Abstract
This study investigates the thermal behavior of nanoalloys with a 13-atom icosahedral core surrounded by a 32-atom Bergman shell using molecular dynamics simulations. Both monometallic (Ni₁₃@Ni₃₂, Pd₁₃@Pd₃₂, Ag₁₃@Ag₃₂) and bimetallic (Ni₁₃@Ag₃₂, Ni₁₃@Pd₃₂) clusters were analyzed to evaluate the effects of atomic size mismatch and cohesive energy on melting behavior. Simulations were performed from 1 K to 1300 K under constant-temperature conditions. Caloric curves and Lindemann indices were used to identify structural transitions. Among all systems, only the Ni₁₃@Ag₃₂ cluster maintained its quasi-spherical shell integrity during heating and showed clear surface-driven melting. Other systems, including those with ideal size matching, experienced structural instabilities or rearrangements before melting. These results demonstrate that the Bergman shell offers thermal and structural stability specifically for the Ni-Ag combination, despite its moderate (~16%) size mismatch. The findings highlight the importance of both geometric compatibility and energetic favorability in the design of stable core-shell nanoalloys.
Supporting Institution
The author acknowledges the support from Zonguldak Bülent Ecevit University Scientific Research Projects Coordinatorship under project code 2016-22794455-02
Project Number
2016-22794455-02
Thanks
The author thanks Dr. Meral Eryürek for her valuable contributions to the design of the figures presented in this study.
References
- Panizon E, Ferrando R. Strain-induced restructuring of the surface in core@shell nanoalloys. Nanoscale 2016; 8(35): 15911-15919.
- Ferrando R, Jellinek J, Johnston R. Nanoalloys: From Theory to Applications of Alloy Clusters and Nanoparticles. Chem Rev 2008; 108(3): 845-910.
- Ferrando R. Geometric structures and chemical ordering in nanoalloys. In: Ferrando R, editor. Structure and Properties of Nanoalloys. Amsterdam, Netherlands: Elsevier, 2016. pp. 13-45.
- Zhang H, Watanabe T, Okumura M, Haruta M, Toshima N. Catalytically highly active top gold atom on palladium nanocluster. Nat Mater 2012; 11(1): 49-52.
- Cheng D, Wang W, Huang S. The onion-ring structure for Pd-Pt bimetallic clusters. J Phys Chem B 2006; 110(33): 16193-16196.
- Parsina I, Baletto F. Tailoring the structural motif of AgCo nanoalloys: Core/shell versus janus-like. J Phys Chem C 2010; 114(3): 1504-1511.
- Meurig Thomas J, Adams RD, Boswell EM, Captain B, Grönbeck H, Raja R. Synthesis, characterization, electronic structure and catalytic performance of bimetallic and trimetallic nanoparticles containing tin. Faraday Discuss 2008; 138: 301-315.
- Demiroglu I, Li ZY, Piccolo L, Johnston RL. A DFT study of molecular adsorption on Au–Rh nanoalloys. Catal Sci Technol 2016; 6(18): 6916-6931.
- Yan Y, Shan H, Li G, Xiao F, Jiang Y, Yan Y, Jin C, Zhang H, Wu J, Yang D. Epitaxial Growth of Multimetallic Pd@PtM (M = Ni, Rh, Ru) Core-Shell Nanoplates Realized by in Situ-Produced CO from Interfacial Catalytic Reactions. Nano Lett 2016; 16(12): 7999-8004.
- Zhao J, Li H, Liu Z, Hu W, Zhao C, Shi D. An advanced electrocatalyst with exceptional eletrocatalytic activity via ultrafine Pt-based trimetallic nanoparticles on pristine graphene. Carbon N Y 2015; 87(C): 116-127.
- Shakila PB, Jeevanantham V, Nagalakshmi R, Saravanan R. Quick photoresponsive and high quantum yield of Ag/Pd/Ni trimetallic nanocatalyst using Cassia auriculata for removal of fabric dye. Biomass Convers Biorefinery 2024; 14(20): 25533-25543.
