物理化学学报最新文献

{"title":"Insights into the development of 2D covalent organic frameworks as photocatalysts in organic synthesis","authors":"Lewang Yuan ,&nbsp;Yaoyao Peng ,&nbsp;Zong-Jie Guan ,&nbsp;Yu Fang","doi":"10.1016/j.actphy.2025.100086","DOIUrl":"10.1016/j.actphy.2025.100086","url":null,"abstract":"<div><div>Two-dimensional covalent organic frameworks (2D COFs) exhibit distinctive characteristics, including tunable topology, an extensive specific surface area, susceptibility to functionalization, and robust stability, making them frequently utilized in multiphase photocatalytic applications. This article begins with an overview of the synthesis methods for 2D COFs, covering solvothermal, ionothermal, mechanochemical, microwave-assisted, sonochemical, and interfacial synthesis techniques. It provides a concise introduction to various factors influencing photocatalytic performance, such as crystallinity and stability, band structure, charge transfer capability, pore size and specific surface area, and the nature of the light source. Subsequently, the discussion shifts to summarizing and analyzing advancements in the use of 2D COFs as photocatalysts for organic small molecule conversion reactions, particularly in photocatalytic oxidation, reduction, and coupling reactions. Finally, a summary and outlook are presented regarding the opportunities and challenges that 2D COFs face in photocatalytic organic transformations.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100086"},"PeriodicalIF":10.8,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143848761","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":"Tailored cathode electrolyte interphase via ethylene carbonate-free electrolytes enabling stable and wide-temperature operation of high-voltage LiCoO2","authors":"Yu Peng,&nbsp;Jiawei Chen,&nbsp;Yue Yin,&nbsp;Yongjie Cao,&nbsp;Mochou Liao,&nbsp;Congxiao Wang,&nbsp;Xiaoli Dong,&nbsp;Yongyao Xia","doi":"10.1016/j.actphy.2025.100087","DOIUrl":"10.1016/j.actphy.2025.100087","url":null,"abstract":"<div><div>Raising the charge cut-off voltage of LiCoO₂ (LCO) cathodes provides a straightforward approach to increasing the energy density of lithium-ion batteries (LIBs). However, when the charge cut-off voltage exceeds 4.55 ​V (vs. Li/Li⁺), the cathode-electrolyte interphase (CEI) becomes unstable, failing to protect the LCO cathode from severe interfacial side reactions and structural instability. These issues accelerate battery degradation and severely hinder the practical application of high-energy-density LIBs. Moreover, ethylene carbonate (EC)-based electrolytes exhibit more pronounced parasitic reactions than EC-free electrolytes under high voltage, further exacerbating performance limitations. Therefore, optimizing the components and structure of the CEI with EC-free electrolytes remains a challenge. In this work, we aim to construct a robust and chemically stable F-/B-containing CEI on the surface of LCO cathodes using an EC-free electrolyte design. By replacing EC with more anti-oxidative propylene carbonate (PC) and fluoroethylene carbonate (FEC) solvents, the oxidative stability of the electrolyte is significantly improved. This promotes the formation of LiF within the CEI, thereby enhancing its mechanical strength. Meanwhile, the introduction of the sacrificial film-forming additive lithium bis(oxalato)borate (LiBOB) facilitates the generation of oxalates (Li₂C₂O₄) and B-containing crosslinked polymers (LiB_<em>x</em>O_<em>y</em>) within the CEI. These components exhibit high electrochemical stability and flexibility, compensating for the limitations of the LiF-rich CEI and further enhancing the overall structural stability of the CEI. This combination results in a rigid-flexible coupling architecture composed of inorganic-rich components (LiF and Li₂C₂O₄) embedded in B-containing crosslinked polymers (LiB_<em>x</em>O_<em>y</em>), ensuring both mechanical integrity and chemical stability of the CEI. Consequently, this tailored CEI effectively mitigates interfacial layer cracking and regeneration, reducing irreversible structural degradation and interfacial side reactions in high-voltage LCO cathodes. Based on these improvements, the EC-free PC-based electrolyte enables superior performance of LCO cathodes at 4.6 ​V, achieving 82% capacity retention at 0.5<em>C</em> over 200 cycles. Furthermore, graphite||LCO full cells demonstrate enhanced cycling stability at 4.5 ​V and enable operation across a wide temperature range (−40 to 80 ​°C), highlighting the effectiveness of the rigid-flexible coupling CEI derived from the tailored electrolyte. By moving away from conventional EC-based electrolyte formulas, this work provides new insights into designing high-performance, wide-temperature, and sustainable PC-based electrolytes.