ChemPhysMater最新文献_第2页

Oxygen doping induced intramolecular electron acceptor system in red g-C3N4 nanosheets with remarkably enhanced photocatalytic performance 氧掺杂诱导红色g-C3N4纳米片分子内电子受体体系，显著增强了光催化性能

ChemPhysMater Pub Date : 2025-04-01 DOI: 10.1016/j.chphma.2024.09.001

Huihui Gao, Zhixin Yao, Xuan Chen, Mengqing Zhu, Gang Zhao, Shouwei Zhang, Jinghua Guo

{"title":"Oxygen doping induced intramolecular electron acceptor system in red g-C3N4 nanosheets with remarkably enhanced photocatalytic performance","authors":"Huihui Gao, Zhixin Yao, Xuan Chen, Mengqing Zhu, Gang Zhao, Shouwei Zhang, Jinghua Guo","doi":"10.1016/j.chphma.2024.09.001","DOIUrl":"10.1016/j.chphma.2024.09.001","url":null,"abstract":"<div><div>The enhancement of the photocatalytic activity of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) depends on the rational design of its visible-light harvesting and charge separation/migration properties. Herein, an oxygen doping-induced intramolecular electron acceptor system enabling n→π* electronic transitions in red g-C<sub>3</sub>N<sub>4</sub> nanosheets (<em>E</em><sub>g</sub> ∼ 1.89 eV) was prepared via copolymerization with nitrilotriacetic acid (NTA) and urea. The n→π* electronic transition can be controllably tuned, thus broadening the absorption spectrum of the system to ∼750 nm. Simultaneously, doping with oxygen which acts as an electron acceptor, accelerates in-plane charge separation and migration. Moreover, this strategy was confirmed experimentally to be scalable for industrial mass production. Experiments and theoretical calculations demonstrated that the oxygen doping could continuously modulate the band gap (from ∼2.65 to ∼1.32 eV), resulting in the formation of an intramolecular electron acceptor system which enhances charge separation/migration kinetics. The optimized sample exhibited remarkable photocatalytic H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> production rates of ∼144.8 µmol/h and ∼539.76 µM/h, respectively, which are higher than those for currently available g-C<sub>3</sub>N<sub>4</sub>-based photocatalysts. Significantly, the sample exhibited H<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> photocatalytic yields ∼37.3 and ∼30.1 times those of pristine g-C<sub>3</sub>N<sub>4</sub> under long-wavelength excitation (<em>λ</em> = 520 nm). This study developed an effective and scalable strategy for the design and synthesis of full-spectrum photocatalysts for a broad range of applications.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 2","pages":"Pages 137-149"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143839250","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Progress in graphdiyne-based membrane for gas separation and water purification 石墨烯基气体分离和水净化膜的研究进展

ChemPhysMater Pub Date : 2025-03-18 DOI: 10.1016/j.chphma.2025.02.007

Siyuan Li , Yasong Zhao , Dan Wang

引用次数: 0

Electronic perturbation of Pd single-atom catalysts on graphdiyne derivatives toward effective electrocatalytic nitrate reduction 钯单原子催化剂对石墨炔衍生物电催化硝酸还原的电子扰动研究

ChemPhysMater Pub Date : 2025-03-16 DOI: 10.1016/j.chphma.2025.02.005

Cheng Wang , Tao Song , Hao Dai , Siyan Shu , Shenghan Zhang , Hongliang Dong , Yongfei Ji , Lele Duan

