Abstract
Ethanol conversion to C4+ olefins remains a critical yet nonselective process for producing renewable middle distillates. Here, Cu−La/Beta catalysts composed of copper and lanthanum incorporated onto a dealuminated Beta support are reported for ethanol conversion to C4+ olefins (73% selectivity, ∼98% ethanol conversion, 623 K,<4% C1−C3 hydrocarbons) which particularly favors C5+ olefin formation (43% selectivity) as a distinction from the benchmarking Cu−Y/ Beta catalyst. Monometallic Cu/Beta or La/Beta samples are insufficient to catalyze the C4+ olefin formation and primarily form dehydration products (e.g., ethylene and diethyl ether), indicating the necessity of both Cu and La species for butene and C5+ olefin formation. Increasing the bulk La loading at a fixed Cu content yields higher C5+ olefins until the La/Cu molar ratio reaches 3.6. These findings indicate Cu−La/Beta as an effective ethanol conversion catalyst that facilitates multiple C−C bond formation events required for synthesizing C5+ olefins (i.e., hexenes and octenes).
| Original language | English |
|---|---|
| Pages (from-to) | 5702-5707 |
| Number of pages | 6 |
| Journal | ACS Sustainable Chemistry and Engineering |
| Volume | 10 |
| Issue number | 18 |
| DOIs | |
| State | Published - May 9 2022 |
Funding
Funding provided by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (BETO), under contract DE-AC05-00OR22725 (ORNL) with UT-Battle, LLC, and in collaboration with the Chemical Catalysis for Bioenergy (ChemCatBio) Consortium, a member of the Energy Materials Network. Z.L. also acknowledges funding from the Center for Bioenergy Innovation, a U.S. DOE Bioenergy Research Center supported by the Office of Biological and Environmental Research in the DOE Office of Science and led by Oak Ridge National Laboratory. X-ray data measurements and analyses were partly conducted at the Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. We acknowledge Dr. Jong Keum and Dr. Yang He’s help in XRD data measurements. Microscopy was performed as part of a user project at CNMS. The authors thank Jeffrey Baxter for assistance with TEM sample preparation. The views and opinions of the authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights.
Keywords
- Beta zeolite
- Catalysis
- Copper
- Ethanol
- Lanthanum
- Olefins