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100087"},"PeriodicalIF":10.8,"publicationDate":"2025-04-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143843597","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":"Challenges and strategies on high-manganese Li-rich layered oxide cathodes for ultrahigh-energy-density batteries","authors":"Liangliang Song ,&nbsp;Haoyan Liang ,&nbsp;Shunqing Li ,&nbsp;Bao Qiu ,&nbsp;Zhaoping Liu","doi":"10.1016/j.actphy.2025.100085","DOIUrl":"10.1016/j.actphy.2025.100085","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Benefiting from the synergistic participation of transition metals (TMs) and lattice oxygen in redox reactions, Li-rich layered oxides (LLOs) exhibit a capacity exceeding 250 ​mAh ​g&lt;sup&gt;−1&lt;/sup&gt;, positioning them as promising cathode candidates for next-generation high-energy-density lithium-ion batteries. To further enhance capacity and reduce reliance on environmentally hazardous Co and Ni elements, the development of high-Mn LLOs (HM-LLOs) with ultrahigh capacities surpassing 350 ​mAh ​g&lt;sup&gt;−1&lt;/sup&gt; ​has emerged as a viable strategy. Elevated Mn content introduces additional Li–O–Li configurations, facilitating greater lattice oxygen involvement in redox reactions, thereby increasing theoretical capacity. However, practical studies reveal that the achievable capacity of HM-LLOs remains significantly lower than theoretical predictions, severely hindering their application. The discrepancy primarily stems from two factors: activation difficulty and irreversible oxygen loss. Despite the higher initial charge capacity, the lattice oxygen utilization efficiency is still limited by incomplete activation. Meanwhile, irreversible oxygen loss leads to low initial coulombic efficiency (ICE). Given these challenges in HM-LLOs, a systematic review is necessary to unravel the origin of these issues and seek valid strategies to promote their application in power batteries. Herein, we elucidate the relationship between high Mn content and theoretical capacity through compositional, structural, and stoichiometric perspectives. Next, we analyze the roles of elemental components in HM-LLOs at the atomic level, followed by an in-depth investigation of unique structural evolution, particularly the formation of large Li&lt;sub&gt;2&lt;/sub&gt;MnO&lt;sub&gt;3&lt;/sub&gt; domains. These factors collectively restrict practical capacity utilization. Low Co content combined with large Li&lt;sub&gt;2&lt;/sub&gt;MnO&lt;sub&gt;3&lt;/sub&gt; domains exacerbate activation issues, while low Ni content and these domains promote irreversible oxygen loss. Building on this mechanistic understanding, we comprehensively categorize various strategies, from precursor synthesis to active material modifications. The mechanisms of precursor synthesis and structural transformations during the sintering process have been detailed. Optimization methods employed during the synthesis process have been thoroughly reviewed. Furthermore, effective modification methods have been elaborated, from the fundamental principles to practical applications. The advantages and disadvantages of these modification methods, as well as potential future optimization directions, have been outlined. Additionally, novel explorations, such as the construction of O2-type structures, innovative activation methods, and the development of sulfur-based host, are discussed. Finally, we propose future directions to bridge the gap between theoretical and practical capacities, including advanced characterization of oxygen redox dynamics and machine learning","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100085"},"PeriodicalIF":10.