{"title":"Electronic perturbation of Pd single-atom catalysts on graphdiyne derivatives toward effective electrocatalytic nitrate reduction","authors":"Cheng Wang , Tao Song , Hao Dai , Siyan Shu , Shenghan Zhang , Hongliang Dong , Yongfei Ji , Lele Duan","doi":"10.1016/j.chphma.2025.02.005","DOIUrl":"10.1016/j.chphma.2025.02.005","url":null,"abstract":"<div><div>Electrocatalytic reduction of nitrate (NO<sub>3</sub><sup>−</sup>) to ammonia (NH<sub>3</sub>) is a promising approach for addressing water pollution caused by nitrate and producing industrial feedstock NH<sub>3</sub>. However, a significant challenge lies in effectively suppressing the formation of undesired byproducts such as H<sub>2</sub>, N<sub>2</sub>, NO<sub>2</sub><sup>−</sup>, and N<sub>2</sub>H<sub>4</sub>. In this study, three Pd single-atom catalysts (SACs) supported on graphdiyne (GDY) derivatives functionalized with electron-withdrawing and electron-donating groups denoted as Pd/GDY-F, Pd/GDY-H and Pd/GDY-OMe were prepared. Structural characterization showed that due to the electron induction effect of the functional groups, Pd/GDY-F displays the highest Pd valence state, followed by Pd/GDY-H and Pd/GDY-OMe. Interestingly, the nitrate reduction activity also follows the order Pd/GDY-F > Pd/GDY-H > Pd/GDY-OMe, indicating that the nitrate reduction activity of Pd depends on the Pd oxidation state. In addition, the anion exchange ionomers and high nitrate concentrations are beneficial for nitrate reduction. Under optimized conditions, Pd/GDY-F displays a high Faraday efficiency (FE) of 96.2% ± 2.5% toward NH<sub>3</sub>. Mechanistic studies revealed that high-valence Pd atoms favor the adsorption of nitrate reduction intermediates, leading to a high Faraday efficiency for NH<sub>3</sub>.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 321-329"},"PeriodicalIF":0.0,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Stable, high-performance vertical heterojunction ultraviolet photodetectors with Ga2O3-protected Ag nanowires window electrode 稳定，高性能的垂直异质结紫外光电探测器与ga2o3保护银纳米线窗口电极

ChemPhysMater Pub Date : 2025-03-10 DOI: 10.1016/j.chphma.2025.02.004

Xingyuan Yu , Yujie Peng , Di Zhang , Fuqiang Zhai , Hua Tang , Jiang Cheng , Lu Li , Xin Yang , Feng Cheng

{"title":"Stable, high-performance vertical heterojunction ultraviolet photodetectors with Ga2O3-protected Ag nanowires window electrode","authors":"Xingyuan Yu , Yujie Peng , Di Zhang , Fuqiang Zhai , Hua Tang , Jiang Cheng , Lu Li , Xin Yang , Feng Cheng","doi":"10.1016/j.chphma.2025.02.004","DOIUrl":"10.1016/j.chphma.2025.02.004","url":null,"abstract":"<div><div>Large-scale ultraviolet photodetectors are highly promising for detection of weak signals and have the potential for widespread applications in high-tech areas such as aerospace detection and wearable devices. However, the commonly used window electrodes lack transparency to ultraviolet light. Although ultraviolet photodetectors based on Ag nanowires exhibit good response due to their broad transparency range, the sharp interface between the Ag nanowires and the semiconductor renders them extremely unstable. Surface protection is considered to enhance the stability and lifespan of these devices. Our research has revealed that amorphous Ga<sub>2</sub>O<sub>3</sub> can fully encapsulate the surface of Ag nanowires and securely affix it to the NiO film, resulting in a stable performance with a high responsivity of 48 mA W<sup>−</sup><sup>1</sup> and detectivity of 6.1 × 10<sup>11</sup> Jones for 254 nm light. The unpacked device exhibited a stable photocurrent, showing only 6.8% degradation after 3 months in ambient air. Finally, a large-scale (5 cm × 4 cm, with 12 cm<sup>2</sup> of active area) ultraviolet photodetector with a Ga<sub>2</sub>O<sub>3</sub>-protected Ag nanowire electrode was prepared, which demonstrated a milliamp-level photocurrent under weak ultraviolet illumination that can be directly read by a conventional multimeter in practical scenarios, indicating the promising prospects of this device for future commercial applications.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 313-320"},"PeriodicalIF":0.0,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670497","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhanced photocatalytic degradation of Cr(VI) and oxytetracycline using CuFeS₂@Zn composites CuFeS 2 @Zn复合材料增强光催化降解Cr（VI）和土霉素

