Ludmila Ivanova, Olga Bakina, Nikolay Rodkevich, Marat Lerner
{"title":"Heterophase CuO/Cu/Fe nanoparticle incorporated polyurethane coating for combating catheter-induced infection","authors":"Ludmila Ivanova, Olga Bakina, Nikolay Rodkevich, Marat Lerner","doi":"10.1016/j.matchemphys.2024.130154","DOIUrl":"10.1016/j.matchemphys.2024.130154","url":null,"abstract":"<div><div>To combat biofilm formation on the surface of medical devices, a new coatings based on polyurethane filled with heterophase nanoparticles CuO/Cu/Fe composition have been developed. Due to the synergistic antibacterial effect of the nanoparticle constituents, the obtained coatings demonstrated exceptional antibacterial activity. Thus the coating containing 5 % wt. or more of the CuO/Cu/Fe nanoparticles was at least 99.99 % against bacteria <em>S. aureus, A. bumannii, K. pneumonia, P. aeruginosa</em>. For this coating, the value of surface energy was maximum, indicating an increase in its hydrophobicity. The operational life of the catheter samples was more than 30 days, which exceeds the operational life of standard urinary catheters. Based on the results obtained, the application of the developed coating is a promising strategy for solving the catheter-associated urinary tract infection problem. Good biocompatibility was determined <em>in vitro</em> using 3T3 fibroblast cell culture, which is highly sensitive to toxic effects. Compared to other strategies of catheter surface modification, the use of polyurethane coating with nanoparticles of complex composition has a number of advantages: high antibacterial activity of nanoparticles due to the synergistic effect of constituents; biocompatibility of the coating provided by the use of biometals; long-term service life due to good adhesion of the coating to the standard silicon Foley catheter. Thus, the proposed coating containing nanoparticles effectively prevents bacterial colonization on catheters or other implants, thereby reducing the risk of postoperative catheter-induced infection.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"330 ","pages":"Article 130154"},"PeriodicalIF":4.3,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Probing the effect of electrolyte ions on the electrochemical performance of nickel-based metal-organic frameworks","authors":"Shiwani Khokhar , Prakash Chand , Hardeep Anand","doi":"10.1016/j.matchemphys.2024.130144","DOIUrl":"10.1016/j.matchemphys.2024.130144","url":null,"abstract":"<div><div>Understanding the influence of electrolyte ions dimension on electrochemical performance is essential for advancing the development of superior MOF-based devices. Nanosheet-type nickel metal-organic frameworks (Ni-BDC) have emerged as exceptional materials for next-generation supercapacitors. To address this, we investigate the energy storage performance of nickel-1,4-benzene dicarboxylate (Ni-BDC) via an elementary solvothermal approach. The primary objective of the present investigation was to elucidate the influence of distinct cationic components within aqueous electrolytes on the electrochemical efficiency of Ni-BDC. The electrochemical examination was performed using a three-electrode setup in different aqueous electrolytes, comprising LiOH, NaOH, and KOH, each with a concentration of 2 M. The calculated specific capacitance value of Ni-BDC increases in the order of 204 F/g (for LiOH) < 290 F/g (for NaOH) < 1526 F/g (for KOH) at 1 A/g due to the lowest hydration sphere radius, greater ionic mobility of K<sup>+</sup> ion. The material performed better electrochemically in KOH electrolyte with 87 % capacitance preservation. Additionally, an asymmetric supercapacitor (ASSC) device was built using activated carbon (AC) as the negative electrode and nanosheet-like Ni-BDC as the positive electrode. The device, operating within a 1.4 V potential window, demonstrated a capacitance of 39.4 F/g at a current density of 1 A/g. The ASSC device maintained 85 % of its cyclic stability over 4000 charge-discharge cycles at a current density of 8 A/g. This study underscores the vital importance of selecting the optimal electrolyte to significantly enhance the electrochemical performance of Ni-BDC electrode material.