Shubo Tian1,2, Bingxue Wang3, Wanbing Gong4, Zizhan He3, Qi Xu2, Wenxing Chen5, Qinghua Zhang6, Youqi Zhu5, Jiarui Yang2, Qiang Fu7, Chun Chen4, Yuxiang Bu3, Lin Gu6, Xiaoming Sun1, Huijun Zhao4, Dingsheng Wang8, Yadong Li2. 1. State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China. 2. Department of Chemistry, Tsinghua University, Beijing, China. 3. School of Chemistry and Chemical Engineering, Shandong University, Jinan, China. 4. Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, China. 5. Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, China. 6. Institute of Physics, Chinese Academy of Sciences, Beijing, China. 7. School of Chemistry and Chemical Engineering, Shandong University, Jinan, China. qfu@sdu.edu.cn. 8. Department of Chemistry, Tsinghua University, Beijing, China. wangdingsheng@mail.tsinghua.edu.cn.
Abstract
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 Pt2 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 (~2 nm). First-principles calculations revealed that the excellent and unique catalytic performance of the Pt2 species originates from the facile H2 dissociation induced by the diatomic characteristics of Pt and the easy desorption of the aniline product. The produced Pt2/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.
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 graphiticn class="Chemical">carbon nitride (mpg-C3N4) supported dual-atom Pt2 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 (~2 nm). First-principles calculations revealed that the excellent and unique catalytic performance of the Pt2 species originates from the facile H2 dissociation induced by the diatomic characteristics of Pt and the easy desorption of the aniline product. The produced Pt2/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.
Authors: Jilei Liu; Felicia R Lucci; Ming Yang; Sungsik Lee; Matthew D Marcinkowski; Andrew J Therrien; Christopher T Williams; E Charles H Sykes; Maria Flytzani-Stephanopoulos Journal: J Am Chem Soc Date: 2016-05-17 Impact factor: 15.419
Authors: Grazia Malta; Simon A Kondrat; Simon J Freakley; Catherine J Davies; Li Lu; Simon Dawson; Adam Thetford; Emma K Gibson; David J Morgan; Wilm Jones; Peter P Wells; Peter Johnston; C Richard A Catlow; Christopher J Kiely; Graham J Hutchings Journal: Science Date: 2017-03-31 Impact factor: 47.728
Authors: Alexander Okrut; Ron C Runnebaum; Xiaoying Ouyang; Jing Lu; Ceren Aydin; Son-Jong Hwang; Shengjie Zhang; Olayinka A Olatunji-Ojo; Kathleen A Durkin; David A Dixon; Bruce C Gates; Alexander Katz Journal: Nat Nanotechnol Date: 2014-04-20 Impact factor: 39.213
Authors: Bokwon Yoon; Hannu Häkkinen; Uzi Landman; Anke S Wörz; Jean-Marie Antonietti; Stéphane Abbet; Ken Judai; Ueli Heiz Journal: Science Date: 2005-01-21 Impact factor: 47.728
Authors: Cong Liu; Bing Yang; Eric Tyo; Soenke Seifert; Janae DeBartolo; Bernd von Issendorff; Peter Zapol; Stefan Vajda; Larry A Curtiss Journal: J Am Chem Soc Date: 2015-07-02 Impact factor: 15.419
Authors: Manuel Moliner; Jadeene E Gabay; Chris E Kliewer; Robert T Carr; Javier Guzman; Gary L Casty; Pedro Serna; Avelino Corma Journal: J Am Chem Soc Date: 2016-11-23 Impact factor: 15.419