ChemPhysMater Pub Date : 2025-03-02 DOI: 10.1016/j.chphma.2025.01.004

S. Vigneswaran , P. Gowthaman , S. Sangeethavanathi

{"title":"Enhanced photocatalytic degradation of Cr(VI) and oxytetracycline using CuFeS₂@Zn composites","authors":"S. Vigneswaran , P. Gowthaman , S. Sangeethavanathi","doi":"10.1016/j.chphma.2025.01.004","DOIUrl":"10.1016/j.chphma.2025.01.004","url":null,"abstract":"<div><div>Water pollution caused by heavy metals and antibiotics poses a significant global challenge, necessitating the development of efficient remediation strategies. In this study, zinc (Zn) doped CuFeS<sub>2</sub> (copper iron sulfide) composites were used as highly efficient photocatalysts for the degradation of hexavalent chromium (Cr(VI)) and oxytetracycline (OTC) under visible light. The composites were synthesized using a facile hydrothermal method with various Zn doping concentrations (1 mol%, 5 mol%, and 10 mol%). The synthesized composites were comprehensively characterized by X-ray diffraction, field-emission scanning electron microscopy, Fourier-transform infrared spectroscopy, and Ultraviolet-Visible spectroscopy. X-ray photoelectron spectroscopy, and Brunauer-Emmett-Teller analysis revealed their structural, morphological, optical, and surface area properties. Among the composites, 10 mol% CuFeS@Zn exhibited the highest degradation efficiency, achieving 99 % Cr(VI) and OTC removal within 100 min. This performance significantly surpasses the efficiencies of CuFeS₂, and the CuFeS₂@Zn 1 mol%, and CuFeS₂@Zn 5 mol% composites. Kinetic analysis revealed a high reaction rate constant of 3.041 min<sup>−</sup><sup>1</sup>, and optimal photocatalytic activity was observed at pH 6 and a catalyst dosage of 6 mg, with excellent recyclability and stability demonstrated over multiple cycles for the CuFeS₂@Zn 10 mol% composite. The enhanced photocatalytic performance was attributed to the improved charge carrier separation and transfer resulting from Zn incorporation, which facilitated redox reactions at the catalyst-pollutant interface. This study provides valuable insights into the design of Zn-doped CuFeS₂ composites offering a promising pathway for the development of advanced photocatalytic materials for environmental remediation.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 296-312"},"PeriodicalIF":0.0,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670496","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Modulation of electronic structure of metal-free graphdiyne via precise nitrogen modification for oxygen evolution reaction 无金属石墨炔在析氧反应中精确氮修饰的电子结构调制

