Dual-atom Pt heterogeneous catalyst with excellent catalytic performances for the selective hydrogenation and epoxidation

被引:271
作者
Tian, Shubo [1 ,2 ]
Wang, Bingxue [3 ]
Gong, Wanbing [4 ]
He, Zizhan [3 ]
Xu, Qi [2 ]
Chen, Wenxing [5 ]
Zhang, Qinghua [6 ]
Zhu, Youqi [5 ]
Yang, Jiarui [2 ]
Fu, Qiang [3 ]
Chen, Chun [4 ]
Bu, Yuxiang [3 ]
Gu, Lin [6 ]
Sun, Xiaoming [1 ]
Zhao, Huijun [4 ]
Wang, Dingsheng [2 ]
Li, Yadong [2 ]
机构
[1] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing, Peoples R China
[3] Shandong Univ, Sch Chem & Chem Engn, Jinan, Peoples R China
[4] Chinese Acad Sci, Ctr Environm & Energy Nanomat, Inst Solid State Phys, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, Hefei, Peoples R China
[5] Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Construct Tailorable Adv Funct Ma, Beijing, Peoples R China
[6] Chinese Acad Sci, Inst Phys, Beijing, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; DOPED CARBON; SINGLE; OXIDATION; CLUSTERS; REDUCTION; CO; NITROBENZENE; POINTS; OXIDE;
D O I
10.1038/s41467-021-23517-x
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Atomically monodispersed heterogeneous catalysts with uniform active sites and high atom utilization efficiency are ideal heterogeneous catalytic materials. Designing such type of catalysts, however, remains a formidable challenge. Herein, using a wet-chemical method, we successfully achieved a mesoporous graphitic carbon nitride (mpg-C3N4) supported dual-atom Pt-2 catalyst, which exhibited excellent catalytic performance for the highly selective hydrogenation of nitrobenzene to aniline. The conversion of (>)99% is significantly superior to the corresponding values of mpg-C3N4-supported single Pt atoms and ultra-small Pt nanoparticles (similar to 2 nm). First-principles calculations revealed that the excellent and unique catalytic performance of the Pt-2 species originates from the facile H-2 dissociation induced by the diatomic characteristics of Pt and the easy desorption of the aniline product. The produced Pt-2/mpg-C3N4 samples are versatile and can be applied in catalyzing other important reactions, such as the selective hydrogenation of benzaldehyde and the epoxidation of styrene.
引用
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页数:9
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