Selective visible-light photocatalysis of acetylene to ethylene using a cobalt molecular catalyst and water as a proton source

被引:55
作者
Arcudi, Francesca [1 ,2 ]
Dordevic, Luka [1 ,2 ,3 ]
Schweitzer, Neil [4 ]
Stupp, Samuel, I [1 ,2 ,3 ,5 ,6 ,7 ]
Weiss, Emily A. [1 ,2 ,5 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Ctr BioInspired Energy Sci, Evanston, IL 60208 USA
[3] Northwestern Univ, Simpson Querrey Inst BioNanotechnol, Chicago, IL 60611 USA
[4] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL USA
[5] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
[6] Northwestern Univ, Dept Biomed Engn, Evanston, IL 60208 USA
[7] Northwestern Univ, Dept Med, Chicago, IL 60611 USA
关键词
DEUTERIUM-EXCHANGE; HYDROGENATION; REDUCTION; COMPLEXES; BOND; CO; EQUILIBRIUM; SEPARATION; PALLADIUM;
D O I
10.1038/s41557-022-00966-5
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The acetylene contaminant present in ethylene feeds used to produce polymers is typically removed by thermal hydrogenation. Now, it has been shown that the conversion of acetylene to ethylene at room temperature can be achieved in a visible-light-driven process using an earth-abundant metal (cobalt) catalyst and a water proton source. The production of polymers from ethylene requires the ethylene feed to be sufficiently purified of acetylene contaminant. Accomplishing this task by thermally hydrogenating acetylene requires a high temperature, an external feed of H-2 gas and noble-metal catalysts. It is not only expensive and energy-intensive, but also prone to overhydrogenating to ethane. Here we report a photocatalytic system that reduces acetylene to ethylene with >= 99% selectivity under both non-competitive (no ethylene co-feed) and competitive (ethylene co-feed) conditions, and near 100% conversion under the latter industrially relevant conditions. Our system uses a molecular catalyst based on earth-abundant cobalt operating under ambient conditions and sensitized by either [Ru(bpy)(3)](2+) or an inexpensive organic semiconductor (metal-free mesoporous graphitic carbon nitride) under visible light. These features and the use of water as a proton source offer advantages over current hydrogenation technologies with respect to selectivity and sustainability.
引用
收藏
页码:1007 / +
页数:7
相关论文
共 49 条
  • [41] Seven chemical separations to change the world
    Sholl, David S.
    Lively, Ryan P.
    [J]. NATURE, 2016, 532 (7600) : 435 - 437
  • [42] SELECTIVE HYDROGENATION OF THE CC-TRIPLE BOND IN PHC=CPH BY TRIS(TRIPHENYLPHOSPHINE)COBALT ACTIVATED NABH4 - DEUTERIUM TRACING EXPERIMENTS
    STEINBERGER, B
    MICHMAN, M
    SCHWARZ, H
    HOHNE, G
    [J]. JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1983, 244 (03) : 283 - 288
  • [43] Identification of non-precious metal alloy catalysts for selective hydrogenation of acetylene
    Studt, Felix
    Abild-Pedersen, Frank
    Bligaard, Thomas
    Sorensen, Rasmus Z.
    Christensen, Claus H.
    Norskov, Jens K.
    [J]. SCIENCE, 2008, 320 (5881) : 1320 - 1322
  • [44] Heterometallic antenna-reactor complexes for photocatalysis
    Swearer, Dayne F.
    Zhao, Hangqi
    Zhou, Linan
    Zhang, Chao
    Robatjazi, Hossein
    Martirez, John Mark P.
    Krauter, Caroline M.
    Yazdi, Sadegh
    McClain, Michael J.
    Ringe, Emilie
    Carter, Emily A.
    Nordlander, Peter
    Halas, Naomi J.
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2016, 113 (32) : 8916 - 8920
  • [45] State-of-the-art of Coke Formation during Steam Cracking: Anti-Coking Surface Technologies
    Symoens, Steffen H.
    Olahova, Natalia
    Gandarillas, Andres E. Munoz
    Karimi, Hadiseh
    Djokic, Marko R.
    Reyniers, Marie-Francoise
    Marin, Guy B.
    Van Geem, Kevin M.
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2018, 57 (48) : 16117 - 16136
  • [46] Photocatalytic dry reforming: what is it good for?
    Tavasoli, Alexandra Victoria
    Preston, Mikaela
    Ozin, Geoffrey
    [J]. ENERGY & ENVIRONMENTAL SCIENCE, 2021, 14 (05) : 3098 - 3109
  • [47] ELECTROGENERATED CHEMILUMINESCENCE .13. ELECTROCHEMICAL AND ELECTROGENERATED CHEMILUMINESCENCE STUDIES OF RUTHENIUM CHELATES
    TOKELTAK.NE
    HEMINGWA.RE
    BARD, AJ
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1973, 95 (20) : 6582 - 6589
  • [48] Enhancement of Alkyne Semi-Hydrogenation Selectivity by Electronic Modification of Platinum
    Wang, Zhenshu
    Garg, Aaron
    Wang, Linxi
    He, Haoran
    Dasgupta, Anish
    Zanchet, Daniela
    Janik, Michael J.
    Rioux, Robert M.
    Roman-Leshkov, Yuriy
    [J]. ACS CATALYSIS, 2020, 10 (12) : 6763 - 6770
  • [49] Pd Single-Atom Catalysts on Nitrogen-Doped Graphene for the Highly Selective Photothermal Hydrogenation of Acetylene to Ethylene
    Zhou, Shiqi
    Shang, Lu
    Zhao, Yunxuan
    Shi, Run
    Waterhouse, Geoffrey I. N.
    Huang, Yu-Cheng
    Zheng, Lirong
    Zhang, Tierui
    [J]. ADVANCED MATERIALS, 2019, 31 (18)