- Li Z, Lao X, Yang L, Fu A, Guo P. Assembly of trimetallic palladium-silver-copper nanosheets for efficient C2 alcohol electrooxidation. Sci China Mater 2023; 66(1): 150-159.
- Thomson AI, Winterbottom JM. Silica-supported alloy catalysts for triglyceride hydrogenation: The preparation and properties of Pd–Ag and Pd–Ni systems. J Chem Technol \& Biotechnol 1987; 37(4): 257-270.
- Ershov BG, Anan’ev A V, Abkhalimov E V, Kochubei D I, Kriventsov V V, Plyasova L M, Molina I Y, Kozitsyna N Y, Nefedov S E, Vargaftik M N, Moiseev I I. Bimetallic Pd-M (M = Co, Ni, Zn, Ag) nanoparticles containing transition metals: Synthesis, characterization, and catalytic performance. Nanotechnologies Russ 2011; 6(5): 323-329.
- Wojtaszek K, Cebula F, Rutkowski B, Wytrwal M, Csapó E, Wojnicki M. Synthesis and Catalytic Study of NiAg Bimetallic Core–Shell Nanoparticles. Materials (Basel) 2023; 16(2): 659.
- Pei GX, Liu XY, Wang A, Su Y, Li L, Zhang T. Selective hydrogenation of acetylene in an ethylene-rich stream over silica supported Ag-Ni bimetallic catalysts. Appl Catal A Gen 2017; 545: 90-96.
- Holade Y, Morais C, Arrii-Clacens S, Servat K, Napporn TW, Kokoh KB. New Preparation of PdNi/C and PdAg/C Nanocatalysts for Glycerol Electrooxidation in Alkaline Medium. Electrocatalysis 2013; 4(3): 167-178.
- Zhang Z, Nenoff TM, Leung K, Ferreira SR, Huang JY, Berry DT, Provencio PP, Stumpf R. Room-Temperature Synthesis of Ag−Ni and Pd−Ni Alloy Nanoparticles. J Phys Chem C 2010; 114(34): 14309-14318.
- Rapallo A, Rossi G, Ferrando R, Fortunelli A, Curley BC, Lloyd LD, Tarbuck GM, Johnston RL. Global optimization of bimetallic cluster structures. I. Size-mismatched Ag-Cu, Ag-Ni, and Au-Cu systems. J Chem Phys 2005; 122(19): 194308.
- Zhu J, Cheng P, Wang N, Huang S. Insight into the structural and electronic properties of Pd55-nNin (n=0-55) clusters: A density functional theory study. Comput Theor Chem 2015; 1071: 9-17.
- Akbarzadeh H, Abareshi N, Kamrani M. Role of the middle-shell in the stability of three-shell nanoparticles: A molecular dynamics study. Colloids Surfaces A Physicochem Eng Asp 2023; 676(PA): 132163.
- Yıldırım H, Göcen T, Garip AK. Melting behavior of Ir-Ag-Au nanoalloys: a molecular dynamic study. Mol Simul 2022; 48(13): 1155-1162.
- Garip AK. The composition effect for the thermal properties of Pd n Ag (42-n) Pt 13 ternary nanoalloys: a molecular dynamics study. Mol Simul 2019; 45(13): 1004-1013.
- Canestrari N, Nelli D, Ferrando R. General theory for packing icosahedral shells into multi-component aggregates. Nat Commun 2025; 16(1): 1655.
- Gupta RP. Lattice relaxation at a metal surface. Phys Rev B 1981; 23(12): 6265-6270.
- Michaelian K, Rendón N, Garzón IL. Structure and energetics of Ni, Ag, and Au nanoclusters. Phys Rev B 1999; 60(3): 2000-2010.