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"330 ","pages":"Article 130144"},"PeriodicalIF":4.3,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Lac-based-biosynthesis of zinc–copper mixed metal oxide nanoparticles and evaluation of their antifungal activity against A.alternata and F. oxysporum","authors":"Sarla Yadav , Jigyasa Pathak , Purusottam Majhi , Sandeep Kaushik , A.K. Shukla , Raminder Kaur , Ravinder Kumar , Poonam Singh","doi":"10.1016/j.matchemphys.2024.130152","DOIUrl":"10.1016/j.matchemphys.2024.130152","url":null,"abstract":"<div><div>The use of animal-based sources for biosynthesis resonates with the growing market for sustainable and eco-friendly materials, but remains severely unexplored in comparison to plant-based and microbial sources. In this purview, shellac, a bioresin obtained from the <em>Kerria lacca</em> insect, is emerging as an ideal candidate for nanomaterial fabrication due to its abundant availability and anti-microbial properties. It is commonly available in the form of raw seed lac, (SL) and in the processed button lac (BL) form. Therefore, in the current study, the potential of shellac as a green agent for the synthesis of zinc-copper mixed metal oxide nanoparticles, and the anti-fungal activitiy of synthesized nanoparticles was investigated. Two types of zinc copper oxide nanoparticles were synthesized using button lac (ZnCu(BL)O) and seed lac (ZnCu(SL)O), and they were characterised using various techniques such as Powder X-Ray Diffraction (PXRD), Fourier Transform Infrared spectroscopy (FTIR) and Scanning Electron Microscopy-Energy Dispersive X-Ray (SEM-EDX) spectroscopy. PXRD pattern confirmed the hexagonal wurtzite structure of crystalline ZnCuO NPs. FTIR analysis elucidated the presence of functional groups that were potentially involved in the synthesis of MMO nanoparticles, and the formation of Zn–O and Cu–O bonds was suggested by appearance of bands at 559 cm<sup>−1</sup> and 555 cm<sup>−1</sup>. The morphology and elemental composition of the MMONPs were examined using SEM-EDX techniques that revealed the formation of biosynthesized ZnCuO NPs as spherical agglomerates having uniform distribution of Zn, Cu, C and O throughout the material. Further, the antifungal activity of synthesized NPs was evaluated against <em>F. oxysporum</em> and <em>A. alternata</em> fungal pathogens. It was found that the biosynthesized nanoparticles exhibited significant fungicidal potential against both <em>F. oxysporum</em> and <em>A. alternata</em>. Furthermore, the antifungal results indicated that ZnCuSL-(O) NPs exhibited higher antifungal activity against both fungal strains than ZnCuBL-(O) NPs and chemically synthesized ZnCu-O NPs. Thus, ZnCuSL-(O) NPs and ZnCuBL-(O) NPs prepared using shellac may be considered as cost-effective and eco-friendly substitutes over traditional fungicides.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"330 ","pages":"Article 130152"},"PeriodicalIF":4.3,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Radiation-thermal modification of fluoroplastic composite and evaluation of its radiation-protective characteristics","authors":"Vyacheslav Ivanovich Pavlenko , Vitaliy Valerievich Kashibadze , Anton Valerievich Noskov , Roman Vladimirovich Sidelnikov , Daria Aleksandrovna Ryzhikh , Sergey Viktorovich Serebryakov","doi":"10.1016/j.matchemphys.2024.130162","DOIUrl":"10.1016/j.matchemphys.2024.130162","url":null,"abstract":"<div><div>In the work the composite on the basis of fluoroplastic with filler WO<sub>3</sub> is studied and its efficiency for protection against X-ray and gamma radiation is proved. The technological scheme of composite production has been developed and its physical and mechanical characteristics have been studied. The composite with 60 wt% of WO<sub>3</sub> content has the following properties: density 3.35 ± 0.02 g/cm<sup>3</sup>, Vickers microhardness (at 300 g load) 5.38 ± 0.32 HV, flexural strength 18.86 MPa. The γ-radiation sources used were E(<sup>207</sup>Bi) = 0.570 MeV with an activity of 50 kBq, E(<sup>137</sup>Cs) = 0.662 MeV with an activity of 9 kBq, and E(<sup>60</sup>Co) = 1.252 MeV with an activity of 100 kBq. The X-ray radiation sources were isotopes <sup>241</sup>Am (half-life T<sub>1/2</sub> = 432.1 years; photon energy E = 59.5 keV; radioisotope activity 46 μCi) and <sup>109</sup>Cd (half-life T<sub>1/2</sub> = 461.4 years; photon energy E = 88 keV; radioisotope activity 15 μCi). It is shown that for reduction of gamma radiation with energy 1.252 MeV by 50 % a screen from pure fluoroplastic with thickness of 6.301 ± 0.654 cm is required, and for composite with 60 wt% WO<sub>3</sub> the thickness of screen is 1.5 times less (4.077 ± 0.509 cm). Comparison of the linear attenuation coefficient at energy 0.662 MeV with modern analogs confirmed the high efficiency of radiation protection of the developed material. Radiation-thermal modification of the samples was carried out, which allowed to increase their radiation resistance to gamma radiation many times. After radiation-thermal modification the radiation resistance increased up to 1 ± 0.1 MGy and 4.5 ± 0.2 MGy for fluoroplastic and composite with 60 wt% WO<sub>3</sub> content, respectively. And the initial bending strength increased in both materials by 15 % and more.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"330 ","pages":"Article 130162"},"PeriodicalIF":4.3,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Synergistic effects of Carbon@MoS2 core-shell nanostructures on charge dynamics for future optoelectronic applications","authors":"Shreya, Soumya Rai, Peeyush Phogat, Ranjana Jha, Sukhvir Singh","doi":"10.1016/j.matchemphys.2024.130147","DOIUrl":"10.1016/j.matchemphys.2024.130147","url":null,"abstract":"<div><div>The pursuit of advanced materials for enhancing optoelectronic device performance has led to significant interest in core-shell structures, which combine the unique properties of different materials to achieve superior functionality. This study investigates the hydrothermal synthesis of a series of core-shell Carbon@MoS<sub>2</sub> materials with varying carbon concentrations, aiming to identify the optimal carbon content for enhanced optoelectronic applications. XRD analysis revealed the formation of new crystallographic phases, with crystallite sizes ranging from 1.39 nm to 23.1 nm, indicating significant structural modifications. UV–Vis analysis highlighted an expanded light absorption range and a reduction in bandgap up to 0.92 eV, particularly in carbon-loaded samples. Morphological analysis by FESEM and HRTEM confirmed the successful formation of core-shell nanospheres with well-defined MoS<sub>2</sub> layers enveloping carbon cores. Electrochemical studies, including CV and PEIS, demonstrated that the sample CM4, with an optimal carbon concentration, exhibited balanced redox behavior, lower charge transfer resistance of 2860 Ω, and pronounced Warburg diffusion, marking it as the most effective composition for improving optoelectronic performance in future.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"329 ","pages":"Article 130147"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142663138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ciara Byrne , Matjaž Mazaj , Nataša Zabukovec Logar
{"title":"Assessing the heat storage potential of zeolitic imidazolate frameworks (ZIFs) using water and ethanol as working fluids","authors":"Ciara Byrne , Matjaž Mazaj , Nataša Zabukovec Logar","doi":"10.1016/j.matchemphys.2024.130143","DOIUrl":"10.1016/j.matchemphys.2024.130143","url":null,"abstract":"<div><div>Zeolitic imidazolate frameworks (ZIFs) are comprised of transition metal cations such as Zn(II) and imidazolate-based ligands. Due to their inherent properties, including large surface areas, well-defined and stable porous structure, ZIFs hold significant promise for adsorption applications. Sorption-based heat storage and transformation with porous materials and water as working fluid has been recently recognized as one of the most promising approaches to address more efficient use of energy. In this study, we examined seven different ZIFs (ZIF-8, ZIF-62, ZIF-71, ZIF-74, ZIF-76, ZIF-90 and ZIF-93) and their heat storage potential using water and ethanol as working fluids. It has been demonstrated that storage performance is governed by several factors, including pore dimensions, type and distribution of functional groups on imidazolate ligands, chemical stability of the framework as well as the type of the working fluid. Ethanol sorption data demonstrates inflection points in sorption isotherms at lower relative pressures, enhancement of uptakes for ZIFs with hydrophobic properties, but lower desorption enthalpies if compared to water sorption. We found that ZIF-93 was the most promising material for both working fluids.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"332 ","pages":"Article 130143"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142743728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
