Literature DB >> 24812398

Direct, nonoxidative conversion of methane to ethylene, aromatics, and hydrogen.

Xiaoguang Guo1, Guangzong Fang, Gang Li, Hao Ma, Hongjun Fan, Liang Yu, Chao Ma, Xing Wu, Dehui Deng, Mingming Wei, Dali Tan, Rui Si, Shuo Zhang, Jianqi Li, Litao Sun, Zichao Tang, Xiulian Pan, Xinhe Bao.   

Abstract

The efficient use of natural gas will require catalysts that can activate the first C-H bond of methane while suppressing complete dehydrogenation and avoiding overoxidation. We report that single iron sites embedded in a silica matrix enable direct, nonoxidative conversion of methane, exclusively to ethylene and aromatics. The reaction is initiated by catalytic generation of methyl radicals, followed by a series of gas-phase reactions. The absence of adjacent iron sites prevents catalytic C-C coupling, further oligomerization, and hence, coke deposition. At 1363 kelvin, methane conversion reached a maximum at 48.1% and ethylene selectivity peaked at 48.4%, whereas the total hydrocarbon selectivity exceeded 99%, representing an atom-economical transformation process of methane. The lattice-confined single iron sites delivered stable performance, with no deactivation observed during a 60-hour test.

Entities:  

Year:  2014        PMID: 24812398     DOI: 10.1126/science.1253150

Source DB:  PubMed          Journal:  Science        ISSN: 0036-8075            Impact factor:   47.728


  64 in total

1.  Catalysis on singly dispersed bimetallic sites.

Authors:  Shiran Zhang; Luan Nguyen; Jin-Xia Liang; Junjun Shan; Jingyue Jimmy Liu; Anatoly I Frenkel; Anitha Patlolla; Weixin Huang; Jun Li; Franklin Feng Tao
Journal:  Nat Commun       Date:  2015-08-21       Impact factor: 14.919

2.  Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles.

Authors:  Lichen Liu; Avelino Corma
Journal:  Chem Rev       Date:  2018-04-16       Impact factor: 60.622

3.  Design and Application of a High-Temperature Linear Ion Trap Reactor.

Authors:  Li-Xue Jiang; Qing-Yu Liu; Xiao-Na Li; Sheng-Gui He
Journal:  J Am Soc Mass Spectrom       Date:  2017-10-27       Impact factor: 3.109

4.  Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C-H activation.

Authors:  Matthew D Marcinkowski; Matthew T Darby; Jilei Liu; Joshua M Wimble; Felicia R Lucci; Sungsik Lee; Angelos Michaelides; Maria Flytzani-Stephanopoulos; Michail Stamatakis; E Charles H Sykes
Journal:  Nat Chem       Date:  2018-01-08       Impact factor: 24.427

5.  "Soft" oxidative coupling of methane to ethylene: Mechanistic insights from combined experiment and theory.

Authors:  Shanfu Liu; Sagar Udyavara; Chi Zhang; Matthias Peter; Tracy L Lohr; Vinayak P Dravid; Matthew Neurock; Tobin J Marks
Journal:  Proc Natl Acad Sci U S A       Date:  2021-06-08       Impact factor: 11.205

6.  Design, Identification, and Evolution of a Surface Ruthenium(II/III) Single Site for CO Activation.

Authors:  Liqun Kang; Bolun Wang; Adam Thetford; Ke Wu; Mohsen Danaie; Qian He; Emma K Gibson; Ling-Dong Sun; Hiroyuki Asakura; C Richard A Catlow; Feng Ryan Wang
Journal:  Angew Chem Int Ed Engl       Date:  2020-11-13       Impact factor: 15.336

7.  Achieving industrial ammonia synthesis rates at near-ambient conditions through modified scaling relations on a confined dual site.

Authors:  Tao Wang; Frank Abild-Pedersen
Journal:  Proc Natl Acad Sci U S A       Date:  2021-07-27       Impact factor: 11.205

Review 8.  Atomically Dispersed Reactive Centers for Electrocatalytic CO2 Reduction and Water Splitting.

Authors:  Huabin Zhang; Weiren Cheng; Deyan Luan; Xiong Wen David Lou
Journal:  Angew Chem Int Ed Engl       Date:  2021-02-24       Impact factor: 15.336

9.  Understanding the Preparation and Reactivity of Mo/ZSM-5 Methane Dehydroaromatization Catalysts.

Authors:  Yujie Liu; Hao Zhang; Alexandra S G Wijpkema; Ferdy J A G Coumans; Lingqian Meng; Evgeny A Uslamin; Alessandro Longo; Emiel J M Hensen; Nikolay Kosinov
Journal:  Chemistry       Date:  2021-12-16       Impact factor: 5.020

Review 10.  Catalytic Methane Decomposition to Carbon Nanostructures and COx-Free Hydrogen: A Mini-Review.

Authors:  Ahmed Gamal; Kamel Eid; Muftah H El-Naas; Dharmesh Kumar; Anand Kumar
Journal:  Nanomaterials (Basel)       Date:  2021-05-06       Impact factor: 5.076

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