パラジウム－希土類金属間化合物ナノ粒子による炭素―炭素クロスカップリング反応

使用钯-稀土金属间化合物纳米粒子的碳-碳交叉偶联反应

• 批准号: 18F18361
• 负责人: 細野 秀雄
• 金额: $ 1.41万
• 依托单位: Tokyo Institute of Technology
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for JSPS Fellows
• 财政年份: 2018
• 资助国家: 日本
• 起止时间: 2018-10-12 至 2021-03-31
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-18F18361/
• 关键词: Suzuki-coupling reaction; Single atom catalyst; Hydrogenation reaction; Ni-based catalysts; Metal nitrides; Nitrogen vacancy; Ammonia synthesis; Rare-earth elements; Low work function; High carrier density; Intermetallic electride; Pd系不均一触媒; N

Based on the topic of our JSPS project, we developed a series of Pd-bearing intermetallic catalysts, including Y3Pd2 electride, and Y3Pd, Y3Pd4, YPd3 compounds, in which Pd actives sites were implanted into the intermetallic crystal lattice with low work function and high carrier density features. All of them showed extremely chemical stability and served as efficient catalysts for Suzuki coupling reactions. Besides the Pd intermetallic catalysts, we also proposed a new strategy for trapping Pt single atoms through the coulomb interaction between Pt anions and positively charged surface cavities of C12A7. The stabilized Pt single atoms exhibited exceptionally high thermal stability and superior catalytic activity for the hydrogenation of nitroarenes. After these two works, we moved our focus on metal nitride catalysts for ammonia synthesis. We made an intriguing discovery that the combination of nickel and lanthanum nitride enables stable and highly efficient ammonia synthesis. After that, we continuously established a general rule for the design of nitride-based catalysts towards ammonia synthesis, and demonstrate that nitrogen vacancy formation energy as the key factor that affect the reaction barrier of the rate determining step of the ammonia synthesis process.

基于我们JSPS项目的主题，我们开发了一系列含Pd的金属间化合物催化剂，包括Y3Pd2电子催化剂和Y3Pd、Y3Pd4、YPd3化合物，其中Pd的活性中心被注入到具有低功函数和高载流子密度的金属间化合物晶格中。它们都表现出极高的化学稳定性，是铃木偶联反应的有效催化剂。除了Pd金属间化合物催化剂外，我们还提出了一种通过铂阴离子与C12A7表面正电空穴之间的库仑相互作用来捕获铂单原子的新策略。稳定的铂单原子表现出极高的热稳定性和优异的硝基芳烃加氢催化活性。在这两项工作之后，我们将注意力转移到氨合成的金属氮化物催化剂上。我们发现了一个耐人寻味的发现，镍和氮化镧的结合可以实现稳定和高效的氨合成。之后，我们继续建立了氮化物基氨合成催化剂设计的一般规律，并论证了氮空位形成能是影响氨合成反应速率决定步骤反应势垒的关键因素。

项目成果

Electride Compounds for Advanced Catalytic Applications

用于高级催化应用的电子化合物

• 发表时间: 2019
• 作者: Ye Tian-Nan;Lu Yangfan;Xiao Zewen;Li Jiang;Nakao Takuya;Abe Hitoshi;Niwa Yasuhiro;Kitano Masaaki;Tada Tomofumi;Hosono Hideo;Tian-Nan Ye
• 通讯作者: Tian-Nan Ye

Intermetallic ZrPd3-Embedded Nanoporous ZrC as an Efficient and Stable Catalyst of the Suzuki Cross-Coupling Reaction

• DOI: 10.1021/acscatal.0c03416
• 发表时间: 2020-11
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Yangfan Lu;Tiannan Ye;Sang-Won Park;Jiang Li;M. Sasase;H. Abe;Y. Niwa;M. Kitano;H. Hosono