H.J. Yashwanth , M. Madhukara Naik , M.S. Dileep , Murthy Muniyappa , M. Navya Rani
{"title":"Nitrogen, phosphorous co-doped carbon quantum dots as glucose and lactate sensor","authors":"H.J. Yashwanth , M. Madhukara Naik , M.S. Dileep , Murthy Muniyappa , M. Navya Rani","doi":"10.1016/j.matchemphys.2024.130149","DOIUrl":"10.1016/j.matchemphys.2024.130149","url":null,"abstract":"<div><div>The present work emphases on the development of a sensor constructed based on the carbon quantum dots (CQDs) doped with heteroatoms such as nitrogen and phosphorous (NPCQDs) by one step microwave radiation assisted method. Cyclic voltammetry and chronoamperometry are used to investigate and compare the sensing performance of CQDs, nitrogen doped CQDs (NCQDs), phosphorous doped CQDs (CQDs) and NPCQDs towards glucose and lactate. It is observed that NPCQDs shows enhanced current response compared to CQDs, NCQDs and PCQDs due to the injection of extra electrons by dopants. Further, NPCQDs sensor exhibited good stability over 5000 s which is excellent in its class.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"331 ","pages":"Article 130149"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Victor A. Brotsman , Natalia S. Lukonina , Andrei A. Eliseev , Ilya N. Ioffe , Alexey A. Goryunkov , Fedor S. Khorobrykh , Sergei A. Klimin , Boris A. Kulnitskiy , Elena A. Skryleva , Igor B. Kutuza , Pavel V. Zinin , Mikhail Yu Popov
{"title":"Thermal/pressure-induced transformation of C60(CF2)","authors":"Victor A. Brotsman , Natalia S. Lukonina , Andrei A. Eliseev , Ilya N. Ioffe , Alexey A. Goryunkov , Fedor S. Khorobrykh , Sergei A. Klimin , Boris A. Kulnitskiy , Elena A. Skryleva , Igor B. Kutuza , Pavel V. Zinin , Mikhail Yu Popov","doi":"10.1016/j.matchemphys.2024.130142","DOIUrl":"10.1016/j.matchemphys.2024.130142","url":null,"abstract":"<div><div>Homofullerenes are the class of fullerene derivatives where all fullerene carbon atoms remain in the <em>sp</em><sup>2</sup>-state. This is facilitated by cleavage of the skeletal C–C bonds between the adjacent sites of attachment of divalent addends, e.g. certain types of >CX<sub>2</sub> groups. Homofullerenes rarely reveal any important differences in optical and chemical properties compared to pristine fullerenes. Here we report an important novel example of such rare differences: formation of new fullerene polymer phases under thermal and high-pressure treatment as evidenced by the <em>in situ</em> and <em>ex situ</em> studies by means of Raman spectroscopy, HRTEM and XPS. Initially, C<sub>60</sub>(CF<sub>2</sub>) molecules undergo dimerization yielding double-caged multiply linked [C<sub>60</sub>(CF<sub>2</sub>)]<sub>2</sub> dimers. High-pressure treatment of C<sub>60</sub>(CF<sub>2</sub>) with additional shear stress leads to phase transitions observed up to 27 GPa yielding high-pressure phases (IV and V) with partial defluorination. This behavior is qualitatively similar to that of pristine C<sub>60</sub>, but due to the presence of the CF<sub>2</sub> moiety, the pressures required are 5–8 GPa higher compared to pristine C<sub>60</sub>. While the shear loads distort the crystal lattice of the C<sub>60</sub>(CF<sub>2</sub>) sample, interplane distances are preserved, indicatively of the lack of long polymeric fullerene chains typical of pristine C<sub>60</sub>. Most importantly, high-pressure phase V of C<sub>60</sub>(CF<sub>2</sub>) demonstrates a transition at 45 GPa yielding an even harder phase which remains stable under 45–80 GPa loads.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"331 ","pages":"Article 130142"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kgwajana B. Molala, Peace P. Mkhonto, Mofuti A. Mehlape, Phuti E. Ngoepe