- Cleri F, Rosato V. Tight-binding potentials for transition metals and alloys. Phys Rev B 1993; 48(1): 22-33.
- Todorov IT, Ellison L, Smith W. Rigid body molecular dynamics within the domain decomposition framework of DL_POLY_4. In: Malyshkin V, editor. Parallel Computing Technologies. Berlin, Germany: Springer, 2013. pp. 429-435.
- Todorov IT, Smith W, Trachenko K, Dove MT. DL_POLY_3: new dimensions in molecular dynamics simulations via massive parallelism. J Mater Chem 2006; 16(20): 1911.
- Bush IJ, Todorov IT, Smith W. A DAFT DL_POLY distributed memory adaptation of the Smoothed Particle Mesh Ewald method. Comput Phys Commun 2006; 175(5): 323-329.
- Boateng HA, Todorov IT. Arbitrary order permanent Cartesian multipolar electrostatic interactions. J Chem Phys 2015; 142(3): 034117.
- Lee MS, Chacko S, Kanhere DG. First-principles investigation of finite-temperature behavior in small sodium clusters. J Chem Phys 2005; 123(16): 164310.
- Alavi S, Thompson DL. Molecular Dynamics Simulations of the Melting of Aluminum Nanoparticles. J Phys Chem A 2006; 110(4): 1518-1523.
- Wen YH, Huang R, Zeng XM, Shao GF, Sun SG. Tetrahexahedral Pt–Pd alloy nanocatalysts with high-index facets: an atomistic perspective on thermodynamic and shape stabilities. J Mater Chem A 2014; 2(5): 1375-1382.
- Shibuta Y, Suzuki T. Phase transition in substrate-supported molybdenum nanoparticles: a molecular dynamics study. Phys Chem Chem Phys 2010; 12(3): 731-739.
- Kittel C. Introduction to Solid State Physics. 8th ed. New York, NY, USA: Wiley, 2004.
- Ackland GJ, Jones AP. Applications of local crystal structure measures in experiment and simulation. Phys Rev B 2006; 73(5): 54104.
Abstract
Bu çalışmada, 13 atomlu bir ikosahedral çekirdek üzerine yerleştirilmiş 32 atomlu Bergman kabuğa sahip nanoalaşımların termal davranışı moleküler dinamik simülasyonları ile incelenmiştir. Atomik boyut uyumsuzluğu ve kohezyon enerjisinin erime davranışı üzerindeki etkilerini değerlendirmek amacıyla, tek elementli (Ni₁₃@Ni₃₂, Pd₁₃@Pd₃₂, Ag₁₃@Ag₃₂) ve iki elementli (Ni₁₃@Ag₃₂, Ni₁₃@Pd₃₂) kümeler analiz edilmiştir. Simülasyonlar sabit sıcaklık koşullarında 1 K ile 1300 K arasında gerçekleştirilmiştir. Yapısal geçişleri belirlemek için kalorik eğriler ve Lindemann indisleri kullanılmıştır. Tüm sistemler arasında yalnızca Ni₁₃@Ag₃₂ kümesi ısıtma süresince küreselimsi kabuk yapısını korumuş ve belirgin bir yüzey kaynaklı erime davranışı sergilemiştir. İdeal boyut uyumu gösteren sistemler de dahil olmak üzere diğer yapılar, erime öncesinde yapısal kararsızlık veya yeniden düzenlenme göstermiştir. Bu sonuçlar, yaklaşık %16’lık bir boyut uyumsuzluğuna rağmen Bergman kabuğunun yalnızca Ni-Ag kombinasyonu için termal ve yapısal açıdan kararlı olduğunu ortaya koymaktadır. Bulgular, kararlı iç-kabuk nanoalaşımlar tasarımında geometrik uyumun ve enerjik uygunluğun birlikte önem taşıdığını göstermektedir.