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143848653","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":"Accelerating the reconstruction of NiSe2 by Co/Mn/Mo doping for enhanced urea electrolysis","authors":"Mingjie Lei ,&nbsp;Wenting Hu ,&nbsp;Kexin Lin ,&nbsp;Xiujuan Sun ,&nbsp;Haoshen Zhang ,&nbsp;Ye Qian ,&nbsp;Tongyue Kang ,&nbsp;Xiulin Wu ,&nbsp;Hailong Liao ,&nbsp;Yuan Pan ,&nbsp;Yuwei Zhang ,&nbsp;Diye Wei ,&nbsp;Ping Gao","doi":"10.1016/j.actphy.2025.100083","DOIUrl":"10.1016/j.actphy.2025.100083","url":null,"abstract":"<div><div>As a highly promising renewable energy technology, the urea oxidation reaction (UOR) not only enables efficient utilization of urea wastewater but also provides an effective alternative for hydrogen production via water electrolysis, thereby reducing the energy consumption of conventional electrolysis. Therefore, the development of UOR catalysts with high catalytic activity and long-term stability is of great significance for advancing clean energy technologies. In this study, a nickel-based selenide catalyst (NiCoMnMo–Se) with coexisting nanoparticles and nanosheets was synthesized using a NaBH₄ reduction and selenization strategy. X-ray photoelectron spectroscopy (XPS), ultraviolet–visible (UV–vis) and in-situ bode phase plots, revealed that the synergistic effect of Mn and Mo regulated the electronic structure of Ni, enhancing the conductivity of nickel selenide and accelerating charge transfer kinetics, which facilitates the rapid transformation of Ni²⁺/Co²⁺ into active Ni³⁺/Co³⁺ and significantly reduces the onset potential of NiCoMnMo–Se. During the UOR process, Mo and Se are oxidized to form molybdate and selenate, which subsequently dissolve into the electrolyte. This transformation results in the partial conversion of the original spherical nanoparticle surfaces into nanosheets, thereby exposing more Ni(Co)OOH active sites and significantly enhancing the UOR reaction. Additionally, the introduction of Mn stabilizes the active sites, thereby improving the overall stability of the catalyst. As anticipated, the synthesized NiCoMnMo–Se catalyst demonstrates outstanding electrocatalytic performance and stability in the UOR process, achieving a current density of 50 ​mA ​cm⁻² at a potential of only 1.38 ​V vs. RHE (reversible hydrogen electrode), with a voltage increase of only 3.0% after 50 ​h of operation at a 50 ​mA ​cm⁻². When NiCoMnMo–Se and commercial Pt/C were assembled into a dual-electrode system for alkaline urea electrolysis, it only requires 1.59 ​V vs. RHE to achieve a current density of 50 ​mA ​cm⁻². This paper designs an efficient and stable Ni-based selenide catalyst, which is expected to promote the further development of selenides in relevant energy technologies.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100083"},"PeriodicalIF":10.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838082","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":"CdS/DBTSO-BDTO S-scheme photocatalyst for H2 production and its charge transfer dynamics","authors":"Jiajie Cai ,&nbsp;Chang Cheng ,&nbsp;Bowen Liu ,&nbsp;Jianjun Zhang ,&nbsp;Chuanjia Jiang ,&nbsp;Bei Cheng","doi":"10.1016/j.actphy.2025.100084","DOIUrl":"10.1016/j.actphy.2025.100084","url":null,"abstract":"<div><div>Photocatalytic hydrogen (H₂) production is a clean energy technology, with great potential for addressing the global energy crisis and related environmental problems. However, single-component photocatalysts often suffer from low efficiency primarily due to fast charge carrier recombination and the tradeoff between light-absorbing capacity and redox capabilities. Constructing heterojunctions provides a promising strategy to overcome these drawbacks, and S-scheme heterojunctions have recently stood out, demonstrating the capability to efficiently facilitate electron/hole separation, while maximizing the redox capability. Among them, polymer-based S-scheme photocatalysts are emerging, though the charge carrier dynamics in inorganic-organic S-scheme heterojunctions remain to be elucidated. Herein, we fabricated an S-scheme heterojunction comprised of the conjugated polymer dibenzothiophene-S,S-dioxide-<em>alt</em>-benzodithiophene (DBTSO-BDTO) and cadmium sulfide (CdS) for photocatalytic H₂ production. The S-scheme mechanism was verified using <em>in situ</em> irradiated X-ray photoelectron spectroscopy, and the charge carrier transfer dynamics were analyzed in depth using femtosecond transient absorption spectroscopy, which revealed that a considerable fraction of electrons undergo interfacial charge transfer in the CdS/DBTSO-BDTO composite. Owing to the improved charge separation efficiency and redox capability, the performance of the composite surpassed that of DBTSO-BDTO and CdS, and the H₂ evolution rate of the optimized CdS/DBTSO-BDTO material reached 3313 ​μmol ​h⁻¹ g⁻¹, three times that of pure CdS. The findings provide new insights into the electron transfer mechanisms of S-scheme heterojunctions, and can guide the design of polymer-based photocatalysts for solar fuel production.