{"title":"过渡金属单原子催化剂在 Rh(111) 上催化动力学生长半金属六方氮化硼-石墨烯横向异质结构","authors":"Yandi Zhu, Weihu Li, Xiaoyan Ren, Lili Zhang, Xingju Zhao, Shunfang Li","doi":"10.1039/d4ta05741d","DOIUrl":null,"url":null,"abstract":"Deciphering the precise catalytic growth mechanism of atomically thin graphene-based lateral heterostructures is of great interest in low-dimensional physics and materials. Here, based on first-principles calculations and extensive screenings, we reveal that the deposited transition metal atoms (TM=Mn, Zr, Nb, Mo, Hf, Ta, and W), particularly Mo, act as single-atom catalysts (SACs) to effectively promote C adatoms dimerization both energetically and kinetically on C-dimer-unpreferred Rh(111) substrate. Meanwhile, the TM-SAC increases the stability of boron-nitride (BN) dimer, which promotes rapid growth of hexagonal boron nitride-graphene (<em>h</em>-BN-G) lateral heterostructure. Specifically, taking TM=Mo as a typical example, we demonstrate that the Mo-C(BN) couplings weaken the C(BN)-substrate interactions, which sharply reduces the kinetic barriers for both C and BN nucleation and migration in the initial stage of growing <em>h</em>-BN-G lateral heterostructure on Rh(111). Interestingly, Mo-SAC can dynamically involve and migrate out of the <em>h</em>-BN-G interface during the growth processes for C<small><sub>2</sub></small> dimers as feeding blocks. Moreover, the presence of Mo-SAC can effectively tune the patching boundary of the 1D <em>h</em>-BN-G heterostructure, <em>i.e.</em>, from C-N to C-B linking with half-metallicity. The present findings provide significantly new insights into controllable catalytic growth of two-dimensional (2D) lateral heterostructures with various important potential applications, such as transport in spintronic devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic kinetic growth of half-metallic hexagonal boron nitride-graphene lateral heterostructure by transition metal single-atom catalyst on Rh(111)\",\"authors\":\"Yandi Zhu, Weihu Li, Xiaoyan Ren, Lili Zhang, Xingju Zhao, Shunfang Li\",\"doi\":\"10.1039/d4ta05741d\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Deciphering the precise catalytic growth mechanism of atomically thin graphene-based lateral heterostructures is of great interest in low-dimensional physics and materials. Here, based on first-principles calculations and extensive screenings, we reveal that the deposited transition metal atoms (TM=Mn, Zr, Nb, Mo, Hf, Ta, and W), particularly Mo, act as single-atom catalysts (SACs) to effectively promote C adatoms dimerization both energetically and kinetically on C-dimer-unpreferred Rh(111) substrate. Meanwhile, the TM-SAC increases the stability of boron-nitride (BN) dimer, which promotes rapid growth of hexagonal boron nitride-graphene (<em>h</em>-BN-G) lateral heterostructure. Specifically, taking TM=Mo as a typical example, we demonstrate that the Mo-C(BN) couplings weaken the C(BN)-substrate interactions, which sharply reduces the kinetic barriers for both C and BN nucleation and migration in the initial stage of growing <em>h</em>-BN-G lateral heterostructure on Rh(111). Interestingly, Mo-SAC can dynamically involve and migrate out of the <em>h</em>-BN-G interface during the growth processes for C<small><sub>2</sub></small> dimers as feeding blocks. Moreover, the presence of Mo-SAC can effectively tune the patching boundary of the 1D <em>h</em>-BN-G heterostructure, <em>i.e.</em>, from C-N to C-B linking with half-metallicity. The present findings provide significantly new insights into controllable catalytic growth of two-dimensional (2D) lateral heterostructures with various important potential applications, such as transport in spintronic devices.\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2024-10-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4ta05741d\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta05741d","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Catalytic kinetic growth of half-metallic hexagonal boron nitride-graphene lateral heterostructure by transition metal single-atom catalyst on Rh(111)
Deciphering the precise catalytic growth mechanism of atomically thin graphene-based lateral heterostructures is of great interest in low-dimensional physics and materials. Here, based on first-principles calculations and extensive screenings, we reveal that the deposited transition metal atoms (TM=Mn, Zr, Nb, Mo, Hf, Ta, and W), particularly Mo, act as single-atom catalysts (SACs) to effectively promote C adatoms dimerization both energetically and kinetically on C-dimer-unpreferred Rh(111) substrate. Meanwhile, the TM-SAC increases the stability of boron-nitride (BN) dimer, which promotes rapid growth of hexagonal boron nitride-graphene (h-BN-G) lateral heterostructure. Specifically, taking TM=Mo as a typical example, we demonstrate that the Mo-C(BN) couplings weaken the C(BN)-substrate interactions, which sharply reduces the kinetic barriers for both C and BN nucleation and migration in the initial stage of growing h-BN-G lateral heterostructure on Rh(111). Interestingly, Mo-SAC can dynamically involve and migrate out of the h-BN-G interface during the growth processes for C2 dimers as feeding blocks. Moreover, the presence of Mo-SAC can effectively tune the patching boundary of the 1D h-BN-G heterostructure, i.e., from C-N to C-B linking with half-metallicity. The present findings provide significantly new insights into controllable catalytic growth of two-dimensional (2D) lateral heterostructures with various important potential applications, such as transport in spintronic devices.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.