ChemPhysMater Pub Date : 2025-02-26 DOI: 10.1016/j.chphma.2025.02.003

Mei Wang , Xinliang Fu , Mengyu Lu , Guodong Shi , Xiufan Liu , Mingjian Yuan

{"title":"Modulation of electronic structure of metal-free graphdiyne via precise nitrogen modification for oxygen evolution reaction","authors":"Mei Wang , Xinliang Fu , Mengyu Lu , Guodong Shi , Xiufan Liu , Mingjian Yuan","doi":"10.1016/j.chphma.2025.02.003","DOIUrl":"10.1016/j.chphma.2025.02.003","url":null,"abstract":"<div><div>The oxygen evolution reaction (OER) is essential for energy conversion and storage but is hindered by sluggish kinetics, low efficiency, and high overpotentials. Although RuO₂ and IrO₂ are efficient catalysts, their high cost and scarcity limit their large-scale application. In contrast, nonmetallic catalysts have gained traction as promising alternatives due to their cost-effectiveness, high stability, and environmental sustainability. The OER efficiency depends on optimal adsorption/desorption of oxygen intermediates, such as *O, OH*, and OOH*, on the catalyst surface. The electronic structure of carbon materials can be optimized via nitrogen doping, which introduces a higher polarity than carbon atoms, thereby optimizing the adsorption free energy of oxygen species during an OER. However, conventional high-temperature pyrolysis methods suffer from limitations such as inaccuracy and high energy consumption. The unique and facile bottom-up synthesis of graphdiyne (GDY) enables precise control over the doping positions of the three sp²-N atoms in GDY (1NGDY, 2NGDY, and 3NGDY) via monomer design engineering. By integrating density functional theory (DFT) calculations with experimental validation, we tailored the adsorption free energy of the oxygen intermediates in the OER, thereby optimizing the rate-determining step of *OOH generation. Among these three kinds of nitrogen-doped GDY catalysts, 3NGDY which incorporates three sp<sup>2</sup>-N atoms exhibited the optimal electrocatalytic performance, achieving a current density of 10 mA cm⁻² in 1 M KOH with a low overpotential of approximately 310 mV. This study demonstrates the significant potential of GDY-based metal-free catalysts in the development of cost-effective, high-performance electrocatalysts.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 289-295"},"PeriodicalIF":0.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Graphdiyne-based nanomaterials: Synthesis, properties, and biomedical applications 石墨烯基纳米材料：合成、性能和生物医学应用

ChemPhysMater Pub Date : 2025-02-24 DOI: 10.1016/j.chphma.2025.01.002

Zhuo Wang , Hui Wang , Xiaoyu Zhang , Yifan Yuan , Longwei Wang , Jing Liu , Chunying Chen

{"title":"Graphdiyne-based nanomaterials: Synthesis, properties, and biomedical applications","authors":"Zhuo Wang , Hui Wang , Xiaoyu Zhang , Yifan Yuan , Longwei Wang , Jing Liu , Chunying Chen","doi":"10.1016/j.chphma.2025.01.002","DOIUrl":"10.1016/j.chphma.2025.01.002","url":null,"abstract":"<div><div>Graphdiyne (GDY)-based nanomaterials are a novel class of two-dimensional carbon structures characterized by a distinctive arrangement of sp<em>-</em> and sp²<em>-</em>hybridized carbon atoms that have garnered significant interest because of their unique properties. The presence of alkyne linkages in these materials leads to a highly conjugated system with uniform pores, offering a plethora of opportunities in diverse technological applications. This review delves into the intrinsic properties of GDY, including its electronic, mechanical, and optical characteristics, which are pivotal for its biomedical utility in fields such as sensing and detection, bio-imaging, tumor therapy, drug delivery, and antibacterial treatments. Despite these promising attributes, the field faces ongoing challenges, including a deeper comprehension of the formation mechanisms, development of scalable synthesis routes for single- or few-layer GDY sheets, and thorough investigation of the basic physical and chemical properties. This paper highlights the existing applications of GDY-based nanomaterials in nanotechnology and identifies the critical research directions necessary for harnessing the full potential of this emerging material.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 207-233"},"PeriodicalIF":0.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pressure induced crossover from 2D-like to 3D structural arrangement in van der Waals magnet CrBr3 范德华磁体CrBr3中二维到三维结构排列的压力诱导交叉

ChemPhysMater Pub Date : 2025-02-24 DOI: 10.1016/j.chphma.2025.02.002

D.P. Kozlenko , O.N. Lis , N.T. Dang , S.E. Kichanov , E.V. Lukin , I.Yu. Zel , N.O. Golosova , B.N. Savenko , T.L. Phan , T.K. Dinh , T.A. Tran