Supporting Institution
Yazar, bu çalışmanın Zonguldak Bülent Ecevit Üniversitesi Bilimsel Araştırma Projeleri Koordinatörlüğü tarafından 2016-22794455-02 numaralı proje kapsamında desteklendiğini belirtir.
Project Number
2016-22794455-02
Thanks
Yazar, bu çalışmada sunulan şekillerin tasarımına yaptığı değerli katkılarından dolayı Dr. Meral Eryürek’e içtenlikle teşekkür eder.
References
- Panizon E, Ferrando R. Strain-induced restructuring of the surface in core@shell nanoalloys. Nanoscale 2016; 8(35): 15911-15919.
- Ferrando R, Jellinek J, Johnston R. Nanoalloys: From Theory to Applications of Alloy Clusters and Nanoparticles. Chem Rev 2008; 108(3): 845-910.
- Ferrando R. Geometric structures and chemical ordering in nanoalloys. In: Ferrando R, editor. Structure and Properties of Nanoalloys. Amsterdam, Netherlands: Elsevier, 2016. pp. 13-45.
- Zhang H, Watanabe T, Okumura M, Haruta M, Toshima N. Catalytically highly active top gold atom on palladium nanocluster. Nat Mater 2012; 11(1): 49-52.
- Cheng D, Wang W, Huang S. The onion-ring structure for Pd-Pt bimetallic clusters. J Phys Chem B 2006; 110(33): 16193-16196.
- Parsina I, Baletto F. Tailoring the structural motif of AgCo nanoalloys: Core/shell versus janus-like. J Phys Chem C 2010; 114(3): 1504-1511.
- Meurig Thomas J, Adams RD, Boswell EM, Captain B, Grönbeck H, Raja R. Synthesis, characterization, electronic structure and catalytic performance of bimetallic and trimetallic nanoparticles containing tin. Faraday Discuss 2008; 138: 301-315.
- Demiroglu I, Li ZY, Piccolo L, Johnston RL. A DFT study of molecular adsorption on Au–Rh nanoalloys. Catal Sci Technol 2016; 6(18): 6916-6931.
- Yan Y, Shan H, Li G, Xiao F, Jiang Y, Yan Y, Jin C, Zhang H, Wu J, Yang D. Epitaxial Growth of Multimetallic Pd@PtM (M = Ni, Rh, Ru) Core-Shell Nanoplates Realized by in Situ-Produced CO from Interfacial Catalytic Reactions. Nano Lett 2016; 16(12): 7999-8004.
- Zhao J, Li H, Liu Z, Hu W, Zhao C, Shi D. An advanced electrocatalyst with exceptional eletrocatalytic activity via ultrafine Pt-based trimetallic nanoparticles on pristine graphene. Carbon N Y 2015; 87(C): 116-127.
- Shakila PB, Jeevanantham V, Nagalakshmi R, Saravanan R. Quick photoresponsive and high quantum yield of Ag/Pd/Ni trimetallic nanocatalyst using Cassia auriculata for removal of fabric dye. Biomass Convers Biorefinery 2024; 14(20): 25533-25543.
- Li Z, Lao X, Yang L, Fu A, Guo P. Assembly of trimetallic palladium-silver-copper nanosheets for efficient C2 alcohol electrooxidation. Sci China Mater 2023; 66(1): 150-159.
- Thomson AI, Winterbottom JM. Silica-supported alloy catalysts for triglyceride hydrogenation: The preparation and properties of Pd–Ag and Pd–Ni systems. J Chem Technol \& Biotechnol 1987; 37(4): 257-270.
- Ershov BG, Anan’ev A V, Abkhalimov E V, Kochubei D I, Kriventsov V V, Plyasova L M, Molina I Y, Kozitsyna N Y, Nefedov S E, Vargaftik M N, Moiseev I I. Bimetallic Pd-M (M = Co, Ni, Zn, Ag) nanoparticles containing transition metals: Synthesis, characterization, and catalytic performance. Nanotechnologies Russ 2011; 6(5): 323-329.