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 8","pages":"Article 100084"},"PeriodicalIF":10.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143817443","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":"PEG-VN modified PP separator for high-stability and high-efficiency lithium-sulfur batteries","authors":"Yingtong Shi ,&nbsp;Guotong Xu ,&nbsp;Guizeng Liang ,&nbsp;Di Lan ,&nbsp;Siyuan Zhang ,&nbsp;Yanru Wang ,&nbsp;Daohao Li ,&nbsp;Guanglei Wu","doi":"10.1016/j.actphy.2025.100082","DOIUrl":"10.1016/j.actphy.2025.100082","url":null,"abstract":"<div><div>Lithium-sulfur (Li-S) batteries are regarded as one of the most promising candidates for next generation energy storage systems due to their high theoretical energy density. However, the practical application of Li-S batteries is limited by the low lithium ion (Li⁺) transport efficiency and the rapid capacity decay caused by the shuttle effect. Herein, we report a composite comprising Polyethylene glycol (PEG) and vanadium nitride (VN) nanosheets coated onto a commercial polypropylene (PP) separator, called PEG-VN@PP separator. The supercatalytic effect and adsorption properties exhibited by the VN nanosheets significantly enhance the conversion of polysulfides, thereby improving both the capacity and stability of Li-S batteries. Due to the coating of PEG, Li⁺ are attracted to the polar functional groups, enabling selective transport, which improves the transport efficiency of Li⁺ and the rate capability of Li-S batteries. The Li-S battery assembled with PEG-VN@PP exhibits a high specific capacity of 782.0 mAh·g⁻¹ and an average capacity decay of 0.048% per cycle at 1<em>C</em> (1675 ​mA·g⁻¹) for 700 cycles, using the carbon nanotubes/sulfur cathode with a sulfur mass loading of 1.2 ​mg·cm⁻².</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100082"},"PeriodicalIF":10.8,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hollow AgPt@Pt core-shell cocatalyst with electron-rich Ptδ− shell for boosting selectivity of photocatalytic H2O2 production for faceted BiVO4","authors":"Yu Wang ,&nbsp;Haiyang Shi ,&nbsp;Zihan Chen ,&nbsp;Feng Chen ,&nbsp;Ping Wang ,&nbsp;Xuefei Wang","doi":"10.1016/j.actphy.2025.100081","DOIUrl":"10.1016/j.actphy.2025.100081","url":null,"abstract":"<div><div>Platinum (Pt) is an excellent oxygen reduction cocatalyst with great potential for the photocatalytic production of H₂O₂. However, its catalytic efficiency is limited by the strong adsorption of O₂, which facilitates O–O bond cleavage and reduces selectivity for the 2-electron oxygen reduction reaction (ORR). Fortunately, the strength of the Pt–O bond can be weakened by adjusting the structure of the cocatalyst to modify the electronic structure of Pt. In this paper, Pt and Ag cocatalysts are successively modified on the (010) facet of BiVO₄ through a two-step photodeposition method. Due to the occurrence of a displacement reaction during the process, a synergistic catalyst with a hollow AgPt alloy core and an electron-rich Pt^{<em>δ</em>−} shell (AgPt@Pt) structure is ultimately synthesized. Photocatalytic experiments demonstrated that the H₂O₂ production from BiVO₄ modified with hollow AgPt@Pt reached an impressive 1021.5 ​μmol ​L⁻¹. This corresponds to an AQE of 5.1%, which is 28.6 times higher than that of the Pt/BiVO₄ photocatalyst with only 35.7 ​μmol ​L⁻¹. Furthermore, research results show that AgPt can transfer electrons to the Pt shell to generate electron-rich Pt^{<em>δ</em>−} active sites, thus increasing the antibonding orbital occupancy of Pt–O_ads in AgPt@Pt catalysts. This electron redistribution weakens the adsorption strength of O₂ on Pt, promoting the 2-electron ORR and facilitating the efficient generation of H₂O₂. This synthesis strategy offers a versatile approach for preparing other Pt-based nano-alloy cocatalysts with improved activity for the selective reduction of O₂ to H₂O₂.