{"title":"Pressure induced crossover from 2D-like to 3D structural arrangement in van der Waals magnet CrBr3","authors":"D.P. Kozlenko , O.N. Lis , N.T. Dang , S.E. Kichanov , E.V. Lukin , I.Yu. Zel , N.O. Golosova , B.N. Savenko , T.L. Phan , T.K. Dinh , T.A. Tran","doi":"10.1016/j.chphma.2025.02.002","DOIUrl":"10.1016/j.chphma.2025.02.002","url":null,"abstract":"<div><div>The evolution of the structural and electronic properties of the van der Waals layered ferromagnet CrBr<sub>3</sub> across the semiconductor-metal transition was investigated using X-ray powder diffraction and Raman spectroscopy at high pressures up to 38 GPa and by density functional theory (DFT) calculations at high pressures up to 120 GPa. The pressure behavior of the structural parameters and vibrational modes revealed a crossover from the quasi-two-dimensional system with weakly interacting atomic layers to the three-dimensional-like system with strongly interacting layers at <em>P</em> ≈ 15 GPa. This resulted in a significant modification of the pressure coefficients of the lattice parameters and interlayer distances. DFT calculations using first-principles generalized gradient approximations of the Perdew-Burke-Ernzerhof (PBE) and Perdew–Burke–Ernzerhof-sol (PBEsol) functionals qualitatively reproduced the high pressure effects on the structural and electronic properties of CrBr<sub>3</sub>, with more accurately results obtained by PBEsol. The relative increase of the binding energy absolute value between the van der Waals layers by 75 times in the pressure range up to 60 GPa was evaluated. Band gap closure associated with the semiconductor–metal transition was found at <em>P</em> = 60 GPa, which is higher than the experimentally determined value.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 280-288"},"PeriodicalIF":0.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670931","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Porous nitrogen-doped graphdiyne templated from zinc acetylacetonate for enhanced oxygen reduction reaction 以乙酰丙酮锌为模板制备的多孔掺氮石墨烯增强氧还原反应

ChemPhysMater Pub Date : 2025-02-20 DOI: 10.1016/j.chphma.2025.01.003

Wenyan Si , Meiping Li , Xingru Yan , Qing Lv , Changshui Huang

引用次数: 0

3D printed 2D materials for tissue engineering applications 用于组织工程应用的3D打印2D材料

ChemPhysMater Pub Date : 2025-01-04 DOI: 10.1016/j.chphma.2024.12.004

Muhammad Bagas Ananda , Maradhana Agung Marsudi , Indra Jaya Budiarso , Akfiny Hasdi Aimon , Ferry Iskandar , Cian Vyas , Glen Cooper , Paulo J.D.S. Bartolo , Arie Wibowo

{"title":"3D printed 2D materials for tissue engineering applications","authors":"Muhammad Bagas Ananda , Maradhana Agung Marsudi , Indra Jaya Budiarso , Akfiny Hasdi Aimon , Ferry Iskandar , Cian Vyas , Glen Cooper , Paulo J.D.S. Bartolo , Arie Wibowo","doi":"10.1016/j.chphma.2024.12.004","DOIUrl":"10.1016/j.chphma.2024.12.004","url":null,"abstract":"<div><div>The field of tissue engineering has witnessed significant progress with the emergence of three-dimensional (3D) printing technologies. The ability to fabricate precise structures with complex geometries combined with the integration of two-dimensional (2D) materials, including graphene, graphene oxide, and transition metal dichalcogenides, has provided novel opportunities. This integration enables the fabrication of functional structures with tailored properties, leveraging the exceptional mechanical, electrical, and chemical characteristics of these materials, in conjunction with the design flexibility offered by 3D printing. Herein, we review the recent advancements in the selection of appropriate 2D materials, diverse 3D printing methods employed for integration, and characterization techniques used to evaluate the performance of the resulting constructs. The successful integration of 3D printing and 2D materials holds immense potential for advancing tissue engineering and paving the way for personalized medicine, regenerative therapies, and point-of-care diagnostics.</div></div>","PeriodicalId":100236,"journal":{"name":"ChemPhysMater","volume":"4 3","pages":"Pages 251-273"},"PeriodicalIF":0.0,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670933","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0