3866/PKU.WHXB202309045","url":null,"abstract":"<div><div>Metal halide perovskites show immense promise in photodetection applications, having been employed in the research of photodiodes, photoconductors, and phototransistors. However, the majority of current photodetectors utilizing perovskite materials rely on polycrystalline thin films, and the presence of grain boundaries and defects hinders their photoelectric performance, creating a bottleneck in further advancements. To address this issue, researchers have employed techniques such as inverse temperature crystallization (ITC) and anti-solvent vapor-assisted crystallization (AVC) to synthesize various perovskite single crystals. Bulk single crystal perovskite structures are advantageous due to their lack of grain boundaries, resulting in lower dark current and noise in photodetectors, thereby enhancing their weak light detection capabilities. Additionally, the diminished presence of grain boundaries extends the lifetime of photo-generated carriers, providing a foundation for improved detector performance. However, due to the excellent optical absorption coefficient of perovskites, the excessive thickness of bulk single crystals can only increase the probability of carrier recombination, impacting the photodetector's performance. Consequently, perovskite thin single crystal materials prepared by controlling longitudinal size have garnered significant interest in novel detector research. Various techniques, such as space-confined method, surface tension-assisted method, and vapor phase epitaxy, have been proposed to growth thin single crystals with controllable thickness. These methods have been continually optimized to enhance crystal quality. Thin single crystal perovskites not only enhance photodetector performance but also hold potential for large-area single crystal production, supporting the development of photodetector imaging arrays. This paper outlines the fundamental principles behind perovskite single crystal growth, introduces various technological approaches developed for thin perovskite single crystal growth, and analyzes the resulting materials from different growth methods. It further reviews notable studies in the realm of perovskite thin single crystal photodetectors for different device types. Finally, the paper discusses current challenges and issues in this field while offering insights into potential future directions of development.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 4","pages":"Article 100030"},"PeriodicalIF":10.8,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093642","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":"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}