{"title":"Plasmon assisted synthesis of TiN-supported single-atom nickel catalysts","authors":"","doi":"10.1186/s11671-024-03992-z","DOIUrl":null,"url":null,"abstract":"<h3>Abstract</h3> <p>We report the deposition of single atom nickel catalyst on refractory plasmonic titanium nitride (TiN) nanomaterials supports using the wet synthesis method under visible light irradiation. TiN nanoparticles efficiently absorb visible light to generate photoexcited electrons and holes. Photoexcited electrons reduce nickel precursor to deposit Ni atoms on TiN nanoparticles’ surface. The generated hot holes are scavenged by the methanol. We studied the Ni deposition on TiN nanoparticles by varying light intensity, light exposure time, and metal precursor concentration. These studies confirmed the photodeposition method is driven by hot electrons and helped us to find optimum synthesis conditions for single atoms deposition. We characterized the nanocatalysts using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). We used density functional theory (DFT) calculations to predict favorable deposition sites and aggregation energy of Ni atoms on TiN. Surface defect sites of TiN are most favorable for single nickel atoms depositions. Interestingly, the oxygen sites on native surface oxide layer of TiN also exhibit strong binding with the single Ni atoms. Plasmon enhanced synthesis method can facilitate photodeposition of single atom catalysts on a wide class of metallic supports with plasmonic properties.</p>","PeriodicalId":715,"journal":{"name":"Nanoscale Research Letters","volume":"100 1","pages":""},"PeriodicalIF":4.7030,"publicationDate":"2024-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanoscale Research Letters","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1186/s11671-024-03992-z","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
Abstract
We report the deposition of single atom nickel catalyst on refractory plasmonic titanium nitride (TiN) nanomaterials supports using the wet synthesis method under visible light irradiation. TiN nanoparticles efficiently absorb visible light to generate photoexcited electrons and holes. Photoexcited electrons reduce nickel precursor to deposit Ni atoms on TiN nanoparticles’ surface. The generated hot holes are scavenged by the methanol. We studied the Ni deposition on TiN nanoparticles by varying light intensity, light exposure time, and metal precursor concentration. These studies confirmed the photodeposition method is driven by hot electrons and helped us to find optimum synthesis conditions for single atoms deposition. We characterized the nanocatalysts using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). We used density functional theory (DFT) calculations to predict favorable deposition sites and aggregation energy of Ni atoms on TiN. Surface defect sites of TiN are most favorable for single nickel atoms depositions. Interestingly, the oxygen sites on native surface oxide layer of TiN also exhibit strong binding with the single Ni atoms. Plasmon enhanced synthesis method can facilitate photodeposition of single atom catalysts on a wide class of metallic supports with plasmonic properties.
摘要 我们报告了在可见光照射下，利用湿合成方法在难熔等离子体氮化钛（TiN）纳米材料载体上沉积单原子镍催化剂的过程。氮化钛纳米颗粒能有效吸收可见光，产生光激发电子和空穴。光激发电子还原镍前驱体，在 TiN 纳米粒子表面沉积镍原子。产生的热空穴被甲醇清除。我们通过改变光照强度、光照时间和金属前驱体浓度来研究镍在 TiN 纳米粒子上的沉积。这些研究证实了光沉积方法是由热电子驱动的，并帮助我们找到了单原子沉积的最佳合成条件。我们使用高角度环形暗场扫描透射电子显微镜（HAADF-STEM）、能量色散 X 射线光谱（EDX）和 X 射线光电子能谱（XPS）对纳米催化剂进行了表征。我们使用密度泛函理论（DFT）计算来预测 TiN 上镍原子的有利沉积位点和聚集能。TiN 的表面缺陷位点最有利于单个镍原子的沉积。有趣的是，TiN 原生表面氧化层上的氧位点也表现出与单个镍原子的强结合力。等离子体增强合成方法可促进单原子催化剂在多种具有等离子体特性的金属支撑物上的光沉积。
期刊介绍：
Nanoscale Research Letters (NRL) provides an interdisciplinary forum for communication of scientific and technological advances in the creation and use of objects at the nanometer scale. NRL is the first nanotechnology journal from a major publisher to be published with Open Access.
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