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

基于JSPS项目的课题，我们开发了一系列含Pd的金属间催化剂，包括Y3Pd2电化物和Y3Pd、Y3Pd4、YPd3化合物，其中Pd活性位点植入到金属间晶格中，具有低功函数和高载流子密度的特点。它们都表现出极好的化学稳定性，是铃木偶联反应的有效催化剂。除了钯金属间催化剂外，我们还提出了一种通过铂阴离子与C12A7带正电的表面空腔之间的库仑相互作用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对硝基芳烃加氢的优异催化活性。经过这两项工作，我们将重点转移到氨合成的金属氮化物催化剂上。我们有一个有趣的发现，镍和氮化镧的结合可以稳定高效地合成氨。此后，我们不断建立氮化物基合成氨催化剂设计的通则，并论证了氮空位形成能是影响合成氨过程定速步骤反应势垒的关键因素。

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.