- Wojtaszek K, Cebula F, Rutkowski B, Wytrwal M, Csapó E, Wojnicki M. Synthesis and Catalytic Study of NiAg Bimetallic Core–Shell Nanoparticles. Materials (Basel) 2023; 16(2): 659.
- Pei GX, Liu XY, Wang A, Su Y, Li L, Zhang T. Selective hydrogenation of acetylene in an ethylene-rich stream over silica supported Ag-Ni bimetallic catalysts. Appl Catal A Gen 2017; 545: 90-96.
- Holade Y, Morais C, Arrii-Clacens S, Servat K, Napporn TW, Kokoh KB. New Preparation of PdNi/C and PdAg/C Nanocatalysts for Glycerol Electrooxidation in Alkaline Medium. Electrocatalysis 2013; 4(3): 167-178.
- Zhang Z, Nenoff TM, Leung K, Ferreira SR, Huang JY, Berry DT, Provencio PP, Stumpf R. Room-Temperature Synthesis of Ag−Ni and Pd−Ni Alloy Nanoparticles. J Phys Chem C 2010; 114(34): 14309-14318.
- Rapallo A, Rossi G, Ferrando R, Fortunelli A, Curley BC, Lloyd LD, Tarbuck GM, Johnston RL. Global optimization of bimetallic cluster structures. I. Size-mismatched Ag-Cu, Ag-Ni, and Au-Cu systems. J Chem Phys 2005; 122(19): 194308.
- Zhu J, Cheng P, Wang N, Huang S. Insight into the structural and electronic properties of Pd55-nNin (n=0-55) clusters: A density functional theory study. Comput Theor Chem 2015; 1071: 9-17.
- Akbarzadeh H, Abareshi N, Kamrani M. Role of the middle-shell in the stability of three-shell nanoparticles: A molecular dynamics study. Colloids Surfaces A Physicochem Eng Asp 2023; 676(PA): 132163.
- Yıldırım H, Göcen T, Garip AK. Melting behavior of Ir-Ag-Au nanoalloys: a molecular dynamic study. Mol Simul 2022; 48(13): 1155-1162.
- Garip AK. The composition effect for the thermal properties of Pd n Ag (42-n) Pt 13 ternary nanoalloys: a molecular dynamics study. Mol Simul 2019; 45(13): 1004-1013.
- Canestrari N, Nelli D, Ferrando R. General theory for packing icosahedral shells into multi-component aggregates. Nat Commun 2025; 16(1): 1655.
- Gupta RP. Lattice relaxation at a metal surface. Phys Rev B 1981; 23(12): 6265-6270.
- Michaelian K, Rendón N, Garzón IL. Structure and energetics of Ni, Ag, and Au nanoclusters. Phys Rev B 1999; 60(3): 2000-2010.
- Cleri F, Rosato V. Tight-binding potentials for transition metals and alloys. Phys Rev B 1993; 48(1): 22-33.
- Todorov IT, Ellison L, Smith W. Rigid body molecular dynamics within the domain decomposition framework of DL_POLY_4. In: Malyshkin V, editor. Parallel Computing Technologies. Berlin, Germany: Springer, 2013. pp. 429-435.
- Todorov IT, Smith W, Trachenko K, Dove MT. DL_POLY_3: new dimensions in molecular dynamics simulations via massive parallelism. J Mater Chem 2006; 16(20): 1911.
- Bush IJ, Todorov IT, Smith W. A DAFT DL_POLY distributed memory adaptation of the Smoothed Particle Mesh Ewald method. Comput Phys Commun 2006; 175(5): 323-329.
- Boateng HA, Todorov IT. Arbitrary order permanent Cartesian multipolar electrostatic interactions. J Chem Phys 2015; 142(3): 034117.
