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Cooperative Rh-O5/Ni(Fe) Site for Efficient Biomass Upgrading Coupled with H2 Production
Abstract
Designing efficient and durable bifunctional catalysts for 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) and hydrogen evolution reaction (HER) is desirable for the co-production of biomass-upgraded chemicals and sustainable hydrogen, which is limited by the competitive adsorption of hydroxyl species (OH ads ) and HMF molecules. Here, we report a class of Rh–O 5 /Ni(Fe) atomic site on nanoporous mesh-type layered double hydroxides with atomic-scale cooperative adsorption centers for highly active and stable alkaline HMFOR and HER catalysis. A low cell voltage of 1.48 V is required to achieve 100 mA cm –2 in an integrated electrolysis system along with excellent stability (>100 h). Operando infrared and X-ray absorption spectroscopic probes unveil that HMF molecules are selectively adsorbed and activated over the single-atom Rh sites and oxidized by in situ-formed electrophilic OH ads species on neighboring Ni sites. Theoretical studies further demonstrate that the strong d–d orbital coupling interactions between atomic-level Rh and surrounding Ni atoms in the special Rh–O 5 /Ni(Fe) structure can greatly facilitate surface electronic exchange-and-transfer capabilities with the adsorbates (OH ads and HMF molecules) and intermediates for efficient HMFOR and HER. We also reveal that the Fe sites in Rh–O 5 /Ni(Fe) structure can promote the electrocatalytic stability of the catalyst. Our findings provide new insights into catalyst design for complex reactions involving competitive adsorptions of multiple intermediates.
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Metadata
- Authors
- Zeng, L., Chen, Y., Sun, M., Huang, Q., Sun, K., Ma, J., Li, J., Tan, H., Li, M., Pan, Y., Liu, Y., Luo, M., Huang, B., & Guo, S.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2023-05-30
- Volume
- 145
- Issue
- 32
- Pages
- 17577-17587
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4378781696
- Cited by
- 265
- References
- 37
- FWCI
- 12.40
- Type
- journal article
- Language
- en
- Open access
- closed
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