{"title":"A DFT and cluster expansion study of (Fe,Ni)9S8 pentlandite and unravelling doping with Mn, Co, Cu and precious metals","authors":"Kgwajana B. Molala, Peace P. Mkhonto, Mofuti A. Mehlape, Phuti E. Ngoepe","doi":"10.1016/j.matchemphys.2024.130146","DOIUrl":"10.1016/j.matchemphys.2024.130146","url":null,"abstract":"<div><div>This study used density functional theory (DFT) adopting the universal cluster expansion (UNCLE) technique to generate different structures for (Fe,Ni)<sub>9</sub>S<sub>8</sub> pentlandite and doped with Mn, Co, Cu and precious metals (Ru, Rh, Pd, Os, Ir and Pt) on the Ni and Fe tetrahedral (T) sites. The cluster expansion (CE) depicted the Fe-rich Fe<sub>5</sub>Ni<sub>4</sub>S<sub>8</sub> structure with space-group of P4<sub>2</sub>/nmc (tetragonal) as the most stable. The doped Fe<sub>5</sub>Ni<sub>4</sub>S<sub>8</sub> structure on the Fe(T) with Mn, Cu, Rh, Pd, Ir and Pt changed from tetragonal to cubic structures, while doping with Co, Ru and Os remained tetragonal. Doping on the Ni(T) with Co, the structure changed from tetragonal to cubic, while doping with Mn, Cu, Ru, Rh, Pd, Os, Ir and Pt the structure remained tetragonal. It was found that doping with Pd on the Fe(T) generated the most thermodynamically stable compound (Fe<sub>3</sub>Pd<sub>2</sub>Ni<sub>4</sub>S<sub>8</sub>) with heats of formation of −130.24 meV. The density of states (DOS) showed that the Pd and Pt were the most preferred substitution of Fe(T) in the pentlandite structure, while the Co preferred the Ni(T) sites. In addition doping with Mn on Fe(T) and Ru doped on Ni(T) induced magnetism to the structure. This study predicted various compositions of dopants on pentlandite and laid a foundation for prediction of new mineral-compounds using DFT-CE method.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"331 ","pages":"Article 130146"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142721514","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xuankai Zhao, Zhejie Ma, Xueru Li, Yujie Guo, Ping Li
{"title":"Optimization of atomic layer deposited Pt-shell thickness of PtCu3@Pt/C catalyst for oxygen reduction reaction","authors":"Xuankai Zhao, Zhejie Ma, Xueru Li, Yujie Guo, Ping Li","doi":"10.1016/j.matchemphys.2024.130145","DOIUrl":"10.1016/j.matchemphys.2024.130145","url":null,"abstract":"<div><div>A series of PtCu<sub>3</sub>@Pt/C catalysts with core@shell structure applicable to oxygen reduction reaction (ORR) were successfully synthesized by combining wet chemistry method for supported PtCu<sub>3</sub>/C preparation and atomic layer deposition (ALD) technique for Pt-shell covering PtCu<sub>3</sub> nanoparticles. The oxygen adsorption energy on the surface of model PtCu<sub>3</sub>@Pt(111) based on density functional theory calculation revealed that the optimal oxygen adsorption strength suitable for ORR appears on the PtCu<sub>3</sub>@Pt(111) having few layers of Pt-shell. For this purpose, the Pt-shell thickness was precisely adjusted by varying the number of ALD cycles between 1 and 6, and four ALD cycles were found to deposit approximately one layer of Pt atoms on the surface of PtCu<sub>3</sub> nanoparticles. In-depth investigation through material characterization verified the formation of PtCu<sub>3</sub> alloy and the adjustability of Pt-shell thickness. Strain effect and electronic effects were observed between the PtCu<sub>3</sub> core and Pt-shell, manifested as lattice compression of the Pt-shell and electron transfer from Pt band to Cu, both of which can downshift d-band center of the Pt-shell thus weakening the adsorption of oxygen species. The electrocatalytic performance of various PtCu<sub>3</sub>@Pt<sub>ALD-n</sub>/C (n = 1–6) catalysts was tested in the ORR process using rotating disk electrode approach. PtCu<sub>3</sub>@Pt<sub>ALD-4</sub>/C exhibited the maximum mass and specific activity among all catalysts, being 3.2 and 2.6 times higher than a commercial Pt/C catalyst, and much better as well than the PtCu<sub>3</sub>/C without Pt-shell. The durability of the PtCu<sub>3</sub>@Pt<sub>ALD-4</sub>/C catalyst was also superior to that of the PtCu<sub>3</sub>/C and Pt/C catalysts.</div></div>","PeriodicalId":18227,"journal":{"name":"Materials Chemistry and Physics","volume":"329 ","pages":"Article 130145"},"PeriodicalIF":4.3,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142663139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}