Ru-Sn/AC for the Aqueous-Phase Reduction of Succinic Acid to 1,4-Butanediol under Continuous Process Conditions
Succinic acid is a biomass-derived platform chemical that can be catalytically converted in the aqueous phase to 1,4-butanediol (BDO), a prevalent building block used in the polymer and chemical industries. Despite significant interest, limited work has been reported regarding sustained catalyst performance and stability under continuous aqueous-phase process conditions. As such, this work examines Ru-Sn on activated carbon (AC) for the aqueous-phase conversion of succinic acid to BDO under batch and flow reactor conditions. Initially, powder Ru-Sn catalysts were screened to determine the most effective bimetallic ratio and provide a comparison to other monometallic (Pd, Pt, Ru) and bimetallic (Pt-Sn, Pd-Re) catalysts. Batch reactor tests determined that a ~1:1 metal weight ratio of Ru to Sn was effective for producing BDO in high yields, with complete conversion resulting in 82% molar yield. Characterization of the fresh Ru-Sn catalyst suggests that the sequential loading method results in Ru sites that are colocated and surface-enriched with Sn. Postbatch reaction characterization confirmed stable Ru-Sn material properties; however, upon a transition to continuous conditions, significant Ru-Sn/AC deactivation occurred due to stainless steel leaching of Ni that resulted in Ru-Sn metal crystallite restructuring to form discrete Ni-Sn sites. Computational modeling confirmed favorable energetics for Ru-Snmore »
- Authors:
-
[1] ; [1]; [1]; [1]; [1]; [2]; [3]; [3]; [1]; [1]; [1];
[1]
- National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, United States
- Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
- Interfacial and Surface Science, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, United States
- Publication Date:
- Report Number(s):
- NREL/JA-5100-70060
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- AC36-08GO28308; AC05-00OR22725; MCB09159
- Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 9; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Research Org:
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B); USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5); National Science Foundation (NSF)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; biobased chemical; catalyst stability; leaching; lignocellulose; restructuring; Ru-Sn/AC; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
- OSTI Identifier:
- 1394395
- Alternate Identifier(s):
- OSTI ID: 1389739