- Lee MS, Chacko S, Kanhere DG. First-principles investigation of finite-temperature behavior in small sodium clusters. J Chem Phys 2005; 123(16): 164310.
- Alavi S, Thompson DL. Molecular Dynamics Simulations of the Melting of Aluminum Nanoparticles. J Phys Chem A 2006; 110(4): 1518-1523.
- Wen YH, Huang R, Zeng XM, Shao GF, Sun SG. Tetrahexahedral Pt–Pd alloy nanocatalysts with high-index facets: an atomistic perspective on thermodynamic and shape stabilities. J Mater Chem A 2014; 2(5): 1375-1382.
- Shibuta Y, Suzuki T. Phase transition in substrate-supported molybdenum nanoparticles: a molecular dynamics study. Phys Chem Chem Phys 2010; 12(3): 731-739.
- Kittel C. Introduction to Solid State Physics. 8th ed. New York, NY, USA: Wiley, 2004.
- Ackland GJ, Jones AP. Applications of local crystal structure measures in experiment and simulation. Phys Rev B 2006; 73(5): 54104.
Details
| Primary Language | English |
|---|---|
| Subjects | Atomic and Molecular Physics |
| Journal Section | Research Article |
| Authors | |
| Project Number | 2016-22794455-02 |
| Submission Date | December 15, 2025 |
| Acceptance Date | January 15, 2026 |
| Early Pub Date | January 16, 2026 |
| Publication Date | January 16, 2026 |
| Published in Issue | Year 2026 Issue: Advanced Online Publication |
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- Prof. Dr. Resul DAŞ
Ferhat Uçar, 1983 yılında Adana'da doğdu. Lisans eğitiminin ardından dört yıl süresince Adana, Gaziantep, Mersin ve İskenderun bölgelerinde uluslararası firmalarda yazılım satış mühendisi, otomasyon mühendisi ve proje mühendisi olarak görev yaptı. 2009 yılında akademik kariyere adım atan Uçar, 2018 yılında Fırat Üniversitesi Elektrik Elektronik Mühendisliği Anabilim Dalında makine öğrenmesi üzerine doktorasını tamamladı.
Şu anda Fırat Üniversitesi Teknoloji Fakültesi Yazılım Mühendisliği bölümünde öğretim üyesi olarak görev yapmakta olan Uçar, aynı zamanda Sam Houston State Üniversitesi ile uluslararası ortak lisans anlaşması bulunan programda İngilizce olarak yazılım mühendisliği dersleri vermektedir. Dergipark bünyesinde TR Dizinde taranan "Turkish Journal of Science & Technology", "Fırat Üniversitesi Mühendislik Bilimleri Dergisi" ve yine Dergipark'ta bulunan "Fırat Üniversitesi Fen Bilimleri Dergisi"nin baş editörlüğünü de yürütmektedir. Akademik kariyeri boyunca idari görevler de üstlenen Uçar, Teknoloji Fakültesi Dekan Yardımcılığı görevinin ardından Fırat Üniversitesi Fen Bilimleri Enstitüsü'nde müdür yardımcısı olarak görev yapmaktadır.
Uçar, IEEE, Elsevier, Wiley, Taylor and Francis ve Nature gibi prestijli platformlarda çok sayıda hakemlik görevini üstlenmiş, devam eden TÜBİTAK projelerinde ve bir COST aksiyonu projesinde araştırmacı olarak yer almaktadır. Fırat Üniversitesi'nin en büyük bütçeli projelerinden biri olan Code23 Fırat Yazılım Atölyesi'nin proje yönetim ekibinde de yer alan Uçar, mobil uygulama geliştirme eğitimi mentörü olarak da görev yapmaktadır.
Yapay zeka ve veri bilimi üzerine yoğunlaşan akademik çalışmalarına devam eden Ferhat Uçar, sektör ve akademi arasında köprü oluşturmayı hedefleyen çalışma ve projelerle kariyer yoluna devam etmektedir.