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100081"},"PeriodicalIF":10.8,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714321","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 dz2-orbital occupancy of Au cocatalysts for enhanced photocatalytic H2O2 production","authors":"Xiaofang Li,&nbsp;Zhigang Wang","doi":"10.1016/j.actphy.2025.100080","DOIUrl":"10.1016/j.actphy.2025.100080","url":null,"abstract":"","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100080"},"PeriodicalIF":10.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759075","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":"Exploring Zn doped NiBP microspheres as efficient and stable electrocatalyst for industrial-scale water splitting","authors":"Sumiya Akter Dristy,&nbsp;Md Ahasan Habib,&nbsp;Shusen Lin,&nbsp;Mehedi Hasan Joni,&nbsp;Rutuja Mandavkar,&nbsp;Young-Uk Chung,&nbsp;Md Najibullah,&nbsp;Jihoon Lee","doi":"10.1016/j.actphy.2025.100079","DOIUrl":"10.1016/j.actphy.2025.100079","url":null,"abstract":"<div><div>Green hydrogen holds great promise for the future energy ecosystem and designing alternative electrocatalysts is essential for industrial-scale green hydrogen production for high-current water splitting under industrial conditions. Herein, the Zn-doped NiBP microsphere electrocatalyst is fabricated <em>via</em> a multi-step process combining hydrothermal and electrochemical approaches, followed by post-annealing. The optimized Zn/NiBP electrode outperforms the majority of previously reported catalysts, with low overpotentials of 95 ​mV for HER (hydrogen evolution reaction) and 280 ​mV for OER (oxygen evolution reaction) at 100 ​mA ​cm⁻² in 1 ​mol ​L⁻¹ KOH. The bifunctional Zn/NiBP || Zn/NiBP demonstrates a 3.10 ​V cell voltage at 2000 ​mA ​cm⁻² in 1 ​mol ​L⁻¹ KOH, surpassing the benchmark Pt/C || RuO₂ systems. The Pt/C || Zn/NiBP hybrid system exhibits exceptionally low cell voltages of 2.50 and 2.30 ​V at 2000 ​mA ​cm⁻² in 1 and 6 ​mol ​L⁻¹ KOH respectively, demonstrating excellent overall water-splitting performance under challenging industrial conditions. Furthermore, the 2-E system shows remarkable stability over 120 ​h at 1000 ​mA ​cm⁻² in 1 and 6 ​mol ​L⁻¹ KOH, indicating the robust anti-corrosion properties of the Zn/NiBP microspheres. Zn-doped NiBP microspheres exhibit enhanced electrochemical conductivity, active surface area and intrinsic electrocatalytic activity due to synergistic interactions among Zn, Ni, B and P, enabling rapid charge transfer and superior electrocatalytic performance for efficient hydrogen generation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100079"},"PeriodicalIF":10.8,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143684740","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":"Accurate and efficient prediction of Schottky barrier heights in 2D semimetal/silicon heterojunctions","authors":"Haiyu Zhu ,&nbsp;Zhuoqun Wen ,&nbsp;Wen Xiong ,&nbsp;Xingzhan Wei ,&nbsp;Zhi Wang","doi":"10.1016/j.actphy.2025.100078","DOIUrl":"10.1016/j.actphy.2025.100078","url":null,"abstract":"<div><div>The accurate prediction of the Schottky barrier height (SBH) holds significant importance for optimizing the performance of semimetal/semiconductor heterojunction devices. Two-dimensional semimetal/semiconductor heterostructures have now been extensively studied experimentally. However, first-principles predictions of the corresponding SBH typically require solving the ab initio Hamiltonian in supercells containing more than 10³ atoms. This high computational complexity not only results in extremely low efficiency but also hinders the design and optimization of heterojunction devices. Herein, we apply density functional theory with a core-level energy alignment method for transition-metal-ditelluride semimetal/silicon junctions, which enables a reduction in supercell size by one order of magnitude. The predicted SBHs show excellent agreement with experiment. We further investigate different 2D semimetal compounds, finding that all candidates exhibit lower SBHs for holes than electrons, with thickness effects becoming negligible beyond three to five layers. This study presents an efficient framework for calculating SBH in complex heterostructures and provides theoretical guidance for the efficient design of high-performance 2D semimetal heterojunction devices.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 7","pages":"Article 100078"},"PeriodicalIF":